WorldWideScience

Sample records for hydrogen adsorption studies

  1. Hydrogen adsorption in metal-decorated silicon carbide nanotubes

    Science.gov (United States)

    Singh, Ram Sevak; Solanki, Ankit

    2016-09-01

    Hydrogen storage for fuel cell is an active area of research and appropriate materials with excellent hydrogen adsorption properties are highly demanded. Nanotubes, having high surface to volume ratio, are promising storage materials for hydrogen. Recently, silicon carbide nanotubes have been predicted as potential materials for future hydrogen storage application, and studies in this area are ongoing. Here, we report a systematic study on hydrogen adsorption properties in metal (Pt, Ni and Al) decorated silicon carbide nanotubes (SiCNTs) using first principles calculations based on density functional theory. The hydrogen adsorption properties are investigated by calculations of adsorption energy, electronic band structure, density of states (DOS) and Mulliken charge population analysis. Our findings show that hydrogen adsorptions on Pt, Ni and Al-decorated SiCNTs undergo spontaneous exothermic reactions with significant modulation of electronic structure of SiCNTs in all cases. Importantly, according to the Mulliken charge population analysis, dipole-dipole interaction causes chemisorptions of hydrogen in Pt, Ni and Al decorated SiCNTs with formation of chemical bonds. The study is a platform for the development of metal decorated SiCNTs for hydrogen adsorption or hydrogen storage application.

  2. Hydrogen purification by periodic adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Barg, Christian; Secchi, Argimiro R.; Trierweiler, Jorge O. [Rio Grande do Sul Univ., Porto Alegre, RS (Brazil). Dept. de Engenharia Quimica]. E-mail: cbarg@enq.ufrgs.br; arge@enq.ufrgs.br; jorge@enq.ufrgs.br

    2000-07-01

    The periodic adsorption processes have been widely used for industrial applications, mainly because it spends less energy than the usual gas separation processes, like the cryogenic distillation. The largest commercial application of periodic adsorption processes is the pressure swing adsorption (PSA) applied to hydrogen purification. Although its wide use in the chemical and petrochemical industry, there are no reports in the open literature about complete modeling studies of a complex commercial unit, with multiple adsorbents and multiple beds and several feed components. This study has as objective the modeling, optimization and dynamical analysis of an industrial PSA unit for hydrogen purification. (author)

  3. Hydrogen adsorption in new carbon materials

    International Nuclear Information System (INIS)

    Zubizarreta, L.; Arenillas, A.; Rubiera, F.; Pis, J.J.

    2006-01-01

    Hydrogen physi-sorption on porous carbon materials is one among the different technologies which could be used for hydrogen storage. In addition hydrogen spillover on a carbon supports can enhance the hydrogen adsorption capacities obtained by physi-sorption. In this study two different carbon supports were synthesised: carbon gels and carbon microspheres. Carbon microspheres were doped with Ni(NO 3 ) 2 to study the hydrogen spillover on carbon support. The texture of the materials was characterised by CO 2 adsorption at 0 C and their hydrogen storage capacity was evaluated at -196 and 10 C with a Micromeritics Tristar 3000, and at room temperature with a high pressure gravimetric analyser. (authors)

  4. Hydrogen adsorption in new carbon materials

    Energy Technology Data Exchange (ETDEWEB)

    Zubizarreta, L.; Arenillas, A.; Rubiera, F.; Pis, J.J. [Instituto Nacional del Carbon, CSIC, Apartado 73, 33080 Oviedo (Spain)

    2006-07-01

    Hydrogen physi-sorption on porous carbon materials is one among the different technologies which could be used for hydrogen storage. In addition hydrogen spillover on a carbon supports can enhance the hydrogen adsorption capacities obtained by physi-sorption. In this study two different carbon supports were synthesised: carbon gels and carbon microspheres. Carbon microspheres were doped with Ni(NO{sub 3}){sub 2} to study the hydrogen spillover on carbon support. The texture of the materials was characterised by CO{sub 2} adsorption at 0 C and their hydrogen storage capacity was evaluated at -196 and 10 C with a Micromeritics Tristar 3000, and at room temperature with a high pressure gravimetric analyser. (authors)

  5. A DFT study of hydrogen adsorption on Be, Mg and Ca frameworks in erionite zeolite

    Energy Technology Data Exchange (ETDEWEB)

    Fellah, Mehmet Ferdi, E-mail: mferdi.fellah@btu.edu.tr

    2017-02-01

    Highlights: • Mg-ERI and Ca-ERI clusters have much lower chemical potential and hardness. • Adsorption enthalpies for Mg- and Ca-ERI are importantly greater than the liquefaction enthalpy of hydrogen. • Mg-ERI and Ca-ERI clusters have much HOMO-LUMO gap indicating higher reactivity. • Ca- and Mg-ERI are potential cryoadsorbent materials for hydrogen storage. - Abstract: The molecular hydrogen adsorption was investigated on additional frameworks with earth alkaline metal atoms (Be, Mg and Ca) in 24T ERI zeolite cluster model by means of Density Functional Theory study. HOMO and LUMO energy values, chemical potential, chemical hardness, electronegativity, adsorption energy and adsorption enthalpy values have been calculated in this study. Mg-ERI and Ca-ERI clusters have much lower chemical potentials with much lower adsorption energy values when compared to the value of Be-ERI cluster. Additionally, they are softer than Be-ERI cluster with respect to their lower chemical hardness values. Hydrogen adsorption enthalpy values were computed as −3.6 and −3.9 kJ/mol on Mg-ERI and Ca-ERI clusters, respectively. These adsorption enthalpy values are significantly larger than the enthalpy value of liquefaction for hydrogen molecule. This consequently specifies that Mg-ERI and Ca-ERI zeolite structures which have higher chemical reactivity appear to be a promising candidate cryoadsorbent for hydrogen storage.

  6. Adsorption of molecular hydrogen on nanostructered surfaces

    International Nuclear Information System (INIS)

    Uranga Piña, Llinersy; Martínez Mesa, Aliezer; Seifert, Gotthard

    2015-01-01

    Were investigated the effect of the structural characteristics of model nanoporous environments on the adsorption of molecular hydrogen. The adsorption properties of the target nanostructures (graphene and ZnO sheets, carbon foams, metal-organic frameworks) are evaluated in a broad range of thermodynamic conditions. The study is carried out within the density functional theory for quantum fluids at finite temperature (QLDFT), which allows to account for the many-body and quantum delocalization effects in a single theoretical framework. The exchange-correlation (excess) functional is derived from the empirical equation of state of the homogeneous system. We focus on the evaluation of hydrogen storage capacities of the substrates and on the emergence of quantum effects triggered by the confinement imposed by the host structure. The approach provides accurate estimates of the hydrogen storage capacities for realistic adsorptive media. The relation between the microscopic structure of the hydrogen fluid and the calculated adsorption properties is also addressed. (full text)

  7. Effects of basic nitrogen poisoning on adsorption of hydrogen on a hydrotreatment catalyst

    International Nuclear Information System (INIS)

    Entz, R.W.; Seapan, M.

    1985-01-01

    Activity of a hydrotreatment catalyst depends on the hydrogen adsorption characteristics of the catalyst. In this work, the adsorption of hydrogen on a Ni-Mo/Al/sub 2/O/sub 3/ catalyst (shell 324) has been studied using a TGA at 1 atm pressure and 200-400 0 C temperature. Hydrogen adsorption on a calcined catalyst was shown to be of activated type with a sudden increase in hydrogen adsorption around 350 0 C. When the catalyst is extracted with Tetrahydrofuran (THF), the hydrogen adsorption increases gradually as the temperature is increased, approaching a monolayer coverage of the catalyst surface. It is shown that solvent extraction of catalyst changes its hydrogen adsorption characteristics significantly. Indeed, at 400 0 C, an extracted catalyst adsorbs about four times more hydrogen than an unextracted catalyst. Adsorption of basic nitrogen compounds on the catalyst interferes with the hydrogen adsorption. The adsorption of pyridine, piperidine, n-pentylamine, and ammonia were studied at 400 0 C. It is shown that the strength of adsorption of piperidine and n-pentylamine are relatively similar, however their adsorption strength is higher than pyridine. Ammonia is the weakest adsorbing compound studied. These observations are in agreement with other studies

  8. Hydrogen Adsorption in Zeolite Studied with Sievert and Thermogravimetric Methods

    International Nuclear Information System (INIS)

    Lesnicenoks, P; Sivars, A; Grinberga, L; Kleperis, J

    2012-01-01

    Natural clinoptilolite (mixture from clinoptilolite, quartz and muscovite) is activated with palladium and tested for hydrogen adsorption capability at temperatures RT - 200°C. Thermogravimetric and volumetric methods showed that zeolite activated with palladium (1.25%wt) shows markedly high hydrogen adsorption capacity - up to 3 wt%. Lower amount of adsorbed hydrogen (∼1.5 wt%) was found for raw zeolite and activated with higher amount of palladium sample. Hypothesis is proposed that the heating of zeolite in argon atmosphere forms and activates the pore structure in zeolite material, where hydrogen encapsulation (trapping) is believed to occur when cooling down to room temperature. An effect of catalyst (Pd) on hydrogen sorption capability is explained by spillover phenomena were less-porous fractions of natural clinoptilolite sample (quartz and muscovite) are involved.

  9. Kinetics of hydrogen adsorption on MgH{sub 2}/CNT composite

    Energy Technology Data Exchange (ETDEWEB)

    Rather, Sami ullah, E-mail: rathersami@gmail.com; Taimoor, Aqeel Ahmad; Muhammad, Ayyaz; Alhamed, Yahia Abobakor; Zaman, Sharif Fakhruz; Ali, Arshid Mahmood

    2016-05-15

    Highlights: • Hydrogen adsorption comparisons of commercial, milled, and MgH{sub 2} composite. • Hydrogen adsorption capacity and kinetics improves tremendously by CNT embedding. • Unsteady state modeling and simulation of adsorption kinetics. - Abstract: Magnesium hydride (MgH{sub 2})–carbon nanotubes (CNT) composite has been prepared by high-energy ball milling method and their experimental and kinetic hydrogen adsorption studies was assessed. Hydrogen adsorption studies were performed by Sievert’s volumetric apparatus and kinetic evaluation was conducted by surface chemistry and Langmuir–Hinshelwood–Hougen–Watson (LHHW) type mode. Powder X-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM) were performed. Hydrogen adsorption capacity of commercial MgH{sub 2}, milled MgH{sub 2}, and MgH{sub 2}/CNT composite are found to be 0.04, 0.057, and 0.059 g (H{sub 2})/g (MgH{sub 2}) at 673 K and hydrogen pressure of 4.6 MPa. Addition of 5 wt% of CNTs to MgH{sub 2} proved to be very critical to enhance hydrogen adsorption as well as to improve its kinetics. It was observed that hydrogen adsorption is not in quasi-state equilibrium and is modeled using kinetic rate laws.

  10. Hydrogen and helium adsorption on potassium

    International Nuclear Information System (INIS)

    Garcia, R.; Mulders, N.; Hess, G.

    1995-01-01

    A previous quartz microbalance study of adsorption of helium on sodium indicates that the inert layer is surprisingly small. Similar experiments with hydrogen on sodium show layer by layer growth below a temperature of 7K. These results motivated the authors to extend the experiments to lower temperatures. A suitable apparatus, capable of reaching 0.45 K, while still enabling them to do in situ alkali evaporation, has been constructed. The authors will report on the results of microbalance adsorption experiments of helium and hydrogen on potassium

  11. Hydrogen adsorption on bimetallic PdAu(111) surface alloys

    DEFF Research Database (Denmark)

    Takehiro, Naoki; Liu, Ping; Bergbreiter, Andreas

    2014-01-01

    The adsorption of hydrogen on structurally well defined PdAu-Pd(111) monolayer surface alloys was investigated in a combined experimental and theoretical study, aiming at a quantitative understanding of the adsorption and desorption properties of individual PdAu nanostructures. Combining...... the structural information obtained by high resolution scanning tunneling microscopy (STM), in particular on the abundance of specific adsorption ensembles at different Pd surface concentrations, with information on the adsorption properties derived from temperature programmed desorption (TPD) spectroscopy...... and high resolution electron energy loss spectroscopy (HREELS) provides conclusions on the minimum ensemble size for dissociative adsorption of hydrogen and on the adsorption energies on different sites active for adsorption. Density functional theory (DFT) based calculations give detailed insight...

  12. A study on hydrogen adsorption behaviors of open-tip carbon nanocones

    International Nuclear Information System (INIS)

    Liao Mingliang

    2012-01-01

    Hydrogen adsorption behaviors of single-walled open-tip (tip-truncated) carbon nanocones (CNCs) with apex angles of 19.2° at temperatures of 77 and 300 K were investigated by the molecular dynamics simulations. Four nanomaterials (including three CNCs with different dimensions and a reference CNT) were analyzed to examine the hydrogen adsorption behaviors and influences of cone sharpness on the behaviors of the CNCs. Physisorption of hydrogen molecules could be observed from the distribution pattern of the hydrogen molecules adsorbed on the nanomaterials. Because of the cone geometry effect, the open-tip CNCs could have larger storage weight percentage and less desorption of hydrogen molecules (caused by the temperature growth) on their outer surfaces, as compared with those of the reference CNT. The hydrogen molecules inside the CNCs and the reference CNT, however, were noted to have similar desorption behaviors owing to the confinement effects from the structures of the nanomaterials. In addition, the sharper CNC could have higher storage weight percentage but the cone sharpness does not have evident enhancement in the average adsorption energy of the CNC. Combination of confinement and repulsion effects existing near the tip region of the CNC would be responsible for the non-enhancement feature.

  13. Adsorption methods for hydrogen isotope storage on zeolitic sieves

    International Nuclear Information System (INIS)

    Cristescu, Ioana; Cristescu, Ion; Vasut, F.; Brad, S.; Lazar, A.

    2001-01-01

    For hydrogen isotope separation, adsorption molecular sieves and active carbon were used. Adsorption process proceeds at liquid nitrogen and liquid hydrogen temperatures. Commercial zeolites have the same proprieties with natural zeolites, but they have a regular pore structure. They also have affinity for molecules of different size with defined shapes. Experimental results obtained at liquid nitrogen temperature (77.4 K) and liquid hydrogen revealed the efficient behaviour of the active carbon and zeolitic sieves for hydrogen isotopes temporary storage. We study adsorption of the synthetic zeolites in a wide range of temperatures and pressures and we used the molecular sieves 4A, 5A and active carbon. The 4A and 5A zeolites have a tridimensional structure with 11.4 A diameter. When the hydration water is eliminated, the material keeps a porous structure. The porous volume represents 45% from the zeolite mass for 4A and 5A sieves. The activation temperature of the zeolite and the carbon is very important for obtaining a high adsorption capacity. If the temperature used for activation is low, the structural water will be not eliminated and the adsorption capacity will be low. The excessive temperature will destroy the porous structure. The adsorption capacity for the hydrogen isotopes was calculated with the relation: A = V ads /m (cm 3 /g). The adsorption capacity and efficiency for the adsorbent materials, are given. Physical adsorption process of the hydrogen isotopes was carried out at liquid nitrogen temperature. The flux gas used in the adsorption system is composed of dry deuterium and protium. This mixture is cooled in liquid nitrogen and then is passed to the adsorbent getter at the same temperature (77.4 K). The gas flux in the adsorbent getter is 5 and 72 l/h (which correspond to 0.008 and 0.134 discharge velocity, respectively). (authors)

  14. A density functional study on the adsorption of hydrogen molecule

    Indian Academy of Sciences (India)

    An all-electron scalar relativistic calculation on the adsorption of hydrogen molecule onto small copper clusters has been performed by using density functional theory with the generalized gradient approximation (GGA) at PW91 level. Our results reveal that after adsorption of H2 molecule, the Cu-Cu interaction is ...

  15. Adsorption and diffusion of hydrogen in Zircaloy-4

    International Nuclear Information System (INIS)

    Torres, E.; Desquines, J.; Baietto, M.C.; Coret, M.; Wehling, F.; Blat-Yrieix, M.; Ambard, A.

    2015-01-01

    Hydrogen in zirconium alloys is considered in many nuclear safety issues. Below 500 Celsius degrees, rather limited knowledge is available on the combined hydrogen adsorption at the sample surface and diffusion in the metal. A modeling of hydrogen gaseous charging has been established starting with a set of relevant laws and parameters derived from open literature. Simulating the hydrogen charging process requires simultaneous analysis of gaseous surface adsorption, hydrogen solid-solution diffusion and precipitation, when exceeding the material solubility limit. The modeling has been extended to reproduce the solid-gas exchange. Gaseous charging experiments have been performed at 420 C. degrees on Stress Relieved Annealed (SRA) Zircaloy-4 cladding samples to validate the model. The sample hydrogen content has been systematically measured after charging and compared to the calculated value thus providing a validation of the adsorption modeling. Complementary tests have been carried out on Recrystallized Annealed (RXA) Zircaloy-4 rods to characterize the combined diffusion and adsorption process. The hydrogen concentration distribution has been characterized using an inverse technique based on destructive analyses of the samples. This additional set of data was relevant for the validation of the hydrogen combined adsorption/diffusion modeling up to 420 C. degrees. (authors)

  16. Multiscale Study of Hydrogen Adsorption on Six Designed Covalent Organic Frameworks Based on Porphyrazine, Cyclobutane and Scandium

    International Nuclear Information System (INIS)

    Li Le-Le; Gao Teng-Fei; Zhang Ruan-Yu; Zhang Hong

    2014-01-01

    The first-principles method of hydrogen adsorption is used to investigate the interaction of H_2 with the scandium-porphyrazine (Sc-Pz) and porphyrazine (Pz) clusters. The result shows that the interaction of H_2 with Sc-Pz is stronger than with Pz. Then grand canonical Monte Carlo simulations are used to investigate hydrogen adsorption in six designed covalent organic frameworks (COFs), which are designed based on porphyrazine, cyclobutane and scandium. When the pressure is from 0.1 to 100 bar and the temperature is 298 K and 77 K, the hydrogen adsorption capacities of the six COFs are calculated. We further study the importance of Sc and fillers to improve the H_2 uptake in the modified COFs by analyzing the isosteric heat of hydrogen adsorption. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

  17. Atomic hydrogen and oxygen adsorptions in single-walled zigzag silicon nanotubes

    International Nuclear Information System (INIS)

    Chen, Haoliang; Ray, Asok K.

    2013-01-01

    Ab initio calculations have been performed to study the electronic and geometric structure properties of zigzag silicon nanotubes. Full geometry and spin optimizations have been performed without any symmetry constraints with an all electron 3-21G* basis set and the B3LYP hybrid functional. The largest zigzag SiNT studied here, (12, 0), has a binding energy per atom of 3.584 eV. Atomic hydrogen and oxygen adsorptions on (9, 0) and (10, 0) nanotubes have also been studied by optimizing the distances of the adatoms from both inside and outside the tube. The adatom is initially placed in four adsorption sites-parallel bridge (PB), zigzag bridge (ZB), hollow, and on-top site. The on-top site is the most preferred site for hydrogen atom adsorbed on (9, 0), with an adsorption energy of 3.0 eV and an optimized distance of 1.49 Å from the adatom to the nearest silicon atom. For oxygen adsorption on (9, 0), the most preferred site is the ZB site, with an adsorption energy of 5.987 eV and an optimized distance of 1.72 Å. For atomic hydrogen adsorption on (10, 0), the most preferred site is also the on-top site with an adsorption energy of 3.174 eV and an optimized distance of 1.49 Å. For adsorption of atomic oxygen on (10, 0), the most preferred site is PB site, with an adsorption energy of 6.306 eV and an optimized distance of 1.71 Å. The HOMO–LUMO gaps of (9, 0) after adsorptions of hydrogen and oxygen atoms decrease while the HOMO–LUMO gaps of (10, 0) increase after adsorption of hydrogen and oxygen

  18. A computational study on the hydrogen adsorption capacity of various lithium-doped boron hydrides.

    Science.gov (United States)

    Pan, Sudip; Giri, Santanab; Chattaraj, Pratim K

    2012-02-05

    An aromatic boron hydride B(3)H(3)(2-) and its various Li/Li(+) doped isomers have been studied at the B3LYP/6-311+G(d) and M06/6-311+G(d) levels of theory to assess their hydrogen storage potential. Different types of interaction energies, reaction enthalpies and reaction electrophilicities associated with the hydrogen adsorption process suggest that B(3)H(3)(2-) itself and some of its Li-decorated analogues may turn out to be effective hydrogen storage material. Nucleus independent chemical shift and conceptual density functional theory based reactivity descriptors lend additional support. The temperature-pressure phase diagram identifies the temperature-pressure zone where the reaction Gibbs free energy for the hydrogen adsorption is negative making it a thermodynamically feasible process. Copyright © 2011 Wiley Periodicals, Inc.

  19. Hydrogen adsorption on skeletal rhodium-tantalum electrodes-catalysts

    International Nuclear Information System (INIS)

    Tsinstevich, V.M.; Krejnina, N.M.

    1975-01-01

    Skeleton rhodium-tantalic catalyst electrodes with a tantalum mass percentage of 0 to 100 have been obtained by the methodology of Crupp and others. The hydrogen adsorption is studied through the method of removing the galvano-static and potentiodynamic curves of charging in sulfuric acid and potassium hydroxide. It has been discovered that the maximum adsorption ability relatively to the hydrogen can be observed in an alloy with a 5% tantalum contents. The energetic characteristics of the alloys are higher in alkali than in acid

  20. Hydrogen adsorption in doped porous carbons

    International Nuclear Information System (INIS)

    L Balan; L Duclaux; S Los

    2005-01-01

    Full text of publication follows: Hydrogen is a clean fuel that will be used in automotive transport when the problem of storage will be solved. The difficulties of H 2 storage (available space, security and performance, etc...) require a material that can store 5 weight % of hydrogen. Research is focused on new materials that can assume the constraints imposed by the automotive applications. Among these materials, the nano-structured carbons (nano-fibers and single walled carbon nano-tubes) were claimed to be promising by numerous authors [1-3]. The more promising carbon materials for hydrogen adsorption are those having micropores (i. e. single walled carbon nano-tubes and activated carbon), for which the energy of sorption of hydrogen molecules is theoretically higher [7-8]. Presently, the best performance of hydrogen adsorption was found in super-activated microporous carbons sorbing 5 weight % at 77 K, and almost 0.5 % at room temperature and 6 MPa [9]. Up to now, the performance of these materials can still be improved as the known mechanism of sorption in these carbon materials: physi-sorption controlled by Van der Waals attractive forces through London interaction is efficient at cryogenic temperatures (77 K) where the interaction between adsorbent and adsorbate becomes stronger. One way to improve the attractive interaction between adsorbent and molecule is to increase the forces due to the interaction of electrical field and induced dipole of the molecule. This can be theoretically tailored in carbon materials through the electron charge transfer by electron donors who can provide an increase in the electrical field at the surface of the adsorbent. Then, the doping of carbon substrates, appearing to be a promising method to increase the energy of adsorption has been proposed in recent papers as a solution to obtain good hydrogen adsorption properties at appropriate temperatures close to room temperatures [10-12]. Thus, we have studied the adsorption

  1. Hydrogen adsorption in doped porous carbons

    International Nuclear Information System (INIS)

    Balan, L.; Duchaux, L.; Los, S.

    2005-01-01

    Full text of publication follows: Hydrogen is a clean fuel that will be used in automotive transport when the problem of storage will be solved. The difficulties of H 2 storage (available space, security and performance, etc...) require a material that can store 5 weight % of hydrogen. Research is focused on new materials that can assume the constraints imposed by the automotive applications. Among these materials, the nano-structured carbons (nano-fibers and single walled carbon nano-tubes) were claimed to be promising by numerous authors [1-3]. The more promising carbon materials for hydrogen adsorption are those having micropores (i. e. single walled carbon nano-tubes and activated carbon), for which the energy of sorption of hydrogen molecules is theoretically higher [7- 8]. Presently, the best performance of hydrogen adsorption was found in super-activated micro-porous carbons sorbing 5 weight % at 77 K, and almost 0.5 % at room temperature and 6 MPa [9]. Up to now, the performance of these materials can still be improved as the known mechanism of sorption in these carbon materials: physisorption controlled by Van der Waals attractive forces through London interaction is efficient at cryogenic temperatures (77 K) where the interaction between adsorbent and adsorbate becomes stronger. One way to improve the attractive interaction between adsorbent and molecule is to increase the forces due to the interaction of electrical field and induced dipole of the molecule. This can be theoretically tailored in carbon materials through the electron charge transfer by electron donors who can provide an increase in the electrical field al the surface of the adsorbent. Then, the doping of carbon substrates, appearing to be a promising method to increase the energy of adsorption has been proposed in recent papers as a solution to obtain good hydrogen adsorption properties at appropriate temperatures close to room temperatures [10-12]. Thus, we have studied the adsorption

  2. Adsorption of hydrogen gas and redox processes in clays.

    Science.gov (United States)

    Didier, Mathilde; Leone, Laura; Greneche, Jean-Marc; Giffaut, Eric; Charlet, Laurent

    2012-03-20

    In order to assess the adsorption properties of hydrogen gas and reactivity of adsorbed hydrogen, we measured H(2)(g) adsorption on Na synthetic montmorillonite-type clays and Callovo-Oxfordian (COx) clayrock using gas chromatography. Synthetic montmorillonites with increasing structural Fe(III) substitution (0 wt %, 3.2 wt %, and 6.4 wt % Fe) were used. Fe in the synthetic montmorillonites is principally present as structural Fe(III) ions. We studied the concomitant reduction of structural Fe(III) in the clays using (57)Fe Mössbauer spectrometry. The COx, which mainly contains smectite/illite and calcite minerals, is also studied together with the pure clay fraction of this clayrock. Experiments were performed with dry clay samples which were reacted with hydrogen gas at 90 and 120 °C for 30 to 45 days at a hydrogen partial pressure close to 0.45 bar. Results indicate that up to 0.11 wt % of hydrogen is adsorbed on the clays at 90 °C under 0.45 bar of relative pressure. (57)Fe Mössbauer spectrometry shows that up to 6% of the total structural Fe(III) initially present in these synthetic clays is reduced upon adsorption of hydrogen gas. No reduction is observed with the COx sample in the present experimental conditions.

  3. Adsorption process to recover hydrogen from feed gas mixtures having low hydrogen concentration

    Science.gov (United States)

    Golden, Timothy Christopher; Weist, Jr., Edward Landis; Hufton, Jeffrey Raymond; Novosat, Paul Anthony

    2010-04-13

    A process for selectively separating hydrogen from at least one more strongly adsorbable component in a plurality of adsorption beds to produce a hydrogen-rich product gas from a low hydrogen concentration feed with a high recovery rate. Each of the plurality of adsorption beds subjected to a repetitive cycle. The process comprises an adsorption step for producing the hydrogen-rich product from a feed gas mixture comprising 5% to 50% hydrogen, at least two pressure equalization by void space gas withdrawal steps, a provide purge step resulting in a first pressure decrease, a blowdown step resulting in a second pressure decrease, a purge step, at least two pressure equalization by void space gas introduction steps, and a repressurization step. The second pressure decrease is at least 2 times greater than the first pressure decrease.

  4. Theoretical study of hydrogen adsorption of graphene and carbon nanotubes decorated with palladium

    International Nuclear Information System (INIS)

    Lopez Corral, Ignacio; German, Estefania; Volpe, Maria A; Brizuela, Graciela; Juan, Alfredo

    2008-01-01

    Since their discovery in 1991, carbon nanotubes (CNT) have awakened great interest in materials science thanks to their extraordinary structural, electronic and mechanical properties which facilitate their application in many different areas. One of the most promising applications is the possibility of using CNT to store hydrogen for use in small scale fuel cells. Unfortunately, experimental studies performed some years ago have often led to controversial conclusions, causing a continuing debate that has still not been resolved. The most recent work suggests that the storage of hydrogen for practical purposes can be achieved with CNT decorated with transition metals, for example Pd. In this context, theoretical modeling methods have to be used for a detailed understanding of the influence and scope of this type of modification in the interaction of the nanotubes with atomic or molecular hydrogen. This work studied hydrogen adsorption in single-walled carbon nanotubes (SWCNT) doped with Pd atoms, using density functional theory (DFT) and semi-empirical methods. As a preliminary approximation to the system a graphene sheet was used, modeled with a 190 atom cluster of C in a hexagonal arrangement, on which a single Pd atom was placed in adsorption sites. Then C 190 clusters were used to simulate two different types of SWCNT: the zigzag SWCNT of quirality (10.0) and the armchair SWCNT of quirality (5.5), both decorated similarly on the graphene. Geometric optimization procedures for the system's different components were carried out with these models, and then the changes produced during the adsorption process in the electronic occupation of atomic orbitals and unions, for which crystal orbital overlap population (COOP) curves and overlap population (OP) values were evaluated. The results obtained with the graphene and nanotube approximations are in agreement and show that the SWCNT modified with Pd have more capacity to trap hydrogen than the non doped SWCNT. The

  5. Hydrogen Adsorption on Activated Carbon an Carbon Nanotubes Using Volumetric Differential Pressure Technique

    International Nuclear Information System (INIS)

    Sanip, S. M.; Saidin, M. A. R.; Aziz, M.; Ismail, A. F.

    2010-01-01

    A simple hydrogen adsorption measurement system utilizing the volumetric differential pressure technique has been designed, fabricated and calibrated. Hydrogen adsorption measurements have been carried out at temperatures 298 K and 77 K on activate carbon and carbon nanotubes with different surface areas. The adsorption data obtained will be helpful in understanding the adsorption property of the studied carbon materials using the fundamentals of adsorption theory. The principle of the system follows the Sievert-type method. The system measures a change in pressure between the reference cell, R1 and the sample cell S1, S2, S3 over a certain temperature range, R1, S1, S2, and S3 having known fixed volume. The sample temperatures will be monitored by thermocouple TC while the pressures in R1 an S1, S2, S3 will be measured using a digital pressure transducer. The maximum operating pressure of the pressure transducer is 20 bar and calibrated with an accuracy of ±0.01 bar. High purity hydrogen is being used in the system and the amount of samples for the study is between 1.0-2.0 grams. The system was calibrated using helium gas without any samples in S1, S2 an S3. This will provide a correction factor during the adsorption process providing an adsorption free reference point when using hydrogen gas resulting in a more accurate reading of the adsorption process by eliminating the errors caused by temperature expansion effects and other non-adsorption related phenomena. The ideal gas equation of state is applied to calculate the hydrogen adsorption capacity based on the differential pressure measurements. Activated carbon with a surface area of 644.87 m 2 /g showed a larger amount of adsorption as compared to multiwalled nanotubes (commercial) with a surface area of 119.68 m 2 /g. This study als indicated that there is a direct correlation between the amounts of hydrogen adsorbed an surface area of the carbon materials under the conditions studied and that the adsorption

  6. Hydrogen adsorption on and solubility in graphites

    International Nuclear Information System (INIS)

    Kanashenko, S.L.; Wampler, W.R.

    1996-01-01

    The experimental data on adsorption and solubility of hydrogen isotopes in graphite over a wide range of temperatures and pressures are reviewed. Langmuir adsorption isotherms are proposed for the hydrogen-graphite interaction. The entropy and enthalpy of adsorption are estimated, allowing for effects of relaxation of dangling sp 2 bonds. Three kinds of traps are proposed: edge carbon atoms of interstitial loops with an adsorption enthalpy relative to H 2 gas of -4.4 eV/H 2 (unrelaxed, Trap 1), edge carbon atoms at grain surfaces with an adsorption enthalpy of -2.3 eV/H 2 (relaxed, Trap 2), and basal plane adsorption sites with an enthalpy of +2.43 eV/H 2 (Trap 3). The adsorption capacity of different types of graphite depends on the concentration of traps which depends on the crystalline microstructure of the material. The number of potential sites for the 'true solubility' (Trap 3) is assumed to be about one site per carbon atom in all types of graphite, but the endothermic character of this solubility leads to a negligible H inventory compared to the concentration of hydrogen in type 1 and type 2 traps for temperatures and gas pressures used in the experiments. Irradiation with neutrons or carbon atoms increases the concentration of type 1 and type 2 traps from about 20 and 200 appm respectively for unirradiated (POCO AXF-5Q) graphite to about 1500 and 5000 appm, respectively, at damage levels above 1 dpa. (orig.)

  7. Adsorption methods for hydrogen isotope storage on zeolite sieves

    International Nuclear Information System (INIS)

    Cristescu, Ioana; Cristescu, Ion; Vasut, Felicia; Brad, Sebastian; Lazar, Alin

    2001-01-01

    Adsorption molecular sieves and activated carbon were used for hydrogen isotopes. The adsorption process proceeds at liquid nitrogen and liquid hydrogen temperatures. The synthetic zeolites have similar properties as natural zeolites, but they have a regular pore structure and affinity for molecules of different size with defined shapes. Experimental results obtained at liquid nitrogen and liquid hydrogen temperatures evidenced the efficient behavior of the activated carbon and zeolite sieves for hydrogen isotope temporary storage. (authors)

  8. Direct measurements of adsorption heats of hydrogen on nano-porous carbons

    International Nuclear Information System (INIS)

    Akihiko Matsumoto; Kazumasa Yamamoto; Tomoyuki Miyata

    2005-01-01

    Since a exciting report of hydrogen storage in single-walled carbon nano-tubes by Dillon and his colleagues, nano-porous carbon materials, such as carbon nano-tubes, carbon nano-horns and micro-porous activated carbon, have attracted considerable attention as hydrogen storage materials. Adsorption plays a predominating role in the hydrogen storage process on solid surfaces. The adsorption is a spontaneous process, which is caused by interaction between gas molecules and surface, hence, it is always exothermic process and observed as adsorption heats. For this reason, direct measurement of the adsorption heats by adsorption micro-calorimetry would provide quantitative information on the strength of adsorption interaction and the adsorption mechanism. However, the adsorption amounts of hydrogen on carbon materials are far less than those of condensable vapors near room temperature due to low critical temperature of hydrogen (33.2 K), therefore, the adsorption heats can not be determined accurately at conventional measurement conditions near room temperature and the atmospheric pressure. This contribution reports the calorimetric characterization of hydrogen adsorption on nano-porous carbon materials at low temperature and high-pressure conditions. The high-pressure adsorption apparatus consists of a volumetric adsorption line connected to a twin-conduction type microcalorimeter. Activated carbon fibers (ACF, Ad'all Co.) of different micro-pore sizes (Table 1) were used as model adsorbents. Each ACF has slit-shaped micropores of uniform size. The adsorption isotherms and differential heats of adsorption at high-pressure region from 0 to 10 MPa were simultaneously measured at isothermal condition from 203 to 298 K. The adsorption isotherms on ACF were of Henry type regardless of adsorption temperature and pore width; the uptakes increased linearly with equilibrium pressure. The adsorption isotherm at lower sorption temperature tended to show higher sorptivity. The

  9. Hydrogen Adsorption on Activated Carbon an Carbon Nanotubes Using Volumetric Differential Pressure Technique

    Science.gov (United States)

    Sanip, S. M.; Saidin, M. A. R.; Aziz, M.; Ismail, A. F.

    2010-03-01

    A simple hydrogen adsorption measurement system utilizing the volumetri differential pressure technique has been designed, fabricated and calibrated. Hydroge adsorption measurements have been carried out at temperatures 298 K and 77 K on activate carbon and carbon nanotubes with different surface areas. The adsorption data obtained will b helpful in understanding the adsorption property of the studied carbon materials using th fundamentals of adsorption theory. The principle of the system follows the Sievert-type metho The system measures a change in pressure between the reference cell, R1 and the sample cell S1, S2, S3 over a certain temperature range. R1, S1, S2, and S3 having known fixed volume The sample temperatures will be monitored by thermocouple TC while the pressures in R1 an S1, S2, S3 will be measured using a digital pressure transducer. The maximum operatin pressure of the pressure transducer is 20 bar and calibrated with an accuracy of ±0.01 bar. Hig purity hydrogen is being used in the system and the amount of samples for the study is betwee 1.0-2.0 grams. The system was calibrated using helium gas without any samples in S1, S2 an S3. This will provide a correction factor during the adsorption process providing an adsorption free reference point when using hydrogen gas resulting in a more accurate reading of th adsorption process by eliminating the errors caused by temperature expansion effects and oth non-adsorption related phenomena. The ideal gas equation of state is applied to calculate th hydrogen adsorption capacity based on the differential pressure measurements. Activated carbo with a surface area of 644.87 m2/g showed a larger amount of adsorption as compared to multiwalled nanotubes (commercial) with a surface area of 119.68 m2/g. This study als indicated that there is a direct correlation between the amounts of hydrogen adsorbed an surface area of the carbon materials under the conditions studied and that the adsorption significant at 77

  10. Hydrogen adsorption in metal-organic frameworks

    Energy Technology Data Exchange (ETDEWEB)

    Senkovska, Irena; Kaskel, Stefan [Department of Inorganic Chemistry, Technical University, Dresden (Germany)

    2008-07-01

    Metal-Organic Frameworks (MOFs) have recently received considerable attention because of their high specific micropore volume and the ability to store gas molecules exceeding the storage capacity of traditional adsorbents. A variety of differences in the MOFs structures makes it difficult to analyze the influence of different factors on hydrogen uptake capabilities in MOFs. We have investigated the influence of the minor structural changes of the MOFs on their hydrogen storage capacity. The influence of the incorporated metal was shown for following isostructural compounds: Cu{sub 3}(BTC){sub 2} (BTC=1,3,5-benzenetricarboxylate) and Mo{sub 3}(BTC){sub 2}; Zn{sub 2}(BDC){sub 2}DABCO and Co{sub 2}(BDC){sub 2}DABCO (BDC=1,4-benzenedicarboxylate, DABCO=1,4-diazabicyclo[2.2.2]octane). Our research interest is directed also towards the discovery of new MOFs, as well as adjusting the pore dimensions of MOFs, using different building blocks, solvent and solvent mixtures, in order to improve gas uptake and adsorption properties. Magnesium-based MOFs were found with the same network topology, very small pore size and selective adsorption behaviour. They show a guest-induced reversible structure transformation due to the flexibility of the Mg{sub 3}-cluster and the organic linkers. This effect could be used for fitting the pore sizes and for the increase of gas sorption capability in Mg contained MOFs after all. The hydrogen adsorption was also studied in several Al-based IRMOFs.

  11. Modeling of the thermal effects of hydrogen adsorption on activated carbon

    International Nuclear Information System (INIS)

    Richard, M.-A.; Chahine, R.

    2006-01-01

    'Full text:' Heat management is one of the most critical issues for the design of efficient adsorption-based storage of hydrogen. We present simulations of mass and energy balance for hydrogen and nitrogen adsorption on activated carbon over wide temperature and pressure ranges. First, the Dubinin-Astakhov (DA) model is adapted to model excess hydrogen and nitrogen adsorption isotherms at high pressures and supercritical temperatures assuming a constant microporous adsorption volume. The five parameter modified D-A adsorption model is shown to fit the experimental data over the temperature range (35 K-293 K) for hydrogen and (93 K-298 K) for nitrogen and pressure range (0-6 MPa) within the experimental uncertainties of the measurement system. We derive the thermodynamic properties of the adsorbed phase from this analytical expression of the measured data. The mass and energy rate balance equations in a microporous adsorbent/adsorbate system are then presented and validated with nitrogen desorption experiments. Finally, simulations of adiabatic and isothermal filling of adsorption-based hydrogen storage are presented and discussed. (author)

  12. Adsorption of hydrogen and deuterium on modified molecular sieves

    International Nuclear Information System (INIS)

    Li Jing; Shi Jinsong; Wu Erdong; Li Xiongwei; Peng Lixia

    2013-01-01

    The adsorption characteristics of hydrogen isotopes on 5A, ZSM-5 and their modified molecular sieves were studied at liquid nitrogen temperature with volumetric method. The effects of modification methods such as transition metal salt loading and ball milling on the adsorption behavior were discussed. It is observed that the adsorption amounts on the modified molecular sieves are reduced. but some modifications contribute to the separation between H 2 and D 2 . (authors)

  13. Direct measurements of adsorption heats of hydrogen on nano-porous carbons

    International Nuclear Information System (INIS)

    Akihiko, Matsumoto; Kazumasa, Yamamoto; Tomoyuki, Miyata

    2005-01-01

    Since a exciting report of hydrogen storage in single-walled carbon nano-tubes by Dillon and his colleagues [1], nano-porous carbon materials, such as carbon nano-tubes, carbon nano-horns and micro-porous activated carbon, have attracted considerable attention as hydrogen storage materials. Adsorption plays a predominating role in the hydrogen storage process on solid surfaces. The adsorption is a spontaneous process, which is caused by interaction between gas molecules and surface, hence, it is always exothermic process and observed as adsorption heats. For this reason, direct measurement of the adsorption heats by adsorption microcalorimetry would provide quantitative information on the strength of adsorption interaction and the adsorption mechanism. However, the adsorption amounts of hydrogen on carbon materials are far less than those of condensable vapors near room temperature due to low critical temperature of hydrogen (33.2 K), therefore, the adsorption heats can not be determined accurately at conventional measurement conditions near room temperature and the atmospheric pressure. This contribution reports the calorimetric characterization of hydrogen adsorption on nano-porous carbon materials at low temperature and high-pressure conditions. The high-pressure adsorption apparatus consists of a volumetric adsorption line connected to a twin-conduction type microcalorimeter. Activated carbon fibers (ACF, Ad'all Co.) of different micropore sizes (Table 1) were used as model adsorbents. Each ACF has slit-shaped micropores of uniform size [2]. The adsorption isotherms and differential heats of adsorption at high-pressure region from 0 to 10 MPa were simultaneously measured at isothermal condition from 203 to 298 K. The adsorption isotherms on ACF were of Henry type regardless of adsorption temperature and pore width; the uptakes increased linearly with equilibrium pressure. The adsorption isotherm at lower sorption temperature tended to show higher sorptivity

  14. Optimization Study of Hydrogen Gas Adsorption on Zig-zag Single-walled Carbon Nanotubes: The Artificial Neural Network Analysis

    Science.gov (United States)

    Nasruddin; Lestari, M.; Supriyadi; Sholahudin

    2018-03-01

    The use of hydrogen gas in fuel cell technology has a huge opportunity to be applied in upcoming vehicle technology. One of the most important problems in fuel cell technology is the hydrogen storage. The adsorption of hydrogen in carbon-based materials attracts a lot of attention because of its reliability. This study investigated the adsorption of hydrogen gas in Single-walled Carbon Nano Tubes (SWCNT) with chilarity of (0, 12), (0, 15), and (0, 18) to find the optimum chilarity. Artificial Neural Networks (ANN) can be used to predict the hydrogen storage capacity at different pressure and temperature conditions appropriately, using simulated series of data. The Artificial Neural Network is modeled as a predictor of the hydrogen adsorption capacity which provides solutions to some deficiencies in molecular dynamics (MD) simulations. In a previous study, ANN configurations have been developed for 77k, 233k, and 298k temperatures in hydrogen gas storage. To prepare this prediction, ANN is modeled to find out the configurations that exist in the set of training and validation of specified data selection, the distance between data, and the number of neurons that produce the smallest error. This configuration is needed to make an accurate artificial neural network. The configuration of neural network was then applied to this research. The neural network analysis results show that the best configuration of artificial neural network in hydrogen storage is at 233K temperature i.e. on SWCNT with chilarity of (0.12).

  15. Hydrogen adsorption on partially oxidised microporous carbons

    International Nuclear Information System (INIS)

    J B Parra; C O Ania; C J Duran Valle; M L Sanchez; C Otero Arean

    2005-01-01

    The search for cost effective adsorbents for large scale gas separation, storage and transport constitutes a present day strategic issue in the energy sector, propelled mainly by the potential use of hydrogen as an energy vector in a sustainable (and cleaner) energy scenario. Both, activated carbons and carbon based nano-structured materials have been proposed as potential candidates for reversible hydrogen storage in cryogenically cooled vessels. For that purpose, surface modification so as to enhance the gas solid interaction energy is desirable. We report on hydrogen adsorption on microporous (active) carbons which have been partially oxidised with nitric acid and ammonium persulfate. From the corresponding hydrogen adsorption isotherms (Fig. 1) an isosteric heat of about 3 kJ mol -1 was derived. This value is in agreement with that of about 3 to 4 kJ mol -1 obtained by quantum chemical calculations on the interaction between the hydrogen molecule and simple model systems (Fig. 2) of both, hydroxyl and carboxyl groups. Further research is in progress with a view to further increases the gas solid interaction energy. However, the values so far obtained are significantly larger than the liquefaction enthalpy of hydrogen: 0.90 kJ mol -1 ; and this is relevant to both, hydrogen separation from gas mixtures and cryogenic hydrogen storage. (authors)

  16. A theoretical study of hydrogen atoms adsorption and diffusion on PuO_2 (110) surface

    International Nuclear Information System (INIS)

    Yu, H.L.; Tang, T.; Zheng, S.T.; Shi, Y.; Qiu, R.Z.; Luo, W.H.; Meng, D.Q.

    2016-01-01

    The mechanisms of adsorption and diffusion of hydrogen atoms on the PuO_2 (110) surface are investigated by density functional theory corrected for onsite Coulombic interactions (GGA + U). In order to find out the energetically more favorable adsorption site and optimum diffusion path, adsorption energy of atomic H on various sites and the diffusion energy barrier are derived and compared. Our results show that both chemisorption and physisorption exist for H atoms adsorption configurations on PuO_2 (110) surface. Two processes for H diffusion are investigated using the climbing nudged-elastic-band (cNEB) approach. We have identified two diffusion mechanisms, leading to migration of atomic H on the surface and diffusion from surface to subsurface. The energy barriers indicate that it is energetically more favorable for H atom to be on the surface. Hydrogen permeation through purity PuO_2 surface is mainly inhibited from hydrogen atom diffusion from surface to subsurface. - Highlights: • H atoms adsorption on PuO_2 (110) surface are investigated by GGA + U. • Both chemisorption and physisorption exist for H atoms adsorption configurations. • H atoms migration into PuO_2 (100) surface are inhibited with the barrier of 2.15 eV. • H atoms diffusion on PuO_2 (110) surface are difficult at room temperature.

  17. Hydrogen Adsorption on Nanoporous Biocarbon

    Science.gov (United States)

    Wood, M. B.; Burress, J. W.; Lapilli, C. M.; Pfeifer, P.; Shah, P. S.; Suppes, G. J.; Dillon, A. C.; Parilla, P. A.

    2007-03-01

    As a part of the Alliance for Collaborative Research in Alternative Fuel Technology (http://all-craft.missouri.edu) we study activated carbons made from corncob, optimized for storing methane and hydrogen (H2) by physisorption at low pressure. We report here: (a) storage capacities of 73-91 g H2/kg carbon at 77 K and 47 bar, validated in three different laboratories (the 2010 DOE target is 60 g H2/kg system); (b) binding energies from H2 adsorption isotherms (c) temperature-programmed desorption data; (d) degree of graphitization of the carbon surface from Raman spectra; (e) pore structure of carbon from nitrogen and methane adsorption isotherms, and small-angle x-ray scattering. The structural analysis shows that the carbon is highly microporous and that the pore space is highly correlated (micropores do not scatter independently).

  18. A study on hydrogen storage through adsorption in nano-structured carbons; Etude du stockage d'hydrogene par adsorption dans des carbones nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Langohr, D

    2004-10-15

    The aim of this work is to build and calibrate an experimental set-up for the testing of the materials, to produce some carbon materials in large amounts and characterise them, and finally, to test these materials in their ability to store hydrogen. This will help in establishing a link between the hydrogen storage capacities of the carbons and their nano-structure. The script is divided into four chapters. The first chapter will deal with the literature review on the thematic of hydrogen storage through adsorption in the carbon materials, while the second chapter will present the experimental set-up elaborated in the laboratory. The third chapter explains the processes used to produce the two families of carbon materials and finally, the last chapter presents the structural characterisation of the samples as well as the experimental results of hydrogen storage on the materials elaborated. (author)

  19. Adsorption and desorption of hydrogen and carbon monoxide were studied on alumina-supported iridium catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Etherton, B.P.

    1980-01-01

    The adsorption and desorption of hydrogen and carbon monoxide were studied on alumina-supported iridium catalysts which were examined by a scanning transmission electron microscope (STEM). The metal particle size and number of particles per area of catalyst increased with increasing metal loading. The particles were approx. 10 A. in diameter, cubo-octahedral shaped, and approx. 80-90% disperse. The STEM electron beam caused negligible damage to the samples. Hydrogen adsorption measurements showed that the hydrogen-iridium atom ratio was 1.2:1-1.3:1 and increased with decreasing metal loading. Temperature-programed desorption showed four types of adsorbed hydrogen desorbing at -90/sup 0/C (I), 15/sup 0/C (IV), 115/sup 0/C (II), and 245/sup 0/C (III). Types II and IV desorb from single atom sites and Types I and III from multiple atom sites. Type I is in rapid equilibrium with the gas phase. All desorption processes appear to be first order. Carbon monoxide adsorbed nondissociatively at 25/sup 0/C with approx. 0.7:1 CO/Ir atom ratio. It adsorbed primarily in linear forms at low coverage, but a bridged form appeared at high coverage.

  20. Structural and electronic properties of hydrogen adsorptions on BC3 sheet and graphene: a comparative study

    International Nuclear Information System (INIS)

    Chuang, Feng-Chuan; Huang, Zhi-Quan; Lin, Wen-Huan; Albao, Marvin A; Su, Wan-Sheng

    2011-01-01

    We have systematically investigated the effect of hydrogen adsorption on a single BC 3 sheet as well as graphene using first-principles calculations. Specifically, a comparative study of the energetically favorable atomic configurations for both H-adsorbed BC 3 sheets and graphene at different hydrogen concentrations ranging from 1/32 to 4/32 ML and 1/8 to 1 ML was undertaken. The preferred hydrogen arrangement on the single BC 3 sheet and graphene was found to have the same property as that of the adsorbed H atoms on the neighboring C atoms on the opposite sides of the sheet. Moreover, at low coverage of H, the pattern of hydrogen adsorption on the BC 3 shows a proclivity toward formation on the same ring, contrasting their behavior on graphene where they tend to form the elongated zigzag chains instead. Lastly, both the hydrogenated BC 3 sheet and graphene exhibit alternation of semiconducting and metallic properties as the H concentration is increased. These results suggest the possibility of manipulating the bandgaps in a single BC 3 sheet and graphene by controlling the H concentrations on the BC 3 sheet and graphene.

  1. Adsorption of hydrogen in Scandium/Titanium decorated nitrogen doped carbon nanotube

    Energy Technology Data Exchange (ETDEWEB)

    Mananghaya, Michael, E-mail: mikemananghaya@gmail.com [De La Salle University, 2401 Taft Ave, 0922, Manila (Philippines); DLSU STC Laguna Boulevard, LTI Spine Road Barangays Biñan and Malamig, Biñan City, Laguna (Philippines); DOST-ASTHRDP, PCIEERD, Gen. Santos Ave., Bicutan, Taguig City 1631 (Philippines); Belo, Lawrence Phoa; Beltran, Arnel [De La Salle University, 2401 Taft Ave, 0922, Manila (Philippines); DLSU STC Laguna Boulevard, LTI Spine Road Barangays Biñan and Malamig, Biñan City, Laguna (Philippines)

    2016-09-01

    Nitrogen doped Carbon Nanotube with divacancy (4ND-CN{sub x}NT) that is decorated with Scandium and Titanium as potential hydrogen storage medium using the pseudo potential density functional method was investigated. Highly localized states near the Fermi level, which are derived from the nitrogen defects, contribute to strong Sc and Ti bindings, which prevent metal aggregation and improve the material stability. A detailed Comparison of the Hydrogen adsorption capability with promising system-weight efficiency of Sc over Ti was elucidated when functionalized with 4ND-CN{sub x}NT. Finally, the (Sc/4ND){sub 10}-CN{sub x}CNT composite material has a thermodynamically favorable adsorption and consecutive adsorption energy for ideal reversible adsorption and desorption of hydrogen at room temperature such that it can hold at least 5.8 wt% hydrogen molecules at the LDA and GGA level. - Highlights: • Carbon Nanotube with divacancy (4ND-CN{sub x}NT) decorated with Sc and Ti. • Nitrogen defects, contribute to strong Sc and Ti bindings. • H{sub 2} and (Sc/4ND){sub 10}-CN{sub x}CNT has a favorable adsorption. • 5.8 wt% adsorption at the LDA and GGA level.

  2. Grand Canonical Monte Carlo simulations of hydrogen adsorption on aluminophosphate molecular sieves

    Energy Technology Data Exchange (ETDEWEB)

    Song, Mee Kyung [Bioinformatics and Molecular Design Research Center, B138A, Yonsei Engineering Research Complex, Yonsei University, Seoul 120-749 (Korea); No, Kyoung Tai [Department of Biotechnology, College of Life Science and Biotechnology, Yonsei University, Seoul 120-749 (Korea)

    2009-03-15

    The hydrogen adsorption simulations were carried for several model AlPOs (VPI-5, AlPO-5, AlPO-11 and AlPO-25) employing the Grand Canonical Monte Carlo (GCMC) simulations at 77 K to investigate the effect of pore size and the pore volume on the hydrogen uptake. The adsorption capacity showed no relationship with the pore size, surface area and micropore volume of AlPOs. However, the adsorption capacity per unit micropore volume increased as the pore size decreases. The heat of adsorption also increased as the pore size decreases. For all model AlPOs, the hydrogen exists homogeneously near the oxygen atoms in the framework. (author)

  3. Hydrogen adsorption in the series of carbon nanostructures: Graphenes-graphene nanotubes-nanocrystallites

    Science.gov (United States)

    Soldatov, A. P.; Kirichenko, A. N.; Tat'yanin, E. V.

    2016-07-01

    A comparative analysis of hydrogen absorption capability is performed for the first time for three types of carbon nanostructures: graphenes, oriented carbon nanotubes with graphene walls (OCNTGs), and pyrocarbon nanocrystallites (PCNs) synthesized in the pores of TRUMEM ultrafiltration membranes with mean diameters ( D m) of 50 and 90 nm, using methane as the pyrolized gas. The morphology of the carbon nanostructures is studied by means of powder X-ray diffraction, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and transmission electron microscopy (TEM). Hydrogen adsorption is investigated via thermogravimetric analysis (TGA) in combination with mass-spectrometry. It is shown that only OCNTGs can adsorb and store hydrogen, the desorption of which under atmospheric pressure occurs at a temperature of around 175°C. Hydrogen adsorption by OCNTGs is quantitatively determined and found to be about 1.5% of their mass. Applying certain assumptions, the relationship between the mass of carbon required for the formation of single-wall OCNTGs in membrane pores and the surface area of pores is established. Numerical factor Ψ = m dep/ m calc, where m dep is the actual mass of carbon deposited upon the formation of OCNTGs and mcalc is the calculated mass of carbon necessary for the formation of OCNTGs is introduced. It is found that the dependence of specific hydrogen adsorption on the magnitude of the factor has a maximum at Ψ = 1.2, and OCNTGs can adsorb and store hydrogen in the interval 0.4 to 0.6 hydrogen adsorption and its relationship to the structure of carbon nanoformations are examined.

  4. Effect of nitrogen doping of graphene oxide on hydrogen and hydroxyl adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Min, Byeong June; Jeong, Hae Kyung [Daegu University, Kyungsan (Korea, Republic of)

    2014-05-15

    We investigate how nitrogen-doping affects the hydrogen (H) and the hydroxyl (OH) adsorption on graphene oxide (GO) and on nitrogen-doped GO (NGO) via pseudopotential plane wave density functional calculations within the local spin density approximation. We find that the nitrogen doping brings about drastic changes in the hydrogen and the hydroxyl adsorption energetics, but its effects depend sensitively on the nitrogen configuration in NGO. The H and the OH adsorption energies are comparable only for pyrrolic NGO. In GO and quarternary NGO, the H adsorption energy is greater than the OH adsorption energy while the trend is reversed in pyridinic NGO. Also, the OH adsorption process is less affected by nitrogen-doping than the H adsorption is.

  5. Hydrogen Adsorption in Flame Synthesized and Lithium Intercalated Carbon Nanofibers--A Comparative Study.

    Science.gov (United States)

    Dhand, Vivek; Prasad, J Sarada; Rao, Venkateswer M; Kalluri, Sujith; Jain, Pawan Kumar; Sreedhar, B

    2015-01-01

    Carbon nanofibers (CNF) have been synthesized under partial combustion conditions in a flame reactor using different mixtures of hydrocarbon gases in the presence and absence of precursors. The hydrogen (H2) adsorption studies have been carried out using a high pressure Sievert's apparatus maintained at a constant temperature (24 degrees C). The flame synthesized CNFs showed high degree of H2 adsorption capacities at 100 atm pressure. The highest H2 capacities recorded have been 4.1 wt% [for CNF produced by liquefied petroleum gas (LPG)-Air (E-17)], 3.7 wt% [for nano carbons produced by Methane-Acetylene-Air (EMAC-4)] and 5.04 wt% for [Lithium intercalated sample (Li-EMAC-4)] respectively.

  6. Relationship between carbon microstructure, adsorption energy and hydrogen adsorption capacity at different temperatures

    International Nuclear Information System (INIS)

    Jacek Jagiello; Matthias Thommes

    2005-01-01

    Various microporous materials such as activated carbons, nano-tubes, synthetic microporous carbons as well as metal organic framework materials are being considered for hydrogen storage applications by means of physical adsorption. To develop materials of practical significance for hydrogen storage it is important to understand the relationships between pore sizes, adsorption energies and adsorption capacities. The pore size distribution (PSD) characterization is traditionally obtained from the analysis of nitrogen adsorption isotherms measured at 77 K. However, a portion of the pores accessible to H 2 may not be accessible to N 2 at this temperature. Therefore, it was recently proposed to use the DFT analysis of H 2 adsorption isotherms to characterize pore structure of materials considered for hydrogen storage applications. In present work, adsorption isotherms of H 2 and N 2 at cryogenic temperatures are used for the characterization of carbon materials. Adsorption measurements were performed with Autosorb 1 MP (Quantachrome Instruments, Boynton Beach, Florida, USA). As an example, Fig 1 compares PSDs calculated for the activated carbon sample (F400, Calgon Carbon) using combined H 2 and N 2 data, and using N 2 isotherm only. The nitrogen derived PSD does not include certain amount of micropores which are accessible to H 2 but not to N 2 molecules. Obviously, the difference in the calculated PSDs by the two methods will depend on the actual content of small micropores in a given sample. Carbon adsorption properties can also be characterized by the isosteric heat of adsorption, Qst, related to the adsorption energy and dependent on the carbon pore/surface structure. Fig 2 shows Qst data calculated using the Clausius-Clapeyron equation from H 2 isotherms measured at 77 K and 87 K for the carbon molecular sieve CMS 5A (Takeda), oxidized single wall nano-tubes (SWNT), and graphitized carbon black (Supelco). The Qst values decrease with increasing pore sizes. The

  7. A study on hydrogen storage through adsorption in nano-structured carbons

    International Nuclear Information System (INIS)

    Langohr, D.

    2004-10-01

    The aim of this work is to build and calibrate an experimental set-up for the testing of the materials, to produce some carbon materials in large amounts and characterise them, and finally, to test these materials in their ability to store hydrogen. This will help in establishing a link between the hydrogen storage capacities of the carbons and their nano-structure. The script is divided into four chapters. The first chapter will deal with the literature review on the thematic of hydrogen storage through adsorption in the carbon materials, while the second chapter will present the experimental set-up elaborated in the laboratory. The third chapter explains the processes used to produce the two families of carbon materials and finally, the last chapter presents the structural characterisation of the samples as well as the experimental results of hydrogen storage on the materials elaborated. (author)

  8. A study on hydrogen storage through adsorption in nano-structured carbons; Etude du stockage d'hydrogene par adsorption dans des carbones nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Langohr, D

    2004-10-15

    The aim of this work is to build and calibrate an experimental set-up for the testing of the materials, to produce some carbon materials in large amounts and characterise them, and finally, to test these materials in their ability to store hydrogen. This will help in establishing a link between the hydrogen storage capacities of the carbons and their nano-structure. The script is divided into four chapters. The first chapter will deal with the literature review on the thematic of hydrogen storage through adsorption in the carbon materials, while the second chapter will present the experimental set-up elaborated in the laboratory. The third chapter explains the processes used to produce the two families of carbon materials and finally, the last chapter presents the structural characterisation of the samples as well as the experimental results of hydrogen storage on the materials elaborated. (author)

  9. High coverage hydrogen adsorption on the Fe{sub 3}O{sub 4}(1 1 0) surface

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Xiaohu, E-mail: yuxiaohu950203@126.com [College of Physics and Electrical Engineering, Anyang Normal University, Anyang, Henan 455000 (China); State Key laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001 (China); Zhang, Xuemei [College of Physics and Electrical Engineering, Anyang Normal University, Anyang, Henan 455000 (China); Wang, Shengguang [State Key laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001 (China); Synfuels China Co., Ltd., Huairou, Beijing 101407 (China)

    2015-10-30

    Graphical abstract: - Highlights: • Hydrogen adsorption on the A and B termination layers of the Fe{sub 3}O{sub 4}(1 1 0) surface at different coverage has been studied by DFT + U method. • The adsorption of hydrogen prefers surface oxygen atoms on both Fe{sub 3}O{sub 4}(1 1 0) surface layers. • The more stable A layer has stronger adsorption energy than the less stable B layer. • The saturation coverage has two dissociatively adsorbed H{sub 2} on the A layer, and one dissociatively adsorbed H{sub 2} on the B layer. - Abstract: Hydrogen adsorption on the A and B termination layers of the Fe{sub 3}O{sub 4}(1 1 0) surface at different coverage has been systematically studied by density functional theory calculations including an on-site Hubbard term (GGA + U). The adsorption of hydrogen prefers surface oxygen atoms on both layers. The more stable A layer has stronger adsorption energy than the less stable B layer. The saturation coverage has two dissociatively adsorbed H{sub 2} on the A layer, and one dissociatively adsorbed H{sub 2} on the B layer. The adsorption mechanism has been analyzed on the basis of projected density of states (PDOS).

  10. Hydrogen adsorption and desorption in carbon nanotube systems and its mechanisms

    Energy Technology Data Exchange (ETDEWEB)

    Shiraishi, M.; Takenobu, T.; Ata, M. [Materials Laboratories, SONY Corporation, Shin-Sakuragaoka 2-1-1, Hodogaya-ku, 240-0036, Yokohama (Japan); Kataura, H. [Department of Physics, Faculty of Science, Tokyo Metropolitan University, Minami-Osawa, Hachioji, 192-0397, Tokyo (Japan)

    2004-04-01

    The hydrogen physisorption properties in single-walled carbon nanotube (SWNT) based materials were characterized. The SWNTs were highly purified and three useful pores for hydrogen physisorption were activated. Hydrogen was physisorbed in intra-tube pores at room temperature and the capacity was estimated to be about 0.3-0.4 wt. % at room temperature. The adsorption capacity can be explained by the Langmuir model. The intra-tube pores have large adsorption potential and this induces hydrogen physisorption at comparatively higher temperatures. This fact indicates the importance of fabricating sub-nanometer ordered pores for this phenomena. (orig.)

  11. Study of the secondary electron energy spectrum of clean aluminium modification during oxygen adsorption, hydrogen adsorption or carbon segregation

    International Nuclear Information System (INIS)

    Pellerin, Francois

    1981-01-01

    The first part of this work is a review of both theoretical and experimental aspects of the fine structure appearing in the Secondary Electron Spectrum (SES) and in the electron energy loss spectrum. In the second part, we report the results of a study of the SES and ELS spectra of clean and gas covered aluminium. The use of very low primary electron energies (E p ≤ 30 eV) enables the detection of previously unobserved peaks in the ELS spectra of clean and oxygen covered aluminium. They are attributed to single electron excitations. Furthermore, a very large peak appears in the SES spectrum during oxygen or carbon adsorption on aluminium. It is interpreted in terms of interaction of the background electrons with the valence electrons of the surface. Molecular hydrogen adsorption is observed on Ta, Pt, Al 2 O 3 , Si. It is responsible for an ELS peak located 13 eV below the elastic peak. Furthermore, on silicon, the chemisorbed hydrogen form can be distinguished from the molecular form with the help of ELS. Finally, some examples are given of the application of these results to surface imaging. (author) [fr

  12. Benzene adsorption and hydrogenation on Pd-Ru alloy by pulse chromatography

    International Nuclear Information System (INIS)

    Dobrokhotov, V.G.; Pavlova, L.F.; Gryaznov, V.M.

    1983-01-01

    Pulse chromatography has been applied to investigate benzene adsorption and hydrogenation on the Walls of a capillary of the Pd-6% Ru alloy at different hydrogen contents in the alloy and various methods of hydrogen supply: as a mixture with benzene vapors or by diffusion through the walls of the capillary. It is stated that reversible adsorption of benzene vapors on the Pd-6% Ru alloy at 303 K under the conditions of the β-phase existence in the alloy-hydrogen system does not change whereas in the region of the α-phase existence it slightly increases with a growth of hydrogen pressure. Strongly adsorbed benzene occupies approximately 7% of the surface. Only strongly adsorbed benzene is hydrogenated on the α-phase of the alloy-hydrogen system. Hydrogen supply to the hydrogenation zone by diffusion throUgh the alloy results in supersaturation of the surface active in the reaction of benzene hydrogenation with a chemisorbed hydrogen form

  13. A model for the physical adsorption of atomic hydrogen

    NARCIS (Netherlands)

    Bruch, L.W.; Ruijgrok, Th.W.

    1979-01-01

    The formation of the holding potential of physical adsorption is studied with a model in which a hydrogen atom interacts with a perfectly imaging substrate bounded by a sharp planar surface; the exclusion of the atomic electron from the substrate is an important boundary condition in the model. The

  14. Relationship between carbon microstructure, adsorption energy and hydrogen adsorption capacity at different temperatures

    International Nuclear Information System (INIS)

    Jagiello, J.; Thommes, M.

    2005-01-01

    Various microporous materials such as activated carbons, nano-tubes, synthetic micro-porous carbons as well as metal organic framework materials are being considered for hydrogen storage applications by means of physical adsorption. To develop materials of practical significance for hydrogen storage it is important to understand the relationships between pore sizes, adsorption energies and adsorption capacities. The pore size distribution (PSD) characterization is traditionally obtained from the analysis of nitrogen adsorption isotherms measured at 77 K. However, a portion of the pores accessible to H 2 may not be accessible to N 2 at this temperature. Therefore, it was recently proposed to use the DFT analysis of H 2 adsorption isotherms to characterize pore structure of materials considered for hydrogen storage applications [1]. In present work, adsorption isotherms of H 2 and N 2 at cryogenic temperatures are used for the characterization of carbon materials. Adsorption measurements were performed with Autosorb 1 MP [Quantachrome Instruments, Boynton Beach, Florida, USA]. As an example, Fig 1 compares PSDs calculated for the activated carbon sample (F400, Calgon Carbon) using combined H 2 and N 2 data, and using N 2 isotherm only. The nitrogen derived PSD does not include certain amount of micro-pores which are accessible to H 2 but not to N 2 molecules. Obviously, the difference in the calculated PSDs by the two methods will depend on the actual content of small micro-pores in a given sample. Carbon adsorption properties can also be characterized by the isosteric heat of adsorption, Qst, related to the adsorption energy and dependent on the carbon pore/surface structure. Fig 2 shows Qst data calculated using the Clausius-Clapeyron equation from H 2 isotherms measured at 77 K and 87 K for the carbon molecular sieve CMS 5A (Takeda), oxidized single wall nano-tubes (SWNT) [2], and graphitized carbon black (Supelco). The Qst values decrease with increasing pore

  15. Hydrogen adsorption and desorption with 3D silicon nanotube-network and film-network structures: Monte Carlo simulations

    International Nuclear Information System (INIS)

    Li, Ming; Kang, Zhan; Huang, Xiaobo

    2015-01-01

    Hydrogen is clean, sustainable, and renewable, thus is viewed as promising energy carrier. However, its industrial utilization is greatly hampered by the lack of effective hydrogen storage and release method. Carbon nanotubes (CNTs) were viewed as one of the potential hydrogen containers, but it has been proved that pure CNTs cannot attain the desired target capacity of hydrogen storage. In this paper, we present a numerical study on the material-driven and structure-driven hydrogen adsorption of 3D silicon networks and propose a deformation-driven hydrogen desorption approach based on molecular simulations. Two types of 3D nanostructures, silicon nanotube-network (Si-NN) and silicon film-network (Si-FN), are first investigated in terms of hydrogen adsorption and desorption capacity with grand canonical Monte Carlo simulations. It is revealed that the hydrogen storage capacity is determined by the lithium doping ratio and geometrical parameters, and the maximum hydrogen uptake can be achieved by a 3D nanostructure with optimal configuration and doping ratio obtained through design optimization technique. For hydrogen desorption, a mechanical-deformation-driven-hydrogen-release approach is proposed. Compared with temperature/pressure change-induced hydrogen desorption method, the proposed approach is so effective that nearly complete hydrogen desorption can be achieved by Si-FN nanostructures under sufficient compression but without structural failure observed. The approach is also reversible since the mechanical deformation in Si-FN nanostructures can be elastically recovered, which suggests a good reusability. This study may shed light on the mechanism of hydrogen adsorption and desorption and thus provide useful guidance toward engineering design of microstructural hydrogen (or other gas) adsorption materials

  16. Adsorption, hydrogenation and dehydrogenation of C2H on a CoCu bimetallic layer

    Science.gov (United States)

    Wu, Donghai; Yuan, Jinyun; Yang, Baocheng; Chen, Houyang

    2018-05-01

    In this paper, adsorption, hydrogenation and dehydrogenation of C2H on a single atomic layer of bimetallic CoCu were investigated using first-principles calculations. The CoCu bimetallic layer is formed by Cu replacement of partial Co atoms on the top layer of a Co(111) surface. Our adsorption and reaction results showed those sites, which have stronger adsorption energy of C2H, possess higher reactivity. The bimetallic layer possesses higher reactivity than either of the pure monometallic layer. A mechanism of higher reactivity of the bimetallic layer is proposed and identified, i.e. in the bimetallic catalyst, the catalytic performance of one component is promoted by the second component, and in our work, the catalytic performance of Co atoms in the bimetallic layer are improved by introducing Cu atoms, lowing the activation barrier of the reaction of C2H. The bimetallic layer could tune adsorption and reaction of C2H by modulating the ratio of Co and Cu. Results of adsorption energies and adsorption configurations reveal that C2H prefers to be adsorbed in parallel on both the pure Co metallic and CoCu bimetallic layers, and Co atoms in subsurface which support the metallic or bimetallic layer have little effect on C2H adsorption. For hydrogenation reactions, the products greatly depend on the concentration and initial positions of hydrogen atoms, and the C2H hydrogenation forming acetylene is more favorable than forming vinylidene in both thermodynamics and kinetics. This study would provide fundamental guidance for hydrocarbon reactions on Co-based and/or Cu-based bimetallic surface chemistry and for development of new bimetallic catalysts.

  17. Thermodynamics of hydrogen adsorption in MOF-177 at low temperatures: measurements and modelling

    Energy Technology Data Exchange (ETDEWEB)

    Poirier, Eric [College of Engineering, Purdue University, West Lafayette, IN 47907 (United States); Dailly, Anne [Chemical and Environmental Sciences Laboratory, General Motors Corporation, Warren, MI 48090 (United States)], E-mail: poirierem@gmail.com, E-mail: anne.dailly@gm.com

    2009-05-20

    Hydrogen adsorption measurements and modelling for the Zn-based microporous metal-organic framework (MOF) Zn{sub 4}O(1,3,5-benzenetribenzoate){sub 2}, MOF-177, were performed over the 50-77 K and 0-40 bar ranges. The maximum excess adsorption measured under these conditions varies over about 105-70 mg g{sup -1}. An analysis of the isotherms near saturation shows that hydrogen is ultimately adsorbed in an incompressible phase whose density is comparable to that of the bulk liquid. These liquid state properties observed under supercritical conditions reveal a remarkable effect of nanoscale confinement. The entire set of adsorption isotherms can be well described using a micropore filling model. The latter is used, in particular, to determine the absolute amounts adsorbed and the adsorption enthalpy. When expressed in terms of absolute adsorption, the isotherms show considerable hydrogen storage capacities, reaching up to 125 mg g{sup -1} at 50 K and 25 bar. The adsorption enthalpies are calculated as a function of fractional filling and range from 3 to 5 kJ mol{sup -1} in magnitude, in accordance with physisorption. These results are discussed with respect to a similar analysis performed on another Zn-based MOF, Zn{sub 4}O(1,4-benzenedicarboxylate){sub 3}, IRMOF-1, presented recently. It is found that both materials adsorb hydrogen by similar mechanisms.

  18. Thermodynamics of hydrogen adsorption in MOF-177 at low temperatures: measurements and modelling

    International Nuclear Information System (INIS)

    Poirier, Eric; Dailly, Anne

    2009-01-01

    Hydrogen adsorption measurements and modelling for the Zn-based microporous metal-organic framework (MOF) Zn 4 O(1,3,5-benzenetribenzoate) 2 , MOF-177, were performed over the 50-77 K and 0-40 bar ranges. The maximum excess adsorption measured under these conditions varies over about 105-70 mg g -1 . An analysis of the isotherms near saturation shows that hydrogen is ultimately adsorbed in an incompressible phase whose density is comparable to that of the bulk liquid. These liquid state properties observed under supercritical conditions reveal a remarkable effect of nanoscale confinement. The entire set of adsorption isotherms can be well described using a micropore filling model. The latter is used, in particular, to determine the absolute amounts adsorbed and the adsorption enthalpy. When expressed in terms of absolute adsorption, the isotherms show considerable hydrogen storage capacities, reaching up to 125 mg g -1 at 50 K and 25 bar. The adsorption enthalpies are calculated as a function of fractional filling and range from 3 to 5 kJ mol -1 in magnitude, in accordance with physisorption. These results are discussed with respect to a similar analysis performed on another Zn-based MOF, Zn 4 O(1,4-benzenedicarboxylate) 3 , IRMOF-1, presented recently. It is found that both materials adsorb hydrogen by similar mechanisms.

  19. Influence of surface treatments on micropore structure and hydrogen adsorption behavior of nanoporous carbons.

    Science.gov (United States)

    Kim, Byung-Joo; Park, Soo-Jin

    2007-07-15

    The scope of this work was to control the pore sizes of porous carbons by various surface treatments and to investigate the relation between pore structures and hydrogen adsorption capacity. The effects of various surface treatments (i.e., gas-phase ozone, anodic oxidation, fluorination, and oxygen plasma) on the micropore structures of porous carbons were investigated by N(2)/77 K isothermal adsorption. The hydrogen adsorption capacity was measured by H(2) isothermal adsorption at 77 K. In the result, the specific surface area and micropore volume of all of the treated samples were slightly decreased due to the micropore filling or pore collapsing behaviors. It was also found that in F(2)-treated carbons the center of the pore size distribution was shifted to left side, meaning that the average size of the micropores decreased. The F(2)- and plasma-treated samples showed higher hydrogen storage capacities than did the other samples, the F(2)-treated one being the best, indicating that the micropore size of the porous carbons played a key role in the hydrogen adsorption at 77 K.

  20. Adsorption and temperature-programmed desorption of hydrogen with dispersed platinum and platinum-gold catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, J.R.; Foger, K.; Breakspere, R.J.

    1979-05-01

    Adsorption and temperature-programmed desorption of hydrogen with dispersed platinum and platinum-gold catalysts was studied with 0.9-3Vertical Bar3< platinum on silica gel, aerosil, sodium and lanthanum Y zeolites, and ..gamma..-alumina, and on aerosil-supported gold-platinum alloys containing 2, 10, 24, 33, and 85Vertical Bar3< gold. Surface enrichment with gold in the alloy systems, as derived from hydrogen adsorption data and predicted from surface enrichment theory and electron microscopic measurements of particle size, were in good agreement, which indicated that equilibrium was achieved by the thermal treatment (oxygen at 573/sup 0/K, hydrogen at 620/sup 0/K, repeated cycles) used. Hydrogen spillover to gold was observed at the higher hydrogen pressures tested on the alloys with high gold content, and to the zeolite supports. The temperature-programed desorption profiles were independent of gold content, which indicated that gold acts only as diluent, and that isolated surface platinum atoms become populated with hydrogen atoms either by hydrogen atom spillover from platinum ensembles to gold and from the gold to the isolated platinum, and/or by adsorption of a molecule directly on the isolated platinum and chemisorption of one H atom at an adjacent gold atom. The distribution of surface platinum ensembles was evaluated by a computer simulation method.

  1. Hydrogen adsorption on N-decorated single wall carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Rangel, Eduardo [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, Apartado Postal 20-364, Codigo Postal 01000, Mexico D.F. (Mexico); Ruiz-Chavarria, Gregorio [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, Apartado Postal 20-364, Codigo Postal 01000, Mexico D.F. (Mexico); Departamento de Fisica, Facultad de Ciencias, Universidad Nacional Autonoma de Mexico Ciudad Universitaria, Codigo Postal 04510, Mexico D.F. (Mexico); Magana, L.F., E-mail: fernando@fisica.unam.m [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, Apartado Postal 20-364, Codigo Postal 01000, Mexico D.F. (Mexico); Arellano, J.S. [Departamento de Ciencias Basicas, Universidad Autonoma Metropolitana, Unidad Azcapotzalco. Avenida San Pablo No. 180, Col. Reynosa Tamaulipas Codigo Postal 02200, Mexico D.F. (Mexico)

    2009-07-06

    Using density functional theory and molecular dynamics we found that N-decorated single walled (8,0) carbon nanotubes are potential high capacity hydrogen storage media. This system could store up to 6.0 wt% hydrogen at 300 K and ambient pressure, with average adsorption energy of -80 meV/(H{sub 2}). Nitrogen coverage was C{sub 8}N.

  2. Hydrogen adsorption on N-decorated single wall carbon nanotubes

    International Nuclear Information System (INIS)

    Rangel, Eduardo; Ruiz-Chavarria, Gregorio; Magana, L.F.; Arellano, J.S.

    2009-01-01

    Using density functional theory and molecular dynamics we found that N-decorated single walled (8,0) carbon nanotubes are potential high capacity hydrogen storage media. This system could store up to 6.0 wt% hydrogen at 300 K and ambient pressure, with average adsorption energy of -80 meV/(H 2 ). Nitrogen coverage was C 8 N.

  3. Hydrogen adsorption in carbon nanostructures compared

    International Nuclear Information System (INIS)

    Schimmel, H.G.; Nijkamp, G.; Kearley, G.J.; Rivera, A.; Jong, K.P. de; Mulder, F.M.

    2004-01-01

    Recent reports continue to suggest high hydrogen storage capacities for some carbon nanostructures due to a stronger interaction between hydrogen and carbon. Here the interaction of hydrogen with activated charcoal, carbon nanofibers, single walled carbon nanotubes (SWNT), and electron beam 'opened' SWNT are compared and shown to be similar. The storage capacity below 77 K of these materials correlates with the surface area of the material with the activated charcoal having the largest. SWNT and 'opened' SWNT have a relatively low accessible surface area due to bundling of the tubes. Pressure-temperature curves give the interaction potential, which was found to be ∼580 K or 50 meV in all samples, leading to significant adsorption below ∼50 K. Using the inelastic neutron scattering signal associated with rotation of the hydrogen molecule as a sensitive probe for the surroundings of the molecule, no difference was found between the hydrogen molecules adsorbed in the investigated materials. These combined spectroscopic and macroscopic results show that SWNT, nanofibers and activated carbons store molecular hydrogen due to their graphitic nature and not because they possess special morphologies. Results from a density functional theory computer calculation suggest molecular hydrogen bonding to an aromatic C-C bond of graphite, irrespective of the surface morphology farther away

  4. Hydrogen adsorption in HKUST-1: a combined inelastic neutron scattering and first-principles study

    International Nuclear Information System (INIS)

    Brown, Craig M; Liu Yun; Yildirim, Taner; Peterson, Vanessa K; Kepert, Cameron J

    2009-01-01

    Hydrogen adsorption in high surface area nanoporous coordination polymers has attracted a great deal of interest in recent years due to the potential applications in energy storage. Here we present combined inelastic neutron scattering measurements and detailed first-principles calculations aimed at unraveling the nature of hydrogen adsorption in HKUST-1 (Cu 3 (1,3,5-benzenetricarboxylate) 2 ), a metal-organic framework (MOF) with unsaturated metal centers. We reveal that, in this system, the major contribution to the overall binding comes from the classical Coulomb interaction which is not screened due to the open metal site; this explains the relatively high binding energies and short H 2 -metal distances observed in MOFs with exposed metal sites as compared to traditional ones. Despite the short distances, there is no indication of an elongation of the H-H bond for the bound H 2 molecule at the metal site. We find that both the phonon and rotational energy levels of the hydrogen molecule are closely similar, making the interpretation of the inelastic neutron scattering data difficult. Finally, we show that the orientation of H 2 has a surprisingly large effect on the binding potential, reducing the classical binding energy by almost 30%. The implication of these results for the development of MOF materials for better hydrogen storage is discussed.

  5. Hydrogen adsorption in HKUST-1: a combined inelastic neutron scattering and first-principles study

    Energy Technology Data Exchange (ETDEWEB)

    Brown, Craig M; Liu Yun; Yildirim, Taner [National Institute of Standards and Technology Center for Neutron Research, 100 Bureau Drive, MS 6102 (United States); Peterson, Vanessa K [Bragg Institute, Australian Nuclear Science and Technology Organisation, Menai, NSW 2234 (Australia); Kepert, Cameron J [School of Chemistry, The University of Sydney, NSW 2006 (Australia)], E-mail: craig.brown@nist.gov

    2009-05-20

    Hydrogen adsorption in high surface area nanoporous coordination polymers has attracted a great deal of interest in recent years due to the potential applications in energy storage. Here we present combined inelastic neutron scattering measurements and detailed first-principles calculations aimed at unraveling the nature of hydrogen adsorption in HKUST-1 (Cu{sub 3}(1,3,5-benzenetricarboxylate){sub 2}), a metal-organic framework (MOF) with unsaturated metal centers. We reveal that, in this system, the major contribution to the overall binding comes from the classical Coulomb interaction which is not screened due to the open metal site; this explains the relatively high binding energies and short H{sub 2}-metal distances observed in MOFs with exposed metal sites as compared to traditional ones. Despite the short distances, there is no indication of an elongation of the H-H bond for the bound H{sub 2} molecule at the metal site. We find that both the phonon and rotational energy levels of the hydrogen molecule are closely similar, making the interpretation of the inelastic neutron scattering data difficult. Finally, we show that the orientation of H{sub 2} has a surprisingly large effect on the binding potential, reducing the classical binding energy by almost 30%. The implication of these results for the development of MOF materials for better hydrogen storage is discussed.

  6. Hydrogen adsorption in HKUST-1: a combined inelastic neutron scattering and first-principles study

    Science.gov (United States)

    Brown, Craig M.; Liu, Yun; Yildirim, Taner; Peterson, Vanessa K.; Kepert, Cameron J.

    2009-05-01

    Hydrogen adsorption in high surface area nanoporous coordination polymers has attracted a great deal of interest in recent years due to the potential applications in energy storage. Here we present combined inelastic neutron scattering measurements and detailed first-principles calculations aimed at unraveling the nature of hydrogen adsorption in HKUST-1 (Cu3(1,3,5-benzenetricarboxylate)2), a metal-organic framework (MOF) with unsaturated metal centers. We reveal that, in this system, the major contribution to the overall binding comes from the classical Coulomb interaction which is not screened due to the open metal site; this explains the relatively high binding energies and short H2-metal distances observed in MOFs with exposed metal sites as compared to traditional ones. Despite the short distances, there is no indication of an elongation of the H-H bond for the bound H2 molecule at the metal site. We find that both the phonon and rotational energy levels of the hydrogen molecule are closely similar, making the interpretation of the inelastic neutron scattering data difficult. Finally, we show that the orientation of H2 has a surprisingly large effect on the binding potential, reducing the classical binding energy by almost 30%. The implication of these results for the development of MOF materials for better hydrogen storage is discussed.

  7. Adsorption of triton X100 and potassium hydrogen phthalate on granular activated carbon from date pits

    Energy Technology Data Exchange (ETDEWEB)

    Merzougui, Z.; Nedjah, S.; Azoudj, Y.; Addoun, F. [Laboratoire d' etude physic-chimique des materiaux et application a l' environnement, Faculte de Chimie, USTHB (Algeria)], E-mail: zmerzougi@yahoo.fr

    2011-07-01

    Activated carbons, thanks to their versatility, are being used in the water treatment sector to absorb pollutants. Several factors influence the adsorption capacity of activated carbon and the aim of this study was to assess the effects of the porous texture and chemical nature of activated carbons on the adsorption of triton X100 and potassium hydrogen phthalate. Activated carbons used in this study were prepared from date pits with ZnCl2, KOH and H3PO4 by carbonization without adjuvant and adsorption of triton X100 and potassium hydrogen phthalate was conducted at 298K. Results showed that activated carbons prepared from date pits have a great potential for removing organic and inorganic pollutants from water and that the adsorption potential depends on the degree of activation of the activated carbons and on the compounds to absorb. This study highlighted that an increase of the carbon surface area and porosity results in a better adsorption capacity.

  8. Hydrogen adsorption properties of polymer-derived nanoporous SiC{sub x} fibers

    Energy Technology Data Exchange (ETDEWEB)

    Chu, Zengyong; He, Rongan; Zhang, Xiaobin; Cheng, Haifeng; Li, Xiaodong; Wang, Yingde [State Key Laboratory of Advanced Ceramic Fibers and Composites, National University of Defense Technology, Changsha 410073 (China)

    2010-04-15

    In an effort to prepare new hydrogen storage materials, we successfully obtained three types of polymer-derived nanoporous SiC{sub x} (x = 5-7) fibers, whose specific surface areas (SSAs) are larger than 580 m{sup 2}/g. Their hydrogen adsorption properties were studied with a comparison of multi-walled carbon nanotubes (MWCNTs). The results reveal that micropores play a predominant role in hydrogen adsorptions at 77 K and at pressures below 0.5 MPa, and mesopores begin to take greater effect when the pressure increases beyond 0.5 MPa. The maximum hydrogen storage capacity (HSC), 0.33 wt% at 302 K and 4 MPa, was achieved for SiC{sub x}-KN fibers with SSA of 990 m{sup 2}/g, while the HSC of the MWCNTs is 0.09 wt% at the same conditions. For these new materials, this work demonstrates that small pore size, large micropore volume and large SSA are all beneficial for the high hydrogen uptake. It can also be deduced from the work that the HSC of the SiC{sub x} fibers could be further increased if the crystallinity and the composition are better controlled. (author)

  9. Comparison of reactivity on step and terrace sites of Pd (3 3 2) surface for the dissociative adsorption of hydrogen: A quantum chemical molecular dynamics study

    International Nuclear Information System (INIS)

    Ahmed, Farouq; Nagumo, Ryo; Miura, Ryuji; Ai, Suzuki; Tsuboi, Hideyuki; Hatakeyama, Nozomu; Endou, Akira; Takaba, Hiromitsu; Kubo, Momoji; Miyamoto, Akira

    2011-01-01

    The notion of 'active sites' is fundamental to heterogeneous catalysis. However, the exact nature of the active sites, and hence the mechanism by which they act, are still largely a matter of speculation. In this study, we have presented a systematic quantum chemical molecular dynamics (QCMD) calculations for the interaction of hydrogen on different step and terrace sites of the Pd (3 3 2) surface. Finally the dissociative adsorption of hydrogen on step and terrace as well as the influence of surface hydrogen vacancy for the dissociative adsorption of hydrogen has been investigated through QCMD. This is a state-of-the-art method for calculating the interaction of atoms and molecules with metal surfaces. It is found that fully hydrogen covered (saturated) step sites can dissociate hydrogen moderately and that a monovacancy surface is suitable for significant dissociative adsorption of hydrogen. However in terrace site of the surface we have found that dissociation of hydrogen takes place only on Pd sites where the metal atom is not bound to any pre-adsorbed hydrogen atoms. Furthermore, from the molecular dynamics and electronic structure calculations, we identify a number of consequences for the interpretation and modeling of diffusion experiments demonstrating the coverage and directional dependence of atomic hydrogen diffusion on stepped palladium surface.

  10. Hydrogen spillover phenomenon: Enhanced reversible hydrogen adsorption/desorption at Ta{sub 2}O{sub 5}-coated Pt electrode in acidic media

    Energy Technology Data Exchange (ETDEWEB)

    Sata, Shunsuke [Department of Electronic Chemistry, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259-G1-5 Nagatsuta, Midori-ku, Yokohama 226-8502 (Japan); Awad, Mohamed I.; El-Deab, Mohamed S. [Department of Electronic Chemistry, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259-G1-5 Nagatsuta, Midori-ku, Yokohama 226-8502 (Japan); Department of Chemistry, Faculty of Science, Cairo University, Cairo (Egypt); Okajima, Takeyoshi [Department of Electronic Chemistry, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259-G1-5 Nagatsuta, Midori-ku, Yokohama 226-8502 (Japan); Ohsaka, Takeo, E-mail: ohsaka@echem.titech.ac.j [Department of Electronic Chemistry, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259-G1-5 Nagatsuta, Midori-ku, Yokohama 226-8502 (Japan)

    2010-04-01

    The current study is concerned with the preparation and characterization of tantalum oxide-loaded Pt (TaO{sub x}/Pt) electrodes for hydrogen spillover application. XPS, SEM, EDX and XRD techniques are used to characterize the TaO{sub x}/Pt surfaces. TaO{sub x}/Pt electrodes were prepared by galvanostatic electrodeposition of Ta on Pt from LiF-NaF (60:40 mol%) molten salts containing K{sub 2}TaF{sub 7} (20 wt%) at 800 deg. C and then by annealing in air at various temperatures (200, 400 and 600 deg. C). The thus-fabricated TaO{sub x}/Pt electrodes were compared with the non-annealed Ta/Pt and the unmodified Pt electrodes for the hydrogen adsorption/desorption (H{sub ads}/H{sub des}) reaction. The oxidation of Ta to the stoichiometric oxide (Ta{sub 2}O{sub 5}) increases with increasing the annealing temperature as revealed from XPS and X-ray diffraction (XRD) measurements. The higher the annealing temperature the larger is the enhancement in the H{sub ads}/H{sub des} reaction at TaO{sub x}/Pt electrode. The extraordinary increase in the hydrogen adsorption/desorption at the electrode annealed at 600 deg. C is explained on the basis of a hydrogen spillover-reverse spillover mechanism. The hydrogen adsorption at the TaO{sub x}/Pt electrode is a diffusion-controlled process.

  11. FTIR spectroscopic and computational studies on hydrogen adsorption on the zeolite Li-FER

    Czech Academy of Sciences Publication Activity Database

    Nachtigall, Petr; Garrone, E.; Palomino, G. T.; Delgado, M. R.; Nachtigallová, Dana; Areán, C. O.

    2006-01-01

    Roč. 8, č. 19 (2006), s. 2286-2292 ISSN 1463-9076 R&D Projects: GA MŠk(CZ) LC512; GA ČR(CZ) GA203/06/0324 Grant - others:UIB(ES) MAT-2005-05350; MIUR(IT) FISR2004 Institutional research plan: CEZ:AV0Z40550506 Keywords : adsorption * hydrogen storage * spectroscopy Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.892, year: 2006

  12. Hydrogen adsorption on metal-organic frameworks (MOFs) and single-walled carbon nanotubes (SWNTs)

    Energy Technology Data Exchange (ETDEWEB)

    Poirier, E.; Chahine, R.; Benard, P.; Lafi, L.; Dorval-Douville, G.; Chandonia, P.-A. [Univ. du Quebec a Trois-Rivieres, Inst. de recherche sur l' hydrogene, Trois-Rivieres, Quebec (Canada)]. E-mail: Lyubov.Lafi@uqtr.ca

    2006-07-01

    'Full text:' In recent years, several novel carbon-based microporous materials such as single-walled carbon nanotubes (SWNTs) and metal-organic frameworks (MOFs) have been proposed as promising adsorbents for hydrogen. Hydrogen adsorption measurements on Al-, Cr- and Zn-based metal-organic frameworks (MOFs) and single-walled carbon nanotubes (SWNTs) are presented. The measurements were performed at temperatures ranging from 77 to 300K and pressures up to 50 atm using a volumetric approach. The maximum excess adsorption at 77K ranges from 2,8 to 3,9 wt % for the MOFs and from 1,5 to 2,5 wt % for the SWNTs. These values are reached at pressures below 40 atm. At room temperature and 40 atm, modest amounts of hydrogen are adsorbed (< 0,4 wt %). A Dubinin-Astakhov (DA) approach is used to investigate the measured adsorption isotherms and retrieve energetic and structural parameters. The adsorption enthalpy averaged over filling is found to be about 2,9 kJ/mol for the MOF-5 and about 3,6 - 4,2 kJ/mol for SWNTs. The uptake of hydrogen on SWNTs and MOF-5 appears to be due to physisorption and can be described, through the DA-model, by a traditional theory of micropore filling. (author)

  13. Effect on hydrogen adsorption due to a lonely or a pair of carbon vacancies on the graphene layer

    International Nuclear Information System (INIS)

    Arellano, J S

    2017-01-01

    The influence on the hydrogen molecule adsorption on a pristine and a defective graphene layer is compared. The different lengths for the C-C bonds on the graphene layer with one vacancy are visualized and compared respect to pristine graphene. The energy of formation of one vacancy is calculated and a comparison of the binding energy for the hydrogen molecule is presented when the molecule is adsorbed on pristine graphene or on the defective graphene layer. The adsorption is studied for a single vacancy and at least for two different pairs of carbon vacancies. The qualitative general result, and contrary to the expected effect of the carbon vacancies on the hydrogen adsorption is that the rearrangement of the carbon atoms on the defective graphene layer allows only a relatively small increase in the magnitude of the binding energy for the hydrogen molecule. (paper)

  14. Design and synthesis of vanadium hydrazide gels for Kubas-type hydrogen adsorption: a new class of hydrogen storage materials.

    Science.gov (United States)

    Hoang, Tuan K A; Webb, Michael I; Mai, Hung V; Hamaed, Ahmad; Walsby, Charles J; Trudeau, Michel; Antonelli, David M

    2010-08-25

    In this paper we demonstrate that the Kubas interaction, a nondissociative form of weak hydrogen chemisorption with binding enthalpies in the ideal 20-30 kJ/mol range for room-temperature hydrogen storage, can be exploited in the design of a new class of hydrogen storage materials which avoid the shortcomings of hydrides and physisorpion materials. This was accomplished through the synthesis of novel vanadium hydrazide gels that use low-coordinate V centers as the principal Kubas H(2) binding sites with only a negligible contribution from physisorption. Materials were synthesized at vanadium-to-hydrazine ratios of 4:3, 1:1, 1:1.5, and 1:2 and characterized by X-ray powder diffraction, X-ray photoelectron spectroscopy, nitrogen adsorption, elemental analysis, infrared spectroscopy, and electron paramagnetic resonance spectroscopy. The material with the highest capacity possesses an excess reversible storage of 4.04 wt % at 77 K and 85 bar, corresponding to a true volumetric adsorption of 80 kg H(2)/m(3) and an excess volumetric adsorption of 60.01 kg/m(3). These values are in the range of the ultimate U.S. Department of Energy goal for volumetric density (70 kg/m(3)) as well as the best physisorption material studied to date (49 kg H(2)/m(3) for MOF-177). This material also displays a surprisingly high volumetric density of 23.2 kg H(2)/m(3) at room temperature and 85 bar--roughly 3 times higher than that of compressed gas and approaching the DOE 2010 goal of 28 kg H(2)/m(3). These materials possess linear isotherms and enthalpies that rise on coverage and have little or no kinetic barrier to adsorption or desorption. In a practical system these materials would use pressure instead of temperature as a toggle and can thus be used in compressed gas tanks, currently employed in many hydrogen test vehicles, to dramatically increase the amount of hydrogen stored and therefore the range of any vehicle.

  15. Analysis of oxygen and hydrogen adsorption on Nb(100) surface by scanning tunneling microscopy

    International Nuclear Information System (INIS)

    An, Bai; Wen, Mao; Fukuyama, Seiji; Yokogawa, Kiyoshi; Ichimura, Shingo; Yoshimura, Masamichi

    2006-01-01

    The surface structure of Nb(100) under the condition of cleaning, oxidation and hydrogen adsorption is observed by STM (scanning tunneling microscopy). The results obtained are followings; (1) (3 x 1)-O→(4 x 1)-O→c(2 x 2)-O→clean(1 x 1)structure was observed by atom level, and these atomic models of structures and STM images were verified by the first-principles calculations, (2) when the clean(1 x 1) structure exposed to hydrogen, dissociative adsorption of hydrogen was observed and Nb hydride cluster formed on the surface at room temperature. It was heated at about 450 - 670 K in UHV, the cluster decomposed into hydrogen and (1 x 1) structure with linear defect was formed. The c(2 x 2)-O structure by oxygen adsorption transformed into (1 x 1)-H structure with OH and Nb hydride cluster under hydrogen gas at room temperature. When it was heated in UHV at 640 K, OH desorbed from the surface and (1 x 1) structure with linear defect was generated. The surface of (3 x 1)-O structure was not changed by hydrogen. (S.Y.)

  16. Ab initio study of hydrogen adsorption on benzenoid linkers in metal-organic framework materials

    International Nuclear Information System (INIS)

    Gao Yi; Zeng, X C

    2007-01-01

    We have computed the energies of adsorption of molecular hydrogen on a number of molecular linkers in metal-organic framework solid materials using density functional theory (DFT) and ab initio molecular orbital methods. We find that the hybrid B3LYP (Becke three-parameter Lee-Yang-Parr) DFT method gives a qualitatively incorrect prediction of the hydrogen binding with benzenoid molecular linkers. Both local-density approximation (LDA) and generalized gradient approximation (GGA) DFT methods are inaccurate in predicting the values of hydrogen binding energies, but can give a qualitatively correct prediction of the hydrogen binding. When compared to the more accurate binding-energy results based on the ab initio Moeller-Plesset second-order perturbation (MP2) method, the LDA results may be viewed as an upper limit while the GGA results may be viewed as a lower limit. Since the MP2 calculation is impractical for realistic metal-organic framework systems, the combined LDA and GGA calculations provide a cost-effective way to assess the hydrogen binding capability of these systems

  17. Adsorption of cadmium ions on nickel surface skeleton catalysts and its effect on reaction of cathodic hydrogen evolution

    International Nuclear Information System (INIS)

    Korovin, N.V.; Udris, E.Ya.; Savel'eva, O.N.

    1986-01-01

    Cadmium adsorption from different concentration CdSO 4 solutions on nickel surface skeleton catalysts (Ni ssc ) is studied by recording of polarization and potentiodynamic curves using electron microscopy and X-ray spectrometry. Main regularities of cadmium adsorption on Ni ssc are shown to be similar to those on smooth and skeleton nickel. A conclusion is drawn that increase of catalytic activity in reaction of cathodic hydrogen evolution from alkali solutions of Ni ssc base electrodes after their treatment in solutions containing Cd 2+ ions is due to irreversible desorption of strongly and averagely bound hydrogen from electrode surface at cadmium adsorption on them

  18. Cryogenic adsorption of low-concentration hydrogen on charcoal, 5A molecular sieve, sodalite, ZSM-5 and Wessalith DAY

    International Nuclear Information System (INIS)

    Willms, R.S.

    1993-01-01

    The separation of low-concentration hydrogen isotopes from helium is a processing step that is required for ceramic lithium breeding blanket processing. Cryogenic adsorption is one method of effecting this separation. In this study live adsorbents were considered for this purpose: charcoal, 5A molecular sieve, UOP S-115, ZSM-5 and Wessalith DAY. The first two adsorbents exhibit good equilibrium loadings and are shown to be quite effective at adsorbing low-concentration hydrogen isotopes. The latter three adsorbents display considerably lower equilibrium loadings. This study concludes that by using either charcoal or 5A molecular sieve, cryogenic adsorption would be an effective means of separating hydrogen isotopes from helium

  19. Final Report: Characterization of Hydrogen Adsorption in Carbon-Based Materials by NMR

    International Nuclear Information System (INIS)

    Wu, Yue; Kleinhammes, Alfred

    2011-01-01

    is well suited for hydrogen storage due to its controlled microporous structure and large surface area; and (4) A new porosimetry method for evaluating the pore landscape using H2 as a probe was developed. 1H NMR can probe the nanoscale pore structure of synthesized material and can assess the pore dimension over a range covering 1.2 nm to 2.5 nm, the size that is desired for H2 adsorption. Analysis of 1H NMR spectra in conjunction with the characterization of the bonding structure of the adsorbent by 13C NMR distinguishes between a heterogeneous and homogeneous pore structure as evidenced by the work on AX21 and activated PEEK. Most of the sorbents studied are suited to hydrogen storage at low temperature (T < 100K). Of the materials investigated, only boron substituted graphite has the potential to work at higher temperatures if the boron content in the favorable planar BC3 configuration that actively contributes to adsorption can be increased.

  20. Final Report: Characterization of Hydrogen Adsorption in Carbon-Based Materials by NMR

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Yue; Kleinhammes, Alfred

    2011-07-11

    activated PEEK is well suited for hydrogen storage due to its controlled microporous structure and large surface area. • A new porosimetry method for evaluating the pore landscape using H2 as a probe was developed. 1H NMR can probe the nanoscale pore structure of synthesized material and can assess the pore dimension over a range covering 1.2 nm to 2.5 nm, the size that is desired for H2 adsorption. • Analysis of 1H NMR spectra in conjunction with the characterization of the bonding structure of the adsorbent by 13C NMR distinguishes between a heterogeneous and homogeneous pore structure as evidenced by the work on AX21 and activated PEEK. • Most of the sorbents studied are suited to hydrogen storage at low temperature (T < 100K). Of the materials investigated, only boron substituted graphite has the potential to work at higher temperatures if the boron content in the favorable planar BC3 configuration that actively contributes to adsorption can be increased.

  1. Effect of controlled deactivation on the thermochemical characteristics of hydrogen adsorption on skeletal nickel from sodium hydroxide-water solutions

    Science.gov (United States)

    Prozorov, D. A.; Lukin, M. V.; Ulitin, M. V.

    2013-04-01

    Differential heats of adsorption in a wide range of surface coverage and maximum amounts of adsorbed hydrogen are determined by adsorption calorimetry on partially deactivated skeletal nickel from aqueous solutions of sodium hydroxide. The effect of the composition of solutions on the values of limiting adsorption and adsorption equilibria of individual forms of hydrogen is shown.

  2. A comparative analysis of the cryo-compression and cryo-adsorption hydrogen storage methods

    Energy Technology Data Exchange (ETDEWEB)

    Petitpas, G [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Benard, P [Universite du Quebec a Trois-Rivieres (Canada); Klebanoff, L E [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Xiao, J [Universite du Quebec a Trois-Rivieres (Canada); Aceves, S M [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2014-07-01

    While conventional low-pressure LH₂ dewars have existed for decades, advanced methods of cryogenic hydrogen storage have recently been developed. These advanced methods are cryo-compression and cryo-adsorption hydrogen storage, which operate best in the temperature range 30–100 K. We present a comparative analysis of both approaches for cryogenic hydrogen storage, examining how pressure and/or sorbent materials are used to effectively increase onboard H₂ density and dormancy. We start by reviewing some basic aspects of LH₂ properties and conventional means of storing it. From there we describe the cryo-compression and cryo-adsorption hydrogen storage methods, and then explore the relationship between them, clarifying the materials science and physics of the two approaches in trying to solve the same hydrogen storage task (~5–8 kg H₂, typical of light duty vehicles). Assuming that the balance of plant and the available volume for the storage system in the vehicle are identical for both approaches, the comparison focuses on how the respective storage capacities, vessel weight and dormancy vary as a function of temperature, pressure and type of cryo-adsorption material (especially, powder MOF-5 and MIL-101). By performing a comparative analysis, we clarify the science of each approach individually, identify the regimes where the attributes of each can be maximized, elucidate the properties of these systems during refueling, and probe the possible benefits of a combined “hybrid” system with both cryo-adsorption and cryo-compression phenomena operating at the same time. In addition the relationships found between onboard H₂ capacity, pressure vessel and/or sorbent mass and dormancy as a function of rated pressure, type of sorbent material and fueling conditions are useful as general designing guidelines in future engineering efforts using these two hydrogen storage approaches.

  3. Textural development and hydrogen adsorption of carbon materials from PET waste

    International Nuclear Information System (INIS)

    Parra, J.B.; Ania, C.O.; Arenillas, A.; Rubiera, F.; Palacios, J.M.; Pis, J.J.

    2004-01-01

    Polyethyleneterephthalate (PET) has become one of the major post-consumer plastic wastes. PET products present a problem of considerable concern due to the huge amount of solid waste produced. The disposal of this waste, together with its low bio- and photo-degradability represents a serious challenge for industrial countries all over the world. Pyrolysis could provide an alternative and economically viable route for processing PET waste due to the potential uses of different by-products: energy from the pyrolysis gases (58% yield in this work), recovery of terephthalic acid and other subproducts (20%), and a solid residue (22%), which has shown a high textural development after activation. The pyrolysis of PET waste was performed in a quartz reactor (i.d. 35 mm) under an inert atmosphere. Further activation was carried out at a temperature of 925 deg. C, with a flow rate of 10 ml min -1 of CO 2 . A series of carbon materials with different burn-off degrees was obtained. Textural characterisation of the samples was carried out by performing N 2 adsorption isotherms at -196 deg. C. Changes in the morphological and structural properties of chars were studied by scanning electron microscopy (SEM) and X-ray diffraction (XRD). The carbons obtained were isotropic and highly microporous materials with apparent BET surface areas of up to 2500 m 2 g -1 . The suitability of the samples for hydrogen storage was studied by performing H 2 adsorption measurements in the 0-1 bar pressure range. Adsorption-desorption experiments showed that reversible physisorption takes place in all the samples. The hydrogen adsorption capacities of the activated PET waste compare favourably well with those attained with high-value carbon materials

  4. The effect of amorphous silicon surface hydrogenation on morphology, wettability and its implication on the adsorption of proteins

    Energy Technology Data Exchange (ETDEWEB)

    Filali, Larbi, E-mail: larbifilali5@gmail.com [Laboratoire de Physique des Couches Minces et Matériaux pour l' Electronique, Université d' Oran 1, Ahmed Ben Bella, BP 1524, El M' naouar 31100 Oran (Algeria); Brahmi, Yamina; Sib, Jamal Dine [Laboratoire de Physique des Couches Minces et Matériaux pour l' Electronique, Université d' Oran 1, Ahmed Ben Bella, BP 1524, El M' naouar 31100 Oran (Algeria); Bouhekka, Ahmed [Laboratoire de Physique des Couches Minces et Matériaux pour l' Electronique, Université d' Oran 1, Ahmed Ben Bella, BP 1524, El M' naouar 31100 Oran (Algeria); Département de Physique, Université Hassiba Ben Bouali, 02000 Chlef (Algeria); Benlakehal, Djamel; Bouizem, Yahya; Kebab, Aissa; Chahed, Larbi [Laboratoire de Physique des Couches Minces et Matériaux pour l' Electronique, Université d' Oran 1, Ahmed Ben Bella, BP 1524, El M' naouar 31100 Oran (Algeria)

    2016-10-30

    Highlights: • Hydrogenation of the surfaces had the effect of reducing the roughness by way of shadow etching. • Roughness was the driving factor affecting the wettability of the hydrogenated surfaces. • Bovine Serum Albumin proteins favored the surfaces with highest hydrogen content. • Surface modification induced secondary structure change of adsorbed proteins. - Abstract: We study the effect of amorphous silicon (a-Si) surface hydrogenation on Bovine Serum Albumin (BSA) adsorption. A set of (a-Si) films was prepared by radio frequency magnetron sputtering (RFMS) and after deposition; they were treated in molecular hydrogen ambient at different pressures (1–3 Pa). Fourier transform infrared attenuated total reflection (FTIR-ATR) spectroscopy and spectroscopic ellipsometry (SE) were used to study the hydrogenation effect and BSA adsorption. Atomic force microscopy (AFM) was used to evaluate morphological changes caused by hydrogenation. The wettability of the films was measured using contact angle measurement, and in the case of the hydrogenated surfaces, it was found to be driven by surface roughness. FTIR-ATR spectroscopy and SE measurements show that proteins had the strongest affinity toward the surfaces with the highest hydrogen content and their secondary structure was affected by a significant decrease of the α-helix component (-27%) compared with the proteins adsorbed on the un-treated surface, which had a predominantly α-helix (45%) structure. The adsorbed protein layer was found to be densely packed with a large thickness (30.9 nm) on the hydrogen-rich surfaces. The most important result is that the surface hydrogen content was the dominant factor, compared to wettability and morphology, for protein adsorption.

  5. Substituent effects in heterogeneous catalysis--4. Adsorption estimations during competitive hydrogenation of cyclohexanone and its 2-alkyl derivatives

    Energy Technology Data Exchange (ETDEWEB)

    Chihara, T; Tanaka, K

    1979-02-01

    Adsorption estimations during competitive hydrogenation of cyclohexanone and its 2-alkyl derivatives alumina-supported ruthenium, rhodium, and platinum catalysts were obtained in a study to determine the relative contributions of the rate constants and the adsorption equilibrium constants to the substituent-dependent constant. The reaction rates obtained during competitive hydrogenation were in the order cyclohexanone (A) Vertical Bar3:Vertical Bar3: 2-methyl cyclohexanone (B) Vertical Bar3: 2-ethyl cyclohexanone (C) Vertical Bar3: 2-propyl cyclohexanone (D) for all catalysts, whereas the rates obtained during individual hydrogenation were in the order A Vertical Bar3: B approx. C approx. D. The adsorption equilibrium constants which were estimated by analyzing the kinetic data agreed well with the theoretical values derived from statistical mechanics by using a model in which the substrate ketones were immobilely adsorbed.

  6. On the nature of gallium species in gallium-modified mordenite and MFI zeolites. A comparative DRIFT study of carbon monoxide adsorption and hydrogen dissociation.

    Science.gov (United States)

    Serykh, Alexander I; Kolesnikov, Stanislav P

    2011-04-21

    The results of a DRIFT study of carbon monoxide molecular adsorption and hydrogen dissociative adsorption on gallium-modified mordenite and MFI (ZSM-5) zeolites are presented. It was found that in the reduced gallium-modified mordenite (Ga-MOR) both Ga(3+) and Ga(+) exchanged cations are present and can be detected by CO adsorption. Ga(3+) cations in Ga-MOR dissociatively adsorb molecular hydrogen at elevated temperatures, resulting in the formation of gallium hydride species and acidic hydroxyl groups. In the reduced Ga-MFI evacuated at 823 K under medium vacuum conditions only Ga(+) exchanged intrazeolite cations were detected. It was found, however, that Ga(3+) intrazeolite exchanged cations which form upon high-temperature disproportionation of Ga(+) cations in the reduced Ga-MFI and Ga-MOR can be stabilized by high-temperature oxidation of these zeolites.

  7. Textural development and hydrogen adsorption of carbon materials from PET waste

    Energy Technology Data Exchange (ETDEWEB)

    Parra, J.B.; Ania, C.O.; Arenillas, A.; Rubiera, F.; Palacios, J.M.; Pis, J.J

    2004-10-06

    Polyethyleneterephthalate (PET) has become one of the major post-consumer plastic wastes. PET products present a problem of considerable concern due to the huge amount of solid waste produced. The disposal of this waste, together with its low bio- and photo-degradability represents a serious challenge for industrial countries all over the world. Pyrolysis could provide an alternative and economically viable route for processing PET waste due to the potential uses of different by-products: energy from the pyrolysis gases (58% yield in this work), recovery of terephthalic acid and other subproducts (20%), and a solid residue (22%), which has shown a high textural development after activation. The pyrolysis of PET waste was performed in a quartz reactor (i.d. 35 mm) under an inert atmosphere. Further activation was carried out at a temperature of 925 deg. C, with a flow rate of 10 ml min{sup -1} of CO{sub 2}. A series of carbon materials with different burn-off degrees was obtained. Textural characterisation of the samples was carried out by performing N{sub 2} adsorption isotherms at -196 deg. C. Changes in the morphological and structural properties of chars were studied by scanning electron microscopy (SEM) and X-ray diffraction (XRD). The carbons obtained were isotropic and highly microporous materials with apparent BET surface areas of up to 2500 m{sup 2} g{sup -1}. The suitability of the samples for hydrogen storage was studied by performing H{sub 2} adsorption measurements in the 0-1 bar pressure range. Adsorption-desorption experiments showed that reversible physisorption takes place in all the samples. The hydrogen adsorption capacities of the activated PET waste compare favourably well with those attained with high-value carbon materials.

  8. Hydrogen molecule on lithium adsorbed graphene: A DFT study

    International Nuclear Information System (INIS)

    Kaur, Gagandeep; Gupta, Shuchi; Gaganpreet; Dharamvir, Keya

    2016-01-01

    Electronic structure calculations for the adsorption of molecular hydrogen on lithium (Li) decorated and pristine graphene have been studied systematically using SIESTA code [1] within the framework of the first-principle DFT under the Perdew-Burke-Ernzerhof (PBE) form of the generalized gradient approximation (GGA)[2], including spin polarization. The energy of adsorption of hydrogen molecule on graphene is always enhanced by the presence of co-adsorbed lithium. The most efficient adsorption configuration is when H 2 is lying parallel to lithium adsorbed graphene which is in contrast to its adsorption on pristine graphene (PG) where it prefers perpendicular orientation.

  9. Adsorption removal of hydrogen sulfide gas. IV. Characteristics of adsorbents for the adsorption removal of hydrogen sulfide gas

    Energy Technology Data Exchange (ETDEWEB)

    Boki, K

    1974-10-25

    The amount of hydrogen sulfide gas adsorbed was affected by the surface properties (surface pH, acid strength, acid amount, and basic amount), the surface structure (pore volume), and the surface form (scanning electron microscopic observation) of 32 tested adsorbents. In general, the amount adsorption increased in the following order, amount of H/sub 2/S adsorbed on the silicate adsorbents, on the active carbon adsorbents, and on the zeolite adsorbents. The amount of H/sub 2/S adsorbed on magnesium silicate and silica gel adsorbents was mainly affected by the surface structure, and the amount adsorbed on the aluminum silicate adsorbents was affected by the distinctions on the surface forms of the adsorbents. The amount of H/sub 2/S adsorbed on 10 kinds of active carbon was determined by the surface properties and the surface structures of the adsorbents. The amount adsorbed on 12 kinds of zeolites was determined by either the surface properties or by the surface structures of the adsorbents. The amount of H/sub 2/S adsorbed on the silicate, active carbon, and zeolite adsorbents interacted with the heat of adsorption, and among the same kinds of adsorbents, the amount adsorbed was linearly related to the heat of adsorption.

  10. A density functional study on the adsorption of hydrogen molecule ...

    Indian Academy of Sciences (India)

    tive adsorption of H2 onto the minimum energy copper clusters by using the density ... theoretical study of molecular oxygen and atomic oxy- gen adsorption onto small ...... the values for all singlet spin states are zero, indicating that no ...

  11. Hydrogen sulfide adsorption on activated carbon fiber. Tests on Parisian subway; Elimination du sulfure d'hydrogene par adsorption sur tissu de charbon actif. Essais sur site RATP

    Energy Technology Data Exchange (ETDEWEB)

    Bouzaza, A.; Marsteau, St.; Laplanche, A. [Ecole Nationale Superieure de Chimie, Lab. Chimie des Nuissances et Genie de l' Environnement - CNGE, 35 - Rennes (France); Garrot, B. [RATP, Dept. Environnement et Securite-Domaines d' Expertises de l' Environnement-Entite Qualite de l' Air, 75 - Paris (France)

    2003-06-01

    Hydrogen sulfide has an unpleasant odor and may cause damage to the electrical materials of the Parisian subway. The activated carbon has some intrinsic catalytic activity, so the removal of hydrogen sulfide is due to an adsorption-oxidation process. In a laboratory scale, some kinetic parameters were acquired, which allowed us to build up two dynamic reactors. These continuous reactors, equipped with activated carbon fibers, were tested on the Madeleine station of the Parisian subway. The feasibility of the elimination of H{sub 2}S by continuous adsorption-oxidation was confirmed. The relative humidity of the gas phase was found to play an important role in the performance of the elimination. The durability of the pilot tested was compatible with an industrial exploitation of the process. (authors)

  12. Combined theoretical and FTIR spectroscopic studies on hydrogen adsorption on the zeolites Na-FER and K-FER

    Czech Academy of Sciences Publication Activity Database

    Areán, C. O.; Palomino, G. T.; Garrone, E.; Nachtigallová, Dana; Nachtigall, Petr

    2006-01-01

    Roč. 110, č. 1 (2006), s. 395-402 ISSN 1520-6106 R&D Projects: GA MŠk(CZ) LC512 Institutional research plan: CEZ:AV0Z40550506 Keywords : adsorption * hydrogen storage * spectroscopy Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 4.115, year: 2006

  13. Site competition on metal surfaces: an electron spectroscopic study of sequential adsorption on W(110)

    International Nuclear Information System (INIS)

    Steinkilberg, M.; Menzel, D.

    1977-01-01

    Using UPS and XPS, the sequential adsorption of hydrogen + carbon monoxide, and of hydrogen + oxygen, on W(110) has been studied at room temperature. Adsorption of CO on a H-covered surface is rapid and leads to total displacement of hydrogen. The resulting CO layer however, is different from that formed on the clean surface under identical conditions, in that it consists of a higher percentage of virgin CO, while considerably more β-CO forms on the clean surface. Oxygen does not adsorb on a H-covered surface, nor displace hydrogen. It is concluded that hydrogen most probably occupies the same sites utilized by dissociative adsorption of CO and oxygen, while virgin CO can also occupy different sites; its adsorption can thus lead to interactional weakening of the H-surface bond. (Auth.)

  14. Theoretical study of molecular hydrogen and spiltover hydrogen storage on two-dimensional covalent-organic frameworks

    International Nuclear Information System (INIS)

    Liu Xiu-Ying; He Jie; Yu Jing-Xin; Fan Zhi-Qin; Li Zheng-Xin

    2014-01-01

    Molecular hydrogen and spiltover hydrogen storages on five two-dimensional (2D) covalent-organic frameworks (COFs) (PPy-COF, TP-COF, BTP-COF, COF-18 Å, and HHTP-DPB COF) are investigated using the grand canonical Monte Carlo (GCMC) simulations and the density functional theory (DFT), respectively. The GCMC simulated results show that HHTP-DPB COF has the best performance for hydrogen storage, followed by BTP-COF, TP-COF, COF-18 Å, and PPy-COF. However, their adsorption amounts at room temperature are all too low to meet the uptake target set by US Department of Energy (US-DOE) and enable practical applications. The effects of pore size, surface area, and isosteric heat of hydrogen on adsorption amount are considered, which indicate that these three factors are all the important factors for determining the H 2 adsorption amount. The chemisorptions of spiltover hydrogen atoms on these five COFs represented by the cluster models are investigated using the DFT method. The saturation cluster models are constructed by considering all possible adsorption sites for these cluster models. The average binding energy of a hydrogen atom and the saturation hydrogen storage density are calculated. The large average binding energy indicates that the spillover process may proceed smoothly and reversibly. The saturation hydrogen storage density is much larger than the physisorption uptake of H 2 molecules at 298 K and 100 bar (1 bar = 10 5 Pa), and is close to or exceeds the 2010 US-DOE target of 6 wt% for hydrogen storage. This suggests that the hydrogen storage capacities of these COFs by spillover may be significantly enhanced. Thus 2D COFs studied in this paper are suitable hydrogen storage media by spillover

  15. Hydrogen adsorption-mediated synthesis of concave Pt nanocubes and their enhanced electrocatalytic activity

    Science.gov (United States)

    Lu, Bang-An; Du, Jia-Huan; Sheng, Tian; Tian, Na; Xiao, Jing; Liu, Li; Xu, Bin-Bin; Zhou, Zhi-You; Sun, Shi-Gang

    2016-06-01

    Concave nanocubes are enclosed by high-index facets and have negative curvature; they are expected to have enhanced reactivity, as compared to nanocubes with flat surfaces. Herein, we propose and demonstrate a new strategy for the synthesis of concave Pt nanocubes with {hk0} high-index facets, by using a hydrogen adsorption-mediated electrochemical square-wave potential method. It was found that Pt atoms prefer to deposit on edge sites rather than terrace sites on Pt surfaces with intensive hydrogen adsorption, resulting in the formation of concave structures. The as-prepared concave Pt nanocubes exhibit enhanced catalytic activity and stability towards oxidation of ethanol and formic acid in acidic solutions, compared to commercial Pt/C catalysts.Concave nanocubes are enclosed by high-index facets and have negative curvature; they are expected to have enhanced reactivity, as compared to nanocubes with flat surfaces. Herein, we propose and demonstrate a new strategy for the synthesis of concave Pt nanocubes with {hk0} high-index facets, by using a hydrogen adsorption-mediated electrochemical square-wave potential method. It was found that Pt atoms prefer to deposit on edge sites rather than terrace sites on Pt surfaces with intensive hydrogen adsorption, resulting in the formation of concave structures. The as-prepared concave Pt nanocubes exhibit enhanced catalytic activity and stability towards oxidation of ethanol and formic acid in acidic solutions, compared to commercial Pt/C catalysts. Electronic supplementary information (ESI) available: Details of DFT calculation, SEM images of concave Pt nanocubes, mass activity and stability characterization of the catalysts. See DOI: 10.1039/c6nr02349e

  16. The effect of atomic hydrogen adsorption on single-walled carbon nano tubes properties

    International Nuclear Information System (INIS)

    Jalili, S.; Majidi, R.

    2007-01-01

    We investigated the adsorption of hydrogen atoms on metallic single-walled carbon nano tubes using ab initio molecular dynamics method. It was found that the geometric structures and the electronic properties of hydrogenated SWNTs can be strongly changed by varying hydrogen coverage. The circular cross sections of the CNTs were changed with different hydrogen coverage. When hydrogen is chemisorbed on the surface of the carbon nano tube, the energy gap will be appeared. This is due to the degree of the Sp 3 hybridization, and the hydrogen coverage can control the band gap of the carbon nano tube

  17. Investigation of hydrogen adsorption centers on Y2O3 by IR-spectroscopy method in diffusive-scattered light

    International Nuclear Information System (INIS)

    Zubkov, S.A.; Borovkov, V.Yu.

    1985-01-01

    Adsorption of hydrogen and carbon oxide at the yttrium oxide at 80 K (5x30 3 PaH 2 ) and 300 K (6.5x10 2 PaCO) respectively are studied by the method of IR spectroscopy. It is shown, that at the surface of yttrium oxide trained in vacuum at 970 K, at least four types of centres of hydrogen adsorption, able to polarize H-H bond in a molecule, exist. Acid-base couple is the highest polarized centre, in the content of which there is a coordination-unsaturated highly-charged yttrium cation. Low-temperature dissociation of hydrogen on Y 2 O 3 surface occurs on the centres which polarized H-H bond in molecule comparatively slow

  18. Hydrogen production from palm kernel shell via integrated catalytic adsorption (ICA) steam gasification

    International Nuclear Information System (INIS)

    Khan, Zakir; Yusup, Suzana; Ahmad, Murni Melati; Chin, Bridgid Lai Fui

    2014-01-01

    Highlights: • The paper presents integrated catalytic adsorption (ICA) steam gasification for H 2 yield. • Effects of adsorbent to biomass, biomass particle size and fluidization velocity on H 2 yield are examined. • The present study produces higher H 2 yield as compared to that obtained in literatures. • The ICA provides enhancement of H 2 yield as compared to independent catalytic and CO 2 adsorption gasification systems. - Abstract: The present study investigates the integrated catalytic adsorption (ICA) steam gasification of palm kernel shell for hydrogen production in a pilot scale atmospheric fluidized bed gasifier. The biomass steam gasification is performed in the presence of an adsorbent and a catalyst in the system. The effect of adsorbent to biomass (A/B) ratio (0.5–1.5 wt/wt), fluidization velocity (0.15–0.26 m/s) and biomass particle size (0.355–2.0 mm) are studied at temperature of 675 °C, steam to biomass (S/B) ratio of 2.0 (wt/wt) and biomass to catalyst ratio of 0.1 (wt/wt). Hydrogen composition and yield, total gas yield, and lower product gas heating values (LHV gas ) increases with increasing A/B ratio, while particle size has no significant effect on hydrogen composition and yield, total gas and char yield, gasification and carbon conversion efficiency. However, gas heating values increased with increasing biomass particle size which is due to presence of high methane content in product gas. Meanwhile, medium fluidization velocity of 0.21 m/s favoured hydrogen composition and yield. The results showed that the maximum hydrogen composition and yield of 84.62 vol% and 91.11 g H 2 /kg biomass are observed at A/B ratio of 1.5, S/B ratio of 2.0, catalyst to biomass ratio of 0.1 and temperature of 675 °C. The product gas heating values are observed in the range of 10.92–17.02 MJ/N m 3 . Gasification and carbon conversion efficiency are observed in the range of 25.66–42.95% and 20.61–41.95%, respectively. These lower

  19. Processes of H{sub 2} adsorption on Fe(1 1 0) surface: A density functional theory study

    Energy Technology Data Exchange (ETDEWEB)

    Xie, Weiwei; Peng, Liang; Peng, Daoling [Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education, School of Chemistry and Environment, South China Normal University, Guangzhou 510006 (China); Gu, Feng Long, E-mail: gu@scnu.edu.cn [Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education, School of Chemistry and Environment, South China Normal University, Guangzhou 510006 (China); Liu, Jun [Material Design and Simulation Technology Co. Ltd., Room 1716, V-Faction, 10 Vanke, 2 Ring Road of North Section, Chengdu (China)

    2014-03-01

    Highlights: • The hydrogen coverages for H{sub 2} adsorption on Fe(1 1 0) surface ranging from 0.125 to 1.000 are prepared by using different surface supercells. • With the reduction of coverage, the average iron atomic energy is increased and the adsorption energy is decreased, leading to the system more stable; while coverage has little effect on the Fe(1 1 0) surface structure and the hydrogen adsorption process. • The most stable absorption site is found to be the on-top site. • DFT calculations show that it is a weak adsorption and the adsorption energy barriers under 4.4 kcal/mol. • The final state is H{sub 2} molecule dissociated into two hydrogen atoms interacting with surface iron atoms to form stable Fe-H bonds. - Abstract: Processes of H{sub 2} adsorption on Fe(1 1 0) surface have been studied by the density functional theory, properties such as surface structure, adsorption position, and adsorption energies are discussed as well. To investigate the atomic geometries and stability under different hydrogen coverages for this adsorption, the hydrogen coverages ranging from 0.125 to 1.000 are prepared by using different surface supercells. It is found that with the reduction of coverage, the average iron atomic energy and the adsorption energy are increased, leading to the system more stable; while coverage has little effect on the Fe(1 1 0) surface structure and the hydrogen adsorption process. The most stable absorption site is found to be the on-top site. Our calculations show that it is a weak adsorption and the adsorption energy barriers under 4.4 kcal/mol. The final state is H{sub 2} molecule dissociated into two hydrogen atoms and interacting with surface iron atoms to form stable Fe-H bonds.

  20. Hydrogen-Induced Adsorption of Carbon Monoxide on the Gold Dimer Cation: A Joint Experimental and DFT Investigation.

    Science.gov (United States)

    Vojkovic, Marin; Rayane, Driss; Antoine, Rodolphe; Broyer, Michel; Allouche, Abdul-Rahman; Mignon, Pierre; Dugourd, Philippe

    2017-06-15

    It is demonstrated, using tandem mass spectrometry and radio frequency ion trap, that the adsorption of a H atom on the gold dimer cation, Au 2 H + , prevents its dissociation and allows for adsorption of CO. Reaction kinetics are measured by employing a radio frequency ion trap, where Au 2 + and CO interact for a given reaction time. The effect of a hydrogen atom is evaluated by comparing reaction rate constants measured for Au 2 + and Au 2 H + . The theoretical results for the adsorption of CO molecules and their reaction characteristics with Au 2 + and Au 2 H + are found to agree with the experimental findings. The joint investigations provide insights into hydrogen atom adsorption effects and consequent reaction mechanisms.

  1. First Principles Study of Adsorption of Hydrogen on Typical Alloying Elements and Inclusions in Molten 2219 Al Alloy

    Directory of Open Access Journals (Sweden)

    Yu Liu

    2017-07-01

    Full Text Available To better understand the effect of the components of molten 2219 Al alloy on the hydrogen content dissolved in it, the H adsorption on various positions of alloying element clusters of Cu, Mn and Al, as well as the inclusion of Al2O3, MgO and Al4C3, were investigated by means of first principles calculation, and the thermodynamic stability of H adsorbed on each possible site was also studied on the basis of formation energy. Results show that the interaction between Al, MgO, Al4C3 and H atoms is mainly repulsive and energetically unfavorable; a favorable interaction between Cu, Mn, Al2O3 and H atoms was determined, with H being more likely to be adsorbed on the top of the third atomic layer of Cu(111, the second atomic layer of Mn(111, and the O atom in the third atomic layer of Al2O3, compared with other sites. It was found that alloying elements Cu and Mn and including Al2O3 may increase the hydrogen adsorption in the molten 2219 Al alloy with Al2O3 being the most sensitive component in this regard.

  2. A green synthetic approach to graphene nanosheets for hydrogen adsorption

    International Nuclear Information System (INIS)

    Yuan Wenhui; Li Baoqing; Li Li

    2011-01-01

    A green and facile strategy of preparing graphene by reducing exfoliated graphite oxide (GO) with glucose was developed in this study. The as-prepared samples were characterized by X-ray diffraction (XRD), Raman spectroscopy, Fourier transform infrared spectroscopy (FT-IR), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM) and Atomic force microscopy (AFM). The characterization results indicated that the graphene sheets (GS) were of high quality with smooth surface, rich pore structure and few layer graphene. The samples have a BET specific surface area of 1205.8 m 2 g -1 measured by N 2 adsorption at 77 K. The hydrogen storage capacity of 2.7 wt.% at 298 K and 25 bar demonstrated that the as-prepared graphene employing glucose as reductant is supposed to be a promising material with outstanding property for hydrogen storage.

  3. A DFT+U investigation of hydrogen adsorption on the LaFeO3(010) surface

    NARCIS (Netherlands)

    Boateng, Isaac W.; Tia, Richard; Adei, Evans; Dzade, N.Y.; Catlow, C. Richard A.; de Leeuw, Nora H.

    2017-01-01

    The ABO3 perovskite lanthanum ferrite (LaFeO3) is a technologically important electrode material for nickel–metal hydride batteries, energy storage and catalysis. However, the electrochemical hydrogen adsorption mechanism on LaFeO3 surfaces remains under debate. In the present study, we have

  4. Effect of Hydrogen Adsorption on the Stone-Wales Transformation in Small-Diameter Carbon Nanotubes

    Science.gov (United States)

    Openov, L. A.; Podlivaev, A. I.

    2018-04-01

    The effect of hydrogenation of (4, 0) and (3, 0) carbon nanotubes on the Stone-Wales transformation is studied in the framework of the nonorthogonal tight-binding model. It is shown that the atomic hydrogen adsorption can lead to both a decrease and an increase in the barriers for the direct and inverse transformations depending on the orientation of a rotating C-C bond with respect to the nanotube axis. The characteristic times of formation and annealing the Stone-Wales defects have been estimated. The Young's moduli have been calculated.

  5. Fundamentals of high pressure adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Y.P.; Zhou, L. [Tianjin University, Tianjin (China). High Pressure Adsorption Laboratory

    2009-12-15

    High-pressure adsorption attracts research interests following the world's attention to alternative fuels, and it exerts essential effect on the study of hydrogen/methane storage and the development of novel materials addressing to the storage. However, theoretical puzzles in high-pressure adsorption hindered the progress of application studies. Therefore, the present paper addresses the major theoretical problems that challenged researchers: i.e., how to model the isotherms with maximum observed in high-pressure adsorption; what is the adsorption mechanism at high pressures; how do we determine the quantity of absolute adsorption based on experimental data. Ideology and methods to tackle these problems are elucidated, which lead to new insights into the nature of high-pressure adsorption and progress in application studies, for example, in modeling multicomponent adsorption, hydrogen storage, natural gas storage, and coalbed methane enrichment, was achieved.

  6. Direct observation and modelling of ordered hydrogen adsorption and catalyzed ortho-para conversion on ETS-10 titanosilicate material.

    Science.gov (United States)

    Ricchiardi, Gabriele; Vitillo, Jenny G; Cocina, Donato; Gribov, Evgueni N; Zecchina, Adriano

    2007-06-07

    Hydrogen physisorption on porous high surface materials is investigated for the purpose of hydrogen storage and hydrogen separation, because of its simplicity and intrinsic reversibility. For these purposes, the understanding of the binding of dihydrogen to materials, of the structure of the adsorbed phase and of the ortho-para conversion during thermal and pressure cycles are crucial for the development of new hydrogen adsorbents. We report the direct observation by IR spectroscopic methods of structured hydrogen adsorption on a porous titanosilicate (ETS-10), with resolution of the kinetics of the ortho-para transition, and an interpretation of the structure of the adsorbed phase based on classical atomistic simulations. Distinct infrared signals of o- and p-H2 in different adsorbed states are measured, and the conversion of o- to p-H2 is monitored over a timescale of hours, indicating the presence of a catalyzed reaction. Hydrogen adsorption occurs in three different regimes characterized by well separated IR manifestations: at low pressures ordered 1:1 adducts with Na and K ions exposed in the channels of the material are formed, which gradually convert into ordered 2:1 adducts. Further addition of H2 occurs only through the formation of a disordered condensed phase. The binding enthalpy of the Na+-H2 1:1 adduct is of -8.7+/-0.1 kJ mol(-1), as measured spectroscopically. Modeling of the weak interaction of H2 with the materials requires an accurate force field with a precise description of both dispersion and electrostatics. A novel three body force field for molecular hydrogen is presented, based on the fitting of an accurate PES for the H2-H2 interaction to the experimental dipole polarizability and quadrupole moment. Molecular mechanics simulations of hydrogen adsorption at different coverages confirm the three regimes of adsorption and the structure of the adsorbed phase.

  7. Effects of buffer agents on hydrogen adsorption and desorption at/within activated carbon for the negative electrode of aqueous asymmetric supercapacitors

    International Nuclear Information System (INIS)

    Chien, Hsiu-Chuan; Wu, Tzu-Ho; Rajkumar, Muniyandi; Hu, Chi-Chang

    2016-01-01

    Highlights: • H adsorption causes local pH increase and negatively shifts the double-layer potential window. • The local pH variation at AC/electrolyte interface can be controlled via adding buffer agents. • H adsorption potential on AC in buffer electrolytes follows the Nernstian dependence. • The pseudocapacitive reversibility of H adsorption/desorption at/within AC is too poor. - Abstract: In this work, the effects of adding buffer agents into aqueous electrolytes on the hydrogen adsorption/desorption behaviour at/within activated carbon are systematically investigated for the negative electrode of asymmetric supercapacitors. Due to the poor electrochemical reversibility of hydrogen adsorption/desorption at/within activated carbon, the hydrogen responses at/within activated carbon are not suitable for pseudo-capacitive energy storage of high-performance asymmetric supercapacitor. The electrochemical adsorption of H atoms consumes protons and causes the local pH change at the activated carbon/electrolyte interface, leading to the negative shift in the H adsorption potential when weakly acidic, neutral, and weakly basic electrolytes without buffer agents are employed. The addition of buffer agents into electrolytes significantly improves the rate of proton supply and promotes the rate of hydrogen adsorption at/within AC. Interestingly, the onset potential of significant H adsorption obtained from the buffered electrolytes generally follows the Nernstian dependence, suggesting the Nerstian dependence of H"+/H_a_d_s on AC at all pH values. In order to obtain the energy storage devices with high coulombic and energy efficiencies, the onset potential of significant H adsorption obtained from the electrolyte containing buffer agents is a reliable lower potential limit of the AC-coated negative electrode for aqueous asymmetric supercapacitors.

  8. STUDY OF HYDROGEN SULFIDE REMOVAL FROM GROUNDWATER

    Directory of Open Access Journals (Sweden)

    T. Lupascu

    2013-06-01

    Full Text Available The process of the hydrogen sulfide removal from the underground water of the Hancesti town has been investigated. By oxygen bubbling through the water containing hydrogen sulfide, from the Hancesti well tube, sulfur is deposited in the porous structure of studied catalysts, which decreases their catalytic activity. Concomitantly, the process of adsorption / oxidation of hydrogen sulfide to sulfate take place. The kinetic research of the hydrogen sulfide removal from the Hancesti underground water, after its treatment by hydrogen peroxide, proves greater efficiency than in the case of modified carbonic adsorbents. As a result of used treatment, hydrogen sulfide is completely oxidized to sulfates

  9. A Biomimetic Approach to New Adsorptive Hydrogen Storage Metal-Organic Frameworks

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Hongcai J [Texas A& M University

    2015-08-12

    In the past decades, there has been an escalation of interest in the study of MOFs due to their fascinating structures and intriguing application potentials. Their exceptionally high surface areas, uniform yet tunable pore sizes, and well-defined adsorbate-MOF interaction sites make them suitable for hydrogen storage. Various strategies to increase the hydrogen capacity of MOFs, such as constructing pore sizes comparable to hydrogen molecules, increasing surface area and pore volume, utilizing catenation, and introducing coordinatively unsaturated metal centers (UMCs) have been widely explored to increase the hydrogen uptake of the MOFs. MOFs with hydrogen uptake approaching the DOE gravimetric storage goal under reasonable pressure but cryo- temperature (typically 77 K) were achieved. However, the weak interaction between hydrogen molecules and MOFs has been the major hurdle limiting the hydrogen uptake of MOFs at ambient temperature. Along the road, we have realized both high surface area and strong interaction between framework and hydrogen are equally essential for porous materials to be practically applicable in Hydrogen storage. Increasing the isosteric heats of adsorption for hydrogen through the introduction of active centers into the framework could have great potential on rendering the framework with strong interaction toward hydrogen. Approaches on increasing the surface areas and improving hydrogen affinity by optimizing size and structure of the pores and the alignment of active centers around the pores in frameworks have been pursued, for example: (a) the introduction of coordinatively UMC (represents a metal center missing multiple ligands) with potential capability of multiple dihydrogen-binding (Kubas type, non-dissociative) per UMC, (b) the design and synthesis of proton-rich MOFs in which a + H3 binds dihydrogen just like a metal ion does, and (c) the preparation of MOFs and PPNs with well aligned internal electric fields. We believe the

  10. Molecular adsorption of hydrogen peroxide on N- and Fe-doped titania nanoclusters

    Energy Technology Data Exchange (ETDEWEB)

    Mohajeri, Afshan, E-mail: amohajeri@shirazu.ac.ir; Dashti, Nasimeh Lari

    2017-06-15

    Highlights: • The stability and electronic properties of N/Fe-doped (TiO{sub 2}){sub n} clusters with n = 5,6 were studied. • The adsorption H{sub 2}O{sub 2} on the surface of doped clusters has been investigated. • This is the first report of H{sub 2}O{sub 2} adsorption onto the (TiO{sub 2}){sub n} cluster in the presence of metal and non-metal dopants. • The effect of N and Fe dopants on interaction strength was studied. - Abstract: Titanium dioxide (titania) nanoparticles have been extensively investigated for photocatalytic applications such as the decomposition and adsorption of pollutant and undesirable compound in air and waste water. In this context, the present article reports the molecular adsorption of hydrogen peroxide on the surface of doped titania clusters. Density functional theory calculations were performed to investigate the structures and electronic properties of two nanoscale (TiO{sub 2}){sub n} clusters (n = 5,6) modified by nitrogen and iron dopants. The relative stability of all possible N-doped and Fe-doped isomers has been compared with each other and with the parent cluster. It was found that the Fe-doped clusters are in general more stable than the N-doped counterparts. Moreover, after N/Fe doping an enhanced in the magnetization of the clusters is observed. In the second part, we have investigated different modes of H{sub 2}O{sub 2} adsorption on the lowest-energy isomers of doped clusters. In almost all the cases, the adsorptions on the doped clusters are found to be less exothermic than on the corresponding undoped parent cluster. Our results highlight the essential role of charge transfer into the interaction between H{sub 2}O{sub 2} and doped (TiO{sub 2}){sub n} clusters, especially for Fe-doped clusters.

  11. Monte-Carlo Simulation of Hydrogen Adsorption in Single-Wall Carbon Nano-Cones

    Directory of Open Access Journals (Sweden)

    Zohreh Ahadi

    2011-01-01

    Full Text Available The properties of hydrogen adsorption in single-walled carbon nano-cones are investigated in detail by Monte Carlo simulations. A great deal of our computational results show that the hydrogen storage capacity in single-walled carbon nano-cones is slightly smaller than the capacity of single-walled carbon nanotubes at any time at the same conditions. This indicates that the hydrogen storage capacity of single-walled carbon nano-cones is related to angles of carbon nano-cones. It seems that these type of nanotubes could not exceed the 2010 goal of 6 wt%, which is presented by the U.S. Department of Energy. In addition, these results are discussed in theory.

  12. Strain effect on the adsorption, diffusion, and molecular dissociation of hydrogen on Mg (0001) surface

    Energy Technology Data Exchange (ETDEWEB)

    Lei, Huaping; Wang, Caizhuang; Yao, Yongxin; Hupalo, Myron [Ames Laboratory, USDOE, Ames, Iowa 50011 (United States); Wang, Yangang [Ames Laboratory, USDOE, Ames, Iowa 50011 (United States); Supercomputing Center of Computer Network Information Center, CAS, Beijing 100190 (China); McDougall, Dan; Tringides, Michael; Ho, Kaiming [Ames Laboratory, USDOE, Ames, Iowa 50011 (United States); Department of Physics and Astronomy, Iowa State University, Ames, Iowa 50011 (United States)

    2013-12-14

    The adsorption, diffusion, and molecular dissociation of hydrogen on the biaxially strained Mg (0001) surface have been systematically investigated by the first principle calculations based on density functional theory. When the strain changes from the compressive to tensile state, the adsorption energy of H atom linearly increases while its diffusion barrier linearly decreases oppositely. The dissociation barrier of H{sub 2} molecule linearly reduces in the tensile strain region. Through the chemical bonding analysis including the charge density difference, the projected density of states and the Mulliken population, the mechanism of the strain effect on the adsorption of H atom and the dissociation of H{sub 2} molecule has been elucidated by an s-p charge transfer model. With the reduction of the orbital overlap between the surface Mg atoms upon the lattice expansion, the charge transfers from p to s states of Mg atoms, which enhances the hybridization of H s and Mg s orbitals. Therefore, the bonding interaction of H with Mg surface is strengthened and then the atomic diffusion and molecular dissociation barriers of hydrogen decrease accordingly. Our works will be helpful to understand and to estimate the influence of the lattice deformation on the performance of Mg-containing hydrogen storage materials.

  13. Hydrogen adsorption strength and sites in the metal organic framework MOF5: Comparing experiment and model calculations

    Science.gov (United States)

    Mulder, F. M.; Dingemans, T. J.; Schimmel, H. G.; Ramirez-Cuesta, A. J.; Kearley, G. J.

    2008-07-01

    Hydrogen adsorption in porous, high surface area, and stable metal organic frameworks (MOF's) appears a novel route towards hydrogen storage materials [N.L. Rosi, J. Eckert, M. Eddaoudi, D.T. Vodak, J. Kim, M. O'Keeffe, O.M. Yaghi, Science 300 (2003) 1127; J.L.C. Rowsell, A.R. Millward, K. Sung Park, O.M. Yaghi, J. Am. Chem. Soc. 126 (2004) 5666; G. Ferey, M. Latroche, C. Serre, F. Millange, T. Loiseau, A. Percheron-Guegan, Chem. Commun. (2003) 2976; T. Loiseau, C. Serre, C. Huguenard, G. Fink, F. Taulelle, M. Henry, T. Bataille, G. Férey, Chem. Eur. J. 10 (2004) 1373]. A prerequisite for such materials is sufficient adsorption interaction strength for hydrogen adsorbed on the adsorption sites of the material because this facilitates successful operation under moderate temperature and pressure conditions. Here we report detailed information on the geometry of the hydrogen adsorption sites, based on the analysis of inelastic neutron spectroscopy (INS). The adsorption energies for the metal organic framework MOF5 equal about 800 K for part of the different sites, which is significantly higher than for nanoporous carbon materials (˜550 K) [H.G. Schimmel, G.J. Kearley, M.G. Nijkamp, C.T. Visser, K.P. de Jong, F.M. Mulder, Chem. Eur. J. 9 (2003) 4764], and is in agreement with what is found in first principles calculations [T. Sagara, J. Klassen, E. Ganz, J. Chem. Phys. 121 (2004) 12543; F.M. Mulder, T.J. Dingemans, M. Wagemaker, G.J. Kearley, Chem. Phys. 317 (2005) 113]. Assignments of the INS spectra is realized using comparison with independently published model calculations [F.M. Mulder, T.J. Dingemans, M. Wagemaker, G.J. Kearley, Chem. Phys. 317 (2005) 113] and structural data [T. Yildirim, M.R. Hartman, Phys. Rev. Lett. 95 (2005) 215504].

  14. Density functional study of manganese atom adsorption on hydrogen-terminated armchair boron nitride nanoribbons

    Energy Technology Data Exchange (ETDEWEB)

    Abdullahi, Yusuf Zuntu [Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Department of Physics, Faculty of Science, Kaduna State University, P.M.B. 2339, Kaduna State (Nigeria); Rahman, Md. Mahmudur, E-mail: mahmudur@upm.edu.my [Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Shuaibu, Alhassan [Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Department of Physics, Faculty of Science, Nigerian Defence Academy, P.M.B 2109 Kaduna (Nigeria); Abubakar, Shamsu [Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Department of Physics, Faculty of Science, Yobe State University, P.M.B. 1144, Yobe State (Nigeria); Zainuddin, Hishamuddin [Department of Physics, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Institute for Mathematical Research, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor (Malaysia); Muhida, Rifki [Department of Physics-Energy Engineering, Surya University, Gedung 01 Scientia Business Park, Jl. Boulevard Gading Serpong Blok O/1, Summarecon Serpong, Tangerang 15810, Banten (Indonesia); Setiyanto, Henry [Analytical Chemistry Research Group, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesha no. 10, Bandung 40132 (Indonesia)

    2014-08-15

    In this paper, we have investigated stable structural, electric and magnetic properties of manganese (Mn) atom adsorption on armchair hydrogen edge-terminated boron nitride nanoribbon (A-BNNRs) using first principles method based on density-functional theory with the generalized gradient approximation. Calculation shows that Mn atom situated on the ribbons of A-BNNRs is the most stable configuration, where the bonding is more pronounced. The projected density of states (PDOS) of the favored configuration has also been computed. It has been found that the covalent bonding of boron (B), nitrogen (N) and Mn is mainly contributed by s, d like-orbitals of Mn and partially occupied by the 2p like-orbital of N. The difference in energy between the inner and the edge adsorption sites of A-BNNRs shows that Mn atoms prefer to concentrate at the edge sites. The electronic structures of the various configurations are wide, narrow-gap semiconducting and half-metallic, and the magnetic moment of Mn atoms are well preserved in all considered configurations. This has shown that the boron nitride (BN) sheet covered with Mn atoms demonstrates additional information on its usefulness in future spintronics, molecular magnet and nanoelectronics devices.

  15. Density functional study of manganese atom adsorption on hydrogen-terminated armchair boron nitride nanoribbons

    International Nuclear Information System (INIS)

    Abdullahi, Yusuf Zuntu; Rahman, Md. Mahmudur; Shuaibu, Alhassan; Abubakar, Shamsu; Zainuddin, Hishamuddin; Muhida, Rifki; Setiyanto, Henry

    2014-01-01

    In this paper, we have investigated stable structural, electric and magnetic properties of manganese (Mn) atom adsorption on armchair hydrogen edge-terminated boron nitride nanoribbon (A-BNNRs) using first principles method based on density-functional theory with the generalized gradient approximation. Calculation shows that Mn atom situated on the ribbons of A-BNNRs is the most stable configuration, where the bonding is more pronounced. The projected density of states (PDOS) of the favored configuration has also been computed. It has been found that the covalent bonding of boron (B), nitrogen (N) and Mn is mainly contributed by s, d like-orbitals of Mn and partially occupied by the 2p like-orbital of N. The difference in energy between the inner and the edge adsorption sites of A-BNNRs shows that Mn atoms prefer to concentrate at the edge sites. The electronic structures of the various configurations are wide, narrow-gap semiconducting and half-metallic, and the magnetic moment of Mn atoms are well preserved in all considered configurations. This has shown that the boron nitride (BN) sheet covered with Mn atoms demonstrates additional information on its usefulness in future spintronics, molecular magnet and nanoelectronics devices.

  16. Theoretical study of hydrogen adsorption of graphene and carbon nanotubes decorated with palladium; Estudio teorico de la adsorcion de hidrogeno sobre grafeno y nanotubos de carbono decorados con paladio

    Energy Technology Data Exchange (ETDEWEB)

    Lopez Corral, Ignacio; German, Estefania [Departamento de Fisica, Universidad Nacional del Sur (UNS), Bahia Blanca (Argentina); Volpe, Maria A [Planta Piloto de Ingenieria Quimica (UNS/CONICET), Bahia Blanca (Argentina); Brizuela, Graciela; Juan, Alfredo [Departamento de Fisica, Universidad Nacional del Sur (UNS), Bahia Blanca (Argentina)

    2008-10-15

    Since their discovery in 1991, carbon nanotubes (CNT) have awakened great interest in materials science thanks to their extraordinary structural, electronic and mechanical properties which facilitate their application in many different areas. One of the most promising applications is the possibility of using CNT to store hydrogen for use in small scale fuel cells. Unfortunately, experimental studies performed some years ago have often led to controversial conclusions, causing a continuing debate that has still not been resolved. The most recent work suggests that the storage of hydrogen for practical purposes can be achieved with CNT decorated with transition metals, for example Pd. In this context, theoretical modeling methods have to be used for a detailed understanding of the influence and scope of this type of modification in the interaction of the nanotubes with atomic or molecular hydrogen. This work studied hydrogen adsorption in single-walled carbon nanotubes (SWCNT) doped with Pd atoms, using density functional theory (DFT) and semi-empirical methods. As a preliminary approximation to the system a graphene sheet was used, modeled with a 190 atom cluster of C in a hexagonal arrangement, on which a single Pd atom was placed in adsorption sites. Then C{sub 190} clusters were used to simulate two different types of SWCNT: the zigzag SWCNT of quirality (10.0) and the armchair SWCNT of quirality (5.5), both decorated similarly on the graphene. Geometric optimization procedures for the system's different components were carried out with these models, and then the changes produced during the adsorption process in the electronic occupation of atomic orbitals and unions, for which crystal orbital overlap population (COOP) curves and overlap population (OP) values were evaluated. The results obtained with the graphene and nanotube approximations are in agreement and show that the SWCNT modified with Pd have more capacity to trap hydrogen than the non doped SWCNT. The

  17. Comparative study of hydrogen storage on metal doped mesoporous materials

    Science.gov (United States)

    Carraro, P. M.; Sapag, K.; Oliva, M. I.; Eimer, G. A.

    2018-06-01

    The hydrogen adsorption capacity of mesoporous materials MCM-41 modified with Co, Fe, Ti, Mg and Ni at 77 K and 10 bar was investigated. Various techniques including XRD, N2 adsorption and DRUV-vis were employed for the materials characterization. The results showed that a low nickel loading on MCM-41 support promoted the presence of hydrogen-favorable sites, increasing the hydrogen storage capacity.

  18. Development of a facility for the recovery of high-purity hydrogen from coke oven gas by pressure swing adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Nakamura, M; Saida, K; Uenoyama, K; Sugishita, M; Imokawa, K

    1985-01-01

    This paper reports 1) a pressure swing adsorption (PSA) system comprising three towers, each packed with three different adsorbents; and 2) studies of the application of this system to the recovery of high-purity hydrogen from coke oven gas. Running the adsorption plant at 35 C and 9.5 kg/cm/sup 2/ gives optimum operating stability and economy. In addition, an optimum time cycle for the three-tower system has been developed. Gas from the PSA equipment proper still contains traces of oxygen. This is removed in a further tower packed with Pd catalyst. The ultimate recovery of hydrogen is closely related to its concentration in the raw coke oven gas and to the degree of purity attained. 3 references.

  19. Study of adsorption properties on lithium doped activated carbon materials

    International Nuclear Information System (INIS)

    Los, S.; Daclaux, L.; Letellier, M.; Azais, P.

    2005-01-01

    A volumetric method was applied to study an adsorption coefficient of hydrogen molecules in a gas phase on super activated carbon surface. The investigations were focused on getting the best possible materials for the energy storage. Several treatments on raw samples were used to improve adsorption properties. The biggest capacities were obtain after high temperature treatment at reduced atmosphere. The adsorption coefficient at 77 K and 2 MPa amounts to 3.158 wt.%. The charge transfer between lithium and carbon surface groups via the doping reaction enhanced the energy of adsorption. It was also found that is a gradual decrease in the adsorbed amount of H 2 molecules due to occupation active sites by lithium ions. (author)

  20. A first-principles study of hydrogen storage capacity based on Li-Na-decorated silicene.

    Science.gov (United States)

    Sheng, Zhe; Wu, Shujing; Dai, Xianying; Zhao, Tianlong; Hao, Yue

    2018-05-23

    Surface decoration with alkali metal adatoms has been predicted to be promising for silicene to obtain high hydrogen storage capacity. Herein, we performed a detailed study of the hydrogen storage properties of Li and Na co-decorated silicene (Li-Na-decorated silicene) based on first-principles calculations using van der Waals correction. The hydrogen adsorption behaviors, including the adsorption order, the maximum capacity, and the corresponding mechanism were analyzed in detail. Our calculations show that up to three hydrogen molecules can firmly bind to each Li atom and six for each Na atom, respectively. The hydrogen storage capacity is estimated to be as high as 6.65 wt% with a desirable average adsorption energy of 0.29 eV/H2. It is confirmed that both the charge-induced electrostatic interaction and the orbital hybridizations play a great role in hydrogen storage. Our results may enhance our fundamental understanding of the hydrogen storage mechanism, which is of great importance for the practical application of Li-Na-decorated silicene in hydrogen storage.

  1. Simulation of oxygen-steam gasification with CO{sub 2} adsorption for hydrogen production from empty fruit bunch

    Energy Technology Data Exchange (ETDEWEB)

    Ahmad, M.M.; Inayat, A.; Yusup, S.; Sabil, K.M. [Universiti Teknologi Petronas, Bandar Seri Iskandar, Tronoh (Malaysia). Center of Biofuel and Biochemical, Green Technology Mission Oriented Research

    2011-07-01

    The world is facing a critical situation in which fossil fuel reservoir is depleting while the demand for energy is increasing worldwide. Scientists globally have shifted their effort towards developing alternative sustainable fuels and quite a number of technologies have been discovered. One potential alternative solution is to produce energy from hydrogen as its energy content per kilogram is three times larger than that of gasoline. The combustion of hydrogen produces water instead of greenhouse gases, along with energy, making hydrogen even more attractive as a clean fuel. Current study focuses on the process development of hydrogen production via gasification of Empty Fruit Bunch (EFB) with in-situ adsorption of CO{sub 2} based on equilibrium modeling approach. The process flowsheet simulation is performed using iCON, PETRONAS process simulation software. This work investigates the influence of the temperature within the range of 600 to 1000 C and steam/biomass ratio between 0.1 and 1.0 on the hydrogen yield and product gas composition. The importance of different reactions involved in the system is also discussed. Using the simulation, the optimal operating conditions are predicted to be at 800 C and steam/biomass ratio of 0.6. Hydrogen yield of 149g kg{sup -1} of EFB can be obtained at 1000 C. The preliminary economic potential per annum of the oxygen-steam gasification system coupled with in situ CO{sub 2} adsorption is RM 6.64 x 10{sup 6} or approximately USD 2 x 10{sup 6}.

  2. Hydrogen adsorption on activated carbon nanotubes with an atomic-sized vanadium catalyst investigated by electrical resistance measurements

    International Nuclear Information System (INIS)

    Im, Ji Sun; Yun, Jumi; Kang, Seok Chang; Lee, Sung Kyu; Lee, Young-Seak

    2012-01-01

    Activated multi-walled carbon nanotubes were prepared with appended vanadium as a hydrogen storage medium. The pore structure was significantly improved by an activation process that was studied using Raman spectroscopy, field emission transmission electron microscopy and pore analysis techniques. X-ray photoelectron spectroscopy and X-ray diffraction results reveal that the vanadium catalyst was introduced into the carbon nanotubes in controlled proportions, forming V 8 C 7 . The improved pore structure functioned as a path through the carbon nanotubes that encouraged hydrogen molecule adsorption, and the introduced vanadium catalyst led to high levels of hydrogen storage through the dissociation of hydrogen molecules via the spill-over phenomenon. The hydrogen storage behavior was investigated by electrical resistance measurements for the hydrogen adsorbed on a prepared sample. The proposed mechanism of hydrogen storage suggests that the vanadium catalyst increases not only the amount of hydrogen that is stored but also the speed at which it is stored. A hydrogen storage capacity of 2.26 wt.% was achieved with the activation effects and the vanadium catalyst at 30 °C and 10 MPa.

  3. Alcohol molecules adsorption on graphane nanosheets - A first-principles investigation

    Science.gov (United States)

    Nagarajan, V.; Chandiramouli, R.

    2018-05-01

    The geometric structure, electronic and adsorption properties of methanol, ethanol and 1-propanol molecules on hydrogenated graphene (graphane) were investigated using first-principles calculations. The stability of graphane base material is confirmed using formation energy and phonon band structures. The adsorption of alcohol molecules on bare graphane and hydrogen vacant graphane nanosheet is found to be prominent and the selectivity of alcohol molecules can be achieved using bare or hydrogen vacant graphane nanosheet. Moreover, the interaction of alcohol molecules on bare and hydrogen vacant graphane nanosheets is studied using the adsorption energy, energy band gap variation, Bader charge transfer and average energy band gap variation. The adsorption energy ranges from -0.149 to -0.383 eV upon alcohol adsorption. The energy gap varies from 4.71 to 2.62 eV for bare graphane and from 4.02 to 3.60 eV for hydrogen vacant graphane nanosheets upon adsorption of alcohol molecules. The adsorption properties of alcohol molecules provide useful information for the possible application of graphane nanosheet as a base material for the detection of alcohol molecules.

  4. Green Hydrogen Production from Raw Biogas: A Techno-Economic Investigation of Conventional Processes Using Pressure Swing Adsorption Unit

    Directory of Open Access Journals (Sweden)

    Gioele Di Marcoberardino

    2018-02-01

    Full Text Available This paper discusses the techno-economic assessment of hydrogen production from biogas with conventional systems. The work is part of the European project BIONICO, whose purpose is to develop and test a membrane reactor (MR for hydrogen production from biogas. Within the BIONICO project, steam reforming (SR and autothermal reforming (ATR, have been identified as well-known technologies for hydrogen production from biogas. Two biogases were examined: one produced by landfill and the other one by anaerobic digester. The purification unit required in the conventional plants has been studied and modeled in detail, using Aspen Adsorption. A pressure swing adsorption system (PSA with two and four beds and a vacuum PSA (VPSA made of four beds are compared. VPSA operates at sub-atmospheric pressure, thus increasing the recovery: results of the simulations show that the performances strongly depend on the design choices and on the gas feeding the purification unit. The best purity and recovery values were obtained with the VPSA system, which achieves a recovery between 50% and 60% at a vacuum pressure of 0.1 bar and a hydrogen purity of 99.999%. The SR and ATR plants were designed in Aspen Plus, integrating the studied VPSA model, and analyzing the behavior of the systems at the variation of the pressure and the type of input biogas. The SR system achieves a maximum efficiency, calculated on the LHV, of 52% at 12 bar, while the ATR of 28% at 18 bar. The economic analysis determined a hydrogen production cost of around 5 €/kg of hydrogen for the SR case.

  5. Remarkable adsorptive removal of nitrogen-containing compounds from a model fuel by a graphene oxide/MIL-101 composite through a combined effect of improved porosity and hydrogen bonding

    Energy Technology Data Exchange (ETDEWEB)

    Ahmed, Imteaz; Jhung, Sung Hwa, E-mail: sung@knu.ac.kr

    2016-08-15

    Highlights: • Metal-organic frameworks (MIL-101) were composed with graphene oxide (GnO). • GnO/MIL-101 showed the highest adsorption capacity for indole and quinoline. • Adsorption mechanism was clearly shown based on adsorption results and FTIR. • GnO/MIL-101 might be applied commercially considering capacity and reusability. - Abstract: A composite was prepared by combining a highly porous metal-organic framework (MOF), MIL-101 (Cr-benzenedicarboxylate), and graphene oxide (GnO). The porosity of the composite increased appreciably by the addition of GnO up to a specific amount in the MOF, though further increases in the quantity of GnO was detrimental to porosity. The improved porosity of the GnO/MIL-101 composite was utilized for adsorptive denitrogenation (ADN) of a model fuel where indole (IND) and quinoline (QUI) were used as nitrogen-containing compounds (NCCs). It was found that both IND and QUI showed improved adsorption on the composite compared with pristine MIL-101 or GnO due to the improved porosity of the composite. Interestingly, the improvement in adsorption of IND was much higher than the quantity estimated for the porosity. Importantly, GnO/MIL-101 showed the highest adsorption capacities for NCCs. Irrespective of the studied solvents and co-presence of IND and QUI, the composite adsorbent performed ADN most effectively. This remarkable improvement is explained by the additional mechanism of hydrogen bonding between the surface functional groups of GnO and the hydrogen attached to the nitrogen atom of IND. This hydrogen bonding mechanism is also supported by the results of the adsorption of pyrrole and methylpyrrole. On the other hand, QUI does not show hydrogen-bonding capability, and therefore, its enhanced adsorption originates from only the increased porosity of the adsorbents.

  6. Remarkable adsorptive removal of nitrogen-containing compounds from a model fuel by a graphene oxide/MIL-101 composite through a combined effect of improved porosity and hydrogen bonding

    International Nuclear Information System (INIS)

    Ahmed, Imteaz; Jhung, Sung Hwa

    2016-01-01

    Highlights: • Metal-organic frameworks (MIL-101) were composed with graphene oxide (GnO). • GnO/MIL-101 showed the highest adsorption capacity for indole and quinoline. • Adsorption mechanism was clearly shown based on adsorption results and FTIR. • GnO/MIL-101 might be applied commercially considering capacity and reusability. - Abstract: A composite was prepared by combining a highly porous metal-organic framework (MOF), MIL-101 (Cr-benzenedicarboxylate), and graphene oxide (GnO). The porosity of the composite increased appreciably by the addition of GnO up to a specific amount in the MOF, though further increases in the quantity of GnO was detrimental to porosity. The improved porosity of the GnO/MIL-101 composite was utilized for adsorptive denitrogenation (ADN) of a model fuel where indole (IND) and quinoline (QUI) were used as nitrogen-containing compounds (NCCs). It was found that both IND and QUI showed improved adsorption on the composite compared with pristine MIL-101 or GnO due to the improved porosity of the composite. Interestingly, the improvement in adsorption of IND was much higher than the quantity estimated for the porosity. Importantly, GnO/MIL-101 showed the highest adsorption capacities for NCCs. Irrespective of the studied solvents and co-presence of IND and QUI, the composite adsorbent performed ADN most effectively. This remarkable improvement is explained by the additional mechanism of hydrogen bonding between the surface functional groups of GnO and the hydrogen attached to the nitrogen atom of IND. This hydrogen bonding mechanism is also supported by the results of the adsorption of pyrrole and methylpyrrole. On the other hand, QUI does not show hydrogen-bonding capability, and therefore, its enhanced adsorption originates from only the increased porosity of the adsorbents.

  7. Doped phosphorene for hydrogen capture: A DFT study

    Science.gov (United States)

    Zhang, Hong-ping; Hu, Wei; Du, Aijun; Lu, Xiong; Zhang, Ya-ping; Zhou, Jian; Lin, Xiaoyan; Tang, Youhong

    2018-03-01

    Hydrogen capture and storage is the core of hydrogen energy application. With its high specific surface area, direct bandgap, and variety of potential applications, phosphorene has attracted much research interest. In this study, density functional theory (DFT) is utilized to study the interactions between doped phosphorenes and hydrogen molecules. The effects of different dopants and metallic or nonmetallic atoms on phosphorene/hydrogen interactions is systematically studied by adsorption energy, electron density difference, partial density of states analysis, and Hirshfeld population. Our results indicate that the metallic dopants Pt, Co, and Ni can help to improve the hydrogen capture ability of phosphorene, whereas the nonmetallic dopants have no effect on it. Among the various metallic dopants, Pt performs very differently, such that it can help to dissociate H2 on phosphorene. Specified doped phosphorene could be a promising candidate for hydrogen storage, with behaviors superior to those of intrinsic graphene sheet.

  8. Prediction of hydrogen storage on Y-decorated graphene: A density functional theory study

    International Nuclear Information System (INIS)

    Liu, Wenbo; Liu, Yang; Wang, Rongguo

    2014-01-01

    Highlight: • Rare earth metal Y has an excellent performance on hydrogen storage. • After decoration, each Y can attach six hydrogen molecules without dissociation. • The Y atoms disperse uniformly and stably on B/graphene. • The enhancement of H binding is caused by hybridization and electrostatic attraction. - Abstract: Yttrium decorated graphene has been investigated as a potential carrier for high density hydrogen storage. The adsorption energy and optimized geometry for yttrium on pristine and boron doped graphene have been studied by DFT calculations. The clustering and stability of isolated yttrium atoms on graphene has also been considered. For yttrium decorated boron doped graphene, each yttrium can attach six hydrogen molecules with average adsorption energy of −0.568 eV per hydrogen molecule and the hydrogen storage capacity of this material is 5.78 wt.%, indicating yttrium decorated boron doped graphene as a promising hydrogen storage candidate

  9. Influence of hydrogen bond accepting ability of anions on the adsorption performance of ionic liquid surface molecularly imprinted polymers.

    Science.gov (United States)

    Zhu, Guifen; Gao, Xia; Wang, Xiaolong; Wang, Jianji; Fan, Jing

    2018-01-12

    To illuminate the influence mechanism of anionic structure of ionic liquids (ILs) on the adsorption performance of surface molecularly imprinted polymers (MIPs), in this work, six newly designed MIPs were prepared on the surface of amino-poly(styrene-divinylbenzene) particles by using imidazolium ILs with the same cation [C 4 mim] + but different anions (Cl, CH 3 SO 3 , PF 6 , BF 4 , C 4 F 7 O 2 , C 4 F 9 SO 3 ) as template molecules, methacrylic acid as functional monomer, and ethylene dimethacrylate as cross-linker. The resulting MIP materials were characterized by IR and SEM, and the influence of hydrogen bond accepting ability of anions on the adsorption performance of the MIPs for the ILs was investigated in acetonitrile. It was found that adsorption capacity of the MIPs towards the ILs decreased in the order MIP [C4mim][Cl]  > MIP [C4mim][C4F7O2]  ≥ MIP [C4mim][BF4] and MIP [C4mim][CH3SO3]  > MIP [C4mim][C4F9SO3]  > MIP [C4mim][PF6] , which is in good agreement with the ability of anions of the ILs to form hydrogen bonds. Ultraviolet, 1 H-NMR and 35 Cl-NMR spectroscopy was then used to study the interactions of anions of the ILs with the functional monomer. It was found that the hydrogen bond interaction between anions of the ILs and acidic proton of the functional monomer was the main driving force for the high adsorption selectivity of the imprinted polymers, and the stronger hydrogen bond interaction indicates higher binding capacity and higher selectivity of the polymers towards the ILs. It was also verified that the ILs with stronger hydrogen bond accepting ability of anions could be selectively extracted by the corresponding IL-MIPs. These results may provide new insight into the recognition mechanism of MIPs for ILs, and are also useful for the rational design of this new class of imprinting materials. Copyright © 2017 Elsevier B.V. All rights reserved.

  10. Activity of iridium-ruthenium and iridium-rhodium adsorption catalysts in decomposition of hydrogen peroxide

    Energy Technology Data Exchange (ETDEWEB)

    Zubovich, I A; Mikhaylov, V A; Migulina, N N [Yaroslavskij Politekhnicheskij Inst. (USSR)

    1976-06-01

    Experimental data for the activities of iridium-ruthenium and iridium-rhodium adsorption catalysts in the decomposition of hydrogen peroxide are considered and the results of magnetic susceptibility measurements are presented. It is concluded that surface structures (complexes) may be formed and that micro-electronic feaures play a role in heterogeneous catalysis.

  11. Adsorption and diffusion characteristics of lithium on hydrogenated α- and β-silicene.

    Science.gov (United States)

    Iyikanat, Fadil; Kandemir, Ali; Bacaksiz, Cihan; Sahin, Hasan

    2017-01-01

    Using first-principles density functional theory calculations, we investigate adsorption properties and the diffusion mechanism of a Li atom on hydrogenated single-layer α- and β-silicene on a Ag(111) surface. It is found that a Li atom binds strongly on the surfaces of both α- and β-silicene, and it forms an ionic bond through the transfer of charge from the adsorbed atom to the surface. The binding energies of a Li atom on these surfaces are very similar. However, the diffusion barrier of a Li atom on H-α-Si is much higher than that on H-β-Si. The energy surface calculations show that a Li atom does not prefer to bind in the vicinity of the hydrogenated upper-Si atoms. Strong interaction between Li atoms and hydrogenated silicene phases and low diffusion barriers show that α- and β-silicene are promising platforms for Li-storage applications.

  12. Influence of metal doping of a MOF-74 framework on hydrogen adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Botas, J.A.; Calleja, G.; Orcajo, M.G. [Rey Juan Carlos Univ., Madrid (Spain). Dept. of Chemical and Energy Technology; Sanchez-Sanchez, M. [CSIC, Madrid (Spain). Inst. de Catalisis y Petroleoquimica

    2010-07-01

    Microporous Metal-Organic Framework (MOF) adsorbents are considered an interesting option for hydrogen storage. Due to their porous nature and unusually high surface areas, these materials show an exceptional H{sub 2} uptake. Unfortunately, their interaction with H{sub 2} molecules is weak, so cryogenic temperatures are required to reach competitive H{sub 2} storage capacities. In this sense, the presence of coordinatively unsaturated and exposed metal centers in some MOF frameworks could increase the affinity for H{sub 2} through stronger metal-H{sub 2} interactions. In this preliminary work, the effect of doping a Zn{sup 2+}-MOF-74 framework with Co{sup 2+}, Cu{sup 2+} and Mg{sup 2+} on its adsorption properties for H{sub 2} has been studied. Characterization studies suggest that the samples prepared have actually the MOF-74 structure, in which the different tested heteroatom ions have been successfully incorporated. The differences in H{sub 2} adsorption at 77 K and 87 K between the MOF-74 samples doped with the mentioned divalent metal ions were discussed as a function of their free pore volume and amount of metal incorporation. (orig.)

  13. Hydrogen storage capacity of lithium-doped KOH activated carbons

    International Nuclear Information System (INIS)

    Minoda, Ai; Oshima, Shinji; Iki, Hideshi; Akiba, Etsuo

    2014-01-01

    Highlights: • The hydrogen adsorption of lithium-doped KOH activated carbons has been studied. • Lithium doping improves their hydrogen adsorption affinity. • Lithium doping is more effective for materials with micropores of 0.8 nm or smaller. • Lithium reagent can alter the pore structure, depending on the raw material. • Optimizing the pore size and functional group is needed for better hydrogen uptake. - Abstract: The authors have studied the hydrogen adsorption performance of several types of lithium-doped KOH activated carbons. In the case of activated cokes, lithium doping improves their hydrogen adsorption affinity from 5.02 kg/m 3 to 5.86 kg/m 3 at 303 K. Hydrogen adsorption density increases by around 17% after lithium doping, likely due to the fact that lithium doping is more effective for materials with micropores of 0.8 nm or smaller. The effects of lithium on hydrogen storage capacity vary depending on the raw material, because the lithium reagent can react with the material and alter the pore structure, indicating that lithium doping has the effect of plugging or filling the micropores and changing the structures of functional groups, resulting in the formation of mesopores. Despite an observed decrease in hydrogen uptake, lithium doping was found to improve hydrogen adsorption affinity. Lithium doping increases hydrogen uptake by optimizing the pore size and functional group composition

  14. Electrocatalytic activity of a mononuclear yttrium(III)–methyl orange complex and Y{sub 2}O{sub 2}SO{sub 4} nanoparticles for adsorption/desorption of hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Shafaie, Fahimeh [Department of Chemistry, Isfahan University of Technology, Isfahan, 84156-83111 (Iran, Islamic Republic of); Hadadzadeh, Hassan, E-mail: hadad@cc.iut.ac.ir [Department of Chemistry, Isfahan University of Technology, Isfahan, 84156-83111 (Iran, Islamic Republic of); Behnamfar, Mohammad Taghi [Department of Chemistry, Isfahan University of Technology, Isfahan, 84156-83111 (Iran, Islamic Republic of); Rudbari, Hadi Amiri [Faculty of Chemistry, University of Isfahan, Isfahan, 81746-73441 (Iran, Islamic Republic of)

    2016-12-01

    A new mononuclear yttrium(III) complex, [Y(MO){sub 3}(DMF){sub 3}(H{sub 2}O){sub 2}] (where MO{sup –} is methyl orange anion (4-[(4-dimethylamino)phenyldiazenyl]benzenesulfonate)), was synthesized in an aqueous solution. The complex was characterized by elemental analysis, UV/Vis, FT-IR, and single-crystal X-ray crystallography. The yttrium oxysulfate nanoparticles (Y{sub 2}O{sub 2}SO{sub 4}) were then prepared by calcination of [Y(MO){sub 3}(DMF){sub 3}(H{sub 2}O){sub 2}]. The obtained nanoparticles were characterized by FT-IR, X-ray diffraction analysis (XRD), and field-emission scanning electron microscopy (FE-SEM). The hydrogen adsorption/desorption (H{sub ads}/H{sub des}) behavior of the Y(III) complex and Y{sub 2}O{sub 2}SO{sub 4} nanoparticles was studied at a carbon paste electrode (CPE) in H{sub 2}SO{sub 4} by cyclic voltammetry (CV). The recorded voltammograms exhibited a pair of peaks corresponding to the adsorption/desorption of hydrogen for the Y(III) complex and Y{sub 2}O{sub 2}SO{sub 4} nanoparticles. The results show a reversible hydrogen adsorption/desorption reaction for both compounds. The voltammograms of the nanoparticles indicate an excellent cycling stability for the adsorption/desorption of hydrogen. In addition, the linear sweep voltammetry (LSV) technique was used to investigate the electrocatalytic activity of both compounds for the hydrogen adsorption reaction. The linear voltammograms of both compounds demonstrate the excellent electrocatalytic activity for the hydrogen adsorption reaction. - Highlights: • Preparation of a new Y(III) complex and Y{sub 2}O{sub 2}SO{sub 4} nanoparticles. • Investigation of the H{sub ads}/H{sub des} reaction for both compounds by voltammetry. • Observation of two peaks corresponding to the H{sub ads}/H{sub des} in both compounds. • An excellent cycling stability for the nanoparticles in H{sub 2}SO{sub 4}.

  15. Hydrogen dissociation and incorporation on Mg{sub 17}Al{sub 12}(100) surface: A density functional theory study

    Energy Technology Data Exchange (ETDEWEB)

    Ning, Hua [Guangxi Key Laboratory for Relativistic Astrophysics, Guangxi Colleges and Universities Key Laboratory of Novel Energy Materials and Related Technology, College of Physics Science and Technology, Guangxi University, Nanning 530004 (China); Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials, School of Material Science and Engineering, Guilin University of Electronic Technology, Guilin 541004 (China); Zhou, Zhiyan; Zhang, Ziyan [Guangxi Key Laboratory for Relativistic Astrophysics, Guangxi Colleges and Universities Key Laboratory of Novel Energy Materials and Related Technology, College of Physics Science and Technology, Guangxi University, Nanning 530004 (China); Zhou, Wenzheng; Li, Guangxu [Guangxi Key Laboratory for Relativistic Astrophysics, Guangxi Colleges and Universities Key Laboratory of Novel Energy Materials and Related Technology, College of Physics Science and Technology, Guangxi University, Nanning 530004 (China); Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials, School of Material Science and Engineering, Guilin University of Electronic Technology, Guilin 541004 (China); Guo, Jin, E-mail: guojin@gxu.edu.cn [Guangxi Key Laboratory for Relativistic Astrophysics, Guangxi Colleges and Universities Key Laboratory of Novel Energy Materials and Related Technology, College of Physics Science and Technology, Guangxi University, Nanning 530004 (China); Guangxi Collaborative Innovation Center of Structure and Property for New Energy and Materials, School of Material Science and Engineering, Guilin University of Electronic Technology, Guilin 541004 (China)

    2017-02-28

    Highlights: • Hydrogen adsorption, dissociation, and penetration on (in) Mg{sub 17}Al{sub 12} (100) surface are studied. • Hydrogen molecules are dissociated on the surface with barrier of 0.63 eV. • The maximum barrier energy for atomic hydrogen penetration into the subsurface is ∼0.7 eV. • The hybridization between the s orbital of H and the s orbitals of Mg is major. - Abstract: Hydrogen adsorption, dissociation, and penetration on (in) Mg{sub 17}Al{sub 12} (100) surface are studied extensively by DFT total-energy calculations. The adsorption geometries, dissociation barriers, various diffusion pathways, penetrative processes, and electronic structures were investigated. Results show that the atomic and molecular hydrogen forms prefer to be adsorbed on the Mg3-Mg3 bridge sites (C sites). Hydrogen molecules are dissociated on the surface with the minimum barrier energy of 0.63 eV. There are two stages in the process of hydrogen incorporation, which are hydrogen diffusion on the surface and the penetration from the surface into the subsurface. Two possible pathways of atomic hydrogen penetration from surface into subsurface are found. The calculations of electronic structures show that the hybridization between the s orbital of H and the s orbitals of Mg is major. The Mg-Mg bond on the outmost surface is shortened from 4.48 Å to 3.30 Å after the hydrogen adsorption on C sites, showing the strong interaction between Mg and H atoms.

  16. Novel alternating polymer adsorption/surface activation self-assembled film based on hydrogen bond

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Yongjun; Yang Shuguang; Guan Ying; Miao Xiaopeng; Cao Weixiao; Xu Jian

    2003-08-01

    By combining hydrogen bonding layer-by-layer self-assembly and the stepwise chemisorption method, a new alternating polymer adsorption/surface activation self-assembly method was developed. First a layer of diphenylamine-4-diazonium-formaldehyde resin (diazo resin or DR) is deposited on a substrate. In the following surface activation step, the diazonium groups on the surface couple with resorcin in the outside solution. The deposition of another layer of DR is feasible due to the formation of hydrogen bond between the diazonium group of DR and the hydroxy group of the resorcin moieties. The resulting film is photosensitive. After UV irradiation, the film becomes very stable towards polar organic solvents.

  17. Enhanced reactive adsorption of hydrogen sulfide on the composites of graphene/graphite oxide with copper (hydr)oxychlorides.

    Science.gov (United States)

    Mabayoje, Oluwaniyi; Seredych, Mykola; Bandosz, Teresa J

    2012-06-27

    Composites of copper (hydr)oxychlorides with graphite oxide or graphene were synthesized and used as adsorbents of hydrogen sulfide at dynamic conditions at ambient temperatures. The materials were extensively characterized before and after adsorption in order to link their performance to the surface features. X-ray diffraction, FTIR, thermal analysis, TEM, SEM/EDX, and adsorption of nitrogen were used. It was found that the composite with graphene has the most favorable surface features enhancing reactive adsorption of hydrogen sulfide. The presence of moisture in the H2S stream has a positive effect on the removal process owing to the dissociation process. H2S is retained on the surface via a direct replacement of OH groups and via acid-base reactions with the copper (hydr)oxide. Highly dispersed reduced copper species on the surface of the composite with graphene enhance activation of oxygen and cause formation of sulfites and sulfates. Higher conductivity of the graphene phase than that of graphite oxide helps in electron transfer in redox reactions.

  18. EFFECT OF DIATOMEAOUS EARTH TREATMENT USING HYDROGEN CHLORIDE AND SULFURIC ACID ON KINETICS OF CADMIUM(II ADSORPTION

    Directory of Open Access Journals (Sweden)

    Nuryono Nuryono

    2010-06-01

    Full Text Available In this research, treatment of diatomaceous earth, Sangiran, Central Java using hydrogen chloride (HCl and sulfuric acid (H2SO4 on kinetics of Cd(II adsorption in aqueous solution has been carried out. The work was conducted by mixing an amount of grounded diatomaceous earth (200 mesh in size with HCl or H2SO4 solution in various concentrations for two hours at temperature range of 100 - 150oC. The mixture was then filtered and washed with water until the filtrate pH is approximately 7 and then the residue was dried for four hours at a temperature of 70oC. The product was used as an adsorbent to adsorb Cd(II in aqueous solution with various concentrations. The Cd(II adsorbed was determined by analyzing the rest of Cd(II in the solution using atomic absorption spectrophotometry. The effect of treatment was evaluated from kinetic parameter of adsorption rate constant calculated based on the simple kinetic model. Results showed  that before equilibrium condition reached, adsorpstion of Cd(II occurred through two steps, i.e. a step tends to follow a reaction of irreversible first order  (step I followed by reaction of reversible first order (step II. Treatment with acids, either hydrogen chloride or sulfuric acid, decreased adsorption rate constant for the step I from 15.2/min to a range of 6.4 - 9.4/min.  However, increasing concentration of acid (in a range of concentration investigated did not give significant and constant change of adsorption rate constant. For step II process,  adsorption involved physical interaction with the sufficient low adsorption energy (in a range of 311.3 - 1001 J/mol.     Keywords: adsorption, cdmium, diatomaceous earth, kinetics.

  19. Adsorption and diffusion characteristics of lithium on hydrogenated α- and β-silicene

    Directory of Open Access Journals (Sweden)

    Fadil Iyikanat

    2017-08-01

    Full Text Available Using first-principles density functional theory calculations, we investigate adsorption properties and the diffusion mechanism of a Li atom on hydrogenated single-layer α- and β-silicene on a Ag(111 surface. It is found that a Li atom binds strongly on the surfaces of both α- and β-silicene, and it forms an ionic bond through the transfer of charge from the adsorbed atom to the surface. The binding energies of a Li atom on these surfaces are very similar. However, the diffusion barrier of a Li atom on H-α-Si is much higher than that on H-β-Si. The energy surface calculations show that a Li atom does not prefer to bind in the vicinity of the hydrogenated upper-Si atoms. Strong interaction between Li atoms and hydrogenated silicene phases and low diffusion barriers show that α- and β-silicene are promising platforms for Li-storage applications.

  20. Nanotube Adsorption for the Capture and Re-liquefaction of Hydrogen Biol-Off During Tanker Transfer Operations, Phase I

    Data.gov (United States)

    National Aeronautics and Space Administration — This proposal discloses an innovative, economically feasible technique to capture and re-liquefy the hydrogen boil-off by using carbon nanotube adsorption prior to...

  1. Enhanced hydrogen storage on Li-doped defective graphene with B substitution: A DFT study

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Yanan [School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan (China); Chu, Wei, E-mail: chuwei1965@scu.edu.cn [School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan (China); Jing, Fangli [School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan (China); Zheng, Jian [State Key Laboratory Cultivation Base for Nonmetal Composites and Functional Materials, Southwest University of Science and Technology, Mianyang, 621010 (China); Sun, Wenjing [China-America Cancer Research Institute, Key Laboratory for Medical Molecular Diagnostics of Guangdong Province, Guangdong Medical University, Dongguan, Guangdong 523808 (China); Xue, Ying [Key Laboratory Green Chemistry & Technology of Ministry of Education (MOE), College of Chemistry, Sichuan University, Chengdu 610064, Sichuan (China)

    2017-07-15

    Highlights: • Li atoms were found to be well dispersed on defective structures without clustering. • First H{sub 2} with five different initial configurations on Li/MV, Li/DV, Li/BMV, Li/BDV were explored in order. • Each system could bind up to three H{sub 2} molecules with hydrogen average adsorption energies close to the range of 0.2–0.4 eV. • H{sub 2} molecules bind with systems through weak electrostatic interaction between Li cation and induced H{sub 2} dipole. • H{sub 2} adsorption and desorption on the studied systems can process under ambient conditions. - Abstract: The characteristics of hydrogen adsorption on Li-doped defective graphene systems were investigated using density functional theory (DFT) calculations. Four types of defective structures were selected. Li atoms were well dispersed on the defective graphene without clustering, evidenced by the binding energy value between Li and defective graphene than that of Li-Li{sub x}. Additionally, as the amount of adsorbed H{sub 2} molecules increase, the H{sub 2} molecules show tilting configuration toward the Li adatom. This is beneficial for more hydrogen adsorption under the electrostatic interaction. On these four stable structures, there were up to three polarized H{sub 2} molecules adsorbed on per Li adatom, with the average hydrogen adsorption energy in the range of approximately 0.2–0.4 eV. These results provide new focus on the nature of Li-doped defective graphene with sometimes B substitution medium, which could be considered as a promising candidate for hydrogen storage.

  2. Excess Adsorption Isotherms of Hydrogen on Activated Carbons from Agricultural Waste Materials.

    Czech Academy of Sciences Publication Activity Database

    Soukup, Karel; Hejtmánek, Vladimír; Cruz, G.J.F.; Jandová, Věra; Šolcová, Olga

    2017-01-01

    Roč. 40, č. 5 (2017), s. 900-906 ISSN 0930-7516. [International Congress of Chemical and Process Engineering CHISA 2016 and the 19th Conference PRES 2016 /22./. Prague, 27.08.2016-31.08.2016] R&D Projects: GA ČR GA15-14228S Grant - others:NUT(PE) 0722-2014/UNT-R Institutional support: RVO:67985858 Keywords : activated carbon * hydrogen * excess adsorption Subject RIV: CI - Industrial Chemistry, Chemical Engineering OBOR OECD: Chemical process engineering Impact factor: 2.051, year: 2016

  3. Carbon dioxide adsorption in graphene sheets

    Directory of Open Access Journals (Sweden)

    Ashish Kumar Mishra

    2011-09-01

    Full Text Available Control over the CO2 emission via automobiles and industrial exhaust in atmosphere, is one of the major concerns to render environmental friendly milieu. Adsorption can be considered to be one of the more promising methods, offering potential energy savings compared to absorbent systems. Different carbon nanostructures (activated carbon and carbon nanotubes have attracted attention as CO2 adsorbents due to their unique surface morphology. In the present work, we have demonstrated the CO2 adsorption capacity of graphene, prepared via hydrogen induced exfoliation of graphitic oxide at moderate temperatures. The CO2 adsorption study was performed using high pressure Sieverts apparatus and capacity was calculated by gas equation using van der Waals corrections. Physical adsorption of CO2 molecules in graphene was confirmed by FTIR study. Synthesis of graphene sheets via hydrogen exfoliation is possible at large scale and lower cost and higher adsorption capacity of as prepared graphene compared to other carbon nanostructures suggests its possible use as CO2 adsorbent for industrial application. Maximum adsorption capacity of 21.6 mmole/g was observed at 11 bar pressure and room temperature (25 ºC.

  4. Effects of hydrogen adsorption on the properties of double wall BN and (BN){sub x}C{sub y} nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Freitas, A. [Departamento de Física, Universidade Federal da Paraíba, Caixa Postal 5008, 58059-900 João Pessoa, PB (Brazil); Azevedo, S., E-mail: sazevedo@fisica.ufpb.br [Departamento de Física, Universidade Federal da Paraíba, Caixa Postal 5008, 58059-900 João Pessoa, PB (Brazil); Kaschny, J.R. [Instituto Federal da Bahia – Campus Vitoria da Conquista, Avenida Amazonas 3150, 45030-220 Vitória da Conquista, BA (Brazil)

    2016-01-15

    In the present contribution, we apply first-principles calculations, based on the density functional theory, to study the effects of hydrogen adsorption on the structural and electronic properties of boron nitride and hybrid carbon–boron nitride double wall nanotubes. The results demonstrate that the hydrogen decoration induces significant structural deformation and an appreciable reduction in the gap energy. When the number of hydrogen atoms introduced on the outer wall is increased, desorption of hydrogen pairs are observed. The calculations indicate that each adsorbed hydrogen atom induces a structural deformation with an energetic cost of about 68 meV/atom. It is also found that the introduction of hydrogen atoms can be applied as an efficient tool for tuning the electronic properties of such structures. - Graphical abstract: Localized density of states of a hydrogenated double wall boron nitride nanotube. Some hydrogen pairs are desorbed, forming H{sub 2} molecules. - Highlights: • Hydrogenation induces structural deformation and reduction in the gap energy. • Each H atom induces a deformation with an energetic cost of about 68 meV/atom. • In some cases, desorption of H pairs from the outer wall is observed.

  5. Studies of effects on determination of trace hydrogen in U-Nb alloy

    International Nuclear Information System (INIS)

    Zou Lexi; Li Yingqiu; Liu Jun; Wu Lunqiang; Qi Lianzhu; Bian Min

    2002-01-01

    The affecting factors for determination of trace hydrogen in U-Nb alloy are studied. The status of samples affects greatly the measured hydrogen content, which has the higher value for scrap sample than cylinder sample. The hydrogen content in cylinder is closer to real value in U-Nb alloy. The hydrogen in U-Nb alloy is mainly from surface adsorption. The results of hydrogen determined by vacuum thermal evolved method, in which the relative standard uncertainty is less than 28%, are in agreement with those by inert-gas fusion method

  6. First-principles study of H, O, and N adsorption on metal embedded carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Li, Detian [Science and Technology on Vacuum Technology and Physics Laboratory, Lanzhou Institute of Physics, Lanzhou, Gansu 730000 (China); Institute of Micro-nano Structures & Optoelectronics, Wenzhou University, Wenzhou, Zhejiang 325035 (China); Luo, Haijun, E-mail: luohaijun@wzu.edu.cn [Institute of Micro-nano Structures & Optoelectronics, Wenzhou University, Wenzhou, Zhejiang 325035 (China); Cai, Jianqiu [Institute of Micro-nano Structures & Optoelectronics, Wenzhou University, Wenzhou, Zhejiang 325035 (China); Cheng, Yongjun [Science and Technology on Vacuum Technology and Physics Laboratory, Lanzhou Institute of Physics, Lanzhou, Gansu 730000 (China); Shao, Xiji [Institute of Micro-nano Structures & Optoelectronics, Wenzhou University, Wenzhou, Zhejiang 325035 (China); Dong, Changkun, E-mail: dck@wzu.edu.cn [Science and Technology on Vacuum Technology and Physics Laboratory, Lanzhou Institute of Physics, Lanzhou, Gansu 730000 (China); Institute of Micro-nano Structures & Optoelectronics, Wenzhou University, Wenzhou, Zhejiang 325035 (China)

    2017-05-01

    Highlights: • Ni or Fe embedment and high atomic adsorption coverage benefit applications like hydrogen storage and field emission. • Ni or Fe embedment could help tune the catalytic properties. • Ni or Fe embedment enhances the adatom-SWNT interaction significantly. - Abstract: The density functional theory calculation has been conducted to investigate the structural and electronic properties, including the adsorption energies, bond structures, work functions, charge transfer behaviors, and density of states for pristine, Ni-, and Fe-embedded capped (5, 5) single-walled carbon nanotubes (SWNTs) with different coverage of atomic hydrogen, oxygen, and nitrogen adsorptions. Ni or Fe embedment enhances the adatom-SWNT interactions significantly for three kinds of gas atoms with the increases of the adsorption energies. The SWNT work function drops with H adsorption, while Ni or Fe embedment assists further the reduction. When increasing the coverage, the adsorption energy decreases and the work function climbs for O adsorption, but the nitrogen adsorption energy increases. The Bader charge transfer analysis implies that the cap possesses higher oxygen reduction activities than the tube, and the density of states analysis shows that Ni or Fe embedment deepens the C-adatom hybridizations.

  7. Kelvin probe force microscopy studies of the charge effects upon adsorption of carbon nanotubes and C60 fullerenes on hydrogen-terminated diamond

    Science.gov (United States)

    Kölsch, S.; Fritz, F.; Fenner, M. A.; Kurch, S.; Wöhrl, N.; Mayne, A. J.; Dujardin, G.; Meyer, C.

    2018-01-01

    Hydrogen-terminated diamond is known for its unusually high surface conductivity that is ascribed to its negative electron affinity. In the presence of acceptor molecules, electrons are expected to transfer from the surface to the acceptor, resulting in p-type surface conductivity. Here, we present Kelvin probe force microscopy (KPFM) measurements on carbon nanotubes and C60 adsorbed onto a hydrogen-terminated diamond(001) surface. A clear reduction in the Kelvin signal is observed at the position of the carbon nanotubes and C60 molecules as compared with the bare, air-exposed surface. This result can be explained by the high positive electron affinity of carbon nanotubes and C60, resulting in electron transfer from the surface to the adsorbates. When an oxygen-terminated diamond(001) is used instead, no reduction in the Kelvin signal is obtained. While the presence of a charged adsorbate or a difference in work function could induce a change in the KPFM signal, a charge transfer effect of the hydrogen-terminated diamond surface, by the adsorption of the carbon nanotubes and the C60 fullerenes, is consistent with previous theoretical studies.

  8. A three-site Langmuir adsorption model to elucidate the temperature, pressure, and support dependence of the hydrogen coverage on supported Pt particles

    NARCIS (Netherlands)

    Ji, Y.; Koot, V.; van der Eerden, A.M.J.; Weckhuysen, B.M.; Koningsberger, D.C.; Ramaker, D.E.

    2007-01-01

    The three-site adsorption model, previously developed to describe H adsorption on small Pt particles, was used to gain insight into dependence of hydrogen coverage on temperature, pressure, and support ionicity. The three sites, in order of decreasing PtH bond strength, involve H in an atop, a

  9. Hydrogen storage by physisorption on porous materials

    Energy Technology Data Exchange (ETDEWEB)

    Panella, B

    2006-09-13

    A great challenge for commercializing hydrogen powered vehicles is on-board hydrogen storage using economic and secure systems. A possible solution is hydrogen storage in light-weight solid materials. Here three principle storage mechanisms can be distinguished: i) absorption of hydrogen in metals ii) formation of compounds with ionic character, like complex hydrides and iii) physisorption (or physical adsorption) of hydrogen molecules on porous materials. Physical adsorption exhibits several advantages over chemical hydrogen storage as for example the complete reversibility and the fast kinetics. Two classes of porous materials were investigated for physical hydrogen storage, i.e. different carbon nanostructures and crystalline metal-organic frameworks possessing extremely high specific surface area. Hydrogen adsorption isotherms were measured using a Sieverts' apparatus both at room temperature and at 77 K at pressures up to the saturation regime. Additionally, the adsorption sites of hydrogen in these porous materials were identified using thermal desorption spectroscopy extended to very low temperatures (down to 20 K). Furthermore, the adsorbed hydrogen phase was studied in various materials using Raman spectroscopy at different pressures and temperatures. The results show that the maximum hydrogen storage capacity of porous materials correlates linearly with the specific surface area and is independent of structure and composition. In addition the pore structure of the adsorbent plays an important role for hydrogen storage since the adsorption sites for H2 could be assigned to pores possessing different dimensions. Accordingly it was shown that small pores are necessary to reach high storage capacities already at low pressures. This new understanding may help to tailor and optimize new porous materials for hydrogen storage. (orig.)

  10. Hydrogen storage by physisorption on porous materials

    Energy Technology Data Exchange (ETDEWEB)

    Panella, B.

    2006-09-13

    A great challenge for commercializing hydrogen powered vehicles is on-board hydrogen storage using economic and secure systems. A possible solution is hydrogen storage in light-weight solid materials. Here three principle storage mechanisms can be distinguished: i) absorption of hydrogen in metals ii) formation of compounds with ionic character, like complex hydrides and iii) physisorption (or physical adsorption) of hydrogen molecules on porous materials. Physical adsorption exhibits several advantages over chemical hydrogen storage as for example the complete reversibility and the fast kinetics. Two classes of porous materials were investigated for physical hydrogen storage, i.e. different carbon nanostructures and crystalline metal-organic frameworks possessing extremely high specific surface area. Hydrogen adsorption isotherms were measured using a Sieverts' apparatus both at room temperature and at 77 K at pressures up to the saturation regime. Additionally, the adsorption sites of hydrogen in these porous materials were identified using thermal desorption spectroscopy extended to very low temperatures (down to 20 K). Furthermore, the adsorbed hydrogen phase was studied in various materials using Raman spectroscopy at different pressures and temperatures. The results show that the maximum hydrogen storage capacity of porous materials correlates linearly with the specific surface area and is independent of structure and composition. In addition the pore structure of the adsorbent plays an important role for hydrogen storage since the adsorption sites for H2 could be assigned to pores possessing different dimensions. Accordingly it was shown that small pores are necessary to reach high storage capacities already at low pressures. This new understanding may help to tailor and optimize new porous materials for hydrogen storage. (orig.)

  11. On the problem of low-temperature air adsorption studies by the volume method

    International Nuclear Information System (INIS)

    Gur'yanov, V.V.; Gashin, V.M.; Shcherbakov, V.P.; Misin, M.S.; Sizova, G.P.

    1975-01-01

    The properties of a porous structure and the adsorption of a series of carbon adsorbents at 77 K were studied. It was shown that isotherms may be constructed within the framework of the theory of volume filling only for a degree of filling of theta>20.5. Deviations from theoretical curves are observed with practically no accumulation in the high-vacuum equipment of carbon-adsorbed helium, hydrogen, and neon. Therefore the initial parts of the air-adsorption isotherm at 77 K may not be used for characterizing the adsorption properties and parameters of the porous structure of a microporous adsorbent. The effect of adsorbent microporosity on the adsorption isotherm begins to appear only when the pressure of the poorly sorbed components of the air is less than the total pressure of the nitrogen and oxygen

  12. Theoretical Investigation of Hydrogen Adsorption and Dissociation on Iron and Iron Carbide Surfaces Using the ReaxFF Reactive Force Field Method

    Energy Technology Data Exchange (ETDEWEB)

    Zou, Chenyu; van Duin, Adri C.T.; Sorescu, Dan C.

    2012-06-01

    We have developed a ReaxFF reactive force field to describe hydrogen adsorption and dissociation on iron and iron carbide surfaces relevant for simulation of Fischer–Tropsch (FT) synthesis on iron catalysts. This force field enables large system (>>1000 atoms) simulations of hydrogen related reactions with iron. The ReaxFF force field parameters are trained against a substantial amount of structural and energetic data including the equations of state and heats of formation of iron and iron carbide related materials, as well as hydrogen interaction with iron surfaces and different phases of bulk iron. We have validated the accuracy and applicability of ReaxFF force field by carrying out molecular dynamics simulations of hydrogen adsorption, dissociation and recombination on iron and iron carbide surfaces. The barriers and reaction energies for molecular dissociation on these two types of surfaces have been compared and the effect of subsurface carbon on hydrogen interaction with iron surface is evaluated. We found that existence of carbon atoms at subsurface iron sites tends to increase the hydrogen dissociation energy barrier on the surface, and also makes the corresponding hydrogen dissociative state relatively more stable compared to that on bare iron. These properties of iron carbide will affect the dissociation rate of H{sub 2} and will retain more surface hydride species, thus influencing the dynamics of the FT synthesis process.

  13. Equilibrium curve determination of HF adsorption by activated carbon

    International Nuclear Information System (INIS)

    Bahrami, H.; Safdari, S. J.; Mousavian, S. M. A.

    2010-01-01

    One of the byproducts of uranium enrichment industry is hydrogen fluoride gas. Due to the toxicity and corrosivity of the molecule, it has adverse effects on the environment and the process. Therefore, it must be removed by adsorption towers. The activated carbon is one of the proposed sorbent for the adsorption. Hydrogen fluoride adsorption equilibrium curve gives important information for designing the adsorption towers. In this article, the hydrogen fluoride adsorption and adsorption factors were determined experimentally, and four different types of carbon have been used. The operating pressure in all tests was less than 30 mbar. Comparison between the obtained experimental equilibrium curves shows that the first, second and fourth types of activated carbon are suitable for the adsorption of hydrogen fluoride. The experimental data were fitted using mathematical models of Langmuir, Freundlich, Toth and Henry. The results show that Toth mathematical model is more suitable than other models. Also, the absolute error were predicted by the model of Toth for the first, second and fourth types of the activated carbon were 12.9, 16.5 and 34 percent, respectively.

  14. Capillary condensation and adsorption of binary mixtures.

    Science.gov (United States)

    Weinberger, B; Darkrim-Lamari, F; Levesque, D

    2006-06-21

    The adsorption of equimolar binary mixtures of hydrogen-carbon dioxide, hydrogen-methane, and methane-carbon dioxide in porous material models is determined by grand canonical Monte Carlo simulations. The material models have an adsorbent surface similar to that of nanofibers with a herringbone structure. Our main result, which is relevant for hydrogen purification and carbon dioxide capture, is that the adsorption selectivities calculated for the mixtures can differ significantly from those deduced from simulations of the adsorption of pure gases, in particular, when one of the adsorbed gases presents a capillary condensation induced by confinement within the pore network. A comparison of our data is also made with theoretical models used in the literature for predicting the properties of the mixture adsorption.

  15. Study of Supported Nickel Catalysts Prepared by Aqueous Hydrazine Method. Hydrogenating Properties and Hydrogen Storage: Support Effect. Silver Additive Effect

    International Nuclear Information System (INIS)

    Wojcieszak, R.

    2006-06-01

    We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports (γ-Al 2 O 3 , amorphous or crystallized SiO 2 , Nb 2 O 5 , CeO 2 and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N 2 , FTIR and FTIR-Pyridine, TEM, STEM, EDS, H 2 -TPR, H 2 -adsorption, H 2 -TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO 2 or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

  16. Adsorption of guanidinium collectors on aluminosilicate minerals - a density functional study.

    Science.gov (United States)

    Nulakani, Naga Venkateswara Rao; Baskar, Prathab; Patra, Abhay Shankar; Subramanian, Venkatesan

    2015-10-07

    In this density functional theory based investigation, we have modelled and studied the adsorption behaviour of guanidinium cations and substituted (phenyl, methoxy phenyl, nitro phenyl and di-nitro phenyl) guanidinium cationic collectors on the basal surfaces of kaolinite and goethite. The adsorption behaviour is assessed in three different media, such as gas, explicit water and pH medium, to understand the affinity of GC collectors to the SiO4 tetrahedral and AlO6 octahedral surfaces of kaolinite. The tetrahedral siloxane surface possesses a larger binding affinity to GC collectors than the octahedral sites due to the presence of surface exposed oxygen atoms that are active in the intermolecular interactions. Furthermore, the inductive electronic effects of substituted guanidinium cations also play a key role in the adsorption mechanism. Highly positive cations result in a stronger electrostatic interaction and preferential adsorption with the kaolinite surfaces than low positive cations. Computed interaction energies and electron densities at the bond critical points suggest that the adsorption of guanidinium cations on the surfaces of kaolinite and goethite is due to the formation of intra/inter hydrogen bonding networks. Also, the electrostatic interaction favours the high adsorption ability of GC collectors in the pH medium than gas phase and water medium. The structures and energies of GC collectors pave an intuitive view for future experimental studies on mineral flotation.

  17. Study on Shale Adsorption Equation Based on Monolayer Adsorption, Multilayer Adsorption, and Capillary Condensation

    Directory of Open Access Journals (Sweden)

    Qing Chen

    2017-01-01

    Full Text Available Shale gas is an effective gas resource all over the world. The evaluation of pore structure plays a critical role in exploring shale gas efficiently. Nitrogen adsorption experiment is one of the significant approaches to analyze pore size structure of shale. Shale is extremely heterogeneous due to component diversity and structure complexity. Therefore, adsorption isotherms for homogeneous adsorbents and empirical isotherms may not apply to shale. The shape of adsorption-desorption curve indicates that nitrogen adsorption on shale includes monolayer adsorption, multilayer adsorption, and capillary condensation. Usually, Langmuir isotherm is a monolayer adsorption model for ideal interfaces; BET (Brunauer, Emmett, Teller adsorption isotherm is a multilayer adsorption model based on specific assumptions; Freundlich isotherm is an empirical equation widely applied in liquid phase adsorption. In this study, a new nitrogen adsorption isotherm is applied to simultaneously depict monolayer adsorption, multilayer adsorption, and capillary condensation, which provides more real and accurate representation of nitrogen adsorption on shale. In addition, parameters are discussed in relation to heat of adsorption which is relevant to the shape of the adsorption isotherm curve. The curve fitting results indicate that our new nitrogen adsorption isotherm can appropriately describe the whole process of nitrogen adsorption on shale.

  18. Effect of active zinc oxide dispersion on reduced graphite oxide for hydrogen sulfide adsorption at mid-temperature

    Science.gov (United States)

    Song, Hoon Sub; Park, Moon Gyu; Croiset, Eric; Chen, Zhongwei; Nam, Sung Chan; Ryu, Ho-Jung; Yi, Kwang Bok

    2013-09-01

    Composites of Zinc oxide (ZnO) with reduced graphite oxide (rGO) were synthesized and used as adsorbents for hydrogen sulfide (H2S) at 300 °C. Various characterization methods (TGA, XRD, FT-IR, TEM and XPS) were performed in order to link their H2S adsorption performance to the properties of the adsorbent's surface. Microwave-assisted reduction process of graphite oxide (GO) provided mild reduction environment, allowing oxygen-containing functional groups to remain on the rGO surface. It was confirmed that for the ZnO/rGO synthesize using the microwave-assisted reduction method, the ZnO particle size and the degree of ZnO dispersion remained stable over time at 300 °C, which was not the case for only the ZnO particles themselves. This stable highly dispersed feature allows for sustained high surface area over time. This was confirmed through breakthrough experiments for H2S adsorption where it was found that the ZnO/rGO composite showed almost four times higher ZnO utilization efficiency than ZnO itself. The effect of the H2 and CO2 on H2S adsorption was also investigated. The presence of hydrogen in the H2S stream had a positive effect on the removal of H2S since it allows a reducing environment for Znsbnd O and Znsbnd S bonds, leading to more active sites (Zn2+) to sulfur molecules. On the other hand, the presence of carbon dioxide (CO2) showed the opposite trend, likely due to the oxidation environment and also due to possible competitive adsorption between H2S and CO2.

  19. Effect of active zinc oxide dispersion on reduced graphite oxide for hydrogen sulfide adsorption at mid-temperature

    International Nuclear Information System (INIS)

    Song, Hoon Sub; Park, Moon Gyu; Croiset, Eric; Chen, Zhongwei; Nam, Sung Chan; Ryu, Ho-Jung; Yi, Kwang Bok

    2013-01-01

    Composites of Zinc oxide (ZnO) with reduced graphite oxide (rGO) were synthesized and used as adsorbents for hydrogen sulfide (H 2 S) at 300 °C. Various characterization methods (TGA, XRD, FT-IR, TEM and XPS) were performed in order to link their H 2 S adsorption performance to the properties of the adsorbent's surface. Microwave-assisted reduction process of graphite oxide (GO) provided mild reduction environment, allowing oxygen-containing functional groups to remain on the rGO surface. It was confirmed that for the ZnO/rGO synthesize using the microwave-assisted reduction method, the ZnO particle size and the degree of ZnO dispersion remained stable over time at 300 °C, which was not the case for only the ZnO particles themselves. This stable highly dispersed feature allows for sustained high surface area over time. This was confirmed through breakthrough experiments for H 2 S adsorption where it was found that the ZnO/rGO composite showed almost four times higher ZnO utilization efficiency than ZnO itself. The effect of the H 2 and CO 2 on H 2 S adsorption was also investigated. The presence of hydrogen in the H 2 S stream had a positive effect on the removal of H 2 S since it allows a reducing environment for Zn-O and Zn-S bonds, leading to more active sites (Zn 2+ ) to sulfur molecules. On the other hand, the presence of carbon dioxide (CO 2 ) showed the opposite trend, likely due to the oxidation environment and also due to possible competitive adsorption between H 2 S and CO 2 .

  20. Detection of hydrogen peroxide with graphyne

    Science.gov (United States)

    Majidi, R.; Karami, A. R.

    2013-12-01

    The effect of hydrogen peroxide on the electronic properties of graphyne has been investigated to explore the possibility of using graphyne based biosensor. We have used density functional theory to study the electronic properties of γ-graphyne in the presence of different number of hydrogen peroxide. The optimal adsorption position, orientation, and distance of hydrogen peroxide adsorbed on the graphyne sheet have been determined by calculating adsorption energy. It is found that γ-graphyne which is an intrinsic semiconductor becomes an n-type semiconductor due to the presence of hydrogen peroxide. The energy band gap of γ-graphyne is decreased by increasing the number of hydrogen peroxide. The results demonstrate that γ-graphyne is a promising candidate for biosensor application because of its electrical sensitivity to hydrogen peroxide.

  1. Water on TiO2 studied by work function change: adsorption in cycles

    International Nuclear Information System (INIS)

    Bundaleski, Nenad; Silva, Ana G; Jean-Shaw, Bobbie; Teodoro, Orlando; Moutinho, Augusto

    2013-01-01

    The nature of water adsorption on TiO 2 (110) rutile surface attracts a lot of attention for quite some time. In spite of the considerable experimental and theoretical efforts a lot of details remain unclear. We have been using work function study to follow the adsorption of water on TiO 2 at room temperature, and interpreted the results in terms of fast dissociative adsorption on bridging oxygen vacancies (BOV) and much slower non-dissociative adsorption on Ti 5f rows. Additionally, we concluded that water from Ti 5f rows efficiently desorbs at room temperature which is not the case for BOV adsorption sites. Here we propose a novel experimental approach which consists of monitoring in real-time the work function change during cycles of water adsorption. Since desorption at BOVs does not take place at room temperature, this method allows us to resolve the adsorption dynamics on the two adsorption sites. The first results changed our understanding of the phenomenon: we show that both, adsorption on BOVs and Ti 5f are both very fast. Additionally, slow exponential decay of the work function is observed, which is not directly related to water adsorption. The possible explanation of the third slow contribution could be related to the migration of hydrogen atoms along the bridging oxygen rows.

  2. Probing the structure, stability and hydrogen adsorption of lithium functionalized isoreticular MOF-5 (Fe, Cu, Co, Ni and Zn) by density functional theory.

    Science.gov (United States)

    Venkataramanan, Natarajan Sathiyamoorthy; Sahara, Ryoji; Mizuseki, Hiroshi; Kawazoe, Yoshiyuki

    2009-04-14

    Li adsorption on isoreticular MOFs with metal Fe, Cu, Co, Ni and Zn was studied using density function theory. Li functionalization shows a considerable structural change associated with a volume change in isoreticular MOF-5 except for the Zn metal center. Hydrogen binding energies on Li functionalized MOFs are seen to be in the range of 0.2 eV, which is the desired value for an ideal reversible storage system. This study has clearly shown that Li doping is possible only in Zn-based MOF-5, which would be better candidate to reversibly store hydrogen.

  3. Probing the Structure, Stability and Hydrogen Adsorption of Lithium Functionalized Isoreticular MOF-5 (Fe, Cu, Co, Ni and Zn by Density Functional Theory

    Directory of Open Access Journals (Sweden)

    Yoshiyuki Kawazoe

    2009-04-01

    Full Text Available Li adsorption on isoreticular MOFs with metal Fe, Cu, Co, Ni and Zn was studied using density function theory. Li functionalization shows a considerable structural change associated with a volume change in isoreticular MOF-5 except for the Zn metal center. Hydrogen binding energies on Li functionalized MOFs are seen to be in the range of 0.2 eV, which is the desired value for an ideal reversible storage system. This study has clearly shown that Li doping is possible only in Zn-based MOF-5, which would be better candidate to reversibly store hydrogen.

  4. Hydrogen storage using microporous carbon materials

    International Nuclear Information System (INIS)

    B Buczek; E Wolak

    2005-01-01

    In the present century hydrogen will be the most important source of energy and will replace petroleum and petroleum-derived products in the next future. Hydrogen is an almost ideal fuel, both because of its unlimited accessibility and for ecological reasons; the product of its combustion - water vapour - is neither any gaseous contamination nor a component of greenhouse gases. Nowadays hydrogen is applied in industrial processes, but may be also used as a source of house lighting and heating energy, for production of electricity, and as fuel for car engines. Fuel cells, applying reaction between hydrogen and oxygen for production of electricity have been for a long time used in the space technology. Application of hydrogen as fuel should give a possibility of storage and transfer of the high quality energy, i.e. the energy of a high exo-energetic ratio. Due to its low density, one of the main obstacles to the widespread use of hydrogen in energy sector is an efficient storage technology. At present, the methods of hydrogen storage are to liquefy and store in refrigerated containers, which is very expensive, or to store it in high - pressure gas cylinders at room temperature. Unfortunately, low storage density of hydrogen for the latter technique is a significant drawback. Between alternatives have been considered (chemical storage in irreversible hydrogen carriers like methanol or ammonia, reversible metal and chemical hydrides and adsorption in porous media), the latter one seems to lie the most promising. Physical adsorption is a method by which more gas can be stored at a lower pressure by means of Van der Waals interactions at the gas solid interface. Adsorptive storage is particularly promising for permanent gases, which need to be stored, transported, or used in ambient temperature. Thanks to the high density of adsorbed phase, adsorptive storage system could allow the storage of a high density of hydrogen at much lower pressures than compression and higher

  5. A comparative study of the adsorption and hydrogenation of acrolein on Pt(1 1 1), Ni(1 1 1) film and Pt Ni Pt(1 1 1) bimetallic surfaces

    Science.gov (United States)

    Murillo, Luis E.; Chen, Jingguang G.

    In this study we have investigated the reaction pathways for the decomposition and hydrogenation of acrolein (CH 2dbnd CH-CH dbnd O) on Ni/Pt(1 1 1) surfaces under ultra-high vacuum (UHV) conditions using temperature programmed desorption (TPD) and high-resolution electron energy loss spectroscopy (HREELS). While gas-phase hydrogenation products are not observed from clean Pt(1 1 1), the subsurface Pt-Ni-Pt(1 1 1), with Ni residing below the first layer of Pt, is active for the self-hydrogenation of the C dbnd O bond to produce unsaturated alcohol (2-propenol) and the C dbnd C bond to produce saturated aldehyde (propanal), with the latter being the main hydrogenation product without the consecutive hydrogenation to saturated alcohol. For a thick Ni(1 1 1) film prepared on Pt(1 1 1), the self-hydrogenation yields for both products are lower than that from the Pt-Ni-Pt(1 1 1) surface. The presence of pre-adsorbed hydrogen further enhances the selectivity toward C dbnd O bond hydrogenation on the Pt-Ni-Pt(1 1 1) surface. In addition, HREELS studies of the adsorption of the two hydrogenation products, 2-propenol and propanal, are performed on the Pt-Ni-Pt(1 1 1) surface to identify the possible surface intermediates during the reaction of acrolein. The results presented here indicate that the hydrogenation activity and selectivity of acrolein on Pt(1 1 1) can be significantly modified by the formation of the bimetallic surfaces.

  6. Adsorption of Phenol from Aqueous Solutions by Carbon Nanomaterials of One and Two Dimensions: Kinetic and Equilibrium Studies

    Directory of Open Access Journals (Sweden)

    M. de la Luz-Asunción

    2015-01-01

    Full Text Available Carbon nanomaterials have a great potential in environmental studies; they are considered as superior adsorbents of pollutants due to their physical and chemical properties. Functionalization and dimension play an important role in many functions of these nanomaterials including adsorption. In this research, adsorption process was achieved with one-dimension nanomaterials: single walled and multiwalled carbon nanotubes were used as received and after oxidation treatment also two-dimensional nanomaterials were used: graphene oxide and reduced graphene oxide. Carbon nanotubes were modified by hydrogen peroxide under microwave irradiation. The reduction of graphene oxide was achieved by using ascorbic acid. R2 values obtained with the pseudo-second-order model are higher than 0.99. The results demonstrate that Freundlich isotherm provides the best fit for the equilibrium data (R2>0.94. RL values are between 0 and 1; this represents favorable adsorption between carbon nanomaterials and phenol. The adsorption process occurs by π-π interactions and hydrogen bonding and not by electrostatic interactions. The results indicate that the adsorption of phenol on carbon nanomaterials depends on the adsorbents’ surface area, and it is negatively influenced by the presence of oxygenated groups.

  7. Adsorption and activation of methane and methanol on Pt(100) surface: a density functional study

    International Nuclear Information System (INIS)

    Moussounda, P.S.

    2006-11-01

    The activation of methane (CH 4 ) and methanol (CH 3 OH) on Pt(100) surface has been investigated using density functional theory calculations based on plane-wave basis and pseudo-potential. We optimised CH 4 /Pt(100) system. The calculated adsorption energies over the top, bridge and hollow sites are small, weakly dependent on the molecular orientation. The nature of the CH 4 -Pt interaction was examined through the electronic structure changes. The adsorption of methyl (CH 3 ) and hydrogen (H) and the co-adsorption of CH 3 +H were also calculated. From these results, we examined the dissociation of CH 4 to CH 3 +H, and the activation energies found are in good agreement with the experimental and theoretical values. The activation of CH 3 OH/Pt(100) has been studied. All the sites have almost the same adsorption energy. The adsorption of oxygen (O) and the co-adsorption of CH 4 and O were also examined. In addition, the formation of CH 3 OH assuming a one-step mechanism step via the co-adsorption of CH 4 +O has been studied and the barrier height was found to be high. (authors)

  8. Hydrogen production from food wastes and gas post-treatment by CO2 adsorption

    International Nuclear Information System (INIS)

    Redondas, V.; Gómez, X.; García, S.; Pevida, C.; Rubiera, F.; Morán, A.; Pis, J.J.

    2012-01-01

    Highlights: ► The dark fermentation process of food wastes was studied over an extended period. ► Decreasing the HRT of the process negatively affected the specific gas production. ► Adsorption of CO 2 was successfully attained using a biomass type activated carbon. ► H 2 concentration in the range of 85–95% was obtained for the treated gas-stream. - Abstract: The production of H 2 by biological means, although still far from being a commercially viable proposition, offers great promise for the future. Purification of the biogas obtained may lead to the production of highly concentrated H 2 streams appropriate for industrial application. This research work evaluates the dark fermentation of food wastes and assesses the possibility of adsorbing CO 2 from the gas stream by means of a low cost biomass-based adsorbent. The reactor used was a completely stirred tank reactor run at different hydraulic retention times (HRTs) while the concentration of solids of the feeding stream was kept constant. The results obtained demonstrate that the H 2 yields from the fermentation of food wastes were affected by modifications in the hydraulic retention time (HRT) due to incomplete hydrolysis. The decrease in the duration of fermentation had a negative effect on the conversion of the substrate into soluble products. This resulted in a lower amount of soluble substrate being available for metabolisation by H 2 producing microflora leading to a reduction in specific H 2 production. Adsorption of CO 2 from a gas stream generated from the dark fermentation process was successfully carried out. The data obtained demonstrate that the column filled with biomass-derived activated carbon resulted in a high degree of hydrogen purification. Co-adsorption of H 2 S onto the activated carbon also took place, there being no evidence of H 2 S present in the bio-H 2 exiting the column. Nevertheless, the concentration of H 2 S was very low, and this co-adsorption did not affect the CO 2

  9. Effect of active zinc oxide dispersion on reduced graphite oxide for hydrogen sulfide adsorption at mid-temperature

    Energy Technology Data Exchange (ETDEWEB)

    Song, Hoon Sub [Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, N2L3G1 (Canada); Greenhouse Gas Department, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 305-343 (Korea, Republic of); Park, Moon Gyu [Department of Chemical Engineering Education, Chungnam National University, 99 Daehak-ro, Yuseong-gu, Daejeon, 305-764 (Korea, Republic of); Croiset, Eric, E-mail: ecroiset@uwaterloo.ca [Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, N2L3G1 (Canada); Chen, Zhongwei [Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, N2L3G1 (Canada); Nam, Sung Chan; Ryu, Ho-Jung [Greenhouse Gas Department, Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Daejeon, 305-343 (Korea, Republic of); Yi, Kwang Bok, E-mail: cosy32@cnu.ac.kr [Department of Chemical Engineering Education, Chungnam National University, 99 Daehak-ro, Yuseong-gu, Daejeon, 305-764 (Korea, Republic of)

    2013-09-01

    Composites of Zinc oxide (ZnO) with reduced graphite oxide (rGO) were synthesized and used as adsorbents for hydrogen sulfide (H{sub 2}S) at 300 °C. Various characterization methods (TGA, XRD, FT-IR, TEM and XPS) were performed in order to link their H{sub 2}S adsorption performance to the properties of the adsorbent's surface. Microwave-assisted reduction process of graphite oxide (GO) provided mild reduction environment, allowing oxygen-containing functional groups to remain on the rGO surface. It was confirmed that for the ZnO/rGO synthesize using the microwave-assisted reduction method, the ZnO particle size and the degree of ZnO dispersion remained stable over time at 300 °C, which was not the case for only the ZnO particles themselves. This stable highly dispersed feature allows for sustained high surface area over time. This was confirmed through breakthrough experiments for H{sub 2}S adsorption where it was found that the ZnO/rGO composite showed almost four times higher ZnO utilization efficiency than ZnO itself. The effect of the H{sub 2} and CO{sub 2} on H{sub 2}S adsorption was also investigated. The presence of hydrogen in the H{sub 2}S stream had a positive effect on the removal of H{sub 2}S since it allows a reducing environment for Zn-O and Zn-S bonds, leading to more active sites (Zn{sup 2+}) to sulfur molecules. On the other hand, the presence of carbon dioxide (CO{sub 2}) showed the opposite trend, likely due to the oxidation environment and also due to possible competitive adsorption between H{sub 2}S and CO{sub 2}.

  10. Advanced nanostructured materials as media for hydrogen storage

    International Nuclear Information System (INIS)

    David, E.; Niculescu, V.; Armeanu, A.; Sandru, C.; Constantinescu, M.; Sisu, C.

    2005-01-01

    Full text: In a future sustainable energy system based on renewable energy, environmentally harmless energy carriers like hydrogen, will be of crucial importance. One of the major impediments for the transition to a hydrogen based energy system is the lack of satisfactory hydrogen storage alternatives. Hydrogen storage in nanostructured materials has been proposed as a solution for adequate hydrogen storage for a number of applications, in particular for transportation. This paper is a preliminary study with the focus on possibilities for hydrogen storage in zeolites, alumina and nanostructured carbon materials. The adsorption properties of these materials were evaluated in correlation with their internal structure. From N 2 physisorption data the BET surface area (S BET ) , total pore volume (PV), micropore volume (MPV) and total surface area (S t ) were derived. H 2 physisorption measurements were performed at 77 K and a pressure value of 1 bar. From these data the adsorption capacities of sorbent materials were determined. Apparently the microporous adsorbents, e.g activated carbons, display appreciable sorption capacities. Based on their micropore volume, carbon-based sorbents have the largest adsorption capacity for H 2 , over 230 cm 3 (STP)/g, at the previous conditions. By increasing the micropore volume (∼ 1 cm 3 /g) of sorbents and optimizing the adsorption conditions it is expected to obtain an adsorption capacity of ∼ 560 cm 3 (STP)/g, close to targets set for mobile applications. (authors)

  11. Hydrogen adsorption and storage on Palladium – functionalized graphene with NH-dopant: A first principles calculation

    Energy Technology Data Exchange (ETDEWEB)

    Faye, Omar, E-mail: omf071@mail.usask.ca [Department of Mechanical Engineering, College of Engineering, University of Saskatchewan, 57 Campus Drive, Saskatoon, S7N 5A9 Saskatchewan (Canada); Department of Condensed Matter Physics, Cheikh Anta Diop University, Dakar (Senegal); Szpunar, Jerzy A; Szpunar, Barbara [Department of Mechanical Engineering, College of Engineering, University of Saskatchewan, 57 Campus Drive, Saskatoon, S7N 5A9 Saskatchewan (Canada); Beye, Aboubaker Chedikh [Department of Condensed Matter Physics, Cheikh Anta Diop University, Dakar (Senegal)

    2017-01-15

    Highlights: • H{sub 2} adsorption in single and double-sided Pd-G(3x3) and the effect of NH radical on graphene were studied. • Strong interaction of Pd and graphene in double-sided Pd-G(3x3) than that in the single-sided Pd-G(3x3). • The storage capacity was 3.622 wt% with a binding energy of 0.658 eV/H2. • The increase of NH radicals on Pd-G(3x3) enhanced the binding of Pd atoms on the graphene sheet. • We predicted that 2NH-dopant at the opposite site of Pd atoms prevents the desorption of Pd atom from graphene sheet. - Abstract: We conducted a detailed theoretical investigation of the structural and electronic properties of single and double sided Pd-functionalized graphene and NH-doped Pd-functionalized graphene, which are shown to be efficient materials for hydrogen storage. Nitrene radical dopant was an effective addition required for enhancing the Pd binding on the graphene sheet as well as the storage of hydrogen. We found that up to eight H{sub 2} molecules could be adsorbed by double-sided Pd-functionalized graphene at 0 K with an average binding energy in the range 1.315–0.567 eVA gravimetric hydrogen density of 3.622 wt% was reached in the Pd-functionalized graphene on both sides. The binding mechanism of H{sub 2} molecules came not only the polarization mechanism between Pd and H atoms but also from the binding of the Pd atoms on the graphene sheet and the orbital hybridization. The most crucial part of our work is measuring the effect of nitrene radical on the H{sub 2} adsorption on Pd-functionalized graphene. Our calculations predicted that the addition of NH radicals on Pd-functionalized graphene enhance the binding of H{sub 2} molecules, which helps also to avoid the desorption of Pd(H{sub 2}){sub n} (n = 1–5) complexes from graphene sheet. Our results also predict Pd-functionalized NH-doped graphene is a potential hydrogen storage medium for on-board applications.

  12. Hydrogen adsorption and storage on Palladium – functionalized graphene with NH-dopant: A first principles calculation

    International Nuclear Information System (INIS)

    Faye, Omar; Szpunar, Jerzy A; Szpunar, Barbara; Beye, Aboubaker Chedikh

    2017-01-01

    Highlights: • H_2 adsorption in single and double-sided Pd-G(3x3) and the effect of NH radical on graphene were studied. • Strong interaction of Pd and graphene in double-sided Pd-G(3x3) than that in the single-sided Pd-G(3x3). • The storage capacity was 3.622 wt% with a binding energy of 0.658 eV/H2. • The increase of NH radicals on Pd-G(3x3) enhanced the binding of Pd atoms on the graphene sheet. • We predicted that 2NH-dopant at the opposite site of Pd atoms prevents the desorption of Pd atom from graphene sheet. - Abstract: We conducted a detailed theoretical investigation of the structural and electronic properties of single and double sided Pd-functionalized graphene and NH-doped Pd-functionalized graphene, which are shown to be efficient materials for hydrogen storage. Nitrene radical dopant was an effective addition required for enhancing the Pd binding on the graphene sheet as well as the storage of hydrogen. We found that up to eight H_2 molecules could be adsorbed by double-sided Pd-functionalized graphene at 0 K with an average binding energy in the range 1.315–0.567 eVA gravimetric hydrogen density of 3.622 wt% was reached in the Pd-functionalized graphene on both sides. The binding mechanism of H_2 molecules came not only the polarization mechanism between Pd and H atoms but also from the binding of the Pd atoms on the graphene sheet and the orbital hybridization. The most crucial part of our work is measuring the effect of nitrene radical on the H_2 adsorption on Pd-functionalized graphene. Our calculations predicted that the addition of NH radicals on Pd-functionalized graphene enhance the binding of H_2 molecules, which helps also to avoid the desorption of Pd(H_2)_n (n = 1–5) complexes from graphene sheet. Our results also predict Pd-functionalized NH-doped graphene is a potential hydrogen storage medium for on-board applications.

  13. Study of Adsorption Mechanism of Congo Red on Graphene Oxide/PAMAM Nanocomposite

    Science.gov (United States)

    Rafi, Mohammad; Samiey, Babak; Cheng, Chil-Hung

    2018-01-01

    Graphene oxide/poly(amidoamine) (GO/PAMAM) nanocomposite adsorbed high quantities of congo red (CR) anionic dye in 0.1 M NaCl solution, with the maximum adsorption capacity of 198 mg·g−1. The kinetics and thermodynamics of adsorption were investigated to elucidate the effects of pH, temperature, shaking rate, ionic strength, and contact time. Kinetic data were analyzed by the KASRA model and the KASRA, ISO, and pore-diffusion equations. Adsorption adsorption isotherms were studied by the ARIAN model and the Henry, Langmuir, and Temkin equations. It was shown that adsorption sites of GO/PAMAM at experimental conditions were phenolic hydroxyl groups of GO sheets and terminal amine groups of PAMAM dendrimer. Analysis of kinetic data indicated that amine sites were located on the surface, and that hydroxyl sites were placed in the pores of adsorbent. CR molecules interacted with the adsorption sites via hydrogen bonds. The molecules were adsorbed firstly on the amine sites, and then on the internal hydroxyl sites. Adsorption kinetic parameters indicated that the interaction of CR to the –NH3+ sites was the rate-controlling step of adsorption of CR on this site and adsorption activation energies calculated for different parts of this step. On the other hand, kinetic parameters showed that the intraparticle diffusion was the rate-controlling step during the interaction of CR molecules to –OH sites and activation energy of this step was not calculable. Finally, the used GO/PAMAM was completely regenerated by using ethylenediamine. PMID:29587463

  14. Study of Adsorption Mechanism of Congo Red on Graphene Oxide/PAMAM Nanocomposite

    Directory of Open Access Journals (Sweden)

    Mohammad Rafi

    2018-03-01

    Full Text Available Graphene oxide/poly(amidoamine (GO/PAMAM nanocomposite adsorbed high quantities of congo red (CR anionic dye in 0.1 M NaCl solution, with the maximum adsorption capacity of 198 mg·g−1. The kinetics and thermodynamics of adsorption were investigated to elucidate the effects of pH, temperature, shaking rate, ionic strength, and contact time. Kinetic data were analyzed by the KASRA model and the KASRA, ISO, and pore-diffusion equations. Adsorption adsorption isotherms were studied by the ARIAN model and the Henry, Langmuir, and Temkin equations. It was shown that adsorption sites of GO/PAMAM at experimental conditions were phenolic hydroxyl groups of GO sheets and terminal amine groups of PAMAM dendrimer. Analysis of kinetic data indicated that amine sites were located on the surface, and that hydroxyl sites were placed in the pores of adsorbent. CR molecules interacted with the adsorption sites via hydrogen bonds. The molecules were adsorbed firstly on the amine sites, and then on the internal hydroxyl sites. Adsorption kinetic parameters indicated that the interaction of CR to the –NH3+ sites was the rate-controlling step of adsorption of CR on this site and adsorption activation energies calculated for different parts of this step. On the other hand, kinetic parameters showed that the intraparticle diffusion was the rate-controlling step during the interaction of CR molecules to –OH sites and activation energy of this step was not calculable. Finally, the used GO/PAMAM was completely regenerated by using ethylenediamine.

  15. Pd Nanoparticles and MOFs Synergistically Hybridized Halloysite Nanotubes for Hydrogen Storage.

    Science.gov (United States)

    Jin, Jiao; Ouyang, Jing; Yang, Huaming

    2017-12-01

    Natural halloysite nanotubes (HNTs) were hybridized with metal-organic frameworks (MOFs) to prepare novel composites. MOFs were transformed into carbon by carbonization calcination, and palladium (Pd) nanoparticles were introduced to build an emerging ternary compound system for hydrogen adsorption. The hydrogen adsorption capacities of HNT-MOF composites were 0.23 and 0.24 wt%, while those of carbonized products were 0.24 and 0.27 wt% at 25 °C and 2.65 MPa, respectively. Al-based samples showed higher hydrogen adsorption capacities than Zn-based samples on account of different selectivity between metal and hydrogen and approximate porous characteristics. More pore structures are generated by the carbonization reaction from metal-organic frameworks into carbon; high specific surface area, uniform pore size, and large pore volume benefited the hydrogen adsorption ability of composites. Moreover, it was also possible to promote hydrogen adsorption capacity by incorporating Pd. The hydrogen adsorption capacity of ternary compound, Pd-C-H3-MOFs(Al), reached 0.32 wt% at 25 °C and 2.65 MPa. Dissociation was assumed to take place on the Pd particles, then atomic and molecule hydrogen spilled over to the structure of carboxylated HNTs, MOFs, and the carbon products for enhancing the hydrogen adsorption capacity.

  16. Pd Nanoparticles and MOFs Synergistically Hybridized Halloysite Nanotubes for Hydrogen Storage

    Science.gov (United States)

    Jin, Jiao; Ouyang, Jing; Yang, Huaming

    2017-03-01

    Natural halloysite nanotubes (HNTs) were hybridized with metal-organic frameworks (MOFs) to prepare novel composites. MOFs were transformed into carbon by carbonization calcination, and palladium (Pd) nanoparticles were introduced to build an emerging ternary compound system for hydrogen adsorption. The hydrogen adsorption capacities of HNT-MOF composites were 0.23 and 0.24 wt%, while those of carbonized products were 0.24 and 0.27 wt% at 25 °C and 2.65 MPa, respectively. Al-based samples showed higher hydrogen adsorption capacities than Zn-based samples on account of different selectivity between metal and hydrogen and approximate porous characteristics. More pore structures are generated by the carbonization reaction from metal-organic frameworks into carbon; high specific surface area, uniform pore size, and large pore volume benefited the hydrogen adsorption ability of composites. Moreover, it was also possible to promote hydrogen adsorption capacity by incorporating Pd. The hydrogen adsorption capacity of ternary compound, Pd-C-H3-MOFs(Al), reached 0.32 wt% at 25 °C and 2.65 MPa. Dissociation was assumed to take place on the Pd particles, then atomic and molecule hydrogen spilled over to the structure of carboxylated HNTs, MOFs, and the carbon products for enhancing the hydrogen adsorption capacity.

  17. Hydrogen storage using microporous carbon materials

    International Nuclear Information System (INIS)

    Buczek, B.; Wolak, E.

    2005-01-01

    In the present century hydrogen will lie the most important source of energy and will replace petroleum and petroleum-derived products in the next future. Hydrogen is an almost ideal fuel, both because of its unlimited accessibility and for ecological reasons; the product of its combustion - water vapour - is neither any gaseous contamination nor a component of greenhouse gases. Nowadays hydrogen is applied in industrial processes, but may be also used as a source of house lighting and heating energy, for production of electricity, and as fuel for car engines. Fuel cells, applying reaction between hydrogen and oxygen for production of electricity have been for a long time used in the space technology. Application of hydrogen as fuel should give a possibility of storage and transfer of the high quality energy, i.e. the energy of a high exo-energetic ratio[l]. Due to its low density, one of the main obstacles to the widespread use of hydrogen in energy sector is an efficient storage technology. At present, the methods of hydrogen storage are to liquefy and store in refrigerated containers, which is very expensive, or to store it in high - pressure gas cylinders at room temperature. Unfortunately, low storage density of hydrogen for the latter technique is a significant drawback. Between alternatives have been considered (chemical storage in irreversible hydrogen carriers like methanol or ammonia, reversible metal and chemical hydrides and adsorption in porous media), the latter one seems to be the most promising [2]. Physical adsorption is a method by which more gas can be stored at a lower pressure by means of Van der Waals interactions at the gas solid interface. Adsorptive storage is particularly promising for permanent gases, which need to be stored, transported, or used in ambient temperature. Thanks to the high density of adsorbed phase, adsorptive storage system could allow the storage of a high density of hydrogen at much lower pressures than compression and

  18. Hydrogen storage in nanostructured materials

    Energy Technology Data Exchange (ETDEWEB)

    Assfour, Bassem

    2011-02-28

    Hydrogen is an appealing energy carrier for clean energy use. However, storage of hydrogen is still the main bottleneck for the realization of an energy economy based on hydrogen. Many materials with outstanding properties have been synthesized with the aim to store enough amount of hydrogen under ambient conditions. Such efforts need guidance from material science, which includes predictive theoretical tools. Carbon nanotubes were considered as promising candidates for hydrogen storage applications, but later on it was found to be unable to store enough amounts of hydrogen under ambient conditions. New arrangements of carbon nanotubes were constructed and hydrogen sorption properties were investigated using state-of-the-art simulation methods. The simulations indicate outstanding total hydrogen uptake (up to 19.0 wt.% at 77 K and 5.52wt.% at 300 K), which makes these materials excellent candidates for storage applications. This reopens the carbon route to superior materials for a hydrogen-based economy. Zeolite imidazolate frameworks are subclass of MOFs with an exceptional chemical and thermal stability. The hydrogen adsorption in ZIFs was investigated as a function of network geometry and organic linker exchange. Ab initio calculations performed at the MP2 level to obtain correct interaction energies between hydrogen molecules and the ZIF framework. Subsequently, GCMC simulations are carried out to obtain the hydrogen uptake of ZIFs at different thermodynamic conditions. The best of these materials (ZIF-8) is found to be able to store up to 5 wt.% at 77 K and high pressure. We expected possible improvement of hydrogen capacity of ZIFs by substituting the metal atom (Zn{sup 2+}) in the structure by lighter elements such as B or Li. Therefore, we investigated the energy landscape of LiB(IM)4 polymorphs in detail and analyzed their hydrogen storage capacities. The structure with the fau topology was shown to be one of the best materials for hydrogen storage. Its

  19. Hydrogen adsorption in carbon nanostructures compared

    NARCIS (Netherlands)

    Schimmel, H.G.; Nijkamp, M.G.; Kearley, G.J.; Rivera, A.; de Jong, K.P.; Mulder, F.M.

    2004-01-01

    Recent reports continue to suggest high hydrogen storage capacities for some carbon nanostructures due to a stronger interaction between hydrogen and carbon. Here the interaction of hydrogen with activated charcoal, carbon nanofibers, single walled carbon nanotubes (SWNT), and electron beam ‘opened’

  20. Effects of van der Waals density functional corrections on trends in furfural adsorption and hydrogenation on close-packed transition metal surfaces

    Science.gov (United States)

    Liu, Bin; Cheng, Lei; Curtiss, Larry; Greeley, Jeffrey

    2014-04-01

    The hydrogenation of furfural to furfuryl alcohol on Pd(111), Cu(111) and Pt(111) is studied with both standard Density Functional Theory (DFT)-GGA functionals and with van der Waals-corrected density functionals. VdW-DF functionals, including optPBE, optB88, optB86b, and Grimme's method, are used to optimize the adsorption configurations of furfural, furfuryl alcohol, and related intermediates resulting from hydrogenation of furfural, and the results are compared to corresponding values determined with GGA functionals, including PW91 and PBE. On Pd(111) and Pt(111), the adsorption geometries of the intermediates are not noticeably different between the two classes of functionals, while on Cu(111), modest changes are seen in both the perpendicular distance and the orientation of the aromatic ring with respect to the planar surface. In general, the binding energies increase substantially in magnitude as a result of van der Waals contributions on all metals. In contrast, however, dispersion effects on the kinetics of hydrogenation are relatively small. It is found that activation barriers are not significantly affected by the inclusion of dispersion effects, and a Brønsted-Evans-Polanyi relationship developed solely from PW91 calculations on Pd(111) is capable of describing corresponding results on Cu(111) and Pt(111), even when the dispersion effects are included. Finally, the reaction energies and barriers derived from the dispersion-corrected and pure GGA calculations are used to plot simple potential energy profiles for furfural hydrogenation to furfuryl alcohol on the three considered metals, and an approximately constant downshift of the energetics due to the dispersion corrections is observed.

  1. Comprehensive Adsorption Studies of Doxycycline and Ciprofloxacin Antibiotics by Biochars Prepared at Different Temperatures

    Science.gov (United States)

    Zeng, Zhi-wei; Tan, Xiao-fei; Liu, Yun-guo; Tian, Si-rong; Zeng, Guang-ming; Jiang, Lu-hua; Liu, Shao-bo; Li, Jiang; Liu, Ni; Yin, Zhi-hong

    2018-01-01

    This paper comparatively investigated the removal efficiency and mechanisms of rice straw biochars prepared under three pyrolytic temperatures for two kinds of tetracycline and quinolone antibiotics (doxycycline and ciprofloxacin). The influencing factors of antibiotic adsorption (including biochar dosage, pH, background electrolytes, humic acid, initial antibiotics concentration, contact time, and temperature) were comprehensively studied. The results suggest that biochars produced at high-temperature [i.e., 700°C (BC700)], have higher adsorption capacity for the two antibiotics than low-temperature (i.e., 300–500°C) biochars (BC300 and BC500). Higher surface area gives rise to greater volume of micropores and mesopores, and higher graphitic surfaces of the BC700 contributed to its higher functionality. The maximum adsorption capacity was found to be in the following order: DOX > CIP. The π-π EDA interaction and hydrogen bonding might be the predominant adsorption mechanisms. Findings in this study highlight the important roles of high-temperature biochars in controlling the contamination of tetracycline and quinolone antibiotics in the environment. PMID:29637067

  2. Comprehensive adsorption studies of doxycycline and ciprofloxacin antibiotics by biochars prepared at different temperatures

    Science.gov (United States)

    Zeng, Zhi-wei; Tan, Xiao-fei; Liu, Yun-guo; Tian, Si-rong; Zeng, Guang-ming; Jiang, Lu-hua; Liu, Shao-bo; Li, Jiang; Liu, Ni; Yin, Zhi-hong

    2018-03-01

    This paper comparatively investigated the removal efficiency and mechanisms of rice straw biochars prepared under three pyrolytic temperatures for two kinds of tetracycline and quinolone antibiotics (doxycycline and ciprofloxacin). The influencing factors of antibiotic adsorption (including biochar dosage, pH, background electrolytes, humic acid, initial antibiotics concentration, contact time, and temperature) were comprehensively studied. The results suggest that biochars produced at high-temperature (i.e., 700°C (BC700)), have higher adsorption capacity for the two antibiotics than low-temperature (i.e., 300-500°C) biochars (BC300 and BC500). Higher surface area gives rise to greater volume of micropores and mesopores, and higher graphitic surfaces of the BC700 contributed to its higher functionality. The maximum adsorption capacity was found to be in the following order: DOX > CIP. The π-π EDA interaction and hydrogen bonding might be the predominant adsorption mechanisms. Findings in this study highlight the important roles of high-temperature biochars in controlling the contamination of tetracycline and quinolone antibiotics in the environment.

  3. Study of heterogeneous catalytic processes over cobalt, molybdenum and cobalt-molybdenum catalysts supported on alumina by temperature-programmed desorption and temperature-programmed reaction. 1. Adsorption of hydrozen

    International Nuclear Information System (INIS)

    Rozanov, V.V.; Tsao Yamin; Krylov, O.V.

    1996-01-01

    Hydrogen adsorption on reduced, sulphidized and reoxidized specimens of molybdenum-and cobalt-molybdenum-containing catalysts applied on aluminium oxide has been studied by the method of thermal desorption (TD). Comparison of TD spectra of hydrogen and data of X-ray phase analysis of the specimens and mass-spectrometric analysis of the products desorbed from the surface of catalysts after their successive reduction sulphidizing, carbonizing and reoxidation permitted a correlation between various forms of hydrogen adsorption and certain centres on the surface of the catalysts. 12 refs., 2 figs

  4. Final Report: Metal Perhydrides for Hydrogen Storage

    Energy Technology Data Exchange (ETDEWEB)

    Hwang, J-Y.; Shi, S.; Hackney, S.; Swenson, D.; Hu, Y.

    2011-07-26

    H molecule contains one hydrogen atom because the valence of a Li ion is +1. One MgH2 molecule contains two hydrogen atoms because the valence of a Mg ion is +2. In metal perhydrides, a molecule could contain more hydrogen atoms than expected based on the metal valance, i.e. LiH1+n and MgH2+n (n is equal to or greater than 1). When n is sufficiently high, there will be plenty of hydrogen storage capacity to meet future requirements. The existence of hydrogen clusters, Hn+ (n = 5, 7, 9, 11, 13, 15) and transition metal ion-hydrogen clusters, M+(H2)n (n = 1-6), such as Sc(H2)n+, Co(H2)n+, etc., have assisted the development of this concept. Clusters are not stable species. However, their existence stimulates our approach on using electric charges to enhance the hydrogen adsorption in a hydrogen storage system in this study. The experimental and modeling work to verify it are reported here. Experimental work included the generation of cold hydrogen plasma through a microwave approach, synthesis of sorbent materials, design and construction of lab devices, and the determination of hydrogen adsorption capacities on various sorbent materials under various electric field potentials and various temperatures. The results consistently show that electric potential enhances the adsorption of hydrogen on sorbents. NiO, MgO, activated carbon, MOF, and MOF and platinum coated activated carbon are some of the materials studied. Enhancements up to a few hundred percents have been found. In general, the enhancement increases with the electrical potential, the pressure applied, and the temperature lowered. Theoretical modeling of the hydrogen adsorption on the sorbents under the electric potential has been investigated with the density functional theory (DFT) approach. It was found that the interaction energy between hydrogen and sorbent is increased remarkably when an electric field is applied. This increase of binding energy offers a potential solution for DOE when looking for a compromise

  5. Techno-economic assessment of biogas plant upgrading by adsorption of hydrogen sulfide on treated sewage–sludge

    International Nuclear Information System (INIS)

    Aguilera, P.G.; Gutiérrez Ortiz, F.J.

    2016-01-01

    Highlights: • Three processes were considered: desulfurization by adsorption, in-situ sorbent regeneration and its production. • The steam for regeneration was studied considering it as a bought external utility and as an in-situ produced utility. • From the cash flow analysis, the cost of the overall desulfurization process was between 2.5 and 4.0 c€/Nm"3. • A sensitivity analysis was carried out to consider the uncertainty of the methodology. • The competitiveness of the technology seems to be promising versus other biogas H_2S removal technologies. - Abstract: Biogas plant upgrading by adsorption of hydrogen sulfide on treated sewage–sludge was techno-economically assessed. Three different processes were included in the study: the desulfurization of biogas by adsorption, the in-situ regeneration of the adsorbent and its production from sewage-sludge. Biogas plant upgrading was performed for a flow rate of 1000 Nm"3/h of biogas with a H_2S concentration of 2000 ppmv and a breakthrough concentration of 200 ppmv, which is the technical limit value for internal combustion engines. The cost due to the steam required for the in-situ regeneration was evaluated in two different scenarios: as a bought external utility and as an in-situ produced utility, installing an electric or a biogas steam boiler. According to the cash flow analysis carried out, all the options require a similar minimum selling price for the upgraded biogas (about 0.27–0.29 €/Nm"3), with a cost of the overall desulfurization process between 2.5 and 4.0 c€/Nm"3.

  6. Interaction of hydrogen with palladium clusters deposited on graphene

    Energy Technology Data Exchange (ETDEWEB)

    Alonso, Julio A.; Granja, Alejandra; Cabria, Iván; López, María J. [Departamento de Física Teórica, Atómica y Optica, Universidad de Valladolid, 47011 Valladolid (Spain)

    2015-12-31

    Hydrogen adsorption on nanoporous carbon materials is a promising technology for hydrogen storage. However, pure carbon materials do not meet the technological requirements due to the week binding of hydrogen to the pore walls. Experimental work has shown that doping with Pd atoms and clusters enhances the storage capacity of porous carbons. Therefore, we have investigated the role played by the Pd dopant on the enhancement mechanisms. By performing density functional calculations, we have found that hydrogen adsorbs on Pd clusters deposited on graphene following two channels, molecular adsorption and dissociative chemisorption. However, desorption of Pd-H complexes competes with desorption of hydrogen, and consequently desorption of Pd-H complexes would spoil the beneficial effect of the dopant. As a way to overcome this difficulty, Pd atoms and clusters can be anchored to defects of the graphene layer, like graphene vacancies. The competition between molecular adsorption and dissociative chemisorption of H{sub 2} on Pd{sub 6} anchored on a graphene vacancy has been studied in detail.

  7. Interaction of hydrogen with palladium clusters deposited on graphene

    Science.gov (United States)

    Alonso, Julio A.; Granja, Alejandra; Cabria, Iván; López, María J.

    2015-12-01

    Hydrogen adsorption on nanoporous carbon materials is a promising technology for hydrogen storage. However, pure carbon materials do not meet the technological requirements due to the week binding of hydrogen to the pore walls. Experimental work has shown that doping with Pd atoms and clusters enhances the storage capacity of porous carbons. Therefore, we have investigated the role played by the Pd dopant on the enhancement mechanisms. By performing density functional calculations, we have found that hydrogen adsorbs on Pd clusters deposited on graphene following two channels, molecular adsorption and dissociative chemisorption. However, desorption of Pd-H complexes competes with desorption of hydrogen, and consequently desorption of Pd-H complexes would spoil the beneficial effect of the dopant. As a way to overcome this difficulty, Pd atoms and clusters can be anchored to defects of the graphene layer, like graphene vacancies. The competition between molecular adsorption and dissociative chemisorption of H2 on Pd6 anchored on a graphene vacancy has been studied in detail.

  8. A first-principles study of lithium-decorated hybrid boron nitride and graphene domains for hydrogen storage

    International Nuclear Information System (INIS)

    Hu, Zi-Yu; Shao, Xiaohong; Wang, Da; Liu, Li-Min; Johnson, J. Karl

    2014-01-01

    First-principles calculations are performed to investigate the adsorption of hydrogen onto Li-decorated hybrid boron nitride and graphene domains of (BN) x C 1−x complexes with x = 1, 0.25, 0.5, 0.75, 0, and B 0.125 C 0.875 . The most stable adsorption sites for the nth hydrogen molecule in the lithium-decorated (BN) x C 1−x complexes are systematically discussed. The most stable adsorption sites were affected by the charge localization, and the hydrogen molecules were favorably located above the C-C bonds beside the Li atom. The results show that the nitrogen atoms in the substrate planes could increase the hybridization between the 2p orbitals of Li and the orbitals of H 2 . The results revealed that the (BN) x C 1−x complexes not only have good thermal stability but they also exhibit a high hydrogen storage of 8.7% because of their dehydrogenation ability

  9. Hydrogen storage by functionalised Poly(ether ether ketone)

    Energy Technology Data Exchange (ETDEWEB)

    Pedicini, R.; Giacoppo, G.; Carbone, A.; Passalacqua, E. [CNR-ITAE, Messina (Italy). Inst. for Advanced Energy Technologies

    2010-07-01

    In this work a functionalised polymer was studied as potential material for hydrogen storage in solid state. A Poly(ether ether ketone) (PEEK) matrix was modified by a manganese oxide in situ formation. Here we report the functionalisation process and the preliminary results on hydrogen storage capability of the synthesised polymer. The polymer was characterized by Scanning Electron Microscopy, X-ray diffraction, Transmission Electron Microscopy and Gravimetric Hydrogen Adsorption measurements. In the functionalised PEEK, morphological changes occur as a function of oxide precursor concentration and reaction time. Promising results by gravimetric measurements were obtained with a hydrogen sorption of 0.24%wt/wt at 50 C and 60 bar, moreover, reversibility hydrogen adsorption and desorption in a wide range of both temperature and pressure was confirmed. (orig.)

  10. The cianimetalatos as model materials for studying the adsorption of H2 and interactions that determine

    International Nuclear Information System (INIS)

    Reguera, E.; Reguera, L.; Rodríguez, C.

    2015-01-01

    An overview of the work done in recent years in the IMRE and the Faculties of Chemistry and Physics at the University of Havana, in collaboration with the Applied Research Center for Advanced Science and Technology at the National Polytechnic Institute of Mexico is presented; on the synthesis, physico-chemical characterization, assessment and modeling of potentially usable as nanoporous materials cianometalatos model to study the adsorption of H2 at high densities, and interactions that determine it. The mechanisms of interaction of the hydrogen molecule with the crystal lattice and its consequences for the adsorption and diffusion of hydrogen in these materials are discussed. The results have been reported in dozens of articles, published in international journals, they were presented at numerous scientific events and contributed to the preparation of several thesis, master's and Ph.D. (full text)

  11. Theoretical study on platinum-catalyzed isotope exchange reaction mechanism of hydrogen and liquid water

    International Nuclear Information System (INIS)

    Hu Sheng; Wang Heyi; Luo Shunzhong

    2009-04-01

    Based on electron and vibration approximate means and the density function theory B3LYP, the ΔG degree and equilibrium pressures of adsorption and dissociation reactions of H 2 and water vapor on Pt surface have been calculated. The adsorption, dissociation and coadsorption actions of H 2 and water were analyzed. According to the ΔG degree, hydrogen molecule combines with metal atoms in single atom, and water vapor molecule has no tendency to dissociate on Pt surface. The dissociation of hydrogen molecule would hold back the direct adsorption of water vapor molecules on Pt surface. The structures of Pt-H (OH 2 ) n + (n=1, 2, 3) hydroniums were optimized. According to the mulliken overlap populations, Pt-H (OH 2 ) + is not stable or produced. Hydrogen isotope exchange occurs between hydration layer and D atoms which adsorb on Pt surface via intermediates (H 2 O) n D + (ads) (n≥2). (authors)

  12. Influence of nitrogen doping in sumanene framework toward hydrogen storage: A computational study.

    Science.gov (United States)

    Reisi-Vanani, Adel; Shamsali, Fatemeh

    2017-09-01

    Two conditions are important to obtain appropriate substances for hydrogen storage; high surface area and fitting binding energy (BE). Doping is a key strategy that improves BE. We investigated hydrogen adsorption onto twenty six nitrogen disubstituted isomers of sumanene (C 19 N 2 H 12 ) by MP2/6-311++G(d,p)//B3LYP/6-31+G(d) and M06-2X/6-31+G(d) levels of theory. Effect of nitrogen doping in different positions of sumanene was checked. To obtain better BE, basis set superposition error (BSSE) and zero point energy (ZPE) corrections were used. Anticipating of adsorption sites and extra details about adsorption process was done by molecular electrostatic potential (MEP) surfaces. Various types of density of state (DOS) diagrams such as total DOS (TDOS), projected DOS (PDOS) and overlap population DOS (OPDOS) and natural bond orbital (NBO) analysis were used to find better insight on the adsorption properties. In addition of temperature depending of the BE, HOMO-LUMO gap (HLG), dipole moment, reactivity and stability, bowl depth and natural population analysis (NPA) of the isomers were studied. A physisorption mechanism for adsorption was proposed and a trivial change was seen. Place of nitrogen atoms in sumanene frame causes to binding energy increases or decreases compared with pristine sumanene. The best and the worst isomers and category of isomers were suggested. Copyright © 2017 Elsevier Inc. All rights reserved.

  13. Adsorption of malachite green and iodine on rice husk-based porous carbon

    International Nuclear Information System (INIS)

    Guo Yupeng; Zhang Hui; Tao Nannan; Liu Yanhua; Qi Juirui; Wang Zichen; Xu Hongding

    2003-01-01

    Adsorption isotherms of I 2 and malachite green (MG) by rice husk-based porous carbons (RHCs) from aqueous medium have been studied. Three samples of carbons prepared by NaOH-activation, three samples prepared by KOH-activation and two samples of commercial carbons have been studied. And the adsorption isotherms have been determined after modifying the carbon surfaces by oxidation with nitric acid and hydrogen peroxide and after degassing at 800 deg. C. The results have been found to follow the Freundlich adsorption isotherm. Three samples of N series have larger capacity for removing I 2 and MG from solution compared to that of the tested commercial carbons. The adsorption capacity of I 2 is similar for K series and commercial carbons. And the capacity of commercial carbons for MG is larger than K series. The adsorption capacity of I 2 on oxidation carbons has increased for hydrogen peroxide treatment and decreased for nitric acid, and that of MG is decreased. But the adsorption capacities of I 2 and MG increase on degassing. On the other hand, the adsorption of I 2 increases after modifying the carbon surfaces by HCl without oxidation. Suitable mechanisms have been proposed

  14. Li-Decorated β12-Borophene as Potential Candidates for Hydrogen Storage: A First-Principle Study.

    Science.gov (United States)

    Liu, Tingting; Chen, Yuhong; Wang, Haifeng; Zhang, Meiling; Yuan, Lihua; Zhang, Cairong

    2017-12-07

    The hydrogen storage properties of pristine β 12 -borophene and Li-decorated β 12 -borophene are systemically investigated by means of first-principles calculations based on density functional theory. The adsorption sites, adsorption energies, electronic structures, and hydrogen storage performance of pristine β 12 -borophene/H₂ and Li- β 12 -borophene/H₂ systems are discussed in detail. The results show that H₂ is dissociated into Two H atoms that are then chemisorbed on β 12 -borophene via strong covalent bonds. Then, we use Li atom to improve the hydrogen storage performance and modify the hydrogen storage capacity of β 12 -borophene. Our numerical calculation shows that Li- β 12 -borophene system can adsorb up to 7 H₂ molecules; while 2Li- β 12 -borophene system can adsorb up to 14 H₂ molecules and the hydrogen storage capacity up to 10.85 wt %.

  15. First-principles study of H2 adsorption and dissociation on Zr(0 0 0 1)

    International Nuclear Information System (INIS)

    Zhang Peng; Wang Shuangxi; Zhao Jian; He Chaohui; Zhang Ping

    2011-01-01

    Highlights: → The stability of the equilibrium adsorption states is determined after the geometry optimization. → The origin of the stable chemisorbed state is analyzed by the electronic structure and charge redistribution calculation. → The dissociation energetics of H2 are investigated in details by the PES and CINEB calculation. - Abstract: The adsorption and dissociation of H 2 molecules on the Zr(0 0 0 1) surface are systematically investigated by using density functional theory within the generalized gradient approximation and a supercell approach. After geometry optimization, the most stable equilibrium adsorption state is found to be along the top-y entrance. By calculating the adiabatic potential energy surface, the chemisorbed molecular adsorption states are also identified to be along the parallel channel at the top site. The electronic properties of the stable chemisorbed molecular state are analyzed, which show that the interaction between the molecule and substrate is of covalent characteristic with a sizeable charge redistribution. On the other hand, the hcp site is turned out to be the most stable equilibrium adsorption site for hydrogen atom on Zr(0 0 0 1) surface after the dissociation of H 2 . The dissociation energetics of H 2 are studied by calculating the potential energy surface and the minimum energy path of the transition state is determined by using the climb image nudged elastic band method, wherein the fcc-y channel is found to be most stable and favorable for dissociative adsorption of H 2 among the five possible dissociative paths. Remarkably, we find that the adiabatic dissociation process of H 2 is an activated type but with a small energy barrier, which is well consistent with the macroscopic phenomenon that the zirconium metal is easily hydrogenated.

  16. On the Hydrogen Cyanide Removal from Air using Metal loaded Polyacrylonitrile Composite Nanofibers

    Directory of Open Access Journals (Sweden)

    Bozorgmehr Maddah

    2017-12-01

    Full Text Available The present study highlights the potential application of electrospun polyacrylonitrile/metal salts (CrO3, CuCO3 nanofibrous filter media impregnated with TEDA (PAN-M-TEDA as an efficient adsorbent for hydrogen cyanide removal from air. The PAN-M-TEDA nanofiber before and after adsorption of hydrogen cyanide was characterized with Fourier transform infrared microscopy (FTIR. The concentration of hydrogen cyanide passes through the samples was determined by measuring the absorption of hydrogen cyanide in the solution containing indicator via UV-Vis spectroscopy. The results showed that introducing metal salts to PAN nanofiber along with their impregnation with TEDA, significantly increases the adsorption capacity of nanofibrous filter media. The adsorption of hydrogen cyanide over PAN-M-TEDA nanofiber was also studied as a function of thickness, PAN concentration and TEDA concentration by response surface methodology (RSM based on central composite design. It is found that the highest adsorption capacity can be achieved at thickness 28.42 mm, PAN concentration 16.19 w/v % and TEDA concentration 14.80 w/v %.

  17. Comment on "Theoretical study of the dynamics of atomic hydrogen adsorbed on graphene multilayers"

    Science.gov (United States)

    Bonfanti, Matteo; Martinazzo, Rocco

    2018-03-01

    It is shown that the theoretical prediction of a transient magnetization in bilayer and multilayer graphene (M. Moaied et al., Phys. Rev. B 91, 155419 (2015), 10.1103/PhysRevB.91.155419) relies on an incorrect physical scenario for adsorption, namely, one in which H atoms adsorb barrierless on graphitic substrates and form a random adsorption pattern of monomers. Rather, according to experimental evidence, H atom sticking is an activated process, and adsorption is under kinetic control, largely ruled by a preferential sticking mechanism that leads to stable, nonmagnetic dimers at all but the smallest coverages (Theory and experiments are reconciled by reconsidering the hydrogen atom adsorption energetics with the help of van der Waals-inclusive density functional calculations that properly account for the basis set superposition error. It is shown that today van der Waals-density functional theory predicts a shallow physisorption well that nicely agrees with available experimental data and suggests that the hydrogen atom adsorption barrier in graphene is 180 meV high, within ˜5 meV accuracy.

  18. Enhanced hydrogen storage by using lithium decoration on phosphorene

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Zhiyuan; Wan, Neng, E-mail: wn@seu.edu.cn, E-mail: lsy@seu.edu.cn; Lei, Shuangying, E-mail: wn@seu.edu.cn, E-mail: lsy@seu.edu.cn; Yu, Hong [Key Laboratory of Microelectromechanical Systems of the Ministry of Education, Southeast University, Nanjing 210096 (China)

    2016-07-14

    The hydrogen storage characteristics of Li decorated phosphorene were systematically investigated based on first-principle density functional theory. It is revealed that the adsorption of H{sub 2} on pristine phosphorene is relatively weak with an adsorption energy of 0.06 eV. While this value can be dramatically enhanced to ∼0.2 eV after the phosphorene was decorated by Li, and each Li atom can adsorb up to three H{sub 2} molecules. The detailed mechanism of the enhanced hydrogen storage was discussed based on our density functional theory calculations. Our studies give a conservative prediction of hydrogen storage capacity to be 4.4 wt. % through Li decoration on pristine phosphorene. By comparing our calculations to the present molecular dynamic simulation results, we expect our adsorption system is stable under room temperature and hydrogen can be released after moderate heating.

  19. Influence of adsorbed carbon dioxide on hydrogen electrosorption in palladium-platinum-rhodium alloys

    International Nuclear Information System (INIS)

    Lukaszewski, M.; Grden, M.; Czerwinski, A.

    2004-01-01

    Carbon dioxide electroreduction was applied to examine the processes of hydrogen electrosorption (adsorption, absorption and desorption) by thin electrodeposits of Pd-Pt-Rh alloys under conditions of cyclic voltammetric (CV) experiments. Due to different adsorption characteristics towards the adsorption product of the electroreduction of CO 2 (reduced CO 2 ) exhibited by the alloy components hydrogen adsorption and hydrogen absorption signals can be distinguished on CV curves. Reduced CO 2 causes partial blocking of hydrogen adsorbed on surface Pt and Rh atoms, without any significant effect on hydrogen absorption into alloy. It reflects the fact that adsorbed hydrogen bonded to Pd atoms does not participate in CO 2 reduction, while hydrogen adsorbed on Pt and Rh surface sites is inactive in the absorption reaction. In contrast, CO is adsorbed on all alloy components and causes a marked inhibition of hydrogen sorption (both adsorption and absorption)/desorption reactions

  20. A computational study on the adsorption configurations and reactions of SiH{sub x}(x = 1-4) on clean and H-covered Si(100) surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Le, Thong N-M [Molecular Science and Nano-Materials Laboratory, Institute for Computational Science and Technology, Quang Trung Software Park, Dist. 12, Ho Chi Minh City (Viet Nam); Raghunath, P. [Center for Interdisciplinary Molecular Science, Department of Applied Chemistry, National Chiao Tung University, Hsinchu 300, Taiwan (China); Huynh, Lam K., E-mail: lamhuynh.us@gmail.com [Department of Applied Chemistry, School of Biotechnology,International University, VNU-HCMC, Quarter 6, Linh Trung, Thu Duc District, Ho Chi Minh City (Viet Nam); Lin, M.C., E-mail: chemmcl@emory.edu [Center for Interdisciplinary Molecular Science, Department of Applied Chemistry, National Chiao Tung University, Hsinchu 300, Taiwan (China)

    2016-11-30

    Highlights: • Possible adsorption configurations of all adsorbates on Si(100) surface are systematically explored. • The mechanisms leading to the formation of silicon adatoms on the surface are proposed. • The barriers for hydrogen abstractions from the surface are negligible comparing to the barriers for the hydrogen migrations. • The barriers for hydrogen abstractions from the adsorbed speices are negligible comparing to the barriers for the decompositions. - Abstract: Possible adsorption configurations of H and SiH{sub x} (x = 1 − 4) on clean and H-covered Si(100) surfaces are determined by using spin-polarized DFT calculations. The results show that, on the clean surface, the gas-phase hydrogen atom and SiH{sub 3} radicals effectively adsorb on the top sites, while SiH and SiH{sub 2} prefer the bridge sites of the first layer. Another possibility for SiH is to reside on the hollow sites with a triple-bond configuration. For a partially H-coverd Si(100) surface, the mechanism is similar but with higher adsorption energies in most cases. This suggests that the surface species become more stable in the presence of surface hydrogens. The minimum energy paths for the adsorption/migration and reactions of H/SiH{sub x} species on the surfaces are explored using the climbing image-nudged elastic band method. The competitive surface processes for Si thin-film formation from SiH{sub x} precursors are also predicted. The study reveals that the migration of hydrogen adatom is unimportant with respect to leaving open surface sites because of its high barriers (>29.0 kcal/mol). Alternatively, the abstraction of hydrogen adatoms by H/SiH{sub x} radicals is more favorable. Moreover, the removal of hydrogen atoms from adsorbed SiH{sub x}, an essential step for forming Si layers, is dominated by abstraction rather than the decomposition processes.

  1. Arsenic Adsorption Equilibrium Concentration and Adsorption Rate of Activated Carbon Coated with Ferric-Aluminum Hydroxides

    Science.gov (United States)

    Zhang, M.; Sugita, H.; Oguma, T.; Hara, J.; Takahashi, S.

    2015-12-01

    In some areas of developing countries, ground or well water contaminated with arsenic has been reluctantly used as drinking water. It is highly desirable that effective and inexpensive arsenic removal agents should be developed and provided to reduce the potential health risk. Previous studies demonstrated that activated carbon coated with ferric-aluminum hydroxides (Fe-Al-C) has high adsorptive potential for removal of arsenic. In this study, a series of experiments using Fe-Al-C were carried to discuss adsorption equilibrium time, adsorption equilibrium concentration and adsorption rate of arsenic for Fe-Al-C. Fe-Al-C used in this study was provided by Astec Co., Ltd. Powder reagent of disodium hydrogen arsenate heptahydrate was dissolved into ion-exchanged water. The solution was then further diluted with ion-exchanged water to be 1 and 10 mg/L as arsenic concentration. The pH of the solution was adjusted to be around 7 by adding HCl and/or NaOH. The solution was used as artificial arsenic contaminated water in two types of experiments (arsenic adsorption equilibrium and arsenic adsorption rate tests). The results of the arsenic equilibrium tests were showed that a time period of about 3 days to reach apparent adsorption equilibrium for arsenic. The apparent adsorption equilibrium concentration and adsorbed amount of arsenic on Fe-Al-C adsorbent could be estimated by application of various adsorption isotherms, but the distribution coefficient of arsenic between solid and liquid varies with experimental conditions such as initial concentration of arsenic and addition concentration of adsorbent. An adsorption rate equation that takes into account the reduction in the number of effective adsorption sites on the adsorbent caused by the arsenic adsorption reaction was derived based on the data obtained from the arsenic adsorption rate tests.

  2. Microporous Metal Organic Materials for Hydrogen Storage

    Energy Technology Data Exchange (ETDEWEB)

    S. G. Sankar; Jing Li; Karl Johnson

    2008-11-30

    We have examined a number of Metal Organic Framework Materials for their potential in hydrogen storage applications. Results obtained in this study may, in general, be summarized as follows: (1) We have identified a new family of porous metal organic framework materials with the compositions M (bdc) (ted){sub 0.5}, {l_brace}M = Zn or Co, bdc = biphenyl dicarboxylate and ted = triethylene diamine{r_brace} that adsorb large quantities of hydrogen ({approx}4.6 wt%) at 77 K and a hydrogen pressure of 50 atm. The modeling performed on these materials agree reasonably well with the experimental results. (2) In some instances, such as in Y{sub 2}(sdba){sub 3}, even though the modeling predicted the possibility of hydrogen adsorption (although only small quantities, {approx}1.2 wt%, 77 K, 50 atm. hydrogen), our experiments indicate that the sample does not adsorb any hydrogen. This may be related to the fact that the pores are extremely small or may be attributed to the lack of proper activation process. (3) Some samples such as Zn (tbip) (tbip = 5-tert butyl isophthalate) exhibit hysteresis characteristics in hydrogen sorption between adsorption and desorption runs. Modeling studies on this sample show good agreement with the desorption behavior. It is necessary to conduct additional studies to fully understand this behavior. (4) Molecular simulations have demonstrated the need to enhance the solid-fluid potential of interaction in order to achieve much higher adsorption amounts at room temperature. We speculate that this may be accomplished through incorporation of light transition metals, such as titanium and scandium, into the metal organic framework materials.

  3. Hydrogen storage property of alkali and alkaline-earth metal atoms decorated C24 fullerene: A DFT study

    Science.gov (United States)

    Zhang, Yafei; Cheng, Xinlu

    2018-04-01

    The hydrogen storage behavior of alkali and alkaline-earth metal (AM = Li, Na, K, Mg, Ca) atoms decorated C24 fullerene was investigated by using density functional theory (DFT) study. Our results indicate that the AM atoms prefer to adsorb atop the center of tetragon of C24 fullerene with the largest binding energy than other possible adsorption sites. Moreover, the hydrogen storage gravimetric density of 24H2/6Li/C24, 24H2/6Na/C24 and 36H2/6Ca/C24 configurations reaches up to 12.7 wt%, 10.1 wt% and 12 wt%, higher than the year 2020 target from the US department of energy (DOE). Also, the average adsorption energies of H2 molecules of the 24H2/6Li/C24, 24H2/6Na/C24 and 36H2/6Ca/C24 configurations are -0.198 eV/H2, -0.164 eV/H2 and -0.138 eV/H2, locate the desirable range under the physical adsorption at near ambient conditions. These findings will have important implications on designing new hydrogen storage materials in the future.

  4. Semiempirical quantum model approach for hydrogen adsorption in ZrNi alloys

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Bin-Hao, E-mail: binhao17@gmail.com [Department of Energy Application Engineering, Far East University, No. 49, Zhonghua Rd., Xinshi Dist., Tainan City 74448, Taiwan, ROC (China); Huang, Chien-Chung [Department of Hydrogen Energy and Fuel Cells, Green Energy and Eco-Technology Center, ITRI, No. 49, Zhonghua Rd., Xinshi Dist., Tainan City 74448, Taiwan, ROC (China); Yeh, Yen-Lian; Jang, Ming-Jyi [Department of Automation and Control Engineering, Far East University, No. 49, Zhonghua Rd., Xinshi Dist., Tainan City 74448, Taiwan, ROC (China)

    2013-12-15

    Highlights: •The hydrogen diffusion behavior in solid ZrNi alloy performs clearly by MD. •Shear and Young’s modulus agree with the experiment study very well. •Current model can apply to hydrogen-tech material development. -- Abstract: Hydrogen storage is an important topic because of its relevance to the future energy economy. Hydrogen diffusivity in materials plays an important role in hydrogen technology both for hydrogen separation and hydrogen storage. To clarify the mechanism of the rate-controlling step, diffusion mechanism of hydrogen in metallic materials is studied by molecular dynamics method. This study performs semi-empirical-quantum molecular dynamic simulations in order to clarify hydrogen atom diffusion behavior in ZrNi alloys materials. We investigate the mechanical properties change associated with temperature variation for ZrNi base alloys and also consider the influence of materials micro-structure change of hydrogen diffusion. Finally, current work presents a theoretically prediction of dynamical diffusion coefficient to compare diffusion kinetics of crystalline and amorphous structure.

  5. Adsorption of hydrogen isotopes by metals in non-equilibrium conditions

    International Nuclear Information System (INIS)

    Livshits, A.I.; Notkin, M.E.; Pustovojt, Yu.M.

    1982-01-01

    To study the interaction of thermonuclear plasma and additions with metallic walls, nonequilibrium system of thermal atomary hydrogen - ''cold'' (300-1100 K) metal is experimentally investigated. Atomary hydrogen was feeded to samples of Ni and Pd in the shape of atomic beam, coming into vacuum from high-frequency gaseous discharge. It is shown that hydrogen solubility under nonequilibrium conditions increases with surface passivation (contamination); in this case it surpasses equilibrium solubility by value orders. Nickel and iron dissolve more hydrogen than palladium at a certain state of surface ( passivation) and gas (atomary hydrogen). The sign of the temperature dependence of hydrogen solubility in passivated N 1 and Fe changes when alterating molecular hydrogen by atomary hydrogen

  6. A computational study on the adsorption configurations and reactions of SiHx(x = 1-4) on clean and H-covered Si(100) surfaces

    Science.gov (United States)

    Le, Thong N.-M.; Raghunath, P.; Huynh, Lam K.; Lin, M. C.

    2016-11-01

    Possible adsorption configurations of H and SiHx (x = 1 - 4) on clean and H-covered Si(100) surfaces are determined by using spin-polarized DFT calculations. The results show that, on the clean surface, the gas-phase hydrogen atom and SiH3 radicals effectively adsorb on the top sites, while SiH and SiH2 prefer the bridge sites of the first layer. Another possibility for SiH is to reside on the hollow sites with a triple-bond configuration. For a partially H-coverd Si(100) surface, the mechanism is similar but with higher adsorption energies in most cases. This suggests that the surface species become more stable in the presence of surface hydrogens. The minimum energy paths for the adsorption/migration and reactions of H/SiHx species on the surfaces are explored using the climbing image-nudged elastic band method. The competitive surface processes for Si thin-film formation from SiHx precursors are also predicted. The study reveals that the migration of hydrogen adatom is unimportant with respect to leaving open surface sites because of its high barriers (>29.0 kcal/mol). Alternatively, the abstraction of hydrogen adatoms by H/SiHx radicals is more favorable. Moreover, the removal of hydrogen atoms from adsorbed SiHx, an essential step for forming Si layers, is dominated by abstraction rather than the decomposition processes.

  7. Adsorption properties of chloropicrin on pristine and borazine-doped nanographenes: A theoretical study

    Science.gov (United States)

    Hosseinian, Akram; Vessally, Esmail; Babazadeh, Mirzaagha; Edjlali, Ladan; Es'haghi, Moosa

    2018-04-01

    Recently, nanographenes were introduced as definite segments of graphene where their end atoms are saturated with hydrogens. In this study, we explored the reactivity and electronic sensitivity of a hexa-peri-hexabenzocoronene (HBC) and newly synthesized borazine-like ring-doped nanographenes (BNG) to the chloropicrin molecule based on density functional theory. We found that chloropicrin is preferentially adsorbed via its N atoms on both HBC and BNG nanographenes. The electronic properties of HBC were predicted to be sensitive to chloropicrin but the adsorption capacity is low because of the small adsorption energy (-7.1 kcal/mol). However, chloropicrin is adsorbed somewhat more strongly on BNG, with an adsorption energy of about -29.9 kcal/mol. After the adsorption of chloropicrin, the lowest unoccupied molecular orbital (LUMO) level of BNG stabilizes and the highest occupied molecular orbital-LUMO gap is decreased by about 85.9%. Thus, BNG converts from a semiconductor into a semimetal with a higher electrical conductivity. The change in electrical conductivity can generate an electrical signal, which is helpful for detecting chloropicrin. In addition, we predicted a short recovery time of 14.6 s at 350 K for this sensor.

  8. Noncatalytic hydrogenation of decene-1 with hydrogen accumulated in a hybrid carbon nanostructure in nanosized membrane reactors

    Science.gov (United States)

    Soldatov, A. P.

    2014-08-01

    Studies on the creation of nanosized membrane reactors (NMRs) of a new generation with accumulated hydrogen and a regulated volume of reaction zone were continued at the next stage. Hydrogenation was performed in the pores of ceramic membranes with hydrogen preliminarily adsorbed in mono- and multilayered orientated carbon nanotubes with graphene walls (OCNTGs)—a new hybrid carbon nanostructure formed on the inner pore surface. Quantitative determination of hydrogen adsorption in OCNTGs was performed using TRUMEM ultrafiltration membranes with D av = 50 and 90 nm and showed that hydrogen adsorption was up to ˜1.5% of the mass of OCNTG. The instrumentation and procedure for noncatalytic hydrogenation of decene-1 at 250-350°C using hydrogen accumulated and stored in OCNTG were developed. The conversion of decene-1 into decane was ˜0.2-1.8% at hydrogenation temperatures of 250 and 350°C, respectively. The rate constants and activation energy of hydrogenation were determined. The latter was found to be 94.5 kJ/mol, which is much smaller than the values typical for noncatalytic hydrogenations and very close to the values characteristic for catalytic reactions. The quantitative distribution of the reacting compounds in each pore regarded as a nanosized membrane reactor was determined. The activity of hydrogen adsorbed in a 2D carbon nanostructure was evaluated. Possible mechanisms of noncatalytic hydrogenation were discussed.

  9. Selective adsorption of a supramolecular structure on flat and stepped gold surfaces

    Science.gov (United States)

    Peköz, Rengin; Donadio, Davide

    2018-04-01

    Halogenated aromatic molecules assemble on surfaces forming both hydrogen and halogen bonds. Even though these systems have been intensively studied on flat metal surfaces, high-index vicinal surfaces remain challenging, as they may induce complex adsorbate structures. The adsorption of 2,6-dibromoanthraquinone (2,6-DBAQ) on flat and stepped gold surfaces is studied by means of van der Waals corrected density functional theory. Equilibrium geometries and corresponding adsorption energies are systematically investigated for various different adsorption configurations. It is shown that bridge sites and step edges are the preferred adsorption sites for single molecules on flat and stepped surfaces, respectively. The role of van der Waals interactions, halogen bonds and hydrogen bonds are explored for a monolayer coverage of 2,6-DBAQ molecules, revealing that molecular flexibility and intermolecular interactions stabilize two-dimensional networks on both flat and stepped surfaces. Our results provide a rationale for experimental observation of molecular carpeting on high-index vicinal surfaces of transition metals.

  10. Density Functional Theory Study of the Interaction of Hydrogen with Li6C60.

    Science.gov (United States)

    Wang, Qian; Jena, Puru

    2012-05-03

    Hydrogen storage properties of Li-coated C60 fullerene have been studied using density functional theory within the local density as well as generalized gradient approximation. Hydrogen atoms are found to bind to Li6C60 in two distinct forms, with the first set attaching to C atoms, not linked to Li, in atomic form. Once all such C atoms are saturated with hydrogen, the second set of hydrogen atoms bind quasi-molecularly to the Li atoms, five of which remain in the exohedral and the sixth in the endohedral position. The corresponding hydrogen gravimetric density in Li6C60H40 is 5 wt %. Desorption of hydrogen takes place in succession, the ones bound quasi-molecularly desorbing at a temperature lower than the ones bound atomically. The results are compared with the recent experiment on hydrogen adsorption in Li6C60.

  11. A study on metal organic framework (MOF-177) synthesis, characterization and hydrogen adsorption -desorption cycles

    Energy Technology Data Exchange (ETDEWEB)

    Viditha, V.; Venkateswer Rao, M.; Srilatha, K.; Himabindu, V. [Centre for Environment, Institute of Science and Technology, Jawaharlal Nehru Technological University Hyderabad, Kukatpally, Hyderabad-500 085, A.P. (India); Yerramilli, Anjaneyulu [Director, TLGVRC, JSU Box 18739, JSU, Jackson, MS 32917-0939 (United States)

    2013-07-01

    Hydrogen has long been considered to be an ideal alternative to fossil-fuel systems and much work has now been done on its storage. There are four main methods of hydrogen storage: as a liquid; as compressed hydrogen; in the form of metal hydrides; and by physisorption. Among all the materials metal organic frameworks (MOFs) are considered to have desirable properties like high porosity, pore volume and high thermal stability. MOF-177 is considered to be an ideal storage material. In this paper we study about its synthesis and hydrogen storage capacities of MOF-177 at different pressures ranging from 25, 50, 75 and 100 bar respectively. The obtained samples are characterized by XRD, BET and SEM. The recorded results show that the obtained hydrogen capacity is 1.1, 2.20, 2.4 and 2.80 wt%. The desorption capacity is 0.9, 2.1, 2.37 and 2.7 wt% at certain temperatures like 373 K.

  12. Theoretical study of hydrogen storage in metal hydrides.

    Science.gov (United States)

    Oliveira, Alyson C M; Pavão, A C

    2018-05-04

    Adsorption, absorption and desorption energies and other properties of hydrogen storage in palladium and in the metal hydrides AlH 3 , MgH 2 , Mg(BH 4 ) 2 , Mg(BH 4 )(NH 2 ) and LiNH 2 were analyzed. The DFT calculations on cluster models show that, at a low concentration, the hydrogen atom remains adsorbed in a stable state near the palladium surface. By increasing the hydrogen concentration, the tetrahedral and the octahedral sites are sequentially occupied. In the α phase the tetrahedral site releases hydrogen more easily than at the octahedral sites, but the opposite occurs in the β phase. Among the hydrides, Mg(BH 4 ) 2 shows the highest values for both absorption and desorption energies. The absorption energy of LiNH 2 is higher than that of the palladium, but its desorption energy is too high, a recurrent problem of the materials that have been considered for hydrogen storage. The release of hydrogen, however, can be favored by using transition metals in the material structure, as demonstrated here by doping MgH 2 with 3d and 4d-transition metals to reduce the hydrogen atomic charge and the desorption energy.

  13. GAT 4 production and storage of hydrogen. Report July 2004; GAT 4 procduction et stockage de l'hydrogene. Rapport juillet 2004

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2004-07-01

    This paper concerns two aspects of the hydrogen: the production and the storage. For both parts the challenges and a state of the art are presented. It discusses also the hydrogen production by renewable energies, by solar energy, the hydrogen of hydrocarbons reforming purification, active phases development, thermal transfer simulation. Concerning the hydrogen storage the hydrogen adsorption by large surface solid, the storage by metallic hydrides, the alanates and light hydrides, the adsorption on carbon nano-tubes, the storage in nano-structures, the thermal and mechanical simulation of the hydrogen are presented. (A.L.B.)

  14. Neutron-reflectometry study of alcohol adsorption on various DLC coatings

    Energy Technology Data Exchange (ETDEWEB)

    Kalin, M., E-mail: mitjan.kalin@tint.fs.uni-lj.si [University of Ljubljana, Faculty of Mechanical Engineering, Laboratory for Tribology and Interface Nanotechnology, Bogišićeva 8, 1000 Ljubljana (Slovenia); Simič, R. [University of Ljubljana, Faculty of Mechanical Engineering, Laboratory for Tribology and Interface Nanotechnology, Bogišićeva 8, 1000 Ljubljana (Slovenia); Hirayama, T. [Department of Mechanical Engineering, Doshisha University, 1-3 Miyakodani, Tatara, Kyotanabe, Kyoto 610-0394 (Japan); Geue, T.; Korelis, P. [Paul Scherrer Institute, 5232 Villigen – PSI (Switzerland)

    2014-01-01

    Diamond-like carbon (DLC) coatings are notable for their excellent tribological properties. Our understanding of the lubrication of DLC coatings has improved drastically over the past decade. However, only a few details are known about the properties of the adsorbed layers on DLC, which crucially affect their tribological properties under lubricated conditions. In this work we used neutron reflectometry to determine the thickness and the density of adsorbed layers of alcohol molecules on several different types of DLC coatings, i.e., non-hydrogenated (a-C) and hydrogenated, of which both non-doped (a-C:H) and doped (a-C:H:F and a-C:H:Si) coatings were used. The results showed that a 0.9-nm-thick and relatively dense (≈45%) layer of alcohol adsorbed on the a-C coating. In contrast, no adsorption layer was found on the a-C:H, confirming the important role of hydrogen, which predominantly acts as a dangling-bond passivation source and affects the reactivity and tribochemistry of DLC coatings. The incorporation of F into a DLC coating also did not cause an increase in the adsorption ability with respect to alcohol molecules. On the contrary, the incorporation of Si increased the reactivity of the DLC coating so that a 1.3-nm-thick alcohol layer with a 35% bulk density was detected on the surface. We also discuss the very good agreement of the current results with the surface energy of selected coatings found in these experiments.

  15. Hydrogen Adsorption on Ga2O3 Surface: A Combined Experimental and Computational Study

    Energy Technology Data Exchange (ETDEWEB)

    Pan, Yun-xiang; Mei, Donghai; Liu, Chang-jun; Ge, Qingfeng

    2011-05-03

    In the present work, hydrogen adsorption on the Ga2O3 surfaces was investigated using Fourier transform infrared spectroscopy (FTIR) measurements and periodic density functional theory (DFT) calculations. Both the FTIR and DFT studies suggest that H2 dissociates on the Ga2O3 surfaces, producing OH and GaH species. The FTIR bands at 3730, 3700, 3630 and 3600 cm-1 are attributed to the vibration of the OH species whereas those at 2070 and 1990 cm-1 to the GaH species. The structures of the species detected in experiments are established through a comparison with the DFT calculated stretching frequencies. The O atom of the experimentally detected OH species is believed to originate from the surface O3c atom. On the other hand, the H atom that binds the coordinately unsaturated Ga atom results in the experimentally detected GaH species. Dissociation of H2 on the perfect Ga2O3 surface, with the formation of both OH and GaH species, is endothermic and has an energy barrier of 0.90 eV. In contrast, H2 dissociation on the defective Ga2O3 surface with oxygen vacancies, which mainly produces GaH species, is exothermic, with an energy barrier of 0.61 eV. Accordingly, presence of the oxygen vacancies promotes H2 dissociation and production of GaH species on the Ga2O3 surfaces. Higher temperatures are expected to favor oxygen vacancy creation on the Ga2O3 surfaces, and thereby benefit the production of GaH species. This analysis is consistent with the FTIR results that the bands assigned to GaH species become stronger at higher temperatures. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.

  16. High-Resolution Electron Energy Loss Studies of Oxygen, Hydrogen, Nitrogen, Nitric Oxide, and Nitrous Oxide Adsorption on Germanium Surfaces.

    Science.gov (United States)

    Entringer, Anthony G.

    The first high resolution electron energy loss spectroscopy (HREELS) studies of the oxidation and nitridation of germanium surfaces are reported. Both single crystal Ge(111) and disordered surfaces were studied. Surfaces were exposed to H, O_2, NO, N _2O, and N, after cleaning in ultra-high vacuum. The Ge surfaces were found to be non-reactive to molecular hydrogen (H_2) at room temperature. Exposure to atomic hydrogen (H) resulted hydrogen adsorption as demonstrated by the presence of Ge-H vibrational modes. The HREEL spectrum of the native oxide of Ge characteristic of nu -GeO_2 was obtained by heating the oxide to 200^circC. Three peaks were observed at 33, 62, and 106 meV for molecular oxygen (O_2) adsorbed on clean Ge(111) at room temperature. These peaks are indicative of dissociative bonding and a dominant Ge-O-Ge bridge structure. Subsequent hydrogen exposure resulted in a shift of the Ge-H stretch from its isolated value of 247 meV to 267 meV, indicative of a dominant +3 oxidation state. A high density of dangling bonds and defects and deeper oxygen penetration at the amorphous Ge surface result in a dilute bridge structure with a predominant +1 oxidation state for similar exposures. Molecules of N_2O decompose at the surfaces to desorbed N_2 molecules and chemisorbed oxygen atoms. In contrast, both oxygen and nitrogen are detected at the surfaces following exposure to NO molecules. Both NO and N_2O appear to dissociate and bond at the top surface layer. Molecular nitrogen (N_2) does not react with the Ge surfaces, however, a precursor Ge nitride is observed at room temperature following exposure to nitrogen atoms and ions. Removal of oxygen by heating of the NO-exposed surface to 550^circC enabled the identification of the Ge-N vibrational modes. These modes show a structure similar to that of germanium nitride. This spectrum is also identical to that of the N-exposed surface heated to 550^circC. Surface phonon modes of the narrow-gap semiconducting

  17. A DFT study of arsine adsorption on palladium doped graphene: Effects of palladium cluster size

    International Nuclear Information System (INIS)

    Kunaseth, Manaschai; Mudchimo, Tanabat; Namuangruk, Supawadee; Kungwan, Nawee; Promarak, Vinich; Jungsuttiwong, Siriporn

    2016-01-01

    Graphical abstract: The relationship between charge difference and adsorption strength demonstrates that charge migration from Pd_n-SDG to AsH_x significantly enhanced adsorption strength, the Pd_6 clusters doped SDG with a steep slope is recommended as a superior adsorbent material for AsH_3 removal from gas stream. - Highlights: • Pd atom and Pd clusters bind strongly onto the defective graphene surface. • Larger size of Pd cluster adsorbs arsine and its hydrogenated products stronger. • Order of adsorption strength on Pd_n doped graphene: As > AsH > AsH_2 > > AsH_3. • Charge migration characterizes the strong adsorption of AsH_2, AsH, and As. • Pd cluster doped graphene is thermodynamically preferable for arsine removal. - Abstract: In this study, we have investigated the size effects of palladium (Pd) doped single-vacancy defective graphene (SDG) surface to the adsorption of AsH_3 and its dehydrogenated products on Pd using density functional theory calculations. Here, Pd cluster binding study revealed that Pd_6 nanocluster bound strongest to the SDG surface, while adsorption of AsH_x (x = 0–3) on the most stable Pd_n doped SDG showed that dehydrogenated arsine compounds adsorbed onto the surface stronger than the pristine AsH_3 molecule. Charge analysis revealed that considerable amount of charge migration from Pd to dehydrogenated arsine molecules after adsorption may constitute strong adsorption for dehydrogenated arsine. In addition, study of thermodynamic pathways of AsH_3 dehydrogenation on Pd_n doped SDG adsorbents indicated that Pd cluster doping on SDG adsorbent tends to be thermodynamically favorable for AsH_3 decomposition than the single-Pd atom doped SDG. Hence, our study has indicated that Pd_6 clusters doped SDG is more advantageous as adsorbent material for AsH_3 removal.

  18. Interaction of Hydrogen with MOF-5.

    Science.gov (United States)

    Bordiga, Silvia; Vitillo, Jenny G; Ricchiardi, Gabriele; Regli, Laura; Cocina, Donato; Zecchina, Adriano; Arstad, Bjørnar; Bjørgen, Morten; Hafizovic, Jasmina; Lillerud, Karl Petter

    2005-10-06

    Hydrogen storage is among the most demanding challenges in the hydrogen-based energy cycle. One proposed strategy for hydrogen storage is based on physisorption on high surface area solids such as metal-organic frameworks (MOFs). Within this class of materials, MOF-5 has been the first structure studied for hydrogen storage. The IR spectroscopy of adsorbed H2 performed at 15 K and ab initio calculations show that the adsorptive properties of this material are mainly due to dispersive interactions with the internal wall structure and to weak electrostatic forces associated with O13Zn4 clusters. Calculated and measured binding enthalpies are between 2.26 and 3.5 kJ/mol, in agreement with the H2 rotational barriers reported in the literature. A minority of binding sites with higher adsorption enthalpy (7.4 kJ/mol) is also observed. These species are probably associated with OH groups on the external surfaces present as termini of the microcrystals.

  19. Amine–mixed oxide hybrid materials for carbon dioxide adsorption from CO2/H2 mixture

    Science.gov (United States)

    Ravi, Navin; Aishah Anuar, Siti; Yusuf, Nur Yusra Mt; Isahak, Wan Nor Roslam Wan; Shahbudin Masdar, Mohd

    2018-05-01

    Bio-hydrogen mainly contains hydrogen and high level of carbon dioxide (CO2). High concentration of CO2 lead to a limitation especially in fuel cell application. In this study, the amine-mixed oxide hybrid materials for CO2 separation from bio-hydrogen model (50% CO2:50% H2) have been studied. Fourier-transform infrared spectroscopy (FTIR) and x-ray diffraction (XRD) characterizations showed that the amine–mixed oxide hybrid materials successfully adsorbed CO2 physically with no chemical adsorption evidence. The dry gas of CO2/H2 mixture adsorbed physically on amine–CuO–MgO hybrid material. No carbonates were detected after several times of adsorption, which indicated the good recyclability of adsorbents. The adsorbent system of diethanolamine (DEA)/15% CuO–75% MgO showed the highest CO2 adsorption capacity of 21.2 wt% due to the presence of polar substance on MgO surface, which can adsorb CO2 at ambient condition. The alcohol group of DEA can enhance the CO2 solubility on the adsorbent surface. In the 20% CuO–50% MgO adsorbent system, DEA as amine type showed a high CO2 adsorption of 19.4 wt%. The 10% amine loading system showed that the DEA adsorption system provided high CO2 adsorption. The BET analysis confirmed that a high amine loading contributed to the decrease in CO2 adsorption due to the low surface area of the adsorbent system.

  20. Natural diatomite modified as novel hydrogen storage material

    Science.gov (United States)

    Jin, Jiao; Zheng, Chenghui; Yang, Huaming

    2014-03-01

    Natural diatomite, subjected to different modifications, is investigated for hydrogen adsorption capacities at room temperature. An effective metal-modified strategy is developed to disperse platinum (Pt) and palladium (Pd) nanoparticles on the surface of diatomite. Hydrogen adsorption capacity of pristine diatomite (diatomite) is 0.463 wt.% at 2.63 MPa and 298 K, among the highest of the known sorbents, while that of acid-thermally activated diatomite (A-diatomite) could reach up to 0.833 wt.% due to the appropriate pore properties by activation. By incorporation with a small amount of Pt and Pd ( 0.5 wt.%), hydrogen adsorption capacities are enhanced to 0.696 wt.% and 0.980 wt.%, respectively, indicating that activated diatomite shows interesting application in the field of hydrogen storage at room temperature.

  1. Experimental Challenges in Studying Hydrogen Absorption in Ultrasmall Metal Nanoparticles

    International Nuclear Information System (INIS)

    Zlotea, Claudia; Oumellal, Yassine; Provost, Karine; Ghimbeu, Camelia Matei

    2016-01-01

    Recent advances on synthesis, characterization, and hydrogen absorption properties of ultrasmall metal nanoparticles (defined here as objects with average size ≤3 nm) are briefly reviewed in the first part of this work. The experimental challenges encountered in performing accurate measurements of hydrogen absorption in Mg- and noble metal-based ultrasmall nanoparticles are addressed. The second part of this work reports original results obtained for ultrasmall bulk-immiscible Pd–Rh nanoparticles. Carbon-supported Pd–Rh nanoalloys in the whole binary chemical composition range have been successfully prepared by liquid impregnation method followed by reduction at 300°C. EXAFS investigations suggested that the local structure of these nanoalloys is partially segregated into Rh-rich core and Pd-rich surface coexisting within the same nanoparticles. Downsizing to ultrasmall dimensions completely suppresses the hydride formation in Pd-rich nanoalloys at ambient conditions, contrary to bulk and larger nanosized (5–6 nm) counterparts. The ultrasmall Pd 90 Rh 10 nanoalloy can absorb hydrogen-forming solid solutions under these conditions, as suggested by in situ X-ray diffraction (XRD). Apart from this composition, common laboratory techniques, such as in situ XRD, DSC, and PCI, failed to clarify the hydrogen interaction mechanism: either adsorption on developed surfaces or both adsorption and absorption with formation of solid solutions. Concluding insights were brought by in situ EXAFS experiments at synchrotron: ultrasmall Pd 75 Rh 25 and Pd 50 Rh 50 nanoalloys absorb hydrogen-forming solid solutions at ambient conditions. Moreover, the hydrogen solubility in these solid solutions is higher with increasing Pd content, and this trend can be understood in terms of hydrogen preferential occupation in the Pd-rich regions, as suggested by in situ EXAFS. The Rh-rich nanoalloys (Pd 25 Rh 75 and Pd 10 Rh 90 ) only adsorb hydrogen on the developed surface of ultrasmall

  2. Adsorption and catalytic properties of skeleton nickel alloyed by tantalum

    Energy Technology Data Exchange (ETDEWEB)

    Erzhanova, M S; Sokol' skii, D V; Popov, N I; Kondratenko, V I

    1977-02-01

    Adsorption properties are studied of Ni-Ta-catalysts composed of 20-50% Ni, 0-30% Ta, 50% Al with respect to hydrogen; their activity in a number of reactions has been tested. The adsorption capacity is characterized with respect to H/sub 2/ by the methods of thermodesorption and conductometry. It is shown that three forms to hydrogen (..beta.., ..gamma.., sigma) adsorb onto the surface of the alloyed catalysts, whose desorption peaks overlap because of their high mobility and interchangeability. Variation of activity, selectivity and isomerizing capacity of the catalysts correlates with the content of a weakly adsorbed mobile form of H/sub 2/.

  3. (Amino acid + silica) adsorption thermodynamics: Effects of temperature

    International Nuclear Information System (INIS)

    Sebben, Damien; Pendleton, Phillip

    2015-01-01

    Highlights: • High resolution, low concentration Gly, Lys and Glu solution adsorption isotherms. • All isotherms fitted with Langmuir–Freundlich isotherm model. • Gly, Lys and Glu show exothermic adsorption processes. • Isosteric heat analyses reveal changes in interaction strength with surface coverage. - Abstract: A thorough understanding of amino acid adsorption by mineral and oxide surfaces has a major impact on a variety of industrial and biomedical applications. Little information currently exists regarding temperature effects on most of these adsorption processes. Deeper thermodynamic analyses of their multiple temperature adsorption isotherms would aid the interpretation of the interfacial interactions. Low solution concentration adsorption isotherms for glycine, lysine and glutamic acid on a silica adsorbent were generated for T = (291, 298 and 310) K. Data analysis via the Clausius–Clapeyron method yielded the isosteric heat of adsorption as a function of fractional monolayer coverage for each adsorptive. Each amino acid showed an exothermic adsorption response. Glycine and lysine experienced a greater negative effect of increased temperature compared with glutamic acid, indicating a greater number of adsorbed molecules than glutamic acid, with the former undergoing intermolecular clustering within the adsorbed phase. Isosteric heat analyses suggest ionic interactions for lysine and hydrogen bonding for glutamic acid, both weakening with increased coverage. In contrast, initial hydrogen bonding led to ionic bonding for glycine with increasing coverage

  4. First-principle study of hydrogenation on monolayer MoS2

    International Nuclear Information System (INIS)

    Xu, Yong; Li, Yin; Chen, Xi; Zhang, Ru; Zhang, Chunfang; Lu, Pengfei

    2016-01-01

    The structural and electronic properties of hydrogenation on 1H-MoS 2 and 1T-MoS 2 have been systematically explored by using density functional theory (DFT) calculations. Our calculated results indicate an energetically favorable chemical interaction between H and MoS 2 monolayer for H adsorption when increasing concentration of H atoms. For 1H-MoS 2 , single H atom adsorption creates midgap approaching the Fermi level which increases the n-type carrier concentration effectively. As a consequence, its electrical conductivity is expected to increase significantly. For 1T-MoS 2 , H atoms adsorption can lead to the opening of a direct gap of 0.13 eV compared to the metallic pristine 1T-MoS 2 .

  5. Theoretical studies of acrolein hydrogenation on Au20 nanoparticle

    Science.gov (United States)

    Li, Zhe; Chen, Zhao-Xu; He, Xiang; Kang, Guo-Jun

    2010-05-01

    Gold nanoparticles play a key role in catalytic processes. We investigated the kinetics of stepwise hydrogenation of acrolein on Au20 cluster model and compared with that on Au(110) surface. The rate-limiting step barrier of CC reduction is about 0.5 eV higher than that of CO hydrogenation on Au(110) surface. On Au20 nanoparticle, however, the energy barrier of the rate-determining step for CC hydrogenation turns out to be slightly lower than the value for the CO reduction. The selectivity difference on the two substrate models are attributed to different adsorption modes of acrolein: via the CC on Au20, compared to through both CC and CO on Au(110). The preference switch implies that the predicted selectivity of competitive hydrogenation depends on substrate model sensitively, and particles with more low-coordinated Au atoms than flat surfaces are favorable for CC hydrogenation, which is in agreement with experimental result.

  6. Reactivity of a reduced metal oxide surface: hydrogen, water and carbon monoxide adsorption on oxygen defective rutile TiO 2( 1 1 0 )

    Science.gov (United States)

    Menetrey, M.; Markovits, A.; Minot, C.

    2003-02-01

    The reactivity at reduced surface differs from that on the stoichiometric perfect surfaces. This does not originate uniquely from the modification of the coordination; electron count also is determining. The general trend is a decrease of the heat of adsorption on the metal cations. The reactivity decreases at sites in the vicinity of the defects due to the reduction induced by the O vacancies. At the defect site the decrease is less pronounced for H, H 2, CO and molecular H 2O. In the case of H 2O dissociative adsorption, the defect site is more reactive than the perfect surface. Thus, a hydration converting the defective-reduced TiO 2 to the hydrogenated non-defective-reduced surface is easy. The resulting structure possesses surface hydroxyl groups. It is probably the easiest way to form the hydrogenated non-defective surface. On TiO 2, the defective surface requires very anhydrous conditions.

  7. Adsorption of H atoms on cubic Er2O3 (0 0 1) surface: A DFT study

    International Nuclear Information System (INIS)

    Mao, Wei; Chikada, Takumi; Shimura, Kenichiro; Suzuki, Akihiro; Yamaguchi, Kenji; Terai, Takayuki

    2013-01-01

    First-principles plane wave calculations based on spin-polarized density functional theory (DFT) and generalized gradient approximation (GGA) have been used to study the adsorption of H atoms on cubic Er 2 O 3 (0 0 1) surface. We identify stable adsorption positions and find that H preferentially adsorbs on top of fourfold-hollow sites and transfers electrons to the surface, resulting in the formations of covalent bonds to the nearest neighboring four oxygen atoms. In the most energetically favorable adsorption sites, It was found that H bonds with O atoms at the cubic Er 2 O 3 (0 0 1) surface with an adsorption energy of −295.68 kJ mol −1 at coverage 1/8 ML, and the adsorption energy is inclined to decrease with the increase of H coverage (>1/4 ML). In addition, our calculations indicate that the dissociative H atom configurations have adsorption energies that are at least 152.64 kJ mol −1 greater than the H 2 molecule configurations on the surface. These results discussed in the context of erbium oxide slabs are employed to rationalize some processes regarding to the hydrogen isotope permeation behavior of tritium permeation barrier

  8. Investigation of adsorption and absorption-induced stresses using microcantilever sensors

    International Nuclear Information System (INIS)

    Hu, Zhiyu; Thundat, T.; Warmack, R. J.

    2001-01-01

    The interaction between a vapor and a thin film adsorbed on one side of a bimaterial microcantilever produces differential stress, resulting in readily measurable curvatures of the cantilever structure. Depending upon the system studied, there exist two types of gas - solid interaction: bulk-like absorption and surface-like adsorption. The absorption of hydrogen into palladium results in film expansion whose magnitude is governed by hydrogen partial pressure. The bending of a bimaterial microcantilever (palladium/silicon) due to hydrogen absorption depends on the thickness of the palladium film and is reversible but rate limited by a surface barrier. In contrast, the stress induced by adsorption of mercury onto a bimaterial (gold/silicon) cantilever is irreversible at room temperature, is rate limited by surface coverage, and is independent of the gold - film thickness. [copyright] 2001 American Institute of Physics

  9. Study on state equation for hydrogen storage measurement by volumetric method

    International Nuclear Information System (INIS)

    Dai Wei; Xu Jiajing; Wang Chaoyang; Tang Yongjian

    2014-01-01

    Volumetric measurement technique is one of the most popular methods for determining the amount of hydrogen storage. A new state equation was established which extended the limitations from the ideal gas state equation, the van der Waals equation and the Gou equation. The new state equation was then employed to describe the p-V-T character of hydrogen and investigate the adsorption quantity of hydrogen storage in resorcin-formaldehyde aerogel under different temperatures and pressures. The new equation was used to describe the density of hydrogen under different temperatures and pressures. The results are in good agreement with the experimental data. The differences arising from various underlying physics were carefully analyzed. (authors)

  10. A DFT and QTAIM study of the adsorption of organic molecules over the copper-doped coronene and circumcoronene

    Science.gov (United States)

    Malček, Michal; Cordeiro, M. Natalia D. S.

    2018-01-01

    Graphene based materials are nowadays extensively studied because of their potential applications as gas sensors, biosensors or adsorbents. Doping the graphene surface with heteroatoms or transition metals can improve its electronic properties and chemical reactivity. Polyaromatic hydrocarbons coronene and circumcoronene can be used as models of tiny graphene quantum dots. The adsorption of a set of organic molecules (water, hydrogen peroxide, hydrogen sulfide, methanol, ethanol and oxygen molecule) over the copper-doped coronene and circumcoronene was theoretically studied using density functional theory (DFT) and quantum theory of atoms in molecules (QTAIM). In the case of coronene, only one site was considered for the Cu-doping, whereas in the case of circumcoronene being a polyaromatic hydrocarbon composed of 54 carbon atoms, three different sites for Cu-doping were considered. For the systems under study, the adsorption of O2 was found energetically the most favorable, with energetic outcome ranging from -3.1 to -3.7 eV related to the position of dopant Cu atom. Changes in the topology of charge densities at Cu and in its vicinity after the adsorption of studied molecules were investigated in the framework of QTAIM. In addition, QTAIM analysis of bond critical points (BCP) was employed to study the character of the newly formed chemical bonds. The results of this study point out the suitability of Cu-doped graphene materials as sensors and/or adsorbents in practical applications.

  11. Hydrogen trapping ability of the pyridine-lithium⁺ (1:1) complex.

    Science.gov (United States)

    Chattaraj, Saparya; Srinivasu, K; Mondal, Sukanta; Ghosh, Swapan K

    2015-03-26

    Theoretical studies have been carried out at different levels of theory to verify the hydrogen adsorption characteristics of pyridine-lithium ion (1:1) complexes. The nature of interactions associated with the bonding between pyridine and lithium as well as that between lithium and adsorbed molecular hydrogen is studied through the calculation of electron density and electron-density-based reactivity descriptors. The pyridine-lithium ion complex has been hydrogenated systematically around the lithium site, and each lithium site is found to adsorb a maximum of four hydrogen molecules with an interaction energy of ∼-4.0 kcal/mol per molecule of H2. The fate of the hydrogen adsorbed in a pyridine-lithium ion complex (corresponding to the maximum adsorption) is studied in the course of a 2 ps time evolution through ab initio molecular dynamics simulation at different temperatures. The results reveal that the complex can hold a maximum of four hydrogen molecules at a temperature of 77 K, whereas it can hold only two molecules of hydrogen at 298 K.

  12. GAT 4 production and storage of hydrogen. Report July 2004

    International Nuclear Information System (INIS)

    2004-01-01

    This paper concerns two aspects of the hydrogen: the production and the storage. For both parts the challenges and a state of the art are presented. It discusses also the hydrogen production by renewable energies, by solar energy, the hydrogen of hydrocarbons reforming purification, active phases development, thermal transfer simulation. Concerning the hydrogen storage the hydrogen adsorption by large surface solid, the storage by metallic hydrides, the alanates and light hydrides, the adsorption on carbon nano-tubes, the storage in nano-structures, the thermal and mechanical simulation of the hydrogen are presented. (A.L.B.)

  13. Cascades for hydrogen isotope separation using metal hydrides

    International Nuclear Information System (INIS)

    Hill, F.B.; Grzetic, V.

    1982-01-01

    Designs are presented for continuous countercurrent hydrogen isotope separation cascades based on the use of metal hydrides. The cascades are made up of pressure swing adsorption (PSA) or temperature swing adsorption (TSA) stages. The designs were evolved from consideration of previously conducted studies of the separation performance of four types of PSA and TSA processes

  14. Cascades for hydrogen isotope separation using metal hydrides

    Energy Technology Data Exchange (ETDEWEB)

    Hill, F B; Grzetic, V [Brookhaven National Lab., Upton, NY (USA)

    1983-02-01

    Designs are presented for continuous countercurrent hydrogen isotope separation cascades based on the use of metal hydrides. The cascades are made up of pressure swing adsorption (PSA) or temperature swing adsorption (TSA) stages. The designs were evolved from consideration of previously conducted studies of the separation performance of four types of PSA and TSA processes.

  15. Kinetic modeling of hydrogenation and hydro-denitrogenation mechanisms on sulfurated catalysts; Etude par modelisation cinetique des mecanismes d'hydrogenation et d'hydrodesazotation sur catalyseurs sulfures

    Energy Technology Data Exchange (ETDEWEB)

    Penet, H.

    1998-10-23

    Toluene hydrogenation on a NiMo/{gamma}-Al{sub 2}O{sub 3} catalyst was studied at 350 deg. C as a function of the partial pressures of H{sub 2}, H{sub 2}S and NH{sub 3}. This experimental study shows the following facts: the effect of the H{sub 2}S partial pressure on the hydrogenation rate is complex. The order with respect to H{sub 2}S varies between -0.05 and -0.5 as the pressure varies between 0.125 and 3 bar; in the presence of NH{sub 3}, the H{sub 2}S inhibiting effect is enhanced. Kinetic modeling was performed with the Chemkin II/Surface Chemkin II software package. On the basis of the effect of contact time and H{sub 2}S on toluene hydrogenation, the adsorption by heterolytic dissociation of H{sub 2} and H{sub 2}S was selected. H{sub 2} provides hydride species (H{sup -}) attacking the aromatic ring in a first step. Proton addition during the hydrogenation of the first double bond is the limiting step. In the presence of ammonia. the kinetic modeling shows that the catalyst surface is modified and that the displacement of the H{sub 2}S adsorption equilibrium is expected. The NH{sub 3} adsorption mode could not be clearly discriminated between a simple adsorption through coordination and an adsorption through protonation. This model was applied to the hydro-denitrogenation of 2,6-diethyl-aniline at 350 deg. C on NiMo/{gamma}-Al{sub 2}O{sub 3} catalyst and showed that the limitation step is the hydrogenation of the aromatic ring. (author)

  16. Effects of hydrogen peroxide pretreatment of clay minerals on the adsorption of Sr-85 and Tc-95m under anoxic conditions

    International Nuclear Information System (INIS)

    Relyea, J.F.; Washburne, C.D.

    1979-01-01

    Treatment of three clay minerals with hydrogen peroxide affects the observed adsorption behavior of technetium relative to untreated clay under anoxic conditions. A possible adsorption mechanism of Tc is the reduction of TcO - 4 to a more positively charged or better adsorbed species. Oxidation of the clay by H 2 O 2 would hinder the reduction of TcO - 4 by buffering the clay-water system at a higher Eh value, although a difference in measured Eh value may go undetected. Sorption of strontium by the clays under the same conditions is not affected by a pretreatment with H 2 O 2 . The behavior of strontium follows that expected from ion exchange theory. 13 tables

  17. H?, D? and HD adsorption upon the metal-organic framework [Cu?Zn?(btc)?]? studied by pulsed ENDOR and HYSCORE spectroscopy

    Science.gov (United States)

    Jee, Bettina; Hartmann, Martin; Pöppl, Andreas

    2013-10-01

    The adsorption of hydrogen has become interesting in terms of gas separation as well as safe and reversible storage of hydrogen as an energy carrier. In this regard, metal-organic framework compounds are potential candidates. The metal-organic framework [Cu?Zn?(btc)?]? as a partially Zn-substituted analogue of the well known compound HKUST-1 is well suited for studying adsorption geometries at cupric ions by electron paramagnetic resonance (EPR) methods due to the formation of few mixed Cu/Zn paddle wheel units with isolated S = 1/2 electron spins. The adsorption of hydrogen (H2) as well as the deuterium (D2) and HD molecules were investigated by continuous wave EPR and pulsed ENDOR and HYSCORE spectroscopy. The principal values of the proton and deuterium hyperfine coupling tensors ? and ? were determined by spectral simulations as well as of the deuterium nuclear quadrupole tensor ? for adsorbed HD and D2. The results show a side-on coordination of HD and D2 with identical Cu-H and Cu-D distances rCuX = 2.8 Å with the tensors ? and ? aligned parallel to the C4 symmetry axis of the paddle wheel unit. A thermodynamic non-equilibrium state with J = 1, mJ = ±1 is indicated by the experimental data with ? and ? averaged by rotation around C4.

  18. Adsorption of Ti on LiAlH4 surfaces studied by band structure calculations

    International Nuclear Information System (INIS)

    Loevvik, O.M.

    2004-01-01

    LiAlH 4 is a potential light-weight hydrogen storage material if hydrogenation can be made reversible. In NaAlH 4 this may be done by adding small amounts of Ti, but the same effect has not yet been observed in LiAlH 4 . To understand these mechanisms, detailed studies of the materials with and without the additive are necessary. In this study, two-dimensional slabs representing the open (0 1 0) and densely packed (1 0 1) surfaces of LiAlH 4 have been used to model adsorption of titanium atoms on those surfaces. The results show that the Ti atom tends to move below the surface towards interstitial sites rather than binding to a Li ion or AlH 4 complex at the surface

  19. Temperature dependent dual hydrogen sensor response of Pd nanoparticle decorated Al doped ZnO surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Gupta, D.; Barman, P. B.; Hazra, S. K., E-mail: surajithazra@yahoo.co.in [Department of Physics and Materials Science, Jaypee University of Information Technology, Waknaghat, Solan, Himachal Pradesh-173234 (India); Dutta, D. [IC Design and Fabrication Centre, Department of Electronics and Telecommunication Engineering, Jadavpur University, Kolkata-700032 (India); Kumar, M.; Som, T. [SUNAG Laboratory, Institute of Physics, Sachivalaya Marg, Bhubaneswar 751005 (India)

    2015-10-28

    Sputter deposited Al doped ZnO (AZO) thin films exhibit a dual hydrogen sensing response in the temperature range 40 °C–150 °C after surface modifications with palladium nanoparticles. The unmodified AZO films showed no response in hydrogen in the temperature range 40 °C–150 °C. The operational temperature windows on the low and high temperature sides have been estimated by isolating the semiconductor-to-metal transition temperature zone of the sensor device. The gas response pattern was modeled by considering various adsorption isotherms, which revealed the dominance of heterogeneous adsorption characteristics. The Arrhenius adsorption barrier showed dual variation with change in hydrogen gas concentration on either side of the semiconductor-to-metal transition. A detailed analysis of the hydrogen gas response pattern by considering the changes in nano palladium due to hydrogen adsorption, and semiconductor-to-metal transition of nanocrystalline Al doped ZnO layer due to temperature, along with material characterization studies by glancing incidence X-ray diffraction, atomic force microscopy, and transmission electron microscopy, are presented.

  20. Floatability of Fe-bearing silicates in the presence of starch: Adsorption and spectroscopic studies

    International Nuclear Information System (INIS)

    Severov, V V; Filippova, I V; Filippov, L O

    2013-01-01

    Natural polysaccharides such as starch, dextrin, cellulose and their derivatives are promising non-toxic and biodegradable organic flocculants and flotation depressants. This paper presents the investigation of mechanism of adsorption of corn starch on quartz and Fe-bearing amphibole, i.e. pargasite. The direct measurement of starch adsorption on the mineral surfaces shows no difference between quartz and pargasite. However, the starch adsorption on the magnetite is more important. FT-IR spectroscopy studies reports different adsorption mechanism of starch on quartz and pargasite surface. The key changes observed in starch absorption on quartz are the major shifts in C-0 stretching frequencies presumed existence of a hydrogen bond between starch and quartz surface. The similar changes were observed in this region of IR-band for pargasite. The appearance and disappearance of the bands in the region 960-920 cm −1 corresponds probably to formation of a new chemical bond between starch O-H groups and metal atoms on pargasite surface with formation of a surface complex. This result confirms that adsorption of the starch on the pargasite surface is droved by two mechanism. Hence, existence of strong chemical bond between starch and pargasite surface explains decrease of its floatability compared to quartz in process of iron ore flotation and forces to search new conditioning reagent modes.

  1. Floatability of Fe-bearing silicates in the presence of starch: Adsorption and spectroscopic studies

    Science.gov (United States)

    Severov, V. V.; Filippova, I. V.; Filippov, L. O.

    2013-03-01

    Natural polysaccharides such as starch, dextrin, cellulose and their derivatives are promising non-toxic and biodegradable organic flocculants and flotation depressants. This paper presents the investigation of mechanism of adsorption of corn starch on quartz and Fe-bearing amphibole, i.e. pargasite. The direct measurement of starch adsorption on the mineral surfaces shows no difference between quartz and pargasite. However, the starch adsorption on the magnetite is more important. FT-IR spectroscopy studies reports different adsorption mechanism of starch on quartz and pargasite surface. The key changes observed in starch absorption on quartz are the major shifts in C-0 stretching frequencies presumed existence of a hydrogen bond between starch and quartz surface. The similar changes were observed in this region of IR-band for pargasite. The appearance and disappearance of the bands in the region 960-920 cm-1 corresponds probably to formation of a new chemical bond between starch O-H groups and metal atoms on pargasite surface with formation of a surface complex. This result confirms that adsorption of the starch on the pargasite surface is droved by two mechanism. Hence, existence of strong chemical bond between starch and pargasite surface explains decrease of its floatability compared to quartz in process of iron ore flotation and forces to search new conditioning reagent modes.

  2. Adsorption of poly(ethylene oxide) on smectite: Effect of layer charge.

    Science.gov (United States)

    Su, Chia-Chi; Shen, Yun-Hwei

    2009-04-01

    The adsorption of polymers on clay is important in many applications. However the mechanisms of poly(ethylene oxide) (PEO) adsorption on smectite is not well elucidated at present. The aim of this study was to investigate the effect of layer charge density on the adsorption of PEO by smectite. The results indicated that both the hydrophobic interaction (between CH(2)CH(2) groups and siloxane surface) and the hydrogen bonding (between ether oxygen of PEO and structure OH of smectite) lead to PEO preferential adsorption on the surface of low-charge smectite. In addition, the delamination of low-charge smectite in water is enhanced upon PEO adsorption presumably due to the hydrophilic ether oxygen of adsorbed PEO.

  3. Adsorption and dissociation of H2S on Mo(1 0 0) surface by first-principles study

    International Nuclear Information System (INIS)

    Luo, Haijun; Cai, Jianqiu; Tao, Xiangming; Tan, Mingqiu

    2014-01-01

    Density-functional theory calculations had been used to investigate the adsorption and dissociation of H 2 S on Mo(1 0 0) surface. Adsorption mechanisms of H 2 S, HS, S and H on the Mo(1 0 0) surface were analyzed. H 2 S was found to be adsorbed at bridge, hollow and top sites with adsorption energies of −1.25, −1.03 and −0.92 eV, respectively. HS was strongly chemically absorbed at hollow, bridge and top sites with adsorption energies of −4.51, −4.08 and −3.45 eV, respectively, and sulfur and hydrogen preferred to be absorbed at hollow and bridge sites, respectively. In addition, potential energy profiles of H 2 S dissociation on Mo(1 0 0) had been constructed by a climbing image nudged elastic band method. Four possible dissociation pathways of the first H 2 S dehydrogenation were examined with reaction barriers of 0.28, 0.37, 0.075, and 0.21 eV, respectively, while the energy barrier to break the S-H bond of HS with or without hydrogen co-adsorption was almost the same low. This work showed that the decomposition of H 2 S on the molybdenum surface was kinetically and thermodynamically facile. Local densities of electronic states were further used to characterize the interaction between H 2 S and substrate.

  4. A DFT study of arsine adsorption on palladium doped graphene: Effects of palladium cluster size

    Energy Technology Data Exchange (ETDEWEB)

    Kunaseth, Manaschai, E-mail: manaschai@nanotec.or.th [National Nanotechnology Center (NANOTEC), National Science and Technology Development Agency (NSTDA) , Pathum Thani 12120 (Thailand); Mudchimo, Tanabat [Department of Chemistry and Center of Excellence for Innovation in Chemistry, Faculty of Science, Ubon Ratchathani University, Ubon Ratchathani 34190 (Thailand); Namuangruk, Supawadee [National Nanotechnology Center (NANOTEC), National Science and Technology Development Agency (NSTDA) , Pathum Thani 12120 (Thailand); Kungwan, Nawee [Department of Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai 50200 (Thailand); Promarak, Vinich [Department of Material Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong 21201 (Thailand); Jungsuttiwong, Siriporn, E-mail: siriporn.j@ubu.ac.th [Department of Chemistry and Center of Excellence for Innovation in Chemistry, Faculty of Science, Ubon Ratchathani University, Ubon Ratchathani 34190 (Thailand)

    2016-03-30

    Graphical abstract: The relationship between charge difference and adsorption strength demonstrates that charge migration from Pd{sub n}-SDG to AsH{sub x} significantly enhanced adsorption strength, the Pd{sub 6} clusters doped SDG with a steep slope is recommended as a superior adsorbent material for AsH{sub 3} removal from gas stream. - Highlights: • Pd atom and Pd clusters bind strongly onto the defective graphene surface. • Larger size of Pd cluster adsorbs arsine and its hydrogenated products stronger. • Order of adsorption strength on Pd{sub n} doped graphene: As > AsH > AsH{sub 2} > > AsH{sub 3}. • Charge migration characterizes the strong adsorption of AsH{sub 2}, AsH, and As. • Pd cluster doped graphene is thermodynamically preferable for arsine removal. - Abstract: In this study, we have investigated the size effects of palladium (Pd) doped single-vacancy defective graphene (SDG) surface to the adsorption of AsH{sub 3} and its dehydrogenated products on Pd using density functional theory calculations. Here, Pd cluster binding study revealed that Pd{sub 6} nanocluster bound strongest to the SDG surface, while adsorption of AsH{sub x} (x = 0–3) on the most stable Pd{sub n} doped SDG showed that dehydrogenated arsine compounds adsorbed onto the surface stronger than the pristine AsH{sub 3} molecule. Charge analysis revealed that considerable amount of charge migration from Pd to dehydrogenated arsine molecules after adsorption may constitute strong adsorption for dehydrogenated arsine. In addition, study of thermodynamic pathways of AsH{sub 3} dehydrogenation on Pd{sub n} doped SDG adsorbents indicated that Pd cluster doping on SDG adsorbent tends to be thermodynamically favorable for AsH{sub 3} decomposition than the single-Pd atom doped SDG. Hence, our study has indicated that Pd{sub 6} clusters doped SDG is more advantageous as adsorbent material for AsH{sub 3} removal.

  5. First-principles study of the interactions of hydrogen with low-index surfaces of PdCu ordered alloy

    Institute of Scientific and Technical Information of China (English)

    Min Tang; Hengbo Li; Wentao Yuan; Shihui Zou; Chenghua Sun; Yong Wang

    2017-01-01

    PdCu catalysts play a key role in several hydrogen-involved processes. Among these reactions, the interaction of hydrogen with PdCu essentially determines the catalytic performance. However, the response of PdCu to surrounding hydrogen has been poorly investigated, especially for specific facets of PdCu at different environment.In this work, taking temperature and hydrogen pressure into account, we studied the hydrogen-surface interactions for four low-index surfaces of PdCu through first-principles calculations. It was found that H-PdCu adsorption strong relies on the facets, hydrogen coverage, and reaction environment (temperature and H-pressure).Our work highlights the importance of the environment on the nature of catalyst surfaces and reactions and offers a plausible way to investigate the interactions between gas and the surfaces of nanocatalysts in real reactions.

  6. Hydrogen storage behaviors of platinum-supported multi-walled carbon nanotubes

    Energy Technology Data Exchange (ETDEWEB)

    Park, Soo-Jin; Lee, Seul-Yi [Department of Chemistry, Inha University, 253 Nam-gu, Incheon 402-751 (Korea, Republic of)

    2010-12-15

    In this work, the hydrogen storage behaviors of multi-walled carbon nanotubes (MWNTs) loaded by crystalline platinum (Pt) particles were studied. The microstructure of the Pt/MWNTs was characterized by X-ray diffraction and transmission electron microscopy. The pore structure and total pore volumes of the Pt/MWNTs were analyzed by N{sub 2}/77 K adsorption isotherms. The hydrogen storage capacity of the Pt/MWNTs was evaluated at 298 K and 100 bar. From the experimental results, it was found that Pt particles were homogeneously distributed on the MWNT surfaces. The amount of hydrogen storage capacity increased in proportion to the Pt content, with Pt-5/MWNTs exhibiting the largest hydrogen storage capacity. The superior amount of hydrogen storage was linked to an increase in the number of active sites and the optimum-controlled micropore volume for hydrogen adsorption due to the well-dispersed Pt particles. Therefore, it can be concluded that Pt particles play an important role in hydrogen storage characteristics due to the hydrogen spillover effect. (author)

  7. Nano-porous inorganic-organic hybrid solids: some new materials for hydrogen storage?

    International Nuclear Information System (INIS)

    Serre, Ch.; Loiseau, Th.; Devic, T.; Ferey, G.; Latroche, M.; Llewellyn, Ph.; Chang, J.S.

    2007-01-01

    Recently have been studied chromium and aluminium carboxylates MIL-53(Cr, Al), formed from an assembly of octahedrons chains and for hybrid solids formed with octahedrons trimers (MIL-100 and MIL-101). The compounds MIL-53(Cr, Al) are microporous (φ ∼ 8 Angstroms, while the solids MIL-100 and MIL-101 have very large porous volumes (V ∼ 380-700000 (Angstroms) 3 ), meso-pores (φ ∼ 25-34 Angstroms) and a zeolitic architecture. The resulting specific surface areas are important (between 1000 m 2 .g -1 for the MIL-53 solids, until 4000 m 2 .g -1 for the MIL-101 compound. Here is presented their hydrogen adsorption properties, at 77 K and 298 K. The hydrogen adsorption kinetics has been tested on the MIL-53(Cr) solid at 77 K. Hydrogen adsorption micro-calorimetry experiments have been carried out on these solids between 0 and 1 bar in order to obtain data on the strongest interactions between hydrogen and the porous basic structure. (O.M.)

  8. Adsorption separation factors for hydrogen--deuterium (H/sub 2/-HD-D/sub 2/) mixtures on synthetic mordenite at 48 to 62/sup 0/K. [Reaction Kinetics

    Energy Technology Data Exchange (ETDEWEB)

    Parbuzin, V S; Kuryakov, Yu N

    1975-07-01

    The temperature dependence of selectivity has been determined for the adsorption of hydrogen isotopes by sodium mordenite. Heats and entropies of exchange of the isotopic molecules in the gas-zeolite system have been calculated from the experimental results. (auth)

  9. Study of 2D MXene Cr{sub 2}C material for hydrogen storage using density functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Yadav, A. [Department of Physics and National Centre for Nanosciences & Nanotechnology, University of Mumbai, Vidyanagari, Santacruz (E), Mumbai 400 098 (India); Dashora, Alpa, E-mail: dashoralpa@gmail.com [UM-DAE Centre for Excellence in Basic Sciences, Vidyanagari, Santacruz (E), Mumbai 400 098 (India); Patel, N. [Department of Physics and National Centre for Nanosciences & Nanotechnology, University of Mumbai, Vidyanagari, Santacruz (E), Mumbai 400 098 (India); Dipartimento di Fisica, Università degli Studi di Trento, I-38123 Povo, Trento (Italy); Miotello, A. [Dipartimento di Fisica, Università degli Studi di Trento, I-38123 Povo, Trento (Italy); Press, M.; Kothari, D.C. [Department of Physics and National Centre for Nanosciences & Nanotechnology, University of Mumbai, Vidyanagari, Santacruz (E), Mumbai 400 098 (India)

    2016-12-15

    Highlights: • First-principles studies showed that Cr{sub 2}C MXene can store 7.6 wt.% of H{sub 2}. • 6.4 wt.% H{sub 2} can be reversibly stored at ambient temperature. • Charge transfer between H and Cr is responsible for the reversible H{sub 2} adsorption. • H-atom on hollow site between three Cr atoms is the most stable site. - Abstract: Hydrogen storage capacity of 2D MXene Cr{sub 2}C has been studied using density functional theory. Possibility to adsorb H{sub 2} molecule on Cr{sub 2}C surface at various sites has been studied. Among the studied adsorption sites on Cr{sub 2}C surface, few sites were found suitable for chemisorption and physisorption of H{sub 2} molecules. Few of the studied sites are also found to be suitable for Kubas-type interaction, which is useful for reversible hydrogen storage at ambient conditions. Electronic structure calculations and charge transfer analysis have been done to understand the interactions of adsorbed hydrogen with the Cr{sub 2}C layer. It has been found that the total hydrogen storage capacity of Cr{sub 2}C is 7.6 wt.% in which 1.2 wt.% of H is due to the chemisorption, 3.2 wt.% is bonded with Kubas-interaction and remaining 3.2 wt.% is bonded through weak electrostatic interactions (with binding energy of 0.26 eV/H{sub 2} and charge transfer of 0.09 e{sup −} to H atom from Cr atom). Thus the reversible hydrogen storage capacity at ambient conditions (controlled by hydrogen bonded with energies ranging from 0.1 to 0.4 eV/H{sub 2}, in the present case through Kubas and weak electrostatic interactions) is 6.4 wt.% which is greater than the 2017 DoE recommended target value of 5.5 wt.%.

  10. Glucose recovery from aqueous solutions by adsorption in metal-organic framework MIL-101: a molecular simulation study.

    Science.gov (United States)

    Gupta, Krishna M; Zhang, Kang; Jiang, Jianwen

    2015-08-05

    A molecular simulation study is reported on glucose recovery from aqueous solutions by adsorption in metal-organic framework MIL-101. The F atom of MIL-101 is identified to be the most favorable adsorption site. Among three MIL-101-X (X = H, NH2 or CH3), the parent MIL-101 exhibits the highest adsorption capacity and recovery efficacy. Upon functionalization by -NH2 or -CH3 group, the steric hindrance in MIL-101 increases; consequently, the interactions between glucose and framework become less attractive, thus reducing the capacity and mobility of glucose. The presence of ionic liquid, 1-ethyl-3-methyl-imidazolium acetate, as an impurity reduces the strength of hydrogen-bonding between glucose and MIL-101, and leads to lower capacity and mobility. Upon adding anti-solvent (ethanol or acetone), a similar adverse effect is observed. The simulation study provides useful structural and dynamic properties of glucose in MIL-101, and it suggests that MIL-101 might be a potential candidate for glucose recovery.

  11. Adsorption studies on Pt(111)

    International Nuclear Information System (INIS)

    Hopster, H.

    1977-06-01

    The adsorption of O 2 , CO, and C 2 H 2 as well as the CO oxidation on Pt(111) were studied by high-resolution electron spectroscopy. Using a platinum monocrystal sample with a contonuous stage density, the adhesion coefficient for O 2 and the reaction probability for CO were determined as a function of stage density and oxygen cover by measuring the oxygen cover and its time behaviour. The study of vibrations of adsorbed CO showed that CO is bound in linear form on two different adsorption sites. The adsorption of acetylene was studied at 140 K and 300 K. The frequencies of the C-H stretching and flexural vibrations as well as the C-C-H bonding angle were determined. (orig./GSC) [de

  12. Adsorption of Zn(II) on the kaolinite(001) surfaces in aqueous environment: A combined DFT and molecular dynamics study

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Qiang; Kong, Xiang-Ping; Zhang, Bao-Hua; Wang, Juan, E-mail: juaner80@163.com

    2017-08-31

    Highlights: • Zn(II) adsorption on two types of neutral kaolinite(001) surfaces is investigated. • Surface “Ou” is found the preferred site for mono- and bi-dentate complexes. • Both Zn(II) and surface oxygen accept electrons from aqua oxygens. • Coupling of O 2p with Zn sp{sup 3}d{sup 2} (or sp{sup 3}) hybridization states is the bonding nature. - Abstract: Adsorption of Zn(II) on two types of neutral (001) surfaces of kaolinite, tetrahedral Si(t) and octahedral Al(o), was studied by means of DFT calculations and classical molecular dynamics simulations. The position and structure for both outer-sphere and mono-/bi-dentate inner-sphere complexes of Zn(II) in aqueous environment were examined, with binding energy and radial distribution function calculated. Outer-sphere complex on the Si(t) surface, monodentate inner-sphere complex of “O{sub u}” (surface oxygen with “upright” hydrogen) site and bidentate complex of “O{sub u}-O{sub u}” site of neighboring Al centers on the Al(o) surface are considered to be the dominant adsorption species. The outer-sphere complex is found six-coordinated with distorted octahedral geometry, while both the inner-sphere complexes exhibit the tetrahedral structure with coordination number of four. Hydrogen bonding interactions between oxygen or hydrogen of the kaolinite(001) surfaces and the aqua ligands of Zn(II) act as the key role for the structure and stability of adsorption complexes. Upon the Mulliken population analysis and partial density of states, both Zn(II) and surface oxygen accept electrons from aqua oxygens, and coupling of O 2p with the sp{sup 3}d{sup 2} or sp{sup 3} hybridization states of Zn(II) is the primary bonding nature of Zn(II) with oxygen in outer- and inner-sphere complexes, respectively.

  13. Cathodic over-potential and hydrogen partial pressure coupling in hydrogen evolution reaction of marine steel under hydrostatic pressure

    International Nuclear Information System (INIS)

    Xiong, X.L.; Zhou, Q.J.; Li, J.X.; Volinsky, Alex A.; Su, Y.J.

    2017-01-01

    Highlights: •Hydrostatic pressure increases the Volmer and the Heyrovsky reactions rates. •Hydrostatic pressure decreases the Tafel reaction rate. •Hydrogen adsorption conditions change with pressure under −1.2 and −1.3 V SSE . •Under −1.2 and −1.3 V SSE , the Heyrovsky reaction dominates the hydrogen recombination. •Under −1.0 and −1.1 V SSE , the Tafel reaction dominates the hydrogen recombination. -- Abstract: A new electrochemical impedance spectroscopy (EIS) model, which considers both the Tafel recombination and the Heyrovsky reaction under permeable boundary conditions, was developed to characterize the kinetic parameters of the hydrogen evolution reaction (HER) under hydrostatic pressure. The effect of the hydrostatic pressure on the kinetic parameters of the HER and the permeation of A514 steel in alkaline solution were measured using potentiodynamic polarization, the Devanathan cell hydrogen permeation, and EIS. The hydrostatic pressure accelerates the Volmer reaction and inhibits the Tafel recombination, which increases the number of adsorbed hydrogen atoms. On the other hand, the pressure accelerates the Heyrovsky reaction, which decreases the amount of adsorbed hydrogen atoms. At 10 to 40 MPa hydrostatic pressure within the −1.0 to −1.1 V SSE cathodic potential region, the HER is controlled by hydrogen partial pressure, and hydrogen adsorption is the Langmuir type. Within the −1.2 to −1.3 V SSE cathodic potential region, the HER is controlled by the potential, and hydrogen adsorption gradually transfers from the Langmuir type to the Temkin type with increasing hydrostatic pressure.

  14. A COMPREHENSIVE STUDY OF HYDROGEN ADSORBING TO AMORPHOUS WATER ICE: DEFINING ADSORPTION IN CLASSICAL MOLECULAR DYNAMICS

    Energy Technology Data Exchange (ETDEWEB)

    Dupuy, John L.; Lewis, Steven P.; Stancil, P. C. [Department of Physics and Astronomy and the Center for Simulational Physics, University of Georgia, Athens, GA 30602 (United States)

    2016-11-01

    Gas–grain and gas–phase reactions dominate the formation of molecules in the interstellar medium (ISM). Gas–grain reactions require a substrate (e.g., a dust or ice grain) on which the reaction is able to occur. The formation of molecular hydrogen (H{sub 2}) in the ISM is the prototypical example of a gas–grain reaction. In these reactions, an atom of hydrogen will strike a surface, stick to it, and diffuse across it. When it encounters another adsorbed hydrogen atom, the two can react to form molecular hydrogen and then be ejected from the surface by the energy released in the reaction. We perform in-depth classical molecular dynamics simulations of hydrogen atoms interacting with an amorphous water-ice surface. This study focuses on the first step in the formation process; the sticking of the hydrogen atom to the substrate. We find that careful attention must be paid in dealing with the ambiguities in defining a sticking event. The technical definition of a sticking event will affect the computed sticking probabilities and coefficients. Here, using our new definition of a sticking event, we report sticking probabilities and sticking coefficients for nine different incident kinetic energies of hydrogen atoms [5–400 K] across seven different temperatures of dust grains [10–70 K]. We find that probabilities and coefficients vary both as a function of grain temperature and incident kinetic energy over the range of 0.99–0.22.

  15. Adsorption of antibiotics on microplastics.

    Science.gov (United States)

    Li, Jia; Zhang, Kaina; Zhang, Hua

    2018-06-01

    Microplastics and antibiotics are two classes of emerging contaminants with proposed negative impacts to aqueous ecosystems. Adsorption of antibiotics on microplastics may result in their long-range transport and may cause compound combination effects. In this study, we investigated the adsorption of 5 antibiotics [sulfadiazine (SDZ), amoxicillin (AMX), tetracycline (TC), ciprofloxacin (CIP), and trimethoprim (TMP)] on 5 types of microplastics [polyethylene (PE), polystyrene (PS), polypropylene (PP), polyamide (PA), and polyvinyl chloride (PVC)] in the freshwater and seawater systems. Scanning Electron Microscope (SEM) and X-ray diffractometer (XRD) analysis revealed that microplastics have different surface characterizes and various degrees of crystalline. Adsorption isotherms demonstrated that PA had the strongest adsorption capacity for antibiotics with distribution coefficient (K d ) values ranged from 7.36 ± 0.257 to 756 ± 48.0 L kg -1 in the freshwater system, which can be attributed to its porous structure and hydrogen bonding. Relatively low adsorption capacity was observed on other four microplastics. The adsorption amounts of 5 antibiotics on PS, PE, PP, and PVC decreased in the order of CIP > AMX > TMP > SDZ > TC with K f correlated positively with octanol-water partition coefficients (Log K ow ). Comparing to freshwater system, adsorption capacity in seawater decreased significantly and no adsorption was observed for CIP and AMX. Our results indicated that commonly observed polyamide particles can serve as a carrier of antibiotics in the aquatic environment. Copyright © 2018 Elsevier Ltd. All rights reserved.

  16. Adsorption of Hydrogen and Potassium on GaAs(110) Studied by Time-of-Flight Scattering and Recoiling Spectrometry

    International Nuclear Information System (INIS)

    Gayone, J.E.

    2000-01-01

    We study the adsorption of H and K on a GaAs(ll0) surface by Time-of-Flight Ion-Scattering (ISS) and Direct Recoiling (DRS) Spectrometry. The method for cleaning and preparation of the surface consists on cycles of grazing bombardment with 20 keV Ar+ combined with annealing. Since this is the first time that this method is applied to a semiconductor surface, the crystallographic structure of the grazing ion bombarded surface is first characterized by ISS and DRS. The variations of the projectile scattered intensity as a function of the incident and azimuthal angles are interpreted in terms of calculated shadowing and focusing effects. The crystallographic structure of the GaAs(ll0) surface prepared by this method presents the surface relaxation observed for cleaved surfaces. The adsorption of H on GaAs(ll0) is studied as a function of the H 2 exposure and the surface temperature.The behavior of the intensity of projectiles scattered from the first two As and Ga layers is consistent with a process of unrelaxation towards the ideal surface termination upon H adsorption. We have determined that for exposures of 1000 L and 2000 L the AsI-GaI splitting corresponding to the unrelaxed surface is reduced to ΔZ = (0.0 n 0.08) A, as it should be expected for the bulk terminated surface. In addition, the fraction of the surface remaining relaxed as in the clean surface decreases strongly with the H 2 exposure. The H atoms adsorbed on the surface can be detected as recoils produced in quasi-single collisions allowing the study of the adsorption kinetics. The variations of the H recoil intensity with the exposure show that the sticking coefficient changes strongly with the H coverage since the beginning the adsorption. Above ∼ 500 L, the adsorption kinetics deviates from the initial behavior and the sticking coefficient becomes almost constant and small. The simultaneous measurements of the H coverage (with DRS) and the changes in the atomic structure (with ISS) as a

  17. First-principles study of the interactions of hydrogen with low-index surfaces of PdCu ordered alloy

    Directory of Open Access Journals (Sweden)

    Min Tang

    2017-12-01

    Full Text Available PdCu catalysts play a key role in several hydrogen-involved processes. Among these reactions, the interaction of hydrogen with PdCu essentially determines the catalytic performance. However, the response of PdCu to surrounding hydrogen has been poorly investigated, especially for specific facets of PdCu at different environment. In this work, taking temperature and hydrogen pressure into account, we studied the hydrogen-surface interactions for four low-index surfaces of PdCu through first-principles calculations. It was found that H-PdCu adsorption strong relies on the facets, hydrogen coverage, and reaction environment (temperature and H-pressure. Our work highlights the importance of the environment on the nature of catalyst surfaces and reactions and offers a plausible way to investigate the interactions between gas and the surfaces of nanocatalysts in real reactions.

  18. Hydrogen Separation by Natural Zeolite Composite Membranes: Single and Multicomponent Gas Transport.

    Science.gov (United States)

    Farjoo, Afrooz; Kuznicki, Steve M; Sadrzadeh, Mohtada

    2017-10-06

    Single and multicomponent gas permeation tests were used to evaluate the performance of metal-supported clinoptilolite membranes. The efficiency of hydrogen separation from lower hydrocarbons (methane, ethane, and ethylene) was studied within the temperature and pressure ranges of 25-600 °C and 110-160 kPa, respectively. The hydrogen separation factor was found to reduce noticeably in the gas mixture compared with single gas experiments at 25 °C. The difference between the single and multicomponent gas results decreased as the temperature increased to higher than 300 °C, which is when the competitive adsorption-diffusion mechanism was replaced by Knudsen diffusion or activated diffusion mechanisms. To evaluate the effect of gas adsorption, the zeolite surface isotherms of each gas in the mixture were obtained from 25 °C to 600 °C. The results indicated negligible adsorption of individual gases at temperatures higher than 300 °C. Increasing the feed pressure resulted in a higher separation efficiency for the individual gases compared with the multicomponent mixture, due to the governing effect of the adsorptive mechanism. This study provides valuable insight into the application of natural zeolites for the separation of hydrogen from a mixture of hydrocarbons.

  19. Microscale Enhancement of Heat and Mass Transfer for Hydrogen Energy Storage

    Energy Technology Data Exchange (ETDEWEB)

    Drost, Kevin [Oregon State Univ., Corvallis, OR (United States); Jovanovic, Goran [Oregon State Univ., Corvallis, OR (United States); Paul, Brian [Oregon State Univ., Corvallis, OR (United States)

    2015-09-30

    The document summarized the technical progress associated with OSU’s involvement in the Hydrogen Storage Engineering Center of Excellence. OSU focused on the development of microscale enhancement technologies for improving heat and mass transfer in automotive hydrogen storage systems. OSU’s key contributions included the development of an extremely compact microchannel combustion system for discharging hydrogen storage systems and a thermal management system for adsorption based hydrogen storage using microchannel cooling (the Modular Adsorption Tank Insert or MATI).

  20. Adsorption and activation of methane and methanol on Pt(100) surface: a density functional study; Adsorption et activation du methane et du methanol sur la surface (100) du platine: une etude par la fonctionnelle de la densite

    Energy Technology Data Exchange (ETDEWEB)

    Moussounda, P.S

    2006-11-15

    The activation of methane (CH{sub 4}) and methanol (CH{sub 3}OH) on Pt(100) surface has been investigated using density functional theory calculations based on plane-wave basis and pseudo-potential. We optimised CH{sub 4}/Pt(100) system. The calculated adsorption energies over the top, bridge and hollow sites are small, weakly dependent on the molecular orientation. The nature of the CH{sub 4}-Pt interaction was examined through the electronic structure changes. The adsorption of methyl (CH{sub 3}) and hydrogen (H) and the co-adsorption of CH{sub 3}+H were also calculated. From these results, we examined the dissociation of CH{sub 4} to CH{sub 3}+H, and the activation energies found are in good agreement with the experimental and theoretical values. The activation of CH{sub 3}OH/Pt(100) has been studied. All the sites have almost the same adsorption energy. The adsorption of oxygen (O) and the co-adsorption of CH{sub 4} and O were also examined. In addition, the formation of CH{sub 3}OH assuming a one-step mechanism step via the co-adsorption of CH{sub 4}+O has been studied and the barrier height was found to be high. (authors)

  1. First-principle study of hydrogenation on monolayer MoS{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Yong; Li, Yin [State Key Laboratory of Information Photonics and Optical Communications, Beijing University of Posts and Telecommunications, Beijing 100876 (China); School of science, Beijing University of Posts and Telecommunications, Beijing 100876 (China); Chen, Xi; Zhang, Ru [State Key Laboratory of Information Photonics and Optical Communications, Beijing University of Posts and Telecommunications, Beijing 100876 (China); School of Ethnic Minority Education, Beijing University of Posts and Telecommunications, Beijing 102209 (China); Zhang, Chunfang [Beijing Computational Science Research Center, Beijing 100094 (China); Lu, Pengfei, E-mail: photon.bupt@gmail.com [State Key Laboratory of Information Photonics and Optical Communications, Beijing University of Posts and Telecommunications, Beijing 100876 (China)

    2016-07-15

    The structural and electronic properties of hydrogenation on 1H-MoS{sub 2} and 1T-MoS{sub 2} have been systematically explored by using density functional theory (DFT) calculations. Our calculated results indicate an energetically favorable chemical interaction between H and MoS{sub 2} monolayer for H adsorption when increasing concentration of H atoms. For 1H-MoS{sub 2}, single H atom adsorption creates midgap approaching the Fermi level which increases the n-type carrier concentration effectively. As a consequence, its electrical conductivity is expected to increase significantly. For 1T-MoS{sub 2}, H atoms adsorption can lead to the opening of a direct gap of 0.13 eV compared to the metallic pristine 1T-MoS{sub 2}.

  2. Electric field improved hydrogen storage of Ca-decorated monolayer MoS{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Song, Nahong [College of Computer and Information Engineering, Henan University of Economics and Law, Zhengzhou 450002 (China); International Joint Research Laboratory for Quantum Functional Materials of Henan, and School of Physics and Engineering, Zhengzhou University, Zhengzhou 450001 (China); Wang, Yusheng [College of Mathematics and Information Science, North China University of Water Resources and Electric Power, Zhengzhou 450011 (China); International Joint Research Laboratory for Quantum Functional Materials of Henan, and School of Physics and Engineering, Zhengzhou University, Zhengzhou 450001 (China); Gao, Haiyan; Jiang, Weifen; Zhang, Jing; Xu, Bin [College of Mathematics and Information Science, North China University of Water Resources and Electric Power, Zhengzhou 450011 (China); Sun, Qiang [International Joint Research Laboratory for Quantum Functional Materials of Henan, and School of Physics and Engineering, Zhengzhou University, Zhengzhou 450001 (China); Jia, Yu, E-mail: jiayu@zzu.edu.cn [International Joint Research Laboratory for Quantum Functional Materials of Henan, and School of Physics and Engineering, Zhengzhou University, Zhengzhou 450001 (China)

    2015-04-17

    Hydrogen storage property of Ca-decorated MoS{sub 2} is carried out using first-principles calculations. Our calculations demonstrate that the preferential binding of Ca atoms on MoS{sub 2} effectively prevent the Ca clustering. Six H{sub 2} molecules per Ca atom can be adsorbed with a desirable adsorption energy of 0.14 eV/H{sub 2}. Both hybridization of the Ca-3d and S-2s with the H-1s orbital and the polarization of the H{sub 2} molecules contribute to the hydrogen adsorption. Our results show that the external electric field can effectively tune the hydrogen adsorption energy, therefore making hydrogen storage and release reversible. - Highlights: • Ca binds with MoS{sub 2} stalely without clustering. • It can operate under ambient thermodynamic conditions. • External electric field can effectively tune the hydrogen adsorption energy.

  3. New template for metal decoration and hydrogen adsorption on graphene-like C3N4

    International Nuclear Information System (INIS)

    Zhang Yi; Sun Hong; Chen Changfeng

    2009-01-01

    From density functional theory calculations we identify a graphene-like C 3 N 4 (g-C 3 N 4 ) as an excellent template for stable and well dispersed decoration of alkali (Li) and 3d transition metal (TM) atoms. The porous sites of g-C 3 N 4 accommodate excessive N lone-pair electrons and promote hybridization between the orbitals of N and the metal atoms. The most stable TM decorations (Ti and Sc) on g-C 3 N 4 exhibit high capacities of hydrogen adsorption with binding energies suitable for mobile applications. These metal decorated g-C 3 N 4 may also prove useful in catalytic and sensing applications for their unique nanoscale structural features unavailable in conventional nano-clusters.

  4. Adsorption and methanation of carbon dioxide on a nickel/silica catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Falconer, J.L.; Zagli, A.E.

    1980-04-01

    Temperature-programed desorption and reaction studies showed that increasing amounts of CO/sub 2/ adsorbed on silica-supported 6.9% nickel with increasing temperature to a maximum adsorption at approx. 443/sup 0/K, i.e., that the adsorption was activated; that CO/sub 2/ desorbed partly as CO/sub 2/ with the peak at 543/sup 0/K, and partly as CO with several peaks; that in the presence of hydrogen, nearly all adsorbed CO/sub 2/ desorbed as methane, and a small amount as CO; and that the methane desorption peaks from adsorbed CO and CO/sub 2/ both occurred at 473/sup 0/K. These results suggested that carbon dioxide adsorbed dissociatively as a carbon monoxide and an oxygen species. An observed absence of higher hydrocarbons in the methanation products of carbon dioxide was attributed to a high hydrogen/carbon monoxide surface ratio caused by the activated carbon dioxide adsorption.

  5. Enhanced competitive adsorption of CO2 and H2 on graphyne: A density functional theory study

    Directory of Open Access Journals (Sweden)

    Hyuk Jae Kwon

    2017-12-01

    Full Text Available Adsorption using carbon-based materials has been established to be a feasible method for separating carbon dioxide and hydrogen to mitigate the emission of carbon dioxide into the atmosphere and for the collection of fuel for energy sources, simultaneously. We carried out density functional theory calculation with dispersion correction to investigate the physisorption characteristics of carbon allotropes such as graphene and graphyne for the competitive adsorption of CO2 and H2. It is worth noting that the graphyne represented preferable adsorption energies, short bond lengths and energy charges for both gases, compared with the characteristics observed with graphene. We found that in graphyne, both the affinitive adsorption of CO2, and the competitive adsorption of CO2 and H2, took place at the hollow site between acetylene links, which do not exist in graphene. We demonstrate that in the presence of H2, the CO2 adsorption selectivity of graphyne is higher than that of graphene, because of the improved electronic properties resulting from the acetylene links.

  6. Surface atomic relaxation and magnetism on hydrogen-adsorbed Fe(110) surfaces from first principles

    Science.gov (United States)

    Chohan, Urslaan K.; Jimenez-Melero, Enrique; Koehler, Sven P. K.

    2016-11-01

    We have computed adsorption energies, vibrational frequencies, surface relaxation and buckling for hydrogen adsorbed on a body-centred-cubic Fe(110) surface as a function of the degree of H coverage. This adsorption system is important in a variety of technological processes such as the hydrogen embrittlement in ferritic steels, which motivated this work, and the Haber-Bosch process. We employed spin-polarised density functional theory to optimise geometries of a six-layer Fe slab, followed by frozen mode finite displacement phonon calculations to compute Fe-H vibrational frequencies. We have found that the quasi-threefold (3f) site is the most stable adsorption site, with adsorption energies of ∼3.0 eV/H for all coverages studied. The long-bridge (lb) site, which is close in energy to the 3f site, is actually a transition state leading to the stable 3f site. The calculated harmonic vibrational frequencies collectively span from 730 to 1220 cm-1, for a range of coverages. The increased first-to-second layer spacing in the presence of adsorbed hydrogen, and the pronounced buckling observed in the Fe surface layer, may facilitate the diffusion of hydrogen atoms into the bulk, and therefore impact the early stages of hydrogen embrittlement in steels.

  7. Nano-porous inorganic-organic hybrid solids: some new materials for hydrogen storage?; Les solides hybrides inorganiques-organiques nanoporeux: de nouveaux materiaux pour le stockage de l'hydrogene?

    Energy Technology Data Exchange (ETDEWEB)

    Serre, Ch.; Loiseau, Th.; Devic, T.; Ferey, G. [Institut Lavoisier, UMR CNRS 8180, 78 - Versailles (France); Latroche, M. [Laboratoire de Chimie Metallurgique des Terres Rares (LCMTR), UPR 209, 94 - Thiais (France); Llewellyn, Ph. [Universite de Provence, Madirel, 13 - Marseille (France); Chang, J.S. [KRICT, Daejon (Korea, Republic of)

    2007-07-01

    Recently have been studied chromium and aluminium carboxylates MIL-53(Cr, Al), formed from an assembly of octahedrons chains and for hybrid solids formed with octahedrons trimers (MIL-100 and MIL-101). The compounds MIL-53(Cr, Al) are microporous ({phi} {approx} 8 Angstroms, while the solids MIL-100 and MIL-101 have very large porous volumes (V {approx} 380-700000 (Angstroms){sup 3}), meso-pores ({phi} {approx} 25-34 Angstroms) and a zeolitic architecture. The resulting specific surface areas are important (between 1000 m{sup 2}.g{sup -1} for the MIL-53 solids, until 4000 m{sup 2}.g{sup -1} for the MIL-101 compound. Here is presented their hydrogen adsorption properties, at 77 K and 298 K. The hydrogen adsorption kinetics has been tested on the MIL-53(Cr) solid at 77 K. Hydrogen adsorption micro-calorimetry experiments have been carried out on these solids between 0 and 1 bar in order to obtain data on the strongest interactions between hydrogen and the porous basic structure. (O.M.)

  8. Adsorption of NO2 molecules on armchair phosphorene nanosheet for nano sensor applications - A first-principles study.

    Science.gov (United States)

    Nagarajan, V; Chandiramouli, R

    2017-08-01

    The electronic and NO 2 adsorption properties of hydrogenated armchair phosphorene nanosheet device is investigated through density functional theory (DFT) and non-equilibrium Green's function method (NEGF). The armchair phosphorene nanosheet is used for the detection of NO 2 gas in phosphorene molecular device. The DOS spectrum demonstrates the change in peak maxima due to transfer of electrons between NO 2 gas and phosphorene base material. The change in the peak amplitude is observed along the valance band as well as in the conduction band in the transmission spectrum of phosphorene device. I-V characteristics support the change in the current upon adsorption of NO 2 gas molecule on phosphorene molecular device. Using formation energy, structural stability of phosphorene nanosheet has been studied. The adsorption properties of NO 2 on phosphorene nanosheet have also been investigated with the help of adsorption energy, Mulliken charge and Bader charge analysis. In order to ascertain the selectivity of NO 2 gas along phosphorene molecular device in the ambient condition, the adsorption behavior of O 2 and CO 2 is also studied. The findings of the present work confirm that phosphorene molecular device can be used as a NO 2 gas sensor and also the influence of Al substitution in phosphorene nanosheet device is explored and reported. Copyright © 2017 Elsevier Inc. All rights reserved.

  9. Spectroscopy, microscopy and theoretical study of NO adsorption on MoS2 and Co-Mo-S hydrotreating catalysts

    DEFF Research Database (Denmark)

    Topsøe, Nan-Yu; Tuxen, Anders Kyrme; Hinnemann, Berit

    2011-01-01

    nfrared (IR) spectroscopy using NO as a probe molecule has been one of the important methods for characterizing hydrotreating catalysts, since this technique provides information on the nature and quantity of active edge sites of these catalysts. However, due to the strong adsorption of NO, which......) calculations, we present new atomic-scale insight into the nature of NO adsorption on MoS2 and Co-Mo-S nanoclusters. The DFT calculations and STM experiments show that NO does not adsorb at fully sulfided MoS2 edges not containing hydrogen. However, typical sulfided catalysts will have hydrogen present...... NO as a probe molecule to obtain detailed atomic-scale information on hydrotreating catalysts and the origins of activity differences. (C) 2011 Published by Elsevier Inc....

  10. Gas separation by pressure swing adsorption

    International Nuclear Information System (INIS)

    Martin, J.R.; Gottzman, C.F.; Notaro, F.; Stewart, H.A.

    1986-01-01

    Over the past twenty years separation processes based upon pressure swing adsorption have replaced cryogenic processes in a number of selected applications such as air separation for production of moderate quantities of nitrogen and oxygen and recovery of hydrogen from refinery and chemical plant gases. Key events contributing to the emergence of PSA as an important process option have been the development of synthetic zeolite molecular sieves by Union Carbide Corporation in the USA and of carbon molecular sieves by Bergbau-Forschung in Germany. Today PSA processes enjoy significant commercial use producing oxygen from 0.1 Nm 3 /h for medical application to 1500 Nm 3 /h for steel mill use, for making nitrogen up to 1000 Nm 3 /h for inerting and in purifying hydrogen streams of up to 100,000 Nm 3 /h for refinery use. In this paper some of the principles of adsorptive separations are reviewed. The history of the technology is traced briefly with emphasis on key material, process and application events. The major commercial processes in the application of adsorption to bulk separation of air and hydrogen purification are reviewed in more detail with comparisons made to cryogenic alternatives in terms of specific characteristics, advantages and disadvantages where appropriate. Information on performance, reliability and comparative economics are discussed where available

  11. Density functional theory based-study of 5-fluorouracil adsorption on β-cristobalite (1 1 1) hydroxylated surface: The importance of H-bonding interactions

    Energy Technology Data Exchange (ETDEWEB)

    Simonetti, S., E-mail: ssimonet@uns.edu.ar [Universidad Nacional del Sur (UNS)—Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), Bahía Blanca (Argentina); Universidad Tecnológica Nacional (UTN), Bahía Blanca (Argentina); Compañy, A. Díaz [Comisión de Investigaciones Científicas (CIC), Buenos Aires (Argentina); Pronsato, E.; Juan, A.; Brizuela, G. [Universidad Nacional del Sur (UNS)—Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), Bahía Blanca (Argentina); Lam, A. [Instituto de Ciencia y Tecnología de Materiales (IMRE), Universidad de La Habana (Cuba)

    2015-12-30

    Graphical abstract: - Highlights: • Favorable energies results in optimum four adsorption geometries. • Silanols are partially weakening and establish H-bonds with polar groups of 5-FU drug. • Dispersion forces approach the 5-FU molecule toward the surface. • Electron exchange is presented after adsorption. • H-bonds stabilize the molecule playing significant role in the adsorption mechanism. - Abstract: Silica-based mesoporous materials have been recently proposed as an efficient support for the controlled release of a popular anticancer drug, 5-fluorouracil (5-FU). Although the relevance of this topic, the atomistic details about the specific surface-drug interactions and the energy of adsorption are almost unknown. In this work, theoretical calculations using the Vienna Ab-initio Simulation Package (VASP) applying Grimme's—D2 correction were performed to elucidate the drug–silica interactions and the host properties that control 5-FU drug adsorption on β-cristobalite (1 1 1) hydroxylated surface. This study shows that hydrogen bonding, electron exchange, and dispersion forces are mainly involved to perform the 5-FU adsorption onto silica. This phenomenon, revealed by favorable energies, results in optimum four adsorption geometries that can be adopted for 5-FU on the hydroxylated silica surface. Silanols are weakening in response to the molecule approach and establish H-bonds with polar groups of 5-FU drug. The final geometry of 5-FU adopted on hydroxylated silica surface is the results of H-bonding interactions which stabilize and fix the molecule to the surface and dispersion forces which approach it toward silica (1 1 1) plane. The level of hydroxylation of the SiO{sub 2} (1 1 1) surface is reflected by the elevated number of hydrogen bonds that play a significant role in the adsorption mechanisms.

  12. Stability and Electronic Properties of Hydrogenated Zigzag Carbon Nanotube Focused on Stone-Wales Defect

    International Nuclear Information System (INIS)

    Pan Li-Jun; Zhang Jie; Chen Wei-Guang; Tang Ya-Nan

    2015-01-01

    We present a first-principles study of the chemisorption of hydrogen on a Stone-Wales (SW) defective carbon nanotube (10,0). The investigated configurations include four configurations covering single defects and double defects. One hydrogen dimer adsorption is energetically favored on bonds shared by carbon heptagon-heptagon for configurations with the defect parallel to the tube axis compared with the carbon pentagon-hexagon sites for ones with a slanted defect. This different behavior is also demonstrated for hydrogen dimer chain adsorption, the favored site for the former ones is through the defect, which is the nearest neighbor site to defect for the latter ones. It is found that the energy band gaps of hydrogenated configurations may be enlarged or decreased by altering the adsorption site or defect position. The semiconductor-to-metal transition may occur for configurations with the defect or defects parallel to the tube axis due to low electronic localization. Our results highlight the interest of the interaction of multi-factor system by providing a detailed bond and position picture of a hydrogenated defective carbon nanotube (10,0). (paper)

  13. Hydrogen storage in N- and B-doped graphene decorated by small platinum clusters: A computational study

    Science.gov (United States)

    Chen, I.-Nan; Wu, Shiuan-Yau; Chen, Hsin-Tsung

    2018-05-01

    In this work, we perform density functional theory (DFT) calculations to investigate the hydrogen adsorption on Pt4 cluster supported on pristine, B-, and N-doped graphene sheets. It is found that the doping B or N atom in the graphene could enhance the interaction between the Pt4 cluster and the supporting substrate. The first H2 molecule is found to be dissociative chemisorption on the three substrates. Further, dissociative and molecular adsorption of multiple H2 molecules are co-adsorbed on the three substrates. In addition, the interaction between Pt4(H2)x and the substrate is illustrated for the stability of Pt4(H2)x on the substrate. AIMD simulation is also performed to verify the stability and hydrogen storage. Accordingly, the B-graphene is predicted to be the most potential materials for hydrogen storage among these three materials.

  14. Adsorptive separation of ethylene/ethane mixtures using carbon nanotubes: a molecular dynamics study

    International Nuclear Information System (INIS)

    Tian, Xingling; Zhou, Bo; Wang, Zhigang; Yang, Zaixing; Xiu, Peng

    2013-01-01

    Ethylene/ethane separation is a very important process in the chemical industry. Traditionally, this process is achieved by cryodistillation, which is extremely energy-intensive. The adsorptive separation is an energy-saving and environmentally benign alternative. In this study, we employ molecular dynamics simulations to study the competitive adsorption of an equimolar mixture of gaseous ethane and ethylene inside single-walled carbon nanotubes (SWNTs) of different diameters at room temperature. We find that for narrow SWNTs, i.e. the (6, 6) and (7, 7) SWNTs, the selectivities towards ethane, f selec , can reach values of 3.1 and 3.7, respectively. Such high selectivities are contrary to the opinion of many researchers that the adsorptive separation of an ethylene/ethane mixture by means of dispersion interaction is difficult due to the same carbon number of ethane and ethylene. The key for our observation is that the role of dispersion interaction of ethane's additional two hydrogen atoms with the SWNT becomes significant under extreme confinement. Interestingly, the (8, 8) SWNT prefers ethylene to ethane with f selec = 0.6. For wider SWNTs, f selec converges to ∼1. The mechanisms behind these observations, as well as the kinetics of single-file nanopore filling and kinetics of confined gas molecules are discussed. Our findings suggest that efficient ethane/ethylene separation can be achieved by using bundles/membranes of SWNTs with appropriate diameters. (paper)

  15. Glucose recovery from aqueous solutions by adsorption in metal–organic framework MIL-101: a molecular simulation study

    Science.gov (United States)

    Gupta, Krishna M.; Zhang, Kang; Jiang, Jianwen

    2015-01-01

    A molecular simulation study is reported on glucose recovery from aqueous solutions by adsorption in metal-organic framework MIL-101. The F atom of MIL-101 is identified to be the most favorable adsorption site. Among three MIL-101-X (X = H, NH2 or CH3), the parent MIL-101 exhibits the highest adsorption capacity and recovery efficacy. Upon functionalization by -NH2 or -CH3 group, the steric hindrance in MIL-101 increases; consequently, the interactions between glucose and framework become less attractive, thus reducing the capacity and mobility of glucose. The presence of ionic liquid, 1-ethyl-3-methyl-imidazolium acetate, as an impurity reduces the strength of hydrogen-bonding between glucose and MIL-101, and leads to lower capacity and mobility. Upon adding anti-solvent (ethanol or acetone), a similar adverse effect is observed. The simulation study provides useful structural and dynamic properties of glucose in MIL-101, and it suggests that MIL-101 might be a potential candidate for glucose recovery. PMID:26242874

  16. A Study of the Mechanism of the Hydrogen Evolution Reaction on Nickel by Surface Interrogation Scanning Electrochemical Microscopy.

    Science.gov (United States)

    Liang, Zhenxing; Ahn, Hyun S; Bard, Allen J

    2017-04-05

    The hydrogen evolution reaction (HER) on Ni in alkaline media was investigated by scanning electrochemical microscopy under two operating modes. First, the substrate generation/tip collection mode was employed to extract the "true" cathodic current associated with the HER from the total current in the polarization curve. Compared to metallic Ni, the electrocatalytic activity of the HER is improved in the presence of the low-valence-state oxide of Ni. This result is in agreement with a previous claim that the dissociative adsorption of water can be enhanced at the Ni/Ni oxide interface. Second, the surface-interrogation scanning electrochemical microscopy (SI-SECM) mode was used to directly measure the coverage of the adsorbed hydrogen on Ni at given potentials. Simulation indicates that the hydrogen coverage follows a Frumkin isotherm with respect to the applied potential. On the basis of the combined analysis of the Tafel slope and surface hydrogen coverage, the rate-determining step is suggested to be the adsorption of hydrogen (Volmer step) in the investigated potential window.

  17. An enhanced hydrogen adsorption enthalpy for fluoride intercalated graphite compounds.

    Science.gov (United States)

    Cheng, Hansong; Sha, Xianwei; Chen, Liang; Cooper, Alan C; Foo, Maw-Lin; Lau, Garret C; Bailey, Wade H; Pez, Guido P

    2009-12-16

    We present a combined theoretical and experimental study on H(2) physisorption in partially fluorinated graphite. This material, first predicted computationally using ab initio molecular dynamics simulation and subsequently synthesized and characterized experimentally, represents a novel class of "acceptor type" graphite intercalated compounds that exhibit significantly higher isosteric heat of adsorption for H(2) at near ambient temperatures than previously demonstrated for commonly available porous carbon-based materials. The unusually strong interaction arises from the semi-ionic nature of the C-F bonds. Although a high H(2) storage capacity (>4 wt %) at room temperature is predicted not to be feasible due to the low heat of adsorption, enhanced storage properties can be envisaged by doping the graphitic host with appropriate species to promote higher levels of charge transfer from graphene to F(-) anions.

  18. Hydrogen storage by carbon materials synthesized from oil seeds and fibrous plant materials

    Energy Technology Data Exchange (ETDEWEB)

    Sharon, Maheshwar; Bhardwaj, Sunil; Jaybhaye, Sandesh [Nanotechnology Research Center, Birla College, Kalyan 421304 (India); Soga, T.; Afre, Rakesh [Graduate School of Engineering, Nagoya Institute of Technology, Nagoya (Japan); Sathiyamoorthy, D.; Dasgupta, K. [Powder Metallurgy Division, BARC, Trombay 400 085 (India); Sharon, Madhuri [Monad Nanotech Pvt. Ltd., A702 Bhawani Tower, Powai, Mumbai 400 076 (India)

    2007-12-15

    Carbon materials of various morphologies have been synthesized by pyrolysis of various oil-seeds and plant's fibrous materials. These materials are characterized by SEM and Raman. Surface areas of these materials are determined by methylene blue method. These carbon porous materials are used for hydrogen storage. Carbon fibers with channel type structure are obtained from baggas and coconut fibers. It is reported that amongst the different plant based precursors studied, carbon from soyabean (1.09 wt%) and baggas (2.05 wt%) gave the better capacity to store hydrogen at 11kg/m{sup 2} pressure of hydrogen at room temperature. Efforts are made to correlate the hydrogen adsorption capacity with intensities and peak positions of G- and D-band obtained with carbon materials synthesized from plant based precursors. It is suggested that carbon materials whose G-band is around 1575cm{sup -1} and the intensity of D-band is less compared to G-band, may be useful material for hydrogen adsorption study. (author)

  19. Recovery of high-purity hydrogen from COG

    Energy Technology Data Exchange (ETDEWEB)

    Tsukiyama, Y

    1982-01-01

    A general account of the latest trends in the recovery of high-purity hydrogen from coke oven gas (COG), the article being based on both Japanese and overseas literature: 1) Deep-freeze separation: impurities are liquefied and removed. This method make use of the fact that hydrogen is hard to liquefy. 2) The PSA method: high-purity hydrogen is recovered by the adsorption of other constituents at high pressures. This technique makes use of the fact that the adsorption capacity of an adsorbent varies with the partial pressure of the substances being adsorbed. 3) Membrane separation: a permeation separation method that uses a functional polymer separation membrane, and that depends on the fact that hydrogen has a low molecular weight in comparison with the other constituents. (19 refs.) (In Japanese)

  20. Adsorption of ammonia at GaN(0001) surface in the mixed ammonia/hydrogen ambient - a summary of ab initio data

    International Nuclear Information System (INIS)

    Kempisty, Paweł; Krukowski, Stanisław

    2014-01-01

    Adsorption of ammonia at NH 3 /NH 2 /H-covered GaN(0001) surface was analyzed using results of ab initio calculations. The whole configuration space of partially NH 3 /NH 2 /H-covered GaN(0001) surface was divided into zones of differently pinned Fermi level: at the Ga broken bond state for dominantly bare surface (region I), at the valence band maximum (VBM) for NH 2 and H-covered surface (region II), and at the conduction band minimum (CBM) for NH 3 -covered surface (region III). The electron counting rule (ECR) extension was formulated for the case of adsorbed molecules. The extensive ab intio calculations show the validity of the ECR in case of all mixed H-NH 2 -NH 3 coverages for the determination of the borders between the three regions. The adsorption was analyzed using the recently identified dependence of the adsorption energy on the charge transfer at the surface. For region I ammonia adsorbs dissociatively, disintegrating into a H adatom and a HN 2 radical for a large fraction of vacant sites, while for region II adsorption of ammonia is molecular. The dissociative adsorption energy strongly depends on the Fermi level at the surface (pinned) and in the bulk (unpinned) while the molecular adsorption energy is determined by bonding to surface only, in accordance to the recently published theory. Adsorption of Ammonia in region III (Fermi level pinned at CBM) leads to an unstable configuration both molecular and dissociative, which is explained by the fact that broken Ga-bonds are doubly occupied by electrons. The adsorbing ammonia brings 8 electrons to the surface, necessitating the transfer of these two electrons from the Ga broken bond state to the Fermi level. This is an energetically costly process. Adsorption of ammonia at H-covered site leads to the creation of a NH 2 radical at the surface and escape of H 2 molecule. The process energy is close to 0.12 eV, thus not large, but the direct inverse process is not possible due to the escape of the

  1. The potential of organic polymer-based hydrogen storage materials.

    Science.gov (United States)

    Budd, Peter M; Butler, Anna; Selbie, James; Mahmood, Khalid; McKeown, Neil B; Ghanem, Bader; Msayib, Kadhum; Book, David; Walton, Allan

    2007-04-21

    The challenge of storing hydrogen at high volumetric and gravimetric density for automotive applications has prompted investigations into the potential of cryo-adsorption on the internal surface area of microporous organic polymers. A range of Polymers of Intrinsic Microporosity (PIMs) has been studied, the best PIM to date (a network-PIM incorporating a triptycene subunit) taking up 2.7% H(2) by mass at 10 bar/77 K. HyperCrosslinked Polymers (HCPs) also show promising performance as H(2) storage materials, particularly at pressures >10 bar. The N(2) and H(2) adsorption behaviour at 77 K of six PIMs and a HCP are compared. Surface areas based on Langmuir plots of H(2) adsorption at high pressure are shown to provide a useful guide to hydrogen capacity, but Langmuir plots based on low pressure data underestimate the potential H(2) uptake. The micropore distribution influences the form of the H(2) isotherm, a higher concentration of ultramicropores (pore size <0.7 nm) being associated with enhanced low pressure adsorption.

  2. Influence of electrolyte nature on steel membrane hydrogen permeability

    International Nuclear Information System (INIS)

    Lisovskij, A.P.; Nazarov, A.P.; Mikhajlovskij, Yu.N.

    1993-01-01

    Effect of electrolyte nature on hydrogen absorption of carbonic steel membrane at its cathode polarization is studied. Electrolyte buffering by anions of subdissociated acids is shown to increase hydrogen flow though the membrane in acid electrolytes. Mechanisms covering dissociation of proton-bearing anion in the electrolyte near-the-electron layer or dissociative adsorption on steel surface are suggested. Effect of proton-bearing bases forming stable complex compounds with iron, is studied. Activation of anode process of iron solution is shown to increase the rate of hydrogen penetration

  3. Adsorption of emerging contaminant metformin using graphene oxide.

    Science.gov (United States)

    Zhu, Shuai; Liu, Yun-Guo; Liu, Shao-Bo; Zeng, Guang-Ming; Jiang, Lu-Hua; Tan, Xiao-Fei; Zhou, Lu; Zeng, Wei; Li, Ting-Ting; Yang, Chun-Ping

    2017-07-01

    The occurrence of emerging contaminants in our water resources poses potential threats to the livings. Due to the poor treatment in wastewater management, treatment technologies are needed to effectively remove these products for living organism safety. In this study, Graphene oxide (GO) was tested for the first time for its capacity to remove a kind of emerging wastewater contaminants, metformin. The research was conducted by using a series of systematic adsorption and kinetic experiments. The results indicated that GO could rapidly and efficiently reduce the concentration of metformin, which could provide a solution in handling this problem. The uptake of metformin on the graphene oxide was strongly dependent on temperature, pH, ionic strength, and background electrolyte. The adsorption kinetic experiments revealed that almost 80% removal of metformin was achieved within 20 min for all the doses studied, corresponding to the relatively high k 1 (0.232 min -1 ) and k 2 (0.007 g mg -1  min -1 ) values in the kinetic models. It indicated that the highest adsorption capacity in the investigated range (q m ) of GO for metformin was at pH 6.0 and 288 K. Thermodynamic study indicated that the adsorption was a spontaneous (ΔG 0  adsorption of metformin increased when the pH values changed from 4.0 to 6.0, and decreased adsorption were observed at pH 6.0-11.0. GO still exhibited excellent adsorption capacity after several desorption/adsorption cycles. Besides, both so-called π-π interactions and hydrogen bonds might be mainly responsible for the adsorption of metformin onto GO. Copyright © 2017 Elsevier Ltd. All rights reserved.

  4. Study of Supported Nickel Catalysts Prepared by Aqueous Hydrazine Method. Hydrogenating Properties and Hydrogen Storage: Support Effect. Silver Additive Effect; Catalyseurs de nickel supportes prepares par la methode de l'hydrazine aqueuse. Proprietes hydrogenantes et stockage d'hydrogene. Effet du support. Effet de l'ajout d'argent

    Energy Technology Data Exchange (ETDEWEB)

    Wojcieszak, R

    2006-06-15

    We have studied Ni or NiAg nano-particles obtained by the reduction of nickel salts (acetate or nitrate) by hydrazine and deposited by simple or EDTA-double impregnation on various supports ({gamma}-Al{sub 2}O{sub 3}, amorphous or crystallized SiO{sub 2}, Nb{sub 2}O{sub 5}, CeO{sub 2} and carbon). Prepared catalysts were characterized by different methods (XRD, XPS, low temperature adsorption and desorption of N{sub 2}, FTIR and FTIR-Pyridine, TEM, STEM, EDS, H{sub 2}-TPR, H{sub 2}-adsorption, H{sub 2}-TPD, isopropanol decomposition) and tested in the gas phase hydrogenation of benzene or as carbon materials in the hydrogen storage at room temperature and high pressure. The catalysts prepared exhibited better dispersion and activity than classical catalysts. TOF's of NiAg/SiO{sub 2} or Ni/carbon catalysts were similar to Pt catalysts in benzene hydrogenation. Differences in support acidity or preparation method and presence of Ag as metal additive play a crucial role in the chemical reduction of Ni by hydrazine and in the final properties of the materials. Ni/carbon catalysts could store significant amounts of hydrogen at room temperature and high pressure (0.53%/30 bars), probably through the hydrogen spillover effect. (author)

  5. Sum Frequency Generation Vibrational Spectroscopy and Kinetic Study of 2-Methylfuran and 2,5-Dimethylfuran Hydrogenation over 7 nm Platinum Cubic Nanoparticles

    KAUST Repository

    Aliaga, Cesar; Tsung, Chia-Kuang; Alayoglu, Selim; Komvopoulos, Kyriakos; Yang, Peidong; Somorjai, Gabor A.

    2011-01-01

    Sum frequency generation vibrational spectroscopy and kinetic measurements obtained from gas chromatography were used to study the adsorption and hydrogenation of 2-methylfuran (MF) and 2,5-dimethylfuran (DMF) over cubic Pt nanoparticles of 7 nm

  6. Separation of hydrogen isotopes via single column pressure swing adsorption

    International Nuclear Information System (INIS)

    Wong, Y.W.; Hill, F.B.

    1981-01-01

    Separation of hydrogen isotopes based on kinetic isotope effects was studied. The mixture separated was hydrogen containing a trace of tritium as HT and the hydride was vanadium monohydride. The separation was achieved using the single-column pressure swing process. Stage separation factors are larger and product cuts smaller than for a two-column pressure swing process operated in the same monohydride phase

  7. Titanium-decorated graphene for high-capacity hydrogen storage studied by density functional simulations

    International Nuclear Information System (INIS)

    Liu Yali; Ren Ling; He Yao; Cheng Haiping

    2010-01-01

    We present results of density functional theory (DFT) calculations of the adsorption of hydrogen molecules on Ti-decorated graphene. Our results indicate that the binding energies of molecular hydrogen on Ti-decorated graphene can be dramatically enhanced to 0.23-0.60 eV. The hybridization of the Ti 3d orbitals with the H 2 σ and σ* orbitals plays a central role in the enhanced binding. There is also a contribution from the attractive interaction between the surface dipole and the dipole of polarized H 2 . It can be expected that Ti-decorated graphene could be considered as a potential high-capacity hydrogen storage medium.

  8. Wettability modification of Wender lignite by adsorption of dodecyl poly ethoxylated surfactants with different degree of ethoxylation: A molecular dynamics simulation study.

    Science.gov (United States)

    Zhang, Lei; Li, Bao; Xia, Yangchao; Liu, Shengyu

    2017-09-01

    Lignite is an important and useful fossil fuel in the world and the strong hydrophilicity of it limits its applications. Surfactant adsorption on lignite is an effective way to make it hydrophobic. In this work, aiming to examine the effect of the degree of ethoxylation on the adsorption behavior of dodecyl poly ethoxylated surfactants on lignite and the wettability modification of modified lignite by surfactant adsorption, different combined systems formed by surfactants, water and a model surface of Wender lignite have been studied using molecular dynamics simulation. The adsorption configurations vary with the degree of ethoxylation. At the same adsorption amounts, increasing the degree of ethoxylation can make the adsorption layer more compactness and bring stronger adsorption strength. The results of binding energy and its components show that the adsorption of alkyl polyoxyethylene ethers surfactant on lignite is physically adsorbed rather than electrostatically or chemisorbed. Meanwhile, van der Waals interaction plays a dominant role in the adsorption. The addition of surfactant could reduce the possibility of the interaction between water and lignite. Compared to the original lignite, the interaction between them is weakened after surfactant adsorption in water/surfactant/lignite system, thus strengthening the hydrophobicity of lignite. Similar to the adsorption strength, hydrophobicity of modified lignite increases with the increase of the degree of ethoxylation. The lignite surface properties are changed due to surfactant adsorption by analyzing the compositions of interaction energy and the change of hydrogen bonds. Copyright © 2017 Elsevier Inc. All rights reserved.

  9. Water-Stable Metal-Organic Framework with Three Hydrogen-Bond Acceptors: Versatile Theoretical and Experimental Insights into Adsorption Ability and Thermo-Hydrolytic Stability.

    Science.gov (United States)

    Roztocki, Kornel; Lupa, Magdalena; Sławek, Andrzej; Makowski, Wacław; Senkovska, Irena; Kaskel, Stefan; Matoga, Dariusz

    2018-03-19

    A new microporous cadmium metal-organic framework was synthesized both mechanochemically and in solution by using a sulfonyl-functionalized dicarboxylate linker and an acylhydrazone colinker. The three-dimensional framework is highly stable upon heating to 300 °C as well as in aqueous solutions at elevated temperatures or acidic conditions. The thermally activated material exhibits steep water vapor uptake at low relative pressures at 298 K and excellent recyclability up to 260 °C as confirmed by both quasi-equilibrated temperature-programmed desorption and adsorption (QE-TPDA) method as well as adsorption isotherm measurements. Reversible isotherms and hysteretic isobars recorded for the desorption-adsorption cycles indicate the maximum uptake of 0.19 g/g (at 298 K, up to p/p 0 = 1) or 0.18 g/g (at 1 bar, within 295-375 K range), respectively. The experimental isosteric heat of adsorption (48.9 kJ/mol) indicates noncoordinative interactions of water molecules with the framework. Exchange of the solvent molecules in the as-made material with water, performed in the single-crystal to single-crystal manner, allows direct comparison of both X-ray crystal structures. The single-crystal X-ray diffraction for the water-loaded framework demonstrates the orientation of water clusters in the framework cavities and reveals their strong hydrogen bonding with sulfonyl, acyl, and carboxylate groups of the two linkers. The grand canonical Monte Carlo (GCMC) simulations of H 2 O adsorption corroborate the experimental findings and reveal preferable locations of guest molecules in the framework voids at various pressures. Additionally, both experimental and GCMC simulation insights into the adsorption of CO 2 (at 195 K) on the activated framework are presented.

  10. Decoration of carbon nano surfaces with hydrogen and hydrogen rich molecules

    International Nuclear Information System (INIS)

    Zöttl, S.

    2013-01-01

    The use of helium nano droplets as a matrix to investigate different atomic and molecular samples is a well established experimental technique. The unique properties of helium allow for different analytical methods and at the same time provide a stable ambient temperature. Cluster growth inside helium nano droplets can be accomplished by repeatedly doping the droplets with sample particles in a controlled environment. The experimental work represented in this thesis was performed using helium nano droplets to create clusters of fullerenes like C 60 and C 70 . The adsorption properties of these fullerene clusters regarding hydrogen and hydrogen rich molecules have been subject to investigation. The observed results suggest that curved carbon nano surfaces offer higher storage densities than planar graphite surfaces. The use of C 60 as a model carbon nano structure provides a well understood molecule for testing and evaluating computational methods to calculate surface properties of various carbon nano materials. The cost effective storage of hydrogen for mobile applications plays a key role in the development of alternatives to fossil fuels. For that reason, the application of carbon nano materials to store hydrogen by adsorption has attracted much scientific attention lately. The insights gained in the presented thesis contribute to the collective efforts and deliver more refined tools to estimate the adsorption properties of future carbon nano materials. In addition to the aforementioned, a time-of-flight mass spectrometer for educational purpose has been designed and constructed in the framework of my PhD thesis. The instrument is successfully used in various lab courses and information on the setup can be found in the Appendix of this work. (author) [de

  11. Theoretical investigation on the alkali-metal doped BN fullerene as a material for hydrogen storage

    International Nuclear Information System (INIS)

    Venkataramanan, Natarajan Sathiyamoorthy; Belosludov, Rodion Vladimirovich; Note, Ryunosuke; Sahara, Ryoji; Mizuseki, Hiroshi; Kawazoe, Yoshiyuki

    2010-01-01

    Graphical abstract: First-principles calculations have been used to investigate hydrogen adsorption on alkali atom doped B 36 N 36 clusters. Adsorption of alkali atoms involves a charge transfer process, creating positively-charged alkali atoms and this polarizes the H 2 molecules and increases their binding energy. The maximum hydrogen storage capacity of Li doped BN fullerene is 8.9 wt.% in which 60 hydrogen atoms were chemisorbed and 12 H 2 were adsorbed in molecular form. - Abstract: First-principles calculations have been used to investigate hydrogen adsorption on alkali atom doped B 36 N 36 clusters. The alkali atom adsorption takes place near the six tetragonal bridge sites available on the cage, thereby avoiding the notorious clustering problem. Adsorption of alkali atoms involves a charge transfer process, creating positively charged alkali atoms and this polarizes the H 2 molecules thereby, increasing their binding energy. Li atom has been found to adsorb up to three hydrogen molecules with an average binding energy of 0.189 eV. The fully doped Li 6 B 36 N 36 cluster has been found to hold up to 18 hydrogen molecules with the average binding energy of 0.146 eV. This corresponds to a gravimetric density of hydrogen storage of 3.7 wt.%. Chemisorption on the Li 6 B 36 N 36 has been found to be an exothermic reaction, in which 60 hydrogen atoms chemisorbed with an average chemisorption energy of -2.13 eV. Thus, the maximum hydrogen storage capacity of Li doped BN fullerene is 8.9 wt.% in which 60 hydrogen atoms were chemisorbed and 12 hydrogen molecules were adsorbed in molecular form.

  12. Isotopic analysis of H{sub 2}, HD, D{sub 2} mixtures and analysis of ortho-para-hydrogen mixtures by gas chromatography; Dosages par chromatographie en phase gazeuse de melanges d'hydrogene, d'hydrogene deutere, de deuterium et de melanges ortho-para-hydrogene

    Energy Technology Data Exchange (ETDEWEB)

    Botter, F; Perriere, G de la; Tistchenko, S [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

    1961-07-01

    This communication describes the present situation concerning the possibilities of vapor phase chromatography for the separation and analysis of mixtures of H{sub 2}, HD and D{sub 2} and of ortho- and para-hydrogen mixtures. Separation factors for physical adsorption of the various varieties of hydrogen have been deduced from chromatograms and have also been measured directly with a static method - the agreements is good. (author) [French] Le present rapport decrit diverses possibilites qu'offre la chromatographie gazeuse d'elution en ce qui concerne le dosage des melanges H{sub 2}, HD, D{sub 2} et des varietes ortho et para de l'hydrogene. On a calcule, a partir des chromatogrammes obtenus, les facteurs de separation par adsorption physique des differentes varietes d'hydrogene, et compare aux facteurs de separation determines par mesure directe. (auteur)

  13. Molecular dynamics simulations of H2 adsorption in tetramethyl ammonium lithium phthalocyanine crystalline structures.

    Science.gov (United States)

    Lamonte, Kevin; Gómez Gualdrón, Diego A; Cabrales-Navarro, Fredy A; Scanlon, Lawrence G; Sandi, Giselle; Feld, William; Balbuena, Perla B

    2008-12-11

    Tetramethyl ammonium lithium phthalocyanine is explored as a potential material for storage of molecular hydrogen. Density functional theory calculations are used to investigate the molecular structure and the dimer conformation. Additional scans performed to determine the interactions of a H2 molecule located at various distances from the molecular sites are used to generate a simple force field including dipole-induced-dipole interactions. This force field is employed in molecular dynamics simulations to calculate adsorption isotherms at various pressures. The regions of strongest adsorption are quantified as functions of temperature, pressure, and separation between molecules in the adsorbent phase, and compared to the regions of strongest binding energy as given by the proposed force field. It is found that the total adsorption could not be predicted only from the spatial distribution of the strongest binding energies; the available volume is the other contributing factor even if the volume includes regions of much lower binding energy. The results suggest that the complex anion is primarily involved in the adsorption process with molecular hydrogen, whereas the cation serves to provide access for hydrogen adsorption in both sides of the anion molecular plane, and spacing between the planes.

  14. Carbon hybridized halloysite nanotubes for high-performance hydrogen storage capacities

    Science.gov (United States)

    Jin, Jiao; Fu, Liangjie; Yang, Huaming; Ouyang, Jing

    2015-01-01

    Hybrid nanotubes of carbon and halloysite nanotubes (HNTs) with different carbon:HNTs ratio were hydrothermally synthesized from natural halloysite and sucrose. The samples display uniformly cylindrical hollow tubular structure with different morphologies. These hybrid nanotubes were concluded to be promising medium for physisorption-based hydrogen storage. The hydrogen adsorption capacity of pristine HNTs was 0.35% at 2.65 MPa and 298 K, while that of carbon coated HNTs with the pre-set carbon:HNTs ratio of 3:1 (3C-HNTs) was 0.48% under the same condition. This carbon coated method could offer a new pattern for increasing the hydrogen adsorption capacity. It was also possible to enhance the hydrogen adsorption capacity through the spillover mechanism by incorporating palladium (Pd) in the samples of HNTs (Pd-HNTs) and 3C-HNTs (Pd-3C-HNTs and 3C-Pd-HNTs are the samples with different location of Pd nanoparticles). The hydrogen adsorption capacity of the Pd-HNTs was 0.50% at 2.65 MPa and 298 K, while those of Pd-3C-HNTs and 3C-Pd-HNTs were 0.58% and 0.63%, respectively. In particular, for this spillover mechanism of Pd-carbon-HNTs ternary system, the bidirectional transmission of atomic and molecular hydrogen (3C-Pd-HNTs) was concluded to be more effective than the unidirectional transmission (Pd-3C-HNTs) in this work for the first time. PMID:26201827

  15. Computational investigation of hydrogen storage on B5V3

    Science.gov (United States)

    Guo, Chen; Wang, Chong

    2018-05-01

    Based on density functional theory method with 6-311+G(d,p) basis set, the structures, stability and hydrogen storage capacity of B5V3 have been theoretically investigated. It is found that a maximum of seven hydrogen molecules can be adsorbed on B5V3 with gravimetric uptake capacity of 6.39 wt%. The uptake capacity exceeds the target set by the US Department of Energy for vehicular application. Moreover, the average adsorption energy of B5V3 01 (7H2) is 0.60 eV/H2 in the desirable range of reversible hydrogen storage. The kinetic stability of H2 adsorbed on B5V3 01 is confirmed by using gap between highest occupied molecular orbital (HOMO)and the lowest unoccupied molecular orbital (LUMO). The gap value of B5V3 01 (7H2) is 2.81 eV, which indicates the compound with high stability. In addition, the thermochemistry calculation (Gibbs free energy corrected adsorption energy) is used to analyse if the adsorption is favourable or not at different temperatures. It can be found that the Gibbs corrected adsorption energy of B5V3 01 (7H2) is still positive at 400 K at 1 atm. It means that the adsorption of seven hydrogen molecules on B5V3 01 is energetically favourable in a fairly wide temperature range. All the results show that B5V3 01 can be considered as a promising material for hydrogen storage.

  16. Ice XVII as a Novel Material for Hydrogen Storage

    Directory of Open Access Journals (Sweden)

    Leonardo del Rosso

    2017-02-01

    Full Text Available Hydrogen storage is one of the most addressed issues in the green-economy field. The latest-discovered form of ice (XVII, obtained by application of an annealing treatment to a H 2 -filled ice sample in the C 0 -phase, could be inserted in the energy-storage context due to its surprising capacity of hydrogen physisorption, when exposed to even modest pressure (few mbars at temperature below 40 K, and desorption, when a thermal treatment is applied. In this work, we investigate quantitatively the adsorption properties of this simple material by means of spectroscopic and volumetric data, deriving its gravimetric and volumetric capacities as a function of the thermodynamic parameters, and calculating the usable capacity in isothermal conditions. The comparison of ice XVII with materials with a similar mechanism of hydrogen adsorption like metal-organic frameworks shows interesting performances of ice XVII in terms of hydrogen content, operating temperature and kinetics of adsorption-desorption. Any application of this material to realistic hydrogen tanks should take into account the thermodynamic limit of metastability of ice XVII, i.e., temperatures below about 130 K.

  17. Hydrogen storage in engineered carbon nanospaces.

    Science.gov (United States)

    Burress, Jacob; Kraus, Michael; Beckner, Matt; Cepel, Raina; Suppes, Galen; Wexler, Carlos; Pfeifer, Peter

    2009-05-20

    It is shown how appropriately engineered nanoporous carbons provide materials for reversible hydrogen storage, based on physisorption, with exceptional storage capacities (approximately 80 g H2/kg carbon, approximately 50 g H2/liter carbon, at 50 bar and 77 K). Nanopores generate high storage capacities (a) by having high surface area to volume ratios, and (b) by hosting deep potential wells through overlapping substrate potentials from opposite pore walls, giving rise to a binding energy nearly twice the binding energy in wide pores. Experimental case studies are presented with surface areas as high as 3100 m(2) g(-1), in which 40% of all surface sites reside in pores of width approximately 0.7 nm and binding energy approximately 9 kJ mol(-1), and 60% of sites in pores of width>1.0 nm and binding energy approximately 5 kJ mol(-1). The findings, including the prevalence of just two distinct binding energies, are in excellent agreement with results from molecular dynamics simulations. It is also shown, from statistical mechanical models, that one can experimentally distinguish between the situation in which molecules do (mobile adsorption) and do not (localized adsorption) move parallel to the surface, how such lateral dynamics affects the hydrogen storage capacity, and how the two situations are controlled by the vibrational frequencies of adsorbed hydrogen molecules parallel and perpendicular to the surface: in the samples presented, adsorption is mobile at 293 K, and localized at 77 K. These findings make a strong case for it being possible to significantly increase hydrogen storage capacities in nanoporous carbons by suitable engineering of the nanopore space.

  18. Development of porous materials for hydrogen storage

    Energy Technology Data Exchange (ETDEWEB)

    Shinji Oshima; Osamu Kato; Takeshi Kataoka; Yoshihiro Kobori; Michiaki Adachi [Hydrogen and New Energy Research Laboratory Nippon Oil Corporation 8, Chidoricho, Naka-ku, Yokohama, 231-0815 (Japan)

    2006-07-01

    To achieve hydrogen storage of more than 5 mass%, we are focusing on porous materials that consist of light elements. At WHEC 15, we reported that KOH-activated bamboo charcoal showed 0.79 mass% hydrogen uptake at 9.5 MPa and 303 K. After examining various carbon materials, we found that carbonized and KOH-activated polyacrylonitrile fibers showed 1.0 mass% hydrogen uptake at 9.5 MPa and 303 K. When the pressure was raised to 35 MPa, this material showed 1.5 mass% hydrogen uptake at 303 K. Besides porous carbon, other materials, such as coordination polymers, were examined. Since these materials contain elements other than carbon, different adsorption phenomena may be expected. Although the values of their hydrogen uptakes are still lower than those of carbon materials, a coordination polymer which showed 0.38 mass% hydrogen uptake at 9.5 MPa and 303 K was revealed to give an adsorption density of 47 kg/m{sup 3} at 0.1 MPa and 77 K, the highest value reported for a coordination polymer. (authors)

  19. p-Chlorophenol adsorption on activated carbons with basic surface properties

    Science.gov (United States)

    Lorenc-Grabowska, Ewa; Gryglewicz, Grażyna; Machnikowski, Jacek

    2010-05-01

    The adsorption of p-chlorophenol (PCP) from aqueous solution on activated carbons (ACs) with basic surface properties has been studied. The ACs were prepared by two methods. The first method was based on the modification of a commercial CWZ AC by high temperature treatment in an atmosphere of ammonia, nitrogen and hydrogen. The second approach comprised the carbonization followed by activation of N-enriched polymers and coal tar pitch using CO 2 and steam as activation agent. The resultant ACs were characterized in terms of porous structure, elemental composition and surface chemistry (pH PZC, acid/base titration, XPS). The adsorption of PCP was carried out from an aqueous solution in static conditions. Equilibrium adsorption isotherm was of L2 type for polymer-based ACs, whereas L3-type isotherm was observed for CWZ ACs series. The Langmuir monolayer adsorption capacity was related to the porous structure and the amount of basic sites. A good correlation was found between the adsorption capacity and the volume of micropores with a width water molecule adsorption on the PCP uptake is discussed.

  20. Early construction and operation of the highly contaminated water treatment system in Fukushima Daiichi Nuclear Power Station (4). Assessment of hydrogen behavior in stored Cs adsorption vessel

    International Nuclear Information System (INIS)

    Kondo, Masahiro; Arai, Takahiro; Nishi, Yoshihisa

    2014-01-01

    Hydrogen diffusion behavior in a cesium adsorption vessel is assessed. The vessel is used to remove radioactive substance from contaminated water, which is proceeded from Fukushima accident. Experiment and numerical calculation are conducted to clarify the characteristics of natural circulation in the vessel. The natural circulation arising from the temperature difference between inside and outside the vessel is confirmed. We develop an evaluation model to predict the natural circulation and its prediction agrees well with the results obtained by the experiment and the calculation. Using the model, we predict steady and transient behavior of hydrogen concentration. Results indicate that hydrogen concentration is kept lower than the flammability limit when the short vent pipe is open. (author)

  1. A DFT investigation on group 8B transition metal-doped silicon carbide nanotubes for hydrogen storage application

    Science.gov (United States)

    Tabtimsai, Chanukorn; Ruangpornvisuti, Vithaya; Tontapha, Sarawut; Wanno, Banchob

    2018-05-01

    The binding of group 8B transition metal (TMs) on silicon carbide nanotubes (SiCNT) hydrogenated edges and the adsorption of hydrogen molecule on the pristine and TM-doped SiCNTs were investigated using the density functional theory method. The B3LYP/LanL2DZ method was employed in all calculations for the considered structural, adsorption, and electronic properties. The Os atom doping on the SiCNT is found to be the strongest binding. The hydrogen molecule displays a weak interaction with pristine SiCNT, whereas it has a strong interaction with TM-doped SiCNTs in which the Os-doped SiCNT shows the strongest interaction with the hydrogen molecule. The improvement in the adsorption abilities of hydrogen molecule onto TM-doped SiCNTs is due to the protruding structure and the induced charge transfer between TM-doped SiCNT and hydrogen molecule. These observations point out that TM-doped SiCNTs are highly sensitive toward hydrogen molecule. Moreover, the adsorptions of 2-5 hydrogen molecules on TM-doped SiCNT were also investigated. The maximum storage number of hydrogen molecules adsorbed on the first layer of TM-doped SiCNTs is 3 hydrogen molecules. Therefore, TM-doped SiCNTs are suitable to be sensing and storage materials for hydrogen gas.

  2. Tetrahedral silsesquioxane-C2H2Ti complex for hydrogen storage

    Science.gov (United States)

    Konda, Ravinder; Tavhare, Priyanka; Ingale, Nilesh; Chaudhari, Ajay

    2018-04-01

    The interaction of molecular hydrogen with tetrahedral silsesquioxane (T4)-C2H2Ti complex has been studied using Density Functional Theory with M06-2X functional and MP2 method with 6-311++G** basis set. T4-C2H2Ti complex can absorb maximum five hydrogen molecules with the gravimetric hydrogen storage capacity of 3.4 wt %. Adsorption energy calculations show that H2 adsorption on T4-C2H2Ti complex is favorable at room temperature by both the methods. We have studied the effect of temperature and pressure on Gibbs free energy corrected adsorption energies. Molecular dynamics simulations for H2 adsorbed T4-C2H2Ti complex have also been performed at 300K and show that loosely bonded H2 molecule flies away within 1fs. Various interaction energies within the complex are studied. Stability of a complex is predicted by means of a gap between Highest Occupied Molecular Orbital (HUMO) and Lowest Unoccupied Molecular Orbital (LUMO). The H2 desorption temperature for T4-C2H2Ti complex is calculated with Van't Hoff equation and it is found to be 229K.

  3. Enhanced Hydrogen Dipole Physisorption, Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Ahn, Channing [California Inst. of Technology (CalTech), Pasadena, CA (United States)

    2014-01-03

    The hydrogen gas adsorption effort at Caltech was designed to probe and apply our understanding of known interactions between molecular hydrogen and adsorbent surfaces as part of a materials development effort to enable room temperature storage of hydrogen at nominal pressure. The work we have performed over the past five years has been tailored to address the outstanding issues associated with weak hydrogen sorbent interactions in order to find an adequate solution for storage tank technology.

  4. Large entropy derived from low-frequency vibrations and its implications for hydrogen storage

    Science.gov (United States)

    Wang, Xiaoxia; Chen, Hongshan

    2018-02-01

    Adsorption and desorption are driven by the energy and entropy competition, but the entropy effect is often ignored in hydrogen storage and the optimal adsorption strength for the ambient storage is controversial in the literature. This letter investigated the adsorption states of the H2 molecule on M-B12C6N6 (M = Li, Na, Mg, Ca, and Sc) and analyzed the correlation among the zero point energy (ZPE), the entropy change, and the adsorption energy and their effects on the delivery capacities. The ZPE has large correction to the adsorption energy due to the light mass of hydrogen. The computations show that the potential energies along the spherical surface centered at the alkali metals are very flat and it leads to large entropy (˜70 J/mol.K) of the adsorbed H2 molecules. The entropy change can compensate the enthalpy change effectively, and the ambient storage can be realized with relatively weak adsorption of ΔH = -12 kJ/mol. The results are encouraging and instructive for the design of hydrogen storage materials.

  5. Study on Shale Adsorption Equation Based on Monolayer Adsorption, Multilayer Adsorption, and Capillary Condensation

    OpenAIRE

    Chen, Qing; Tian, Yuanyuan; Li, Peng; Yan, Changhui; Pang, Yu; Zheng, Li; Deng, Hucheng; Zhou, Wen; Meng, Xianghao

    2017-01-01

    Shale gas is an effective gas resource all over the world. The evaluation of pore structure plays a critical role in exploring shale gas efficiently. Nitrogen adsorption experiment is one of the significant approaches to analyze pore size structure of shale. Shale is extremely heterogeneous due to component diversity and structure complexity. Therefore, adsorption isotherms for homogeneous adsorbents and empirical isotherms may not apply to shale. The shape of adsorption-desorption curve indi...

  6. Adsorption dynamics and equilibrium studies of Zn (II)

    Indian Academy of Sciences (India)

    Batch equilibration studies are conducted to determine the nature of adsorption of zinc (II) over chitosan. The factors affecting the adsorption process like particle size, contact time, dosage, pH, effects of chloride and nitrate are identified. The influence of temperature and co-ions on the adsorption process is verified.

  7. Prospects for hydrogen storage in graphene.

    Science.gov (United States)

    Tozzini, Valentina; Pellegrini, Vittorio

    2013-01-07

    Hydrogen-based fuel cells are promising solutions for the efficient and clean delivery of electricity. Since hydrogen is an energy carrier, a key step for the development of a reliable hydrogen-based technology requires solving the issue of storage and transport of hydrogen. Several proposals based on the design of advanced materials such as metal hydrides and carbon structures have been made to overcome the limitations of the conventional solution of compressing or liquefying hydrogen in tanks. Nevertheless none of these systems are currently offering the required performances in terms of hydrogen storage capacity and control of adsorption/desorption processes. Therefore the problem of hydrogen storage remains so far unsolved and it continues to represent a significant bottleneck to the advancement and proliferation of fuel cell and hydrogen technologies. Recently, however, several studies on graphene, the one-atom-thick membrane of carbon atoms packed in a honeycomb lattice, have highlighted the potentialities of this material for hydrogen storage and raise new hopes for the development of an efficient solid-state hydrogen storage device. Here we review on-going efforts and studies on functionalized and nanostructured graphene for hydrogen storage and suggest possible developments for efficient storage/release of hydrogen under ambient conditions.

  8. Protein Adsorption in Three Dimensions

    Science.gov (United States)

    Vogler, Erwin A.

    2011-01-01

    initially-adsorbed protein. Interphase protein concentration CI increases as VI decreases, resulting in slow reduction in interfacial energetics. Steady-state is governed by a net partition coefficient P=(/CBCI). In the process of occupying space within the interphase, adsorbing protein molecules must displace an equivalent volume of interphase water. Interphase water is itself associated with surface-bound water through a network of transient hydrogen bonds. Displacement of interphase water thus requires an amount of energy that depends on the adsorbent surface chemistry/energy. This “adsorption-dehydration” step is the significant free-energy cost of adsorption that controls the maximum amount of protein that can be adsorbed at steady state to a unit adsorbent-surface area (the adsorbent capacity). As adsorbent hydrophilicity increases, protein adsorption monotonically decreases because the energetic cost of surface dehydration increases, ultimately leading to no protein adsorption near an adsorbent water wettability (surface energy) characterized by a water contact angle θ → 65°. Consequently, protein does not adsorb (accumulate at interphase concentrations greater than bulk solution) to more hydrophilic adsorbents exhibiting θ protein/surface interactions can be highly favorable, causing protein to adsorb in multilayers in a relatively thick interphase. A straightforward, three-component free energy relationship captures salient features of protein adsorption to all surfaces predicting that the overall free energy of protein adsorption ΔGadso is a relatively small multiple of thermal energy for any surface chemistry (except perhaps for bioengineered surfaces bearing specific ligands for adsorbing protein) because a surface chemistry that interacts chemically with proteins must also interact with water through hydrogen bonding. In this way, water moderates protein adsorption to any surface by competing with adsorbing protein molecules. This Leading Opinion ends

  9. H_{2} adsorption on multiwalled carbon nanotubes at low temperatures and low pressures

    Directory of Open Access Journals (Sweden)

    F. Xu

    2008-11-01

    Full Text Available We present an experimental study on H_{2} adsorption on multiwalled carbon nanotubes (MWCNTs at low temperatures (12–30 K and low pressures (2×10^{-5}  Torr using the temperature programmed desorption technique. Our results show that the molecular hydrogen uptake increases nearly exponentially from 6×10^{-9}  wt. % at 24.5 K to 2×10^{-7}  wt. % at 12.5 K and that the desorption kinetics is of the first order. Comparative measurements indicate that MWCNTs have an adsorption capacity about two orders higher than that of activated carbon (charcoal making them a possible candidate as hydrogen cryosorber for eventual applications in accelerators and synchrotrons.

  10. High purity hydrogen production system by the PSA method

    Energy Technology Data Exchange (ETDEWEB)

    1986-01-01

    In a process developed by Nippon Steel, coke oven gas is compressed and purified of tarry matter, sulphur compounds and gum-formers by adsorption. It is then passed through a three-tower pressure-swing adsorption system to recover hydrogen whose purity can be selected in the range 99 to 99.999%. A composite adsorption agent is used.

  11. Environmental protection and processing of feedstocks by adsorption on carbonaceous materials - developments at Bergbau- Forschung GmbH

    Energy Technology Data Exchange (ETDEWEB)

    Knoblauch, K; Richter, E

    1986-06-01

    Activated carbons, active cokes and carbon molecular sieves are used for regenerative processes for environmental protection and for processing of valuable feedstocks. Development of adsorption processes and their layout based on adsorption equilibria, adsorption kinetics, kinetics of desorption by heating, depressurization or purging not only as single steps but in the same combination as in the regenerative process. For example some adsorption processes are decsribed which are applied in pilot scale or industrially. These include: nitrogen production from air by pressure swing adsorption (PSA); hydrogen production from coke oven gas by PSA; upgrading of methane from biogas and from fire damp; removal of hydrogen sulfide from biogas; removal of sulfur dioxide and nitrogen oxides from flue gases and drinking water supply and waste water treatment. (71 refs.)

  12. Ionic liquid-impregnated activated carbon for biohydrogen purification in an adsorption unit

    Science.gov (United States)

    Yusuf, N. Y.; Masdar, M. S.; Isahak, W. N. R. W.; Nordin, D.; Husaini, T.; Majlan, E. H.; Rejab, S. A. M.; Chew, C. L.

    2017-06-01

    Biological methods for hydrogen production (biohydrogen) are known as energy intensive and can be operated at ambient temperature and pressure; however, consecutive productions such as purification and separation processes still remain challenging in the industry. Various techniques are used to purify and separate hydrogen. These techniques include the use of sorbents/solvents, membranes and cryogenic distillation. In this study, carbon dioxide (CO2) was purified and separated from biohydrogen to produce high purity hydrogen gas. CO2 capture was studied using the activated carbon (AC) modified with the ionic liquid (IL) choline chloride as adsorbent. The physical and chemical properties of the adsorbents were characterized through XRD, FTIR, SEM-EDX, TGA, and BET analyses. The effects of IL loading, flow rate, temperature, and gas mixture were also investigated based on the absorption and desorption of CO2. The CO2 level in the biohydrogen composition was analyzed using a CO2 gas analyzer. The SEM image indicated that the IL homogeneously covered the AC surface. High IL dispersion inlet enhanced the capability of the adsorbent to capture CO2 gas. The thermal stability and presence of the functionalized group of ILs on AC were analyzed by TGA and FTIR techniques, respectively. CO2 adsorption experiments were conducted using a 1 L adsorber unit. Hence, adsorption technologies exhibit potential for biohydrogen purification and mainly affected by adsorbent ability and operating parameters. This research presents an improved biohydrogen technique based on adsorption technology with novel adsorbents. Two different types of commercial CO2 adsorbents were used in the experiment. Results show that the IL/AC exhibited properties suitable for CO2 adsorption. The IL/AC sample presented a high CO2 uptake of 30 wt. % IL when treated at 30 °C for 6 h under a flow rate of 1 L/min. The presence of IL increased the selectivity of CO2 removal during the adsorption process. This IL

  13. Quantum Chemical Study of Water Adsorption on the Surfaces of SrTiO3 Nanotubes.

    Science.gov (United States)

    Bandura, Andrei V; Kuruch, Dmitry D; Evarestov, Robert A

    2015-07-20

    We have studied the adsorption of water molecules on the inner and outer surfaces of nanotubes generated by rolling (001) layers of SrTiO3 cubic crystals. The stability and the atomic and electronic structures of the adsorbed layers are determined by using hybrid density functional theory. The absorption energy and the preferred adsorbate structure are essentially governed by the nature of the surface of the nanotube. Dissociative adsorption prevails on the outer nanotube surfaces. The stability of the adsorbed layers on the inner surfaces is related to the possibility of the formation of hydrogen bonds between water molecules and surface oxygen atoms, and depends on the surface curvature. The presence of water molecules on the inner surface of the nanotubes leads to an increase of the electronic band gap. Externally TiO2 -terminated nanotubes could be used for the photocatalytic decomposition of water by ultraviolet radiation. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Metalized T graphene: A reversible hydrogen storage material at room temperature

    International Nuclear Information System (INIS)

    Ye, Xiao-Juan; Zhong, Wei; Du, You-Wei; Liu, Chun-Sheng; Zeng, Zhi

    2014-01-01

    Lithium (Li)-decorated graphene is a promising hydrogen storage medium due to its high capacity. However, homogeneous mono-layer coating graphene with lithium atoms is metastable and the lithium atoms would cluster on the surface, resulting in the poor reversibility. Using van der Waals-corrected density functional theory, we demonstrated that lithium atoms can be homogeneously dispersed on T graphene due to a nonuniform charge distribution in T graphene and strong hybridizations between the C-2p and Li-2p orbitals. Thus, Li atoms are not likely to form clusters, indicating a good reversible hydrogen storage. Both the polarization mechanism and the orbital hybridizations contribute to the adsorption of hydrogen molecules (storage capacity of 7.7 wt. %) with an optimal adsorption energy of 0.19 eV/H 2 . The adsorption/desorption of H 2 at ambient temperature and pressure is also discussed. Our results can serve as a guide in the design of new hydrogen storage materials based on non-hexagonal graphenes.

  15. Hydrogen Storage in Metal-Organic Frameworks

    Energy Technology Data Exchange (ETDEWEB)

    Long, Jeffrey R. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

    2016-04-28

    The design and characterization of new materials for hydrogen storage is an important area of research, as the ability to store hydrogen at lower pressures and higher temperatures than currently feasible would lower operating costs for small hydrogen fuel cell vehicles. In particular, metal-organic frameworks (MOFs) represent promising materials for use in storing hydrogen in this capacity. MOFs are highly porous, three-dimensional crystalline solids that are formed via linkages between metal ions (e.g., iron, nickel, and zinc) and organic molecules. MOFs can store hydrogen via strong adsorptive interactions between the gas molecules and the pores of the framework, providing a high surface area for gas adsorption and thus the opportunity to store hydrogen at significantly lower pressures than with current technologies. By lowering the energy required for hydrogen storage, these materials hold promise in rendering hydrogen a more viable fuel for motor vehicles, which is a highly desirable outcome given the clean nature of hydrogen fuel cells (water is the only byproduct of combustion) and the current state of global climate change resulting from the combustion of fossil fuels. The work presented in this report is the result of collaborative efforts between researchers at Lawrence Berkeley National Lab (LBNL), the National Institute of Standards and Technology (NIST), and General Motors Corporation (GM) to discover novel MOFs promising for H2 storage and characterize their properties. Described herein are several new framework systems with improved gravimetric and volumetric capacity to strongly bind H2 at temperatures relevant for vehicle storage. These materials were rigorously characterized using neutron diffraction, to determine the precise binding locations of hydrogen within the frameworks, and high-pressure H2 adsorption measurements, to provide a comprehensive picture of H2 adsorption at all relevant pressures. A

  16. Square-wave adsorptive stripping voltammetric determination of nanomolar levels of bezafibrate using a glassy carbon electrode modified with multi-walled carbon nanotubes within a dihexadecyl hydrogen phosphate film.

    Science.gov (United States)

    Ardila, Jorge Armando; Oliveira, Geiser Gabriel; Medeiros, Roberta Antigo; Fatibello-Filho, Orlando

    2014-04-07

    A highly sensitive method for bezafibrate determination using a glassy carbon electrode (GCE) modified with multi-walled carbon nanotubes within a dihexadecyl hydrogen phosphate film based on square-wave adsorptive stripping voltammetry (SWAdSV) is proposed. The electrochemical behaviour of bezafibrate has been studied by cyclic voltammetry, showing an irreversible anodic peak at a potential of 1.09 V in 0.1 mol L(-1) phosphate buffer solution (pH 2.0). A study of the scan rate showed that the oxidation of bezafibrate is an adsorptive-controlled process, involving the transfer of two electrons and two protons per molecule. The analytical curve was linear over a bezafibrate concentration range from 50 to 910 nmol L(-1), with a detection limit of 16 nmol L(-1). This analytical method was successfully applied for benzafibrate determination in pharmaceutical formulations, with results showing good agreement with those obtained using a comparative spectrophotometric method, and has the potential for field application.

  17. Study of 63Ni adsorption on NKF-6 zeolite

    International Nuclear Information System (INIS)

    Zhang Hui; Yu Xianjin; Chen Lei; Jing Yongjie; Ge Zhiwei

    2010-01-01

    The adsorption of 63 Ni from aqueous solutions using NKF-6 zeolite was investigated by a batch technique under ambient conditions. The adsorption was investigated as a function of contact time, pH, ionic strength, foreign ions, humic substances (FA/HA) and temperature. The kinetic adsorption was well described by the pseudo-second-order rate equation. The adsorption of 63 Ni on NKF-6 zeolite was strongly dependent on pH and ionic strength, and the adsorption of 63 Ni increased with increasing NKF-6 zeolite content. At low pH values, the presence of FA enhanced the adsorption of 63 Ni on NKF-6 zeolite, but the presence of HA had no drastic effect. At high pH values, the presence of FA or HA decreased the adsorption of 63 Ni on NKF-6 zeolite. The adsorption isotherms were well represented by the Langmuir model. The thermodynamic parameters (i.e., ΔH 0 , ΔS 0 and ΔG 0 ) for the adsorption of 63 Ni were determined from the temperature dependent isotherms at 293.15, 313.15 and 333.15 o K, respectively, and the results indicate that the adsorption reaction was favored at high temperature. The results suggest that the adsorption process of 63 Ni on NKF-6 zeolite is spontaneous and endothermic. - Research highlights: → As an economical and efficient method, adsorption technique has been widely applied in the disposal of wastewaters. The study of 63 Ni on NKF-6 zeolite, especially the thermodynamic data of 63 Ni adsorption on NKF-6 zeolite and the effect of humic substances on 63 Ni uptake to humic-zeolite hybrids, is still scarce. In this paper, the sorption of 63 Ni on NKF-6 zeolite is studied as a function of various environmental conditions such as contact time, pH, ionic strength, foreign ions, humic substances and temperature. Based on the obtained experimental results, the adsorption mechanism of 63 Ni on NKF-6 zeolite is stated in detail. This study will have an important reference value in evaluating the physiochemical behavior of radionuclide 63 Ni.

  18. Kinetic and isotherm studies of bisphenol A adsorption onto orange albedo(Citrus sinensis): Sorption mechanisms based on the main albedo components vitamin C, flavones glycosides and carotenoids.

    Science.gov (United States)

    Kamgaing, Theophile; Doungmo, Giscard; Melataguia Tchieno, Francis Merlin; Gouoko Kouonang, Jimmy Julio; Mbadcam, Ketcha Joseph

    2017-07-03

    Orange albedo and its adsorption capacity towards bisphenol A (BPA) were studied. Adsorption experiments were conducted in batch mode at 25-55°C. Scanning electron microscopy (SEM), Energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) and Fourier transform infrared (FTIR) spectroscopy were used to characterise the biosorbent. The effects of various parameters including adsorption time, equilibrium pH, adsorbent dosage and initial adsorbate concentration were investigated. The optimum contact time and pH for the removal of BPA were 60 min and 2, respectively. It was found that the adsorption isotherms best matched the Freundlich model, the adsorption of BPA being multilayer and that of the albedo surface heterogeneous. From the kinetic studies, it was found that the removal of BPA best matched the pseudo-second order kinetic model. An adsorption mechanism based on the albedo surface molecules is proposed and gives a good account of π-π interactions and hydrogen bonding. Orange albedo, with a maximum BPA loading capacity of 82.36 mg g -1 (significantly higher than that of most agricultural residues), is a good candidate for BPA adsorption in aqueous media.

  19. Adsorption of dodecylamine hydrochloride on graphene oxide in water

    Directory of Open Access Journals (Sweden)

    Peng Chen

    Full Text Available Cationic surfactants in water are difficult to be degraded, leading to serious water pollution. In this work, graphene oxide (GO was used as an adsorbent for removing Dodecylamine Hydrochloride (DACl, a representative cationic surfactant. X-ray diffraction (XRD, FT-IR spectroscopy and atomic force microscope (AFM were used to characterize the prepared GO. The adsorption of DACl on GO have been investigated through measurements of adsorption capacity, zeta potential, FTIR, and X-ray photoelectron spectroscopy (XPS. The experimental results have shown that the adsorption kinetics could be described as a rate-limiting pseudo second-order process, and the adsorption isotherm agreed well with the Freundlich model. GO was a good adsorbent for DACl removal, compared with coal fly ash and powdered activated carbon. The adsorption process was endothermic, and could be attributed to electrostatic interaction and hydrogen bonding between DACl and GO. Keywords: Graphene oxide, Dodecylamine hydrochloride, Adsorption isotherm, Adsorption mechanisms

  20. MODELING STYRENE HYDROGENATION KINETICS USING PALLADIUM CATALYSTS

    Directory of Open Access Journals (Sweden)

    G. T. Justino

    Full Text Available Abstract The high octane number of pyrolysis gasoline (PYGAS explains its insertion in the gasoline pool. However, its use is troublesome due to the presence of gum-forming chemicals which, in turn, can be removed via hydrogenation. The use of Langmuir-Hinshelwood kinetic models was evaluated for hydrogenation of styrene, a typical gum monomer, using Pd/9%Nb2O5-Al2O3 as catalyst. Kinetic models accounting for hydrogen dissociative and non-dissociative adsorption were considered. The availability of one or two kinds of catalytic sites was analyzed. Experiments were carried out in a semi-batch reactor at constant temperature and pressure in the absence of transport limitations. The conditions used in each experiment varied between 16 - 56 bar and 60 - 100 ºC for pressure and temperature, respectively. The kinetic models were evaluated using MATLAB and EMSO software. Models using adsorption of hydrogen and organic molecules on the same type of site fitted the data best.

  1. Ab initio-based approach to reconstruction, adsorption and incorporation on GaN surfaces

    International Nuclear Information System (INIS)

    Ito, T; Akiyama, T; Nakamura, K

    2012-01-01

    Reconstruction, adsorption and incorporation on various GaN surfaces are systematically investigated using an ab initio-based approach that predicts the surface phase diagram as functions of temperature and beam-equivalent pressure (BEP). The calculated results for GaN surface reconstructions with polar (0 0 0 1), nonpolar (1 1 −2 0), semipolar (1 −1 0 1) and semipolar (1 1 −2 2) orientations imply that reconstructions on GaN surfaces with Ga adlayers generally appear on the polar and the semipolar surfaces, while the stable ideal surface without Ga adsorption is found on the nonpolar GaN(1 1 −2 0) surface because it satisfies the electron counting rule. The hydrogen adsorption on GaN(0 0 0 1) and GaN(1 1 −2 0) realizes several surface structures forming N–H and Ga–NH 2 bonds on their surfaces that depend on temperature and Ga BEP during metal-organic vapor-phase epitaxy (MOVPE). In contrast, the stable structures due to hydrogen adsorption on the semipolar GaN(1 −1 0 1) and GaN(1 1 −2 2) surfaces are not varied over the wide range of temperature and Ga BEP. This implies that the hydrogen adsorbed stable structures are expected to emerge on the semipolar surfaces during MOVPE regardless of the growth conditions. Furthermore, we clarify that Mg incorporation on GaN(1 −1 0 1) surfaces is enhanced by hydrogen adsorption consistent with experimental findings

  2. Micro study of the structural modifications induced by absorption of hydrogen in LaNi4.25Co0.75

    International Nuclear Information System (INIS)

    Latroche, M.; Joubert, J.-M.; Percheron-Guegan, A.

    2000-01-01

    Many intermetallic elements (rare earth gold transition metals) have significant properties that will affect the adsorption of hydrogen. Within the properties, particularly of those composed of AB n , hydrogenation is affected by temperature and environmental pressure. Moreover, the reaction can also be done in electrochemical medium. These remarkable properties made it possible to develop batteries of standard nickel hydride which today largely replace the Nickel Cadmium batteries. However, mechanisms brought into play at an atomic scale during the cycles of absorption-desorption are still badly known. We present here a study by X-ray diffraction of substitute compositions for LaNi 4.25 Co 0.75 cobalt subjected to the absorption effects of hydrogen. The evolutions of profile E lines of elements before and after cycling are studied and compared

  3. Photocatalytic hydrogen evolution from aqueous solutions of organophosphorous compounds

    Energy Technology Data Exchange (ETDEWEB)

    Kozlova, Ekaterina A.; Vorontsov, Alexander V. [Boreskov Institute of Catalysis and Novosibirsk State University, Novosibirsk 630090 (Russian Federation)

    2010-07-15

    Photocatalytic hydrogen production from water solutions of dimethyl methylphosphonate (DMMP), trimethyl phosphate (TMP), triethyl phosphate (TEP), and radiation protective amine WR 2721, that imitate nerve chemical warfare agents was studied for the first time. Platinized titianium dioxide Degussa P25 was used as catalyst. No significant hydrogen evolution was detected without organic electron donors - sacrificial agents. The hydrogen evolution rate was shown to grow slowly with the rise of initial DMMP concentration. The initial rate vs. DMMP concentration curve is well fitted by Langmuir-Hinshelwood (L-H) equation. The DMMP adsorption constant obtained from the L-H equation fit is markedly higher than that obtained from the Langmuir adsorption isotherm. Reactions of full destruction into inorganic products of the four organophosphorous compounds were conducted. Amounts of evolved hydrogen and carbon dioxide were completely consistent with stoichiometry of proposed reaction. There were no initial compounds and only trace of total organic carbon after the end of the reaction. Complete water purification and production of an amount of valuable hydrogen was achieved. Intermediates of DMMP oxygen-free destruction were identified by means of GC/MS. They were the same as those in the case of DMMP photocatalytic oxidation. A mechanism of hydrogen evolution that explains smaller rates of mineralization compared to photocatalytic oxidation by oxygen was proposed. (author)

  4. Surface atomic relaxation and magnetism on hydrogen-adsorbed Fe(110) surfaces from first principles

    Energy Technology Data Exchange (ETDEWEB)

    Chohan, Urslaan K.; Jimenez-Melero, Enrique [School of Materials, The University of Manchester, Manchester M13 9PL (United Kingdom); Dalton Cumbrian Facility, The University of Manchester, Moor Row CA24 3HA (United Kingdom); Koehler, Sven P.K., E-mail: sven.koehler@manchester.ac.uk [Dalton Cumbrian Facility, The University of Manchester, Moor Row CA24 3HA (United Kingdom); School of Chemistry, The University of Manchester, Manchester M13 9PL (United Kingdom); Photon Science Institute, The University of Manchester, Manchester M13 9PL (United Kingdom)

    2016-11-30

    Highlights: • Potential energy surfaces for H diffusion on Fe(110) calculated. • Full vibrational analysis of surface modes performed. • Vibrational analysis establishes lb site as a transition state to the 3f site. • Pronounced buckling observed in the Fe surface layer. - Abstract: We have computed adsorption energies, vibrational frequencies, surface relaxation and buckling for hydrogen adsorbed on a body-centred-cubic Fe(110) surface as a function of the degree of H coverage. This adsorption system is important in a variety of technological processes such as the hydrogen embrittlement in ferritic steels, which motivated this work, and the Haber–Bosch process. We employed spin-polarised density functional theory to optimise geometries of a six-layer Fe slab, followed by frozen mode finite displacement phonon calculations to compute Fe–H vibrational frequencies. We have found that the quasi-threefold (3f) site is the most stable adsorption site, with adsorption energies of ∼3.0 eV/H for all coverages studied. The long-bridge (lb) site, which is close in energy to the 3f site, is actually a transition state leading to the stable 3f site. The calculated harmonic vibrational frequencies collectively span from 730 to 1220 cm{sup −1}, for a range of coverages. The increased first-to-second layer spacing in the presence of adsorbed hydrogen, and the pronounced buckling observed in the Fe surface layer, may facilitate the diffusion of hydrogen atoms into the bulk, and therefore impact the early stages of hydrogen embrittlement in steels.

  5. Effect of Humid Aging on the Oxygen Adsorption in SnO₂ Gas Sensors.

    Science.gov (United States)

    Suematsu, Koichi; Ma, Nan; Watanabe, Ken; Yuasa, Masayoshi; Kida, Tetsuya; Shimanoe, Kengo

    2018-01-16

    To investigate the effect of aging at 580 °C in wet air (humid aging) on the oxygen adsorption on the surface of SnO₂ particles, the electric properties and the sensor response to hydrogen in dry and humid atmospheres for SnO₂ resistive-type gas sensors were evaluated. The electric resistance in dry and wet atmospheres at 350 °C was strongly increased by humid aging. From the results of oxygen partial pressure dependence of the electric resistance, the oxygen adsorption equilibrium constants ( K ₁; for O - adsorption, K ₂; for O 2- adsorption) were estimated on the basis of the theoretical model of oxygen adsorption. The K ₁ and K ₂ in dry and wet atmospheres at 350 °C were increased by humid aging at 580 °C, indicating an increase in the adsorption amount of both O - and O 2- . These results suggest that hydroxyl poisoning on the oxygen adsorption is suppressed by humid aging. The sensor response to hydrogen in dry and wet atmosphere at 350 °C was clearly improved by humid aging. Such an improvement of the sensor response seems to be caused by increasing the oxygen adsorption amount. Thus, the humid aging offers an effective way to improve the sensor response of SnO₂ resistive-type gas sensors in dry and wet atmospheres.

  6. Insight into the adsorption of chloramphenicol on a vermiculite surface

    Science.gov (United States)

    Tri, Nguyen Ngoc; Carvalho, A. J. P.; Dordio, A. V.; Nguyen, Minh Tho; Trung, Nguyen Tien

    2018-05-01

    Four stable configurations were found upon adsorption of the chloramphenicol on a period slab model of the vermiculite surface, using the PBE and C09-vdW functionals in a projector-augmented wave (PAW) method approach. The adsorption is a strong chemisorption process, characterized by an adsorption energy of -106.5 kcal mol-1 at the most stable configuration. Stability of configurations contributed mainly by Mg⋯O/Cl attractive electrostatic interactions and C/Osbnd H⋯O hydrogen bonds. It is remarkable that the vermiculite is found to be a solid material with good potential to be used for adsorption and consequent removal of this type of antibiotic drugs.

  7. A DFT study on benzene adsorption over tungsten sulfides: surface model and adsorption geometries

    NARCIS (Netherlands)

    Koide, R.; Hensen, E.J.M.; Paul, J.F.; Cristol, S.; Payen, E.; Nakamura, H.; Santen, van R.A.

    2007-01-01

    Benzene adsorption on a WS2(100) surface was studied by ab initio periodic DFT computations. Benzene adsorption is facile on the bridge site of the bare W edge via ¿2 or ¿3 coordination. Taking into account the stable configuration at the W edge under typical hydrotreating reaction conditions (623

  8. Initial heats of H{sub 2}S adsorption on activated carbons: Effect of surface features

    Energy Technology Data Exchange (ETDEWEB)

    Bagreev, A.; Adib, F.; Bandosz, T.J.

    1999-11-15

    The sorption of hydrogen sulfide was studied on activated carbons of various origins by means of inverse gas chromatography at infinite dilution. The conditions of the experiment were dry and anaerobic. Prior to the experiments the surface of some carbon samples was oxidized using either nitric acid or ammonium persulfate. Then the structural parameters of carbons were evaluated from the sorption of nitrogen. From the IGC experiments at various temperatures, heats of adsorption were calculated. The results showed that the heat of H{sub 2}S adsorption under dry anaerobic conditions does not depend on surface chemistry. The dependence of the heat of adsorption on the characteristic energy of nitrogen adsorption calculated from the Dubinin-Raduskevich equation was found. This correlation can be used to predict the heat of H{sub 2}S adsorption based on the results obtained from nitrogen adsorption.

  9. Hydrogenation of the alpha,beta-Unsaturated Aldehydes Acrolein, Crotonaldehyde, and Prenal over Pt Single Crystals: A Kinetic and Sum-Frequency Generation Vibrational Spectroscopy Study

    Energy Technology Data Exchange (ETDEWEB)

    Kliewer, C.J.; Somorjai, G.A.

    2008-11-26

    Sum-frequency generation vibrational spectroscopy (SFG-VS) and kinetic measurements using gas chromatography have been used to study the surface reaction intermediates during the hydrogenation of three {alpha},{beta}-unsaturated aldehydes, acrolein, crotonaldehyde, and prenal, over Pt(111) at Torr pressures (1 Torr aldehyde, 100 Torr hydrogen) in the temperature range of 295K to 415K. SFG-VS data showed that acrolein has mixed adsorption species of {eta}{sub 2}-di-{sigma}(CC)-trans, {eta}{sub 2}-di-{sigma}(CC)-cis as well as highly coordinated {eta}{sub 3} or {eta}{sub 4} species. Crotonaldehyde adsorbed to Pt(111) as {eta}{sub 2} surface intermediates. SFG-VS during prenal hydrogenation also suggested the presence of the {eta}{sub 2} adsorption species, and became more highly coordinated as the temperature was raised to 415K, in agreement with its enhanced C=O hydrogenation. The effect of catalyst surface structure was clarified by carrying out the hydrogenation of crotonaldehyde over both Pt(111) and Pt(100) single crystals while acquiring the SFG-VS spectra in situ. Both the kinetics and SFG-VS showed little structure sensitivity. Pt(100) generated more decarbonylation 'cracking' product while Pt(111) had a higher selectivity for the formation of the desired unsaturated alcohol, crotylalcohol.

  10. Carbon nanotubes for energy storage using their hydrogen adsorption capacity: state of the art and perspectives; Nanotubos de carbono para estocagem de energia por adsorcao de hidrogenio: estado da arte e perspectivas

    Energy Technology Data Exchange (ETDEWEB)

    Maestro, Luis Fernando; Luengo, Carlos Alberto [Universidade Estadual de Campinas (UNICAMP), SP (Brazil). Inst. de Fisica. Grupo de Combustiveis Alternativos], e-mail: lmaestro@ifi.unicamp.br

    2004-07-01

    It is presented an updated scope of the research in carbon nanotubes synthesis, their purification and a discussion of recent results in energy storage using their hydrogen adsorption capacity. The GCA activities in this area are also discussed. (author)

  11. Ti-decorated graphitic-C{sub 3}N{sub 4} monolayer: A promising material for hydrogen storage

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Weibin [Department of Physics, Dongguk University, Seoul 04620 (Korea, Republic of); Zhang, Zhijun [Department of Physics, Dongguk University, Seoul 04620 (Korea, Republic of); School of Materials Science and Engineering, Shanghai University, Shanghai 200072 (China); Zhang, Fuchun [College of Physics and Electronic Information, Yan’an University, Yan’an 716000 (China); Yang, Woochul, E-mail: wyang@dongguk.edu [Department of Physics, Dongguk University, Seoul 04620 (Korea, Republic of)

    2016-11-15

    Highlights: • Ti atoms are stably decorated at the triangular N hole in g-C{sub 3}N{sub 4} with an adsorption energy of −7.58 eV. • Electron redistribution of Ti-adsorbed porous g-C{sub 3}N{sub 4} significantly enhanced hydrogen adsorption up to five H{sub 2} molecules at each Ti atom. • The hydrogen capacity of the Ti-decorated g-C{sub 3}N{sub 4} system reaches up to 9.70 wt%. • All H{sub 2} absorbed in the Ti/g-C{sub 3}N{sub 4} system can be released at 393 K according to the molecular dynamic analysis. • Ti/g-C{sub 3}N{sub 4} as a hydrogen storage system is suitable and reversible at the temperature range required for practical applications. - Abstract: Ti-decorated graphitic carbon nitride (g-C{sub 3}N{sub 4}) monolayer as a promising material system for high-capacity hydrogen storage is proposed through density functional theory calculations. The stability and hydrogen adsorption of Ti-decorated g-C{sub 3}N{sub 4} is analyzed by computing the adsorption energy, the charge population, and electronic density of states. The most stable decoration site of Ti atom is the triangular N hole in g-C{sub 3}N{sub 4} with an adsorption energy of −7.58 eV. The large diffusion energy barrier of the adsorbed Ti atom of ∼6.00 eV prohibits the cluster formation of Ti atoms. The electric field induced by electron redistribution of Ti-adsorbed porous g-C{sub 3}N{sub 4} significantly enhanced hydrogen adsorption up to five H{sub 2} molecules at each Ti atom with an average adsorption energy of −0.30 eV/H{sub 2}. The corresponding hydrogen capacity reaches up to 9.70 wt% at 0 K. In addition, the hydrogen capacity is predicted to be 6.30 wt% at 233 K and all adsorbed H{sub 2} are released at 393 K according to molecular dynamics simulation. Thus, the Ti-decorated g-C{sub 3}N{sub 4} monolayer is suggested to be a promising material for hydrogen storage suggested by the DOE for commercial applications.

  12. In silico approach to investigating the adsorption mechanisms of short chain perfluorinated sulfonic acids and perfluorooctane sulfonic acid on hydrated hematite surface.

    Science.gov (United States)

    Feng, Hongru; Lin, Yuan; Sun, Yuzhen; Cao, Huiming; Fu, Jianjie; Gao, Ke; Zhang, Aiqian

    2017-05-01

    Short chain perfluorinated sulfonic acids (PFSAs) that were introduced as alternatives for perfluorooctane sulfonic acid (PFOS) have been widely produced and used. However, few studies have investigated the environmental process of short chain PFSAs, and the related adsorption mechanisms still need to be uncovered. The water-oxide interface is one of the major environmental interfaces that plays an important role in affecting the adsorption behaviour and transport potential of the environmental pollutant. In this study, we performed molecular dynamics simulations and quantum chemistry calculations to investigate the adsorption mechanisms of five PFSAs and their adsorption on hydrated hematite surface as well. Different to the vertical configuration reported for PFOS on titanium oxide, all PFSAs share the same adsorption configuration as the long carbon chains parallel to the surface. The formation of hydrogen bonds between F and inter-surface H helps to stabilize the unique configuration. As a result, the sorption capacity increases with increasing C-F chain length. Moreover, both calculated adsorption energy and partial density of states (PDOS) analysis demonstrate a PFSAs adsorption mechanism in between physical and chemical adsorption because the hydrogen bonds formed by the overlap of F (p) orbital and H (s) orbital are weak intermolecular interactions while the physical adsorption are mainly ascribed to the electrostatic interactions. This massive calculation provides a new insight into the pollutant adsorption behaviour, and in particular, may help to evaluate the environmental influence of pollutants. Copyright © 2017. Published by Elsevier Ltd.

  13. Lithium doping on covalent organic framework-320 for enhancing hydrogen storage at ambient temperature

    Energy Technology Data Exchange (ETDEWEB)

    Xia, Liangzhi, E-mail: 15004110853@163.com; Liu, Qing

    2016-12-15

    Density Functional Theory (DFT) combines with grand canonical Monte Carlo (GCMC) simulations are performed to explore the effect of Li doping on the hydrogen storage capability of COF-320. The results show that the interaction energy between the H{sub 2} and the Li-doped COF-320 is about three times higher than that of pristine COF-320. GCMC simulations are employed to study the hydrogen uptake of Li-doped COF-320 at ambient temperature, further confirm that the lithium doping can improve the hydrogen uptake at ambient temperature. Our results demonstrate that Li-doped COFs have good potential in the field of hydrogen storage. - Graphical abstract: Fig. 1. The optimized cluster model used here to represent the COF-320 and possible adsorption sites (A, B, C) for adsorption of metals in the COF-320. The dangling bonds are terminated by H atoms. C, H, and N atoms are shown as gray, white, and blue colors, respectively. Fig. 2. The adsorption isotherm of H{sub 2} in the pristine and Li-doped COF-320 at 298 K. - Highlights: • The binding sites of single and two lithium atoms in COF-320 were studied. • The interaction energy between the H{sub 2} and the Li-doped COF-320 is about three times higher than that of pristine COF-320. • H{sub 2} uptakes on the Li-doped COFs obtain significant improvement at ambient temperature. • Lithium-doping is a successful strategy for improving hydrogen uptake.

  14. Lithium doping on covalent organic framework-320 for enhancing hydrogen storage at ambient temperature

    International Nuclear Information System (INIS)

    Xia, Liangzhi; Liu, Qing

    2016-01-01

    Density Functional Theory (DFT) combines with grand canonical Monte Carlo (GCMC) simulations are performed to explore the effect of Li doping on the hydrogen storage capability of COF-320. The results show that the interaction energy between the H 2 and the Li-doped COF-320 is about three times higher than that of pristine COF-320. GCMC simulations are employed to study the hydrogen uptake of Li-doped COF-320 at ambient temperature, further confirm that the lithium doping can improve the hydrogen uptake at ambient temperature. Our results demonstrate that Li-doped COFs have good potential in the field of hydrogen storage. - Graphical abstract: Fig. 1. The optimized cluster model used here to represent the COF-320 and possible adsorption sites (A, B, C) for adsorption of metals in the COF-320. The dangling bonds are terminated by H atoms. C, H, and N atoms are shown as gray, white, and blue colors, respectively. Fig. 2. The adsorption isotherm of H 2 in the pristine and Li-doped COF-320 at 298 K. - Highlights: • The binding sites of single and two lithium atoms in COF-320 were studied. • The interaction energy between the H 2 and the Li-doped COF-320 is about three times higher than that of pristine COF-320. • H 2 uptakes on the Li-doped COFs obtain significant improvement at ambient temperature. • Lithium-doping is a successful strategy for improving hydrogen uptake.

  15. Characterization of the adsorption of water vapor and chlorine on microcrystalline silica

    Science.gov (United States)

    Skiles, J. A.; Wightman, J. P.

    1979-01-01

    The characterization of water adsorption on silica is necessary to an understanding of how hydrogen chloride interacts with silica. The adsorption as a function of outgas temperatures of silica and as a function of the isotherm temperature was studied. Characterization of the silica structure by infrared analysis, X-ray diffraction and differential scanning calorimetry, surface area determinations, characterization of the sample surface by electron spectroscopy for chemical analysis (ESCA), and determinations of the heat of immersion in water of silica were investigated. The silica with a scanning electron microscope was examined.

  16. Adsorption of volatile polonium species on metals in various gas atmospheres. Pt. II. Adsorption of volatile polonium on platinum, silver and palladium

    Energy Technology Data Exchange (ETDEWEB)

    Maugeri, Emilio Andrea; Joerg Neuhausen; Dressler, Rugard; Piguet, David; Voegele, Alexander; Schumann, Dorothea [Paul Scherrer Institut (PSI), Villigen (Switzerland). Lab. for Radiochemistry; Misiak, Ryszard [The Henryk Niewodniczanski Institute of Nuclear Physics, Krakow (Poland); Eichler, Robert [Paul Scherrer Institut (PSI), Villigen (Switzerland). Lab. for Radiochemistry; Bern Univ. (Switzerland). Dept. for Chemistry and Biochemistry

    2016-07-01

    This work presents the results obtained from studying the interaction between polonium compounds formed in different atmospheres and platinum, palladium and silver surfaces obtained by thermochromatography. These results are of crucial importance for the design of cover gas filter systems for lead-bismuth eutectic (LBE)-based nuclear facilities such as accelerator driven systems (ADS). The results obtained from studying the interaction of polonium and platinum under inert atmosphere and reducing atmospheres with and without addition of moisture show that polonium is deposited at temperatures between 993 and 1221 K, with adsorption enthalpies ranging from -235 to -291 kJ mol{sup -1}, indicating a very strong adsorption of the polonium species present on platinum surfaces. The interaction between polonium and silver was investigated using purified inert, reducing and oxidizing carrier gases. Results show a deposition temperature between 867 and 990 K, with adsorption enthalpies ranging from -205 to -234 kJ mol{sup -1}. The interaction of polonium and palladium was studied in purified helium and purified hydrogen. For both conditions a deposition temperature of 1221 K was observed corresponding to an adsorption enthalpy of -340 kJ mol{sup -1}. No highly volatile polonium species was formed at any of the applied experimental conditions.

  17. Metal-loaded SBA-16-like silica – Correlation between basicity and affinity towards hydrogen

    International Nuclear Information System (INIS)

    Ouargli-Saker, R.; Bouazizi, N.; Boukoussa, B.; Barrimo, Diana; Paola-Nunes-Beltrao, Ana; Azzouz, A.

    2017-01-01

    Highlights: • Metal dispersion in longitudinal channels confers adsorption properties to SBA-16. • Both Fe"0-NPs and Cu"0-NPs seem to be responsible of this effect. • Effect of the repetitive adsorption-desorption cycles on CO_2 and water sorption. • Hydrogen storage on the functionalized materials. - Abstract: Nanoparticles of Cu"o (CuNPs) and Fe"o (FeNPs) were dispersed in SBA-16-like silica, resulting metal-loaded materials (Cu-SBA-16 and Fe-SBA-16) with improved affinity towards hydrogen. Electron microscopy and X-ray diffraction showed that MNP dispersion occurs mainly inside SBA-16 channels. MNP incorporation was found to confer affinity to the silica surface, since higher CO_2 retention capacity (CRC) was registered Cu/SBA-16 and Fe/SBA-16. This was accompanied by a significant improvement of the affinity towards hydrogen, as supported by hydrogen adsorption tests. This was explained in terms of strong hydrogen interaction with MNP and lattice oxygen atoms. The results reported herein open new prospects for SBA-16 as potential adsorbents for hydrogen storage.

  18. Metal-loaded SBA-16-like silica – Correlation between basicity and affinity towards hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Ouargli-Saker, R. [Department of Materials Engineering, University of Science and Technology, El M’naouer, BP 1505, Oran (Algeria); Nanoqam, Department of Chemistry, University of Quebec at Montreal, H3C3P8 (Canada); Bouazizi, N. [Nanoqam, Department of Chemistry, University of Quebec at Montreal, H3C3P8 (Canada); Unité de recherche, Electrochimie, Matériaux et Environnement, Faculté des Sciences de Gabès, Université de Gabès, Cité Erriadh, 6072 Gabès (Tunisia); Boukoussa, B. [Department of Materials Engineering, University of Science and Technology, El M’naouer, BP 1505, Oran (Algeria); Lqamb, Laboratório de Química Analítica Ambiental, Faculdade de Química, Pontifícia Universidade Católica do Rio Grande do Sul (Brazil); Barrimo, Diana [Nanoqam, Department of Chemistry, University of Quebec at Montreal, H3C3P8 (Canada); Paola-Nunes-Beltrao, Ana [Nanoqam, Department of Chemistry, University of Quebec at Montreal, H3C3P8 (Canada); Laboratory of Materials Chemistry L.C.M, University of Oran1 Ahmed Ben Bella, BP 1524, El-Mnaouer, 31000 Oran (Algeria); Azzouz, A., E-mail: azzouz.a@uqam.ca [Nanoqam, Department of Chemistry, University of Quebec at Montreal, H3C3P8 (Canada)

    2017-07-31

    Highlights: • Metal dispersion in longitudinal channels confers adsorption properties to SBA-16. • Both Fe{sup 0}-NPs and Cu{sup 0}-NPs seem to be responsible of this effect. • Effect of the repetitive adsorption-desorption cycles on CO{sub 2} and water sorption. • Hydrogen storage on the functionalized materials. - Abstract: Nanoparticles of Cu{sup o} (CuNPs) and Fe{sup o} (FeNPs) were dispersed in SBA-16-like silica, resulting metal-loaded materials (Cu-SBA-16 and Fe-SBA-16) with improved affinity towards hydrogen. Electron microscopy and X-ray diffraction showed that MNP dispersion occurs mainly inside SBA-16 channels. MNP incorporation was found to confer affinity to the silica surface, since higher CO{sub 2} retention capacity (CRC) was registered Cu/SBA-16 and Fe/SBA-16. This was accompanied by a significant improvement of the affinity towards hydrogen, as supported by hydrogen adsorption tests. This was explained in terms of strong hydrogen interaction with MNP and lattice oxygen atoms. The results reported herein open new prospects for SBA-16 as potential adsorbents for hydrogen storage.

  19. Hydrogen Separation by Natural Zeolite Composite Membranes: Single and Multicomponent Gas Transport

    Directory of Open Access Journals (Sweden)

    Afrooz Farjoo

    2017-10-01

    Full Text Available Single and multicomponent gas permeation tests were used to evaluate the performance of metal-supported clinoptilolite membranes. The efficiency of hydrogen separation from lower hydrocarbons (methane, ethane, and ethylene was studied within the temperature and pressure ranges of 25–600 °C and 110–160 kPa, respectively. The hydrogen separation factor was found to reduce noticeably in the gas mixture compared with single gas experiments at 25 °C. The difference between the single and multicomponent gas results decreased as the temperature increased to higher than 300 °C, which is when the competitive adsorption–diffusion mechanism was replaced by Knudsen diffusion or activated diffusion mechanisms. To evaluate the effect of gas adsorption, the zeolite surface isotherms of each gas in the mixture were obtained from 25 °C to 600 °C. The results indicated negligible adsorption of individual gases at temperatures higher than 300 °C. Increasing the feed pressure resulted in a higher separation efficiency for the individual gases compared with the multicomponent mixture, due to the governing effect of the adsorptive mechanism. This study provides valuable insight into the application of natural zeolites for the separation of hydrogen from a mixture of hydrocarbons.

  20. Adsorption characteristics of Bisphenol-A on tailored activated carbon in aqueous solutions.

    Science.gov (United States)

    Yan, Liang; Lv, Di; Huang, Xinwen; Shi, Huixiang; Zhang, Geshan

    2016-10-01

    The adsorption behavior of pharmaceuticals and personal care product, Bisphenol-A (BPA), according to four coal-based and four wood-based granular activated carbons modified using outgassing treatment, acidic treatment or alkaline treatment was studied. The adsorption isotherm results indicated that carbon surface acidity played a very important role in the adsorption of BPA. It was found that increasing surface acidity would increase the hydrogen bonding effects and increase adsorption of BPA on activated carbon. The acidic modified sample (F600-A and OLC-A) represented the best adsorption capacity, and the equilibrium adsorption amounts reached 346.42 and 338.55 mg/g, respectively. Further, effects of surface charge and surface basicity were examined. It was found that the adsorbed amount of BPA decreased with the increase of surface charge. Finally, there appeared to be a significant oligomerization phenomenon with BPA molecules onto the surface of activated carbon. OLC and OLC-OG, which have higher micropore percentages, are very effective in hampering the oligomerization of BPA under oxic conditions.

  1. Hydrogen storage in carbon nano-materials. Elaboration, characterization and properties

    International Nuclear Information System (INIS)

    Luxembourg, D.

    2004-10-01

    This work deals with hydrogen storage for supplying fuel cells. Hydrogen storage by adsorption in carbon nano-tubes and nano-fibers is a very controversial issue because experimental results are very dispersed and adsorption mechanisms are not yet elucidated. Physi-sorption cannot explain in fact all the experimental results. All the potential adsorption sites, physical and chemical, are discussed as detailed as possible in a state of the art. Experimental works includes the steps of elaboration, characterization, and measurements of the hydrogen storage properties. Nano-fibers are grown using a CVD approach. Single wall carbon nano-tubes (SWNT) synthesis is based on the vaporization/condensation of a carbon/catalysts mixture in a reactor using a fraction of the available concentrated solar energy at the focus of the 1000 kW solar facility of IMP-CNRS at Odeillo. Several samples are produced using different synthesis catalysts (Ni, Co, Y, Ce). SWNT samples are purified using oxidative and acid treatments. Hydrogen storage properties of these materials are carefully investigated using a volumetric technique. The applied pressure is up to 6 MPa and the temperature is 253 K. Hydrogen uptake of the investigated materials are less than 1 % wt. at 253 K and 6 MPa. (author)

  2. Adsorption of dodecylamine hydrochloride on graphene oxide in water

    Science.gov (United States)

    Chen, Peng; Li, Hongqiang; Song, Shaoxian; Weng, Xiaoqing; He, Dongsheng; Zhao, Yunliang

    Cationic surfactants in water are difficult to be degraded, leading to serious water pollution. In this work, graphene oxide (GO) was used as an adsorbent for removing Dodecylamine Hydrochloride (DACl), a representative cationic surfactant. X-ray diffraction (XRD), FT-IR spectroscopy and atomic force microscope (AFM) were used to characterize the prepared GO. The adsorption of DACl on GO have been investigated through measurements of adsorption capacity, zeta potential, FTIR, and X-ray photoelectron spectroscopy (XPS). The experimental results have shown that the adsorption kinetics could be described as a rate-limiting pseudo second-order process, and the adsorption isotherm agreed well with the Freundlich model. GO was a good adsorbent for DACl removal, compared with coal fly ash and powdered activated carbon. The adsorption process was endothermic, and could be attributed to electrostatic interaction and hydrogen bonding between DACl and GO.

  3. A Density Functional Theory Study of the Adsorption of Benzene on Hematite (α-Fe2O3 Surfaces

    Directory of Open Access Journals (Sweden)

    Nelson Y. Dzade

    2014-02-01

    Full Text Available The reactivity of mineral surfaces in the fundamental processes of adsorption, dissolution or growth, and electron transfer is directly tied to their atomic structure. However, unraveling the relationship between the atomic surface structure and other physical and chemical properties of complex metal oxides is challenging due to the mixed ionic and covalent bonding that can occur in these minerals. Nonetheless, with the rapid increase in computer processing speed and memory, computer simulations using different theoretical techniques can now probe the nature of matter at both the atomic and sub-atomic levels and are rapidly becoming an effective and quantitatively accurate method for successfully predicting structures, properties and processes occurring at mineral surfaces. In this study, we have used Density Functional Theory calculations to study the adsorption of benzene on hematite (α-Fe2O3 surfaces. The strong electron correlation effects of the Fe 3d-electrons in α-Fe2O3 were described by a Hubbard-type on-site Coulomb repulsion (the DFT+U approach, which was found to provide an accurate description of the electronic and magnetic properties of hematite. For the adsorption of benzene on the hematite surfaces, we show that the adsorption geometries parallel to the surface are energetically more stable than the vertical ones. The benzene molecule interacts with the hematite surfaces through π-bonding in the parallel adsorption geometries and through weak hydrogen bonds in the vertical geometries. Van der Waals interactions are found to play a significant role in stabilizing the absorbed benzene molecule. Analyses of the electronic structures reveal that upon benzene adsorption, the conduction band edge of the surface atoms is shifted towards the valence bands, thereby considerably reducing the band gap and the magnetic moments of the surface Fe atoms.

  4. Adsorption removal of tannic acid from aqueous solution by polyaniline: Analysis of operating parameters and mechanism.

    Science.gov (United States)

    Sun, Chencheng; Xiong, Bowen; Pan, Yang; Cui, Hao

    2017-02-01

    Polyaniline (PANI) prepared by chemical oxidation was studied for adsorption removal of tannic acid (TA) from aqueous solution. Batch adsorption studies were carried out under different adsorbent dosages, pH, ionic strength, initial TA concentration and coexisting anions. Solution pH had an important impact on TA adsorption onto PANI with optimal removal in the pH range of 8-11. TA adsorption on PANI at three ionic strength levels (0.02, 0.2 and 2molL -1 NaCl) could be well described by Langmuir model (monolayer adsorption process) and the maximum adsorption capacity was 230, 223 and 1023mgg -1 , respectively. Kinetic data showed that TA adsorption on PANI fitted well with pseudo-second-order model (controlled by chemical process). Among the coexisting anions tested, PO 4 3- significantly inhibited TA adsorption due to the enhancement of repulsive interaction. Continuous flow adsorption studies indicated good flexibility and adaptability of the PANI adsorbent under different flow rates and influent TA concentrations. The mechanism controlling TA adsorption onto PANI under different operating conditions was analyzed with the combination of electrostatic interactions, hydrogen bonding, π-π interactions and Van der Waals interactions. Copyright © 2016 Elsevier Inc. All rights reserved.

  5. Development of sustainable dye adsorption system using nutraceutical industrial fennel seed spent-studies using Congo red dye.

    Science.gov (United States)

    Taqui, Syed Noeman; Yahya, Rosiyah; Hassan, Aziz; Nayak, Nayan; Syed, Akheel Ahmed

    2017-07-03

    Fennel seed spent (FSS)-an inexpensive nutraceutical industrial spent has been used as an efficient biosorbent for the removal of Congo red (CR) from aqueous media. Results show that the conditions for maximum adsorption would be pH 2-4 and 30°C were ideal for maximum adsorption. Based on regression fitting of the data, it was determined that the Sips isotherm (R 2 = 0.994, χ 2 = 0.5) adequately described the mechanism of adsorption, suggesting that the adsorption occurs homogeneously with favorable interaction between layers with favorable interaction between layers. Thermodynamic analysis showed that the adsorption is favorable (negative values for ΔG°) and endothermic (ΔH° = 12-20 kJ mol -1 ) for initial dye concentrations of 25, 50, and 100 ppm. The low ΔH° value indicates that the adsorption is a physical process involving weak chemical interactions like hydrogen bonds and van der Waals interactions. The kinetics revealed that the adsorption process showed pseudo-second-order tendencies with the equal influence of intraparticle as well as film diffusion. The scanning electron microscopy images of FSS show a highly fibrous matrix with a hierarchical porous structure. The Fourier transform infrared spectroscopy analysis of the spent confirmed the presence of cellulosic and lignocellulosic matter, giving it both hydrophilic and hydrophobic properties. The investigations indicate that FSS is a cost-effective and efficient biosorbent for the remediation of toxic CR dye.

  6. Effect of Humid Aging on the Oxygen Adsorption in SnO2 Gas Sensors

    Directory of Open Access Journals (Sweden)

    Koichi Suematsu

    2018-01-01

    Full Text Available To investigate the effect of aging at 580 °C in wet air (humid aging on the oxygen adsorption on the surface of SnO2 particles, the electric properties and the sensor response to hydrogen in dry and humid atmospheres for SnO2 resistive-type gas sensors were evaluated. The electric resistance in dry and wet atmospheres at 350 °C was strongly increased by humid aging. From the results of oxygen partial pressure dependence of the electric resistance, the oxygen adsorption equilibrium constants (K1; for O− adsorption, K2; for O2− adsorption were estimated on the basis of the theoretical model of oxygen adsorption. The K1 and K2 in dry and wet atmospheres at 350 °C were increased by humid aging at 580 °C, indicating an increase in the adsorption amount of both O− and O2−. These results suggest that hydroxyl poisoning on the oxygen adsorption is suppressed by humid aging. The sensor response to hydrogen in dry and wet atmosphere at 350 °C was clearly improved by humid aging. Such an improvement of the sensor response seems to be caused by increasing the oxygen adsorption amount. Thus, the humid aging offers an effective way to improve the sensor response of SnO2 resistive-type gas sensors in dry and wet atmospheres.

  7. Production of ultrapure D-T gas by removal of molecular tritium by selective adsorption

    International Nuclear Information System (INIS)

    Maienschein, J.L.; Hudson, R.S.; Tsugawa, R.T.; Fearon, E.M.; Souers, P.C.; Collins, G.W.

    1991-07-01

    The application of selective adsorption to purification of D-T gas by removal of T 2 has been demonstrated for small quantities of gas typical in research applications. This represents a variation on the production of pure spin isomers of deuterium and hydrogen. The use of an adsorption column offers several advantages over conventional separation techniques, such as low tritium inventory, rapid delivery to prevent radiation damage of the accumulated product, compact size, simplicity of design, construction, and operation, and operation without carrier gas. Because a column can have several thousand equilibrium stages, the purity of the product can be very high. The adsorption column has been shown to be an attractive separation tool for small quantities of hydrogen isotopes

  8. Studies of Modified Hydrogen Storage Intermetallic Compounds Used as Fuel Cell Anodes

    Directory of Open Access Journals (Sweden)

    Rui F. M. Lobo

    2011-12-01

    Full Text Available The possibility of substituting Pt/C with the hydrogen storage alloy MlNi3.6Co0.85Al0.3Mn0.3 as the anode active material of a proton exchange membrane fuel cell system has been analyzed. The electrochemical properties indicate that a much more electrochemically active anode is obtained by impregnating the active material loaded anode in a Nafion proton conducting polymer. Such performance improvement might result from the increase of three-phase boundary sites or length in the gas diffusion electrode where the electrochemical reaction occurs. The experimental data revealed that the membrane electrode assembly (MEA shows better results when the anode active material, MlNi3.6Co0.85Al0.3Mn0.3, is treated with a hot alkaline KBH4 solution, and then chemically coated with 3 wt.% Pd. The MEA with the aforesaid modification presents an enhanced surface capability for hydrogen adsorption, and has been studied by molecular beam-thermal desorption spectrometry.

  9. Development of an installation for the production of high-purity hydrogen using the pressure-swing-adsorption process with coke-oven gas as feedstock

    Energy Technology Data Exchange (ETDEWEB)

    Nakamura, M; Sugishita, M

    1986-04-01

    This paper describes how Nippon Steel developed a process for producing high-purity hydrogen using the PSA method with coke-oven gas as a feedstock. The process comprises a gas-compression and gas-cooling stage, a pre-treatment stage, an adsorption stage, a de-oxygenation stage and various control and maintenance devices, etc. The triple-tower plant constructed is the equivalent of a four-tower conventional installation, with a maximum capacity of around 10,000 Nm/sup 3//h. 1 tab., 14 figs., 3 refs.

  10. Hydrogen storage in hybrid of layered double hydroxides/reduced graphene oxide using spillover mechanism

    International Nuclear Information System (INIS)

    Ensafi, Ali A.; Jafari-Asl, Mehdi; Nabiyan, Afshin; Rezaei, Behzad; Dinari, Mohammad

    2016-01-01

    New efficient hydrogen storage hybrids were fabricated based on hydrogen spillover mechanism, including chemisorptions and dissociation of H_2 on the surface of LDH (layered double hydroxides) and diffusion of H to rGO (reduced graphene oxide). The structures and compositions of all of the hybrids (LDHs/rGO) have been verified using different methods including transmission electron microscopy, X ray diffraction spectroscopy, infrared spectroscopy and Brunauer–Emmett–Teller analysis. Then, the abilities of the LDHs/rGOs, as hydrogen spillover, were investigated by electrochemical methods. In addition, the LDHs/rGOs were decorated with palladium, using redox replacement process, and their hydrogen spillover properties were studied. The results showed that the hydrogen adsorption/desorption kinetics, hydrogen storage capacities and stabilities of Pd"#LDH/rGOs are better than Pd/rGO. Finally presence of different polymers (synthesis with monomers, 4–aminophenol, 4–aminothiophenol, o-phenylenediamine and p-phenylenediamine) at the surface of the Pd#LDH/rGOs on hydrogen storage were studied. The results showed that presence of o-phenylenediamine and p-phenylenediamine improves the kinetics of the hydrogen adsorption/desorption and increase the capacity of the hydrogen storage. - Highlights: • Efficient hydrogen storage sorbents are introduced. • The sorbents are synthesized based on hybrids of layered double hydroxide. • The compositions of all of the hybrids are verified using different methods. • Pd nanoparticles modified nanohybrids are investigated for hydrogen storage. • Presence of different polymers beside the hydrogen sorbents are investigated.

  11. Gas-phase formaldehyde adsorption isotherm studies on activated carbon: correlations of adsorption capacity to surface functional group density.

    Science.gov (United States)

    Carter, Ellison M; Katz, Lynn E; Speitel, Gerald E; Ramirez, David

    2011-08-01

    Formaldehyde (HCHO) adsorption isotherms were developed for the first time on three activated carbons representing one activated carbon fiber (ACF) cloth, one all-purpose granular activated carbon (GAC), and one GAC commercially promoted for gas-phase HCHO removal. The three activated carbons were evaluated for HCHO removal in the low-ppm(v) range and for water vapor adsorption from relative pressures of 0.1-0.9 at 26 °C where, according to the IUPAC isotherm classification system, the adsorption isotherms observed exhibited Type V behavior. A Type V adsorption isotherm model recently proposed by Qi and LeVan (Q-L) was selected to model the observed adsorption behavior because it reduces to a finite, nonzero limit at low partial pressures and it describes the entire range of adsorption considered in this study. The Q-L model was applied to a polar organic adsorbate to fit HCHO adsorption isotherms for the three activated carbons. The physical and chemical characteristics of the activated carbon surfaces were characterized using nitrogen adsorption isotherms, X-ray photoelectron spectroscopy (XPS), and Boehm titrations. At low concentrations, HCHO adsorption capacity was most strongly related to the density of basic surface functional groups (SFGs), while water vapor adsorption was most strongly influenced by the density of acidic SFGs.

  12. CoFe2O4@MIL-100(Fe) hybrid magnetic nanoparticles exhibit fast and selective adsorption of arsenic with high adsorption capacity

    Science.gov (United States)

    Yang, Ji-Chun; Yin, Xue-Bo

    2017-01-01

    In this study, we report the synthesis and application of mesoporous CoFe2O4@MIL-100(Fe) hybrid magnetic nanoparticles (MNPs) for the simultaneous removal of inorganic arsenic (iAs). The hybrid adsorbent had a core-shell and mesoporous structure with an average diameter of 260 nm. The nanoscale size and mesoporous character impart a fast adsorption rate and high adsorption capacity for iAs. In total, 0.1 mg L−1 As(V) and As(III) could be adsorbed within 2 min, and the maximum adsorption capacities were 114.8 mg g−1 for As(V) and 143.6 mg g−1 for As(III), higher than most previously reported adsorbents. The anti-interference capacity for iAs adsorption was improved by the electrostatic repulsion and size exclusion effects of the MIL-100(Fe) shell, which also decreased the zero-charge point of the hybrid absorbent for a broad pH adsorption range. The adsorption mechanisms of iAs on the MNPs are proposed. An Fe-O-As structure was formed on CoFe2O4@MIL-100(Fe) through hydroxyl substitution with the deprotonated iAs species. Monolayer adsorption of As(V) was observed, while hydrogen bonding led to the multi-layer adsorption of neutral As(III) for its high adsorption capacity. The high efficiency and the excellent pH- and interference-tolerance capacities of CoFe2O4@MIL-100(Fe) allowed effective iAs removal from natural water samples, as validated with batch magnetic separation mode and a portable filtration strategy. PMID:28102334

  13. Calcium-decorated carbyne networks as hydrogen storage media.

    Science.gov (United States)

    Sorokin, Pavel B; Lee, Hoonkyung; Antipina, Lyubov Yu; Singh, Abhishek K; Yakobson, Boris I

    2011-07-13

    Among the carbon allotropes, carbyne chains appear outstandingly accessible for sorption and very light. Hydrogen adsorption on calcium-decorated carbyne chain was studied using ab initio density functional calculations. The estimation of surface area of carbyne gives the value four times larger than that of graphene, which makes carbyne attractive as a storage scaffold medium. Furthermore, calculations show that a Ca-decorated carbyne can adsorb up to 6 H(2) molecules per Ca atom with a binding energy of ∼0.2 eV, desirable for reversible storage, and the hydrogen storage capacity can exceed ∼8 wt %. Unlike recently reported transition metal-decorated carbon nanostructures, which suffer from the metal clustering diminishing the storage capacity, the clustering of Ca atoms on carbyne is energetically unfavorable. Thermodynamics of adsorption of H(2) molecules on the Ca atom was also investigated using equilibrium grand partition function.

  14. Surface charge effects in protein adsorption on nanodiamonds

    Science.gov (United States)

    Aramesh, M.; Shimoni, O.; Ostrikov, K.; Prawer, S.; Cervenka, J.

    2015-03-01

    Understanding the interaction of proteins with charged diamond nanoparticles is of fundamental importance for diverse biomedical applications. Here we present a thorough study of protein binding, adsorption kinetics and structure on strongly positively (hydrogen-terminated) and negatively (oxygen-terminated) charged nanodiamond particles using a quartz crystal microbalance by dissipation and infrared spectroscopy. By using two model proteins (bovine serum albumin and lysozyme) of different properties (charge, molecular weight and rigidity), the main driving mechanism responsible for the protein binding to the charged nanoparticles was identified. Electrostatic interactions were found to dominate the protein adsorption dynamics, attachment and conformation. We developed a simple electrostatic model that can qualitatively explain the observed adsorption behaviour based on charge-induced pH modifications near the charged nanoparticle surfaces. Under neutral conditions, the local pH around the positively and negatively charged nanodiamonds becomes very high (11-12) and low (1-3) respectively, which has a profound impact on the protein charge, hydration and affinity to the nanodiamonds. Small proteins (lysozyme) were found to form multilayers with significant conformational changes to screen the surface charge, while larger proteins (albumin) formed monolayers with minor conformational changes. The findings of this study provide a step forward toward understanding and eventually predicting nanoparticle interactions with biofluids.Understanding the interaction of proteins with charged diamond nanoparticles is of fundamental importance for diverse biomedical applications. Here we present a thorough study of protein binding, adsorption kinetics and structure on strongly positively (hydrogen-terminated) and negatively (oxygen-terminated) charged nanodiamond particles using a quartz crystal microbalance by dissipation and infrared spectroscopy. By using two model proteins

  15. Adsorption of hydrogen on clean and modified magnesium films

    DEFF Research Database (Denmark)

    Johansson, Martin; Ostenfeld, Christopher Worsøe; Chorkendorff, Ib

    2006-01-01

    films at H/Mg ratios less than 2% is developed. The activation barrier for hydrogen dissociation is 72 +/- 15 kJ/mole H-2, and a stagnant hydrogen uptake is observed. For platinum-catalyzed films, the barrier is significantly reduced, and there is no stagnation in the uptake rate....

  16. Demonstrative study on the production of hydrogen and aromatic compounds originated from biogas in the Dairy area

    International Nuclear Information System (INIS)

    Yukoh Shudo; Takashi Ohkubo; Yoshiaki Hideshima

    2006-01-01

    The biogas yielded by methane fermentation of cow slurry was provided for the experimental facilities and the refined methane was introduced to the methane direct reformer. Dehydrogenation and aromatization of methane generated hydrogen and aromatic compounds, such as benzene. In order to keep the conversion rate, pre-treatment and regeneration of the catalysts were carried out and in order to control coking at the catalysts, hydrogen was added to the material methane. Moreover a part of the un-reacted methane was introduced to the steam reformer and 99.99% pure hydrogen was produced by the pressure swing adsorption (PSA). With the result that, it was supposed that pre-treating by methane and hydrogen, repeating regeneration by hydrogen, and more than 9% hydrogen addition were needed to stabilize the formation of hydrogen and benzene. And furthermore, material balance of the experimental facilities was clarified. (authors)

  17. Study on the adsorption of 233Pa in glass

    International Nuclear Information System (INIS)

    Natsumi, R.R.; Saiki, M.; Lima, F.W. de.

    1982-08-01

    It is intended to examine the adsorption of protactinium on glass in relation to pH, presence of complexing agents concentration and type of electrolytes. The study was made by using carrier-free 233 Pa solution and Pyrex glass tube was selected as adsorbent glass material surface. The adsorption curve of protactinium on glass surface as a function of the pH of the tracer solution showed the existence of two pronounced adsorption regions. It was found that this adsorption can be reduced by using electrolytes or complexing agents. Desorption of protactinium previously adsorbed on the Pyrex glass tube was also studied. Hidrochloric, oxalic and hydrofluoric acid solutions were used for the desorption experiments. (Author) [pt

  18. FINAL REPORT: Room Temperature Hydrogen Storage in Nano-Confined Liquids

    Energy Technology Data Exchange (ETDEWEB)

    VAJO, JOHN

    2014-06-12

    DOE continues to seek solid-state hydrogen storage materials with hydrogen densities of ≥6 wt% and ≥50 g/L that can deliver hydrogen and be recharged at room temperature and moderate pressures enabling widespread use in transportation applications. Meanwhile, development including vehicle engineering and delivery infrastructure continues for compressed-gas hydrogen storage systems. Although compressed gas storage avoids the materials-based issues associated with solid-state storage, achieving acceptable volumetric densities has been a persistent challenge. This project examined the possibility of developing storage materials that would be compatible with compressed gas storage technology based on enhanced hydrogen solubility in nano-confined liquid solvents. These materials would store hydrogen in molecular form eliminating many limitations of current solid-state materials while increasing the volumetric capacity of compressed hydrogen storage vessels. Experimental methods were developed to study hydrogen solubility in nano-confined liquids. These methods included 1) fabrication of composites comprised of volatile liquid solvents for hydrogen confined within the nano-sized pore volume of nanoporous scaffolds and 2) measuring the hydrogen uptake capacity of these composites without altering the composite composition. The hydrogen storage capacities of these nano-confined solvent/scaffold composites were compared with bulk solvents and with empty scaffolds. The solvents and scaffolds were varied to optimize the enhancement in hydrogen solubility that accompanies confinement of the solvent. In addition, computational simulations were performed to study the molecular-scale structure of liquid solvent when confined within an atomically realistic nano-sized pore of a model scaffold. Confined solvent was compared with similar simulations of bulk solvent. The results from the simulations were used to formulate a mechanism for the enhanced solubility and to guide the

  19. Competitive Protein Adsorption - Multilayer Adsorption and Surface Induced Protein Aggregation

    DEFF Research Database (Denmark)

    Holmberg, Maria; Hou, Xiaolin

    2009-01-01

    In this study, competitive adsorption of albumin and IgG (immunoglobulin G) from human serum solutions and protein mixtures onto polymer surfaces is studied by means of radioactive labeling. By using two different radiolabels (125I and 131I), albumin and IgG adsorption to polymer surfaces...... is monitored simultaneously and the influence from the presence of other human serum proteins on albumin and IgG adsorption, as well as their mutual influence during adsorption processes, is investigated. Exploring protein adsorption by combining analysis of competitive adsorption from complex solutions...... of high concentration with investigation of single protein adsorption and interdependent adsorption between two specific proteins enables us to map protein adsorption sequences during competitive protein adsorption. Our study shows that proteins can adsorb in a multilayer fashion onto the polymer surfaces...

  20. A first-principles study of oxygen adsorption on Ir(111) surface

    Energy Technology Data Exchange (ETDEWEB)

    Gao, Hengjiao, E-mail: gaohengjiao@163.com; Xiong, Yuqing, E-mail: xiongyq@hotmail.com; Liu, Xiaoli, E-mail: shantianzi@126.com; Zhao, Dongcai, E-mail: zhaodongc@163.com; Feng, Yudong, E-mail: yudong_feng@sina.com; Wang, Lanxi, E-mail: wanglanxi@live.com; Wang, Jinxiao, E-mail: coldwind716@gmail.com

    2016-12-15

    Highlights: • Adsorption of oxygen on Ir(111) surface was studied by density functional theory. • The most stable adsorption site was determined by adsorption energy calculation. • Adsorption of oxygen at bridge and top site on Ir surface was the most stable ones. • Interaction of O 2p and Ir 5d orbits is relatively strong and formed hybridization. - Abstract: In order to understand deposition mechanism of iridium thin film by atomic layer deposition, the adsorption of oxygen on Ir(111) surface was studied by use of density functional theory and a periodical slab model. By calculating the adsorption energy and structure of oxygen at four adsorption sites (top, bridge, fcc-hollow and hcp-hollow) on Ir(111) surface, the most stable adsorption site was determined. On this basis, the banding mechanism of O and Ir atoms was studied by density of states of oxygen and iridium atoms. Oxygen adsorbed at hcp(parallel) site on Ir(111) surface was the most stable one according to the adsorption energy calculation results. Orbital charge analysis indicate that charge transferred from 5p and 5d orbit to 2p orbit of adsorbed O atoms, and 6s orbit of iridium atoms. Meanwhile, density of state study indicated that adsorption of oxygen on Ir(111) surface is mainly due to the interaction between 2p orbit of O atoms and 5d orbit of iridium atoms.

  1. Adsorption of oxazole and isoxazole on BNNT surface: A DFT study

    Energy Technology Data Exchange (ETDEWEB)

    Kaur, Jasleen, E-mail: jasleen.chem@gmail.com; Singla, Preeti, E-mail: preetisingla21@gmail.com; Goel, Neetu, E-mail: neetugoel@pu.ac.in

    2015-02-15

    Highlights: • The adsorption of oxazole and isoxazole over (6,0) and (5,5) BNNTs is studied. • The adsorption energies and structural changes are inductive of covalent adsorption. • The solvent plays an important role in improving the adsorption properties. • The adsorption witnesses substantial changes in electronic properties of the BNNT. • The functionalization of the BNNTs open up their applicability as drug carrier. - Abstract: The adsorption behavior of oxazole and isoxazole heterocycles over the (6,0) zigzag and (5,5) armchair boron nitride nanotube (BNNT) has been studied within the formalism of density functional theory (DFT). The adsorption energies, the frontier molecular orbital (FMO) analysis and the structural changes at the adsorption site are indicative of covalent adsorption on the zigzag BNNT surface, while the adsorption is physical in nature on the armchair BNNT surface. The role of solvent in improving the adsorption properties over the BNNT surface is elucidated by reoptimizing the structures in aqueous phase. The solvation energy is indicative of remarkable increase in the solubility of BNNTs after adsorption of heterocyclic rings. The Density of states (DOS) Plots, natural bond orbital (NBO) analysis and the quantum molecular descriptors (QMD) are witness to the substantial changes in the electronic properties of the BNNT systems following the attachment of these heterocycles with the tube surface. The study envisages the functionalization of the BNNT as well as its applicability as carrier of the drugs containing heterocyclic rings oxazole and isoxazole with marked sensitivity to the type of adsorbate and the adsorbent.

  2. Functionalized mesoporous silica materials for molsidomine adsorption: Thermodynamic study

    International Nuclear Information System (INIS)

    Alyoshina, Nonna A.; Parfenyuk, Elena V.

    2013-01-01

    A series of unmodified and organically modified mesoporous silica materials was prepared. The unmodified mesoporous silica was synthesized via sol–gel synthesis in the presence of D-glucose as pore-forming agent. The functionalized by phenyl, aminopropyl and mercaptopropyl groups silica materials were prepared via grafting. The fabricated adsorbent materials were characterized by Fourier transform infrared spectroscopy (FTIR) analysis, N 2 adsorption/desorption and elemental analysis methods. Then their adsorption properties for mesoionic dug molsidomine were investigated at 290–313 K and physiological pH value. Thermodynamic parameters of molsidomine adsorption on the synthesized materials have been calculated. The obtained results showed that the adsorption process of molsidomine on the phenyl modified silica is the most quantitatively and energetically favorable. The unmodified and mercaptopropyl modified silica materials exhibit significantly higher adsorption capacities and energies for molsidomine than the aminopropyl modified sample. The effects are discussed from the viewpoint of nature of specific interactions responsible for the adsorption. - Graphical abstract: Comparative analysis of the thermodynamic characteristics of molsidomine adsorption showed that the adsorption process on mesoporous silica materials is controlled by chemical nature of surface functional groups. Molsidomine adsorption on the phenyl modified silica is the most quantitatively and energetically favorable. Taking into account ambiguous nature of mesoionic compounds, it was found that molsidomine is rather aromatic than dipolar. Display Omitted - Highlights: • Unmodified and organically modified mesoporous silica materials were prepared. • Molsidomine adsorption on the silica materials was studied. • Phenyl modified silica shows the highest adsorption capacity and favorable energy. • Molsidomine exhibits the lowest affinity to aminopropyl modified silica

  3. Adsorption on smooth electrodes: A radiotracer study

    International Nuclear Information System (INIS)

    Rice-Jackson, L.M.

    1990-01-01

    Adsorption on solids is a complicated process and in most cases, occurs as the early stage of other more complicated processes, i.e. chemical reactions, electrooxidation, electroreduction. The research reported here combines the electroanalytical method, cyclic voltammetry, and the use of radio-labeled isotopes, soft beta emitters, to study adsorption processes at smooth electrodes. The in-situ radiotracer method is highly anion (molecule) specific and provides information on the structure and composition of the electric double layer. The emphasis of this research was on studying adsorption processes at smooth electrodes of copper, gold, and platinum. The application of the radiotracer method to these smooth surfaces have led to direct in-situ measurements from which surface coverage was determined; anions and molecules were identified; and weak interactions of adsorbates with the surface of the electrodes were readily monitored. 179 refs

  4. Diffusion of hydrogen into and through γ-iron by density functional theory

    Science.gov (United States)

    Chohan, Urslaan K.; Koehler, Sven P. K.; Jimenez-Melero, Enrique

    2018-06-01

    This study is concerned with the early stages of hydrogen embrittlement on an atomistic scale. We employed density functional theory to investigate hydrogen diffusion through the (100), (110) and (111) surfaces of γ-Fe. The preferred adsorption sites and respective energies for hydrogen adsorption were established for each plane, as well as a minimum energy pathway for diffusion. The H atoms adsorb on the (100), (110) and (111) surfaces with energies of ∼4.06 eV, ∼3.92 eV and ∼4.05 eV, respectively. The barriers for bulk-like diffusion for the (100), (110) and (111) surfaces are ∼0.6 eV, ∼0.5 eV and ∼0.7 eV, respectively. We compared these calculated barriers with previously obtained experimental data in an Arrhenius plot, which indicates good agreement between experimentally measured and theoretically predicted activation energies. Texturing austenitic steels such that the (111) surfaces of grains are preferentially exposed at the cleavage planes may be a possibility to reduce hydrogen embrittlement.

  5. Sc-Decorated Porous Graphene for High-Capacity Hydrogen Storage: First-Principles Calculations.

    Science.gov (United States)

    Chen, Yuhong; Wang, Jing; Yuan, Lihua; Zhang, Meiling; Zhang, Cairong

    2017-08-02

    The generalized gradient approximation (GGA) function based on density functional theory is adopted to investigate the optimized geometrical structure, electron structure and hydrogen storage performance of Sc modified porous graphene (PG). It is found that the carbon ring center is the most stable adsorbed position for a single Sc atom on PG, and the maximum number of adsorbed H₂ molecules is four with the average adsorption energy of -0.429 eV/H₂. By adding a second Sc atom on the other side of the system, the hydrogen storage capacity of the system can be improved effectively. Two Sc atoms located on opposite sides of the PG carbon ring center hole is the most suitable hydrogen storage structure, and the hydrogen storage capacity reach a maximum 9.09 wt % at the average adsorption energy of -0.296 eV/H₂. The adsorption of H₂ molecules in the PG system is mainly attributed to orbital hybridization among H, Sc, and C atoms, and Coulomb attraction between negatively charged H₂ molecules and positively charged Sc atoms.

  6. Hydrogen retention properties of lithium film

    International Nuclear Information System (INIS)

    Kanaya, Koh; Yamauchi, Yuji; Hirohata, Yuko; Hino, Tomoaki; Mori, Kintaro

    1998-01-01

    Hydrogen retention properties of Li films and lithium oxide-lithium hydroxide (Li 2 O-LiOH) mixed films were investigated by two methods, hydrogen ion irradiation and hydrogen glow discharge. In a case of the hydrogen ion irradiation, thermal desorption spectrum of hydrogen retained in Li 2 O-LiOH film had two desorption peaks at around 470 K and 570 K. The ratio between retained hydrogen and Li atom was about 0.7. In a case of the hydrogen glow discharge, the hydrogen was also gettered in Li film during the discharge. The ratio of H/Li was almost 0.9. Most of gettered hydrogen desorbed by a baking with a temperature of 370 K. On the contrary, when the Li film exposed to the atmosphere was irradiated by the hydrogen plasma, the desorption of H 2 O was observed in addition to the adsorption of H 2 . (author)

  7. Nanoporous spongy graphene: Potential applications for hydrogen adsorption and selective gas separation

    Energy Technology Data Exchange (ETDEWEB)

    Kostoglou, Nikolaos, E-mail: nikolaos.kostoglou@stud.unileoben.ac.at [Department of Mechanical and Manufacturing Engineering, University of Cyprus, 1678 Nicosia (Cyprus); Department of Physical Metallurgy and Materials Testing, Montanuniversität Leoben, 8700 Leoben (Austria); Constantinides, Georgios [Research Unit for Nanostructured Materials Systems, Department of Mechanical Engineering and Materials Science and Engineering, Cyprus University of Technology, 3036 Lemesos (Cyprus); Charalambopoulou, Georgia; Steriotis, Theodore [National Center for Scientific Research Demokritos, Agia Paraskevi Attikis, 15310 Athens (Greece); Polychronopoulou, Kyriaki [Department of Mechanical Engineering, Khalifa University of Science, Technology and Research, Abu Dhabi (United Arab Emirates); Li, Yuanqing; Liao, Kin [Department of Aerospace Engineering, Khalifa University of Science, Technology and Research, Abu Dhabi (United Arab Emirates); Ryzhkov, Vladislav [Nanotube Production Department, Fibrtec Incorporation, TX, 75551 Atlanta (United States); Mitterer, Christian [Department of Physical Metallurgy and Materials Testing, Montanuniversität Leoben, 8700 Leoben (Austria); Rebholz, Claus, E-mail: claus@ucy.ac.cy [Department of Mechanical and Manufacturing Engineering, University of Cyprus, 1678 Nicosia (Cyprus)

    2015-12-01

    In the present work, a nanoporous (pore width ~ 0.7 nm) graphene-based sponge-like material with large surface area (~ 350 m{sup 2}/g) was synthesized by wet chemical reduction of graphene oxide in combination with freeze-drying. Surface morphology and elemental composition were studied by scanning and transmission electron microscopy combined with energy dispersive X-ray spectroscopy. Surface chemistry was qualitatively examined by Fourier-transform infrared spectroscopy, while the respective structure was investigated by X-ray diffraction analysis. Textural properties, including Brunauer–Emmet–Teller (BET) surface area, micropore volume and surface area as well as pore size distribution, were deduced from nitrogen gas adsorption/desorption data obtained at 77 K and up to 1 bar. Potential use of the spongy graphene for gas storage and separation applications was preliminarily assessed by low-pressure (0–1 bar) H{sub 2}, CO{sub 2} and CH{sub 4} sorption measurements at different temperatures (77, 273 and 298 K). The adsorption capacities for each gas were evaluated up to ~ 1 bar, the isosteric enthalpies of adsorption for CO{sub 2} (28–33 kJ/mol) and CH{sub 4} (30–38 kJ/mol) were calculated using the Clausius–Clapeyron equation, while the CO{sub 2}/CH{sub 4} gas selectivity (up to 95:1) was estimated using the Ideal Adsorbed Solution Theory (IAST). - Highlights: • Nanoporous sponge produced by chemical reduction of graphene oxide and freeze-drying • Characterization performed using SEM, EDS, TEM, FT-IR, BET and XRD methods • Gas storage performance evaluated towards H{sub 2}, CO{sub 2} and CH{sub 4} adsorption up to 1 bar • CO{sub 2} over CH{sub 4} gas selectivity estimated between 45 and 95 at 273 K using the IAST model.

  8. Nanoporous spongy graphene: Potential applications for hydrogen adsorption and selective gas separation

    International Nuclear Information System (INIS)

    Kostoglou, Nikolaos; Constantinides, Georgios; Charalambopoulou, Georgia; Steriotis, Theodore; Polychronopoulou, Kyriaki; Li, Yuanqing; Liao, Kin; Ryzhkov, Vladislav; Mitterer, Christian; Rebholz, Claus

    2015-01-01

    In the present work, a nanoporous (pore width ~ 0.7 nm) graphene-based sponge-like material with large surface area (~ 350 m"2/g) was synthesized by wet chemical reduction of graphene oxide in combination with freeze-drying. Surface morphology and elemental composition were studied by scanning and transmission electron microscopy combined with energy dispersive X-ray spectroscopy. Surface chemistry was qualitatively examined by Fourier-transform infrared spectroscopy, while the respective structure was investigated by X-ray diffraction analysis. Textural properties, including Brunauer–Emmet–Teller (BET) surface area, micropore volume and surface area as well as pore size distribution, were deduced from nitrogen gas adsorption/desorption data obtained at 77 K and up to 1 bar. Potential use of the spongy graphene for gas storage and separation applications was preliminarily assessed by low-pressure (0–1 bar) H_2, CO_2 and CH_4 sorption measurements at different temperatures (77, 273 and 298 K). The adsorption capacities for each gas were evaluated up to ~ 1 bar, the isosteric enthalpies of adsorption for CO_2 (28–33 kJ/mol) and CH_4 (30–38 kJ/mol) were calculated using the Clausius–Clapeyron equation, while the CO_2/CH_4 gas selectivity (up to 95:1) was estimated using the Ideal Adsorbed Solution Theory (IAST). - Highlights: • Nanoporous sponge produced by chemical reduction of graphene oxide and freeze-drying • Characterization performed using SEM, EDS, TEM, FT-IR, BET and XRD methods • Gas storage performance evaluated towards H_2, CO_2 and CH_4 adsorption up to 1 bar • CO_2 over CH_4 gas selectivity estimated between 45 and 95 at 273 K using the IAST model

  9. Adsorption of pharmaceuticals onto isolated polyamide active layer of NF/RO membranes.

    Science.gov (United States)

    Liu, Yan-Ling; Wang, Xiao-Mao; Yang, Hong-Wei; Xie, Yuefeng F

    2018-06-01

    Adsorption of trace organic compounds (TrOCs) onto the membrane materials has a great impact on their rejection by nanofiltration (NF) and reverse osmosis (RO) membranes. This study aimed to investigate the difference in adsorption of various pharmaceuticals (PhACs) onto different NF/RO membranes and to demonstrate the necessity of isolating the polyamide (PA) active layer from the polysulfone (PS) support layer for adsorption characterization and quantification. Both the isolated PA layers and the PA+PS layers of NF90 and ESPA1 membranes were used to conduct static adsorption tests. Results showed that apparent differences existed between the PA layer and the PA+PS layer in the adsorption capacity of PhACs as well as the time necessary to reach the adsorption equilibrium. PhACs with different physicochemical properties could be adsorbed to different extents by the isolated PA layer, which was mainly attributed to electrostatic attraction/repulsion and hydrophobic interactions. The PA layer of ESPA1 exhibited apparently higher adsorption capacities for the positively charged PhACs and similar adsorption capacities for the neutral PhACs although it had significantly less total interfacial area (per unit membrane surface area) for adsorption compared to the PA layer of NF90. The higher affinity of the PA layer of ESPA1 for the PhACs could be due to its higher capacity of forming hydrogen bonds with PhACs resulted from the modified chemistry with more -OH groups. This study provides a novel approach to determining the TrOC adsorption onto the active layer of membranes for the ease of investigating adsorption mechanisms. Copyright © 2018 Elsevier Ltd. All rights reserved.

  10. Study of cesium and strontium adsorption on slovak bentonite

    International Nuclear Information System (INIS)

    Galambos, M.

    2010-01-01

    Bentonite is a natural clay and one of the most promising candidates for use as a buffer material in the geological disposal systems for high-level radioactive waste and spent nuclear fuel. It is intended to isolate metal canisters with highly radioactive waste products from the surrounding rocks because of its ability to retard the movement of radionuclides by adsorption. Slovak Republic avails of many significant deposits of bentonite. Adsorption of Cs and Sr on five Slovak bentonite of deposits (Jelsovy potok, Kopernica, Lieskovec, Lastovce and Dolna Ves) and montmorillonite K10 (Sigma-Aldrich) has been studied with the using batch of radiometric techniques. Natural, irradiated and natrified samples, in three different kinds of grain size: 15, 45 and 250 μm have been used in the experiments. The adsorptions of Cs and Sr on bentonite under various experimental conditions, such as contact time, adsorbent and adsorbate concentrations, pH after adsorption and effect of pH change, chemical modification, competitive ions and organic agents on the adsorption have been studied. The K d have been determined for adsorbent-Cs/Sr solution system as a function of contact time and adsorbate and adsorbent concentration. The data have been interpreted in terms of Langmuir isotherm. The adsorption of Cs and Sr has increased with increasing metal concentrations. Adsorption of Cs and Sr has been suppressed by presence of organic agents; and of bivalent cations more than univalent cations. By adsorption on natrified samples colloidal particles and pH value increase have been formed. Adsorption experiments carried out show that the most suitable materials intended for use as barriers surrounding a canister of spent nuclear fuel are bentonite of the Jelsovy potok and Kopernica deposits. (author)

  11. Shape-dependent hydrogen-storage properties in Pd nanocrystals: which does hydrogen prefer, octahedron (111) or cube (100)?

    Science.gov (United States)

    Li, Guangqin; Kobayashi, Hirokazu; Dekura, Shun; Ikeda, Ryuichi; Kubota, Yoshiki; Kato, Kenichi; Takata, Masaki; Yamamoto, Tomokazu; Matsumura, Syo; Kitagawa, Hiroshi

    2014-07-23

    Pd octahedrons and cubes enclosed by {111} and {100} facets, respectively, have been synthesized for investigation of the shape effect on hydrogen-absorption properties. Hydrogen-storage properties were investigated using in situ powder X-ray diffraction, in situ solid-state (2)H NMR and hydrogen pressure-composition isotherm measurements. With these measurements, it was found that the exposed facets do not affect hydrogen-storage capacity; however, they significantly affect the absorption speed, with octahedral nanocrystals showing the faster response. The heat of adsorption of hydrogen and the hydrogen diffusion pathway were suggested to be dominant factors for hydrogen-absorption speed. Furthermore, in situ solid-state (2)H NMR detected for the first time the state of (2)H in a solid-solution (Pd + H) phase of Pd nanocrystals at rt.

  12. Functionalized mesoporous silica materials for molsidomine adsorption: Thermodynamic study

    Energy Technology Data Exchange (ETDEWEB)

    Alyoshina, Nonna A.; Parfenyuk, Elena V., E-mail: evp@iscras.ru

    2013-09-15

    A series of unmodified and organically modified mesoporous silica materials was prepared. The unmodified mesoporous silica was synthesized via sol–gel synthesis in the presence of D-glucose as pore-forming agent. The functionalized by phenyl, aminopropyl and mercaptopropyl groups silica materials were prepared via grafting. The fabricated adsorbent materials were characterized by Fourier transform infrared spectroscopy (FTIR) analysis, N{sub 2} adsorption/desorption and elemental analysis methods. Then their adsorption properties for mesoionic dug molsidomine were investigated at 290–313 K and physiological pH value. Thermodynamic parameters of molsidomine adsorption on the synthesized materials have been calculated. The obtained results showed that the adsorption process of molsidomine on the phenyl modified silica is the most quantitatively and energetically favorable. The unmodified and mercaptopropyl modified silica materials exhibit significantly higher adsorption capacities and energies for molsidomine than the aminopropyl modified sample. The effects are discussed from the viewpoint of nature of specific interactions responsible for the adsorption. - Graphical abstract: Comparative analysis of the thermodynamic characteristics of molsidomine adsorption showed that the adsorption process on mesoporous silica materials is controlled by chemical nature of surface functional groups. Molsidomine adsorption on the phenyl modified silica is the most quantitatively and energetically favorable. Taking into account ambiguous nature of mesoionic compounds, it was found that molsidomine is rather aromatic than dipolar. Display Omitted - Highlights: • Unmodified and organically modified mesoporous silica materials were prepared. • Molsidomine adsorption on the silica materials was studied. • Phenyl modified silica shows the highest adsorption capacity and favorable energy. • Molsidomine exhibits the lowest affinity to aminopropyl modified silica.

  13. Development of the work function approach to the underpotential deposition of metals. Application to the hydrogen evolution reaction

    International Nuclear Information System (INIS)

    Trasatti, S.

    1975-01-01

    A theory is developed for the underpotential deposition of metals. Concepts are then extended to oxygen and hydrogen adsorption. Analysis of results shows that, unlike oxygen adsorption, hydrogen adsorption in solution probably follows a different pattern with respect to the gas phase situation. The hydrogen evolution reaction is discussed in the light of the above findings and it is shown that usual concepts regarding the reactivity scale of metals towards hydrogen should be reconsidered taking into account solvent and entropy effects. The latters can account for the behaviour of sp-metals. The formers are important with transition metals. The final picture is consistent with the idea that M-H 2 O interactions are much stronger on transition than on sp-metals. (orig.) [de

  14. Diaphite, a new type of surface with mixed sp{sup 2}-sp{sup 3} hybridization for adsorption and functionalization

    Energy Technology Data Exchange (ETDEWEB)

    Radosinski, Lukasz, E-mail: lukasz.radosinski@pwr.edu.pl [Wroclaw University of Science and Technology, Chemistry Department, Group of Bioprocess and Biomedical Engineering, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw (Poland); Formalik, Filip [Wroclaw University of Science and Technology, Chemistry Department, Group of Bioprocess and Biomedical Engineering, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw (Poland); Olejniczak, Adam [Department of Spectroscopy of Excited States, Institute of Low Temperature and Structure Research, Polish Academy of Sciences, Okolna 2, 50-422 Wroclaw (Poland); Radosz, Andrzej [Wroclaw University of Science and Technology, Faculty of Fundamental Problems of Technology, Department of Quantum Technologies, Wybrzeze Wyspianskiego 27, 50-370 Wroclaw (Poland)

    2017-05-15

    Highlights: • Recent discoveries show a possibility of photoinduced formation of a structure of mixed sp{sub 2}-sp{sub 3} hybridization out of graphite and graphene–diaphite. • Ab initio and molecular mechanics calculations indicate that the surface exhibits large enhancement of binding energy due to favorable sp{sub 3} like hybridization. • The binding energy varies upon configuration of occupied adsorption sites and the adsorption sites form a regular bed-like matrix. - Abstract: We theoretically study a new carbon phase with mixed sp{sup 2}-sp{sup 3} bond hybridization called diaphite. Using ab initio calculations and the adaptive intermolecular reactive bond order (AIREBO) potential approach, we show that the surface of this structure exhibits enhanced adsorption capabilities. Specifically, using hydrogen as a test adsorbate, we calculate that the chemical binding energy, depending on the configuration of hydrogen atoms, varies from 2.08 to 2.9 eV. Furthermore, the adsorption sites form a regular matrix; thus, we postulate that this new stable carbon phase may be a universal matrix for functionalization.

  15. Hydrogen energy systems studies

    Energy Technology Data Exchange (ETDEWEB)

    Ogden, J.M.; Steinbugler, M.; Dennis, E. [Princeton Univ., NJ (United States)] [and others

    1995-09-01

    For several years, researchers at Princeton University`s Center for Energy and Environmental Studies have carried out technical and economic assessments of hydrogen energy systems. Initially, we focussed on the long term potential of renewable hydrogen. More recently we have explored how a transition to renewable hydrogen might begin. The goal of our current work is to identify promising strategies leading from near term hydrogen markets and technologies toward eventual large scale use of renewable hydrogen as an energy carrier. Our approach has been to assess the entire hydrogen energy system from production through end-use considering technical performance, economics, infrastructure and environmental issues. This work is part of the systems analysis activity of the DOE Hydrogen Program. In this paper we first summarize the results of three tasks which were completed during the past year under NREL Contract No. XR-11265-2: in Task 1, we carried out assessments of near term options for supplying hydrogen transportation fuel from natural gas; in Task 2, we assessed the feasibility of using the existing natural gas system with hydrogen and hydrogen blends; and in Task 3, we carried out a study of PEM fuel cells for residential cogeneration applications, a market which might have less stringent cost requirements than transportation. We then give preliminary results for two other tasks which are ongoing under DOE Contract No. DE-FG04-94AL85803: In Task 1 we are assessing the technical options for low cost small scale production of hydrogen from natural gas, considering (a) steam reforming, (b) partial oxidation and (c) autothermal reforming, and in Task 2 we are assessing potential markets for hydrogen in Southern California.

  16. Thermal Adsorption Processing Of Hydrocarbon Residues

    Directory of Open Access Journals (Sweden)

    Sudad H. Al.

    2017-04-01

    Full Text Available The raw materials of secondary catalytic processes must be pre-refined. Among these refining processes are the deasphalting and demetallization including their thermo adsorption or thermo-contact adsorption variety. In oil processing four main processes of thermo-adsorption refining of hydrocarbon residues are used ART Asphalt Residual Treating - residues deasphaltizing 3D Discriminatory Destructive Distillation developed in the US ACT Adsorption-Contact Treatment and ETCC Express Thermo-Contact Cracking developed in Russia. ART and ACT are processes with absorbers of lift type reactor while 3D and ETCC processes are with an adsorbing reactor having ultra-short contact time of the raw material with the adsorbent. In all these processes refining of hydrocarbon residues is achieved by partial Thermo-destructive transformations of hydrocarbons and hetero-atomic compounds with simultaneous adsorption of the formed on the surface of the adsorbents resins asphaltene and carboids as well as metal- sulphur - and nitro-organic compounds. Demetallized and deasphalted light and heavy gas oils or their mixtures are a quality raw material for secondary deepening refining processes catalytic and hydrogenation cracking etc. since they are characterized by low coking ability and low content of organometallic compounds that lead to irreversible deactivation of the catalysts of these deepening processes.

  17. Investigations on the heterogenous catalytic hydrogenation using isotope effect and gamma- and neutron radiation

    Energy Technology Data Exchange (ETDEWEB)

    Kudlacek, R; Cabicar, J [Ceske Vysoke Uceni Technicke, Prague (Czechoslovakia). Katedra Jaderne Chemie

    1976-01-01

    The kinetic and solvent isotope effects during the maleic acid heterogeneous catalytic hydrogenation and deuteration in light and heavy water have been studied. Also the effect of the gamma and neutron irradiation on the Ni-ZnO catalysts (with various ratios of components) on the reaction kinetics and mechanism has been measured, as well as the effect of pH on the adsorption behaviour of maleic acid and the temperature dependence of the reaction rate. Existence of different adsorption centers for hydrogen and maleic acid could be deduced from these experiments. A reaction mechanism based on the two-dimensional diffusion of components in the surface is proposed. The catalyst is formed from Ni and ZnO-microspheres. Hydrogen is bound to nickel and maleic acid is adsorbed on the ZnO-microspheres. The reaction takes place on the boundary layers of these microspheres.

  18. Adsorption of U(VI) onto kaolin studied by batch method

    International Nuclear Information System (INIS)

    Hongxia Zhang; Zhi Liu; Peizhuo Hu; Tonghuan Liu; Wangsuo Wu

    2013-01-01

    Adsorption of U(VI) on purified kaolin was studied by batch methods under ambient conditions, including contact time, pH, fulvic acid, etc. Three kinetic models were used to model the kinetic adsorption which was very well described by the pseudo-second-order rate equation, and the activation energy of adsorption was 52.20 kJ/mol. The Freundlich and Dubinin-Radushkevich models fitted the experimental data better than the Langmuir model for the adsorption and desorption isotherms. The thermodynamic parameters indicated that the adsorption of U(VI) on kaolin was an endothermic and spontaneous process. (author)

  19. Equilibrium and kinetics studies of metal ion adsorption on dyed ...

    African Journals Online (AJOL)

    Batch equilibration studies were conducted to determine the nature of adsorption of Zn (II) and Cu (II) onto dyed coconut pollens. The nature of adsorption of metal ions was explained using the Langmuir equation. The calculated values of equilibrium parameter indicated favourable adsorption by the adsorbents. Also the ...

  20. Thermodynamic study on the adsorption of strontium on polyantimonic acid exchanger

    International Nuclear Information System (INIS)

    Li Mingyu; Chen Jing; Wang Jianchen; Zhao Jing

    2007-01-01

    The adsorption of strontium on the polyantimonic acid adsorbent was studied. The equilibrium data for the adsorption of strontium on polyantimonic acid exchanger from aqueous solutions were obtained and correlated with Langmuir-type and Freundlich-type isotherm equation within the temperature range of 293-323 K and the experimental concentration range. Freundlich adsorption isotherms and the isosteric enthalpy indicate that the adsorption of strontium on polyantimonic acid is an endothermic process from aqueous solutions. The enthalpy, free energy, and entropy of adsorption were calculated. The results indicate that the adsorption process is a complex interaction of physical and chemical processes. The adsorption behaviors were reasonably explained. (authors)

  1. Adsorption of alcohols and fatty acids onto hydrogenated (a-C:H) DLC coatings

    Science.gov (United States)

    Simič, R.; Kalin, M.; Kovač, J.; Jakša, G.

    2016-02-01

    Information about the interactions between lubricants and DLC coatings is scarce, despite there having been many studies over the years. In this investigation we used ToF-SIMS, XPS and contact-angle analyses to examine the adsorption ability and mechanisms with respect to two oiliness additives, i.e., hexadecanol and hexadecanoic acid, on an a-C:H coating. In addition, we analyzed the resistance of the adsorbed films to external influences like solvent cleaning. The results show that both molecules adsorb onto surface oxides and hydroxides present on the initial DLC surface and shield these structures with their hydrocarbon tails. This makes the surfaces less polar, which is manifested in a smaller polar component of the surface energy. We also showed that ultrasonic cleaning in heptane has no significant effect on the quantity of adsorbed molecules or on their chemical state. This not only shows the relatively strong adsorption of these molecules, but also provides useful information for future experimental work. Of the two examined molecules, the acid showed a greater adsorption ability than the alcohol, which explains some of the previously reported better tribological properties in the case of the acid with respect to the alcohol.

  2. Application of computational fluid dynamics for the simulation of cryogenic molecular sieve bed absorber of hydrogen isotopes recovery system for Indian LLCB-TBM

    Energy Technology Data Exchange (ETDEWEB)

    Gayathri Devi, V.; Sircar, A.; Sarkar, B. [Institute of Plasma Research, Bhat, Gandhinagar, Gujarar (India)

    2015-03-15

    One of the most challenging tasks in the design of the fuel cycle system lies in the effective design of Tritium Extraction System (TES) which involves proper extraction and purification of tritium in the fuel cycle of the fusion reactor. Indian Lead Lithium cooled Ceramic Breeder Test Blanket Module (LLCB-TBM) would extract hydrogen isotopes through Cryogenic Molecular Sieve Bed (CMSB) adsorber system. A prototype Hydrogen Isotopes Recovery System (HIRS) is being developed to validate the concepts for tritium extraction by adsorption mass transfer mechanism. In this study, a design model has been developed and analyzed to simulate the adsorption mass transfer kinetics in a fixed bed adsorption column. The simulation leads primarily to effective design of HIRS, which is a state-of-the-art technology. The paper describes the process simulation approach and the results of Computational Fluid Dynamics (CFD) analysis. The effects of different operating conditions are studied to investigate their influence on the hydrogen isotopes adsorption capacity. The results of the present simulation study would be used to understand the best optimized transport phenomenon before realizing the TES as a system for LLCB-TBM. (authors)

  3. Nanoengineered Carbon Scaffolds for Hydrogen Storage

    Energy Technology Data Exchange (ETDEWEB)

    Leonard, A. D.; Hudson, J. L.; Fan, H.; Booker, R.; Simpson, L. J.; O' Neill, K. J.; Parilla, P. A.; Heben, M. J.; Pasquali, M.; Kittrell, C.; Tour, J. M.

    2009-01-01

    Single-walled carbon nanotube (SWCNT) fibers were engineered to become a scaffold for the storage of hydrogen. Carbon nanotube fibers were swollen in oleum (fuming sulfuric acid), and organic spacer groups were covalently linked between the nanotubes using diazonium functionalization chemistry to provide 3-dimensional (3-D) frameworks for the adsorption of hydrogen molecules. These 3-D nanoengineered fibers physisorb twice as much hydrogen per unit surface area as do typical macroporous carbon materials. These fiber-based systems can have high density, and combined with the outstanding thermal conductivity of carbon nanotubes, this points a way toward solving the volumetric and heat-transfer constraints that limit some other hydrogen-storage supports.

  4. A study on hydrogen-storage behaviors of nickel-loaded mesoporous MCM-41.

    Science.gov (United States)

    Park, Soo-Jin; Lee, Seul-Yi

    2010-06-01

    The objective of the present work was to investigate the possibility of improving the hydrogen-storage capacity of mesoporous MCM-41 containing nickel (Ni) oxides (Ni/MCM-41). The MCM-41 and Ni/MCM-41 were prepared using a hydrothermal process as a function of Ni content (2, 5, and 10 wt.% in the MCM-41). The surface functional groups of the Ni/MCM-41 were identified by Fourier transform infrared spectroscopy (FTIR). The structure and morphology of the Ni/MCM-41 were characterized by X-ray diffraction (XRD) and field emission transmission electron microscopy (FE-TEM). XRD results showed a well-ordered hexagonal pore structure; FE-TEM also revealed, as a complementary technique, the structure and pore size. The textural properties of the Ni/MCM-41 were analyzed using N(2) adsorption isotherms at 77 K. The hydrogen-storage capacity of the Ni/MCM-41 was evaluated at 298 K/100 bar. It was found that the presence of Ni on mesoporous MCM-41 created hydrogen-favorable sites that enhanced the hydrogen-storage capacity by a spillover effect. Furthermore, it was concluded that the hydrogen-storage capacity was greatly influenced by the amount of nickel oxide, resulting in a chemical reaction between Ni/MCM-41 and hydrogen molecules. Crown Copyright © 2010. Published by Elsevier Inc. All rights reserved.

  5. Theoretical study of cisplatin adsorption on silica

    Energy Technology Data Exchange (ETDEWEB)

    Simonetti, S., E-mail: ssimonet@uns.edu.ar [Departamento de Fisica and IFISUR, Universidad Nacional del Sur-CONICET, Av. Alem 1253, 8000 Bahia Blanca (Argentina); Departamentos de Ciencias Basicas e Ingenieria Mecanica, Universidad Tecnologica Nacional, 11 de Abril 461, 8000 Bahia Blanca (Argentina); Company, A. Diaz; Brizuela, G.; Juan, A. [Departamento de Fisica and IFISUR, Universidad Nacional del Sur-CONICET, Av. Alem 1253, 8000 Bahia Blanca (Argentina)

    2011-11-15

    The adsorption of cisplatin and its complexes, cis-[PtCl(NH{sub 3}){sub 2}]{sup +} and cis-[Pt(NH{sub 3}){sub 2}]{sup 2+}, on a SiO{sub 2}(1 1 1) hydrated surface has been studied by the Atom Superposition and Electron Delocalization method. The adiabatic energy curves for the adsorption of the drug and its products on the delivery system were considered. The electronic structure and bonding analysis were also performed. The molecule-surface interactions are formed at expenses of the OH surface bonds. The more important interactions are the Cl-H bond for cis-[PtCl{sub 2}(NH{sub 3}){sub 2}] and cis-[PtCl(NH{sub 3}){sub 2}]{sup +} adsorptions, and the Pt-O interaction for cis-[Pt(NH{sub 3}){sub 2}]{sup 2+} adsorption. The Cl p orbitals and Pt s, p y d orbitals of the molecule and its complexes, and the s H orbital and, the s and p orbitals of the O atoms of the hydrated surface are the main contribution to the surface bonds.

  6. Pt-decorated graphene as superior media for H2S adsorption: A first-principles study

    International Nuclear Information System (INIS)

    Ganji, Masoud Darvish; Sharifi, Narges; Ardjmand, Mahdi; Ahangari, Morteza Ghorbanzadeh

    2012-01-01

    Highlights: ► We report the first DFT study in the H 2 S/Pt–graphene system. ► The adsorption properties of H 2 S at different possible site on the surface of pristine graphene are slightly stable presenting energies from 0.02 to 0.06 eV. ► When Pt decorates the graphene sheet on the single and double sides the H 2 S adsorption energy increase to −3.2 eV. ► A single Pt atom can locate up to seven H 2 S molecules stably binded with energies from −6.73 to −0.95 eV. ► The DOS plot indicates strong hybridization between H 2 S molecules and Pt–graphene sheet. - Abstract: The adsorption mechanism of hydrogen sulfide (H 2 S) molecules on pristine and Pt-decorated graphene sheets was studied using density functional theory calculations based on local density approximation and generalized gradient approximation methods. Our calculations show that a Pt-decorated graphene system has much higher binding energy, higher net charge transfer values and shorter connecting distances than pristine graphene due to chemisorption of the H 2 S molecule. Furthermore, the calculated density of states show that orbital hybridization is visible between the H 2 S and Pt-decorated graphene sheets, while there is no evidence for hybridization between the H 2 S molecule and the pristine graphene sheet. Interestingly, we find that up to seven H 2 S molecules can stably bind to a Pt atom on each side of the graphene sheet with desirable binding energy.

  7. Hydrogen energy systems studies

    Energy Technology Data Exchange (ETDEWEB)

    Ogden, J.M.; Kreutz, T.G.; Steinbugler, M. [Princeton Univ., NJ (United States)] [and others

    1996-10-01

    In this report the authors describe results from technical and economic assessments carried out during the past year with support from the USDOE Hydrogen R&D Program. (1) Assessment of technologies for small scale production of hydrogen from natural gas. Because of the cost and logistics of transporting and storing hydrogen, it may be preferable to produce hydrogen at the point of use from more readily available energy carriers such as natural gas or electricity. In this task the authors assess near term technologies for producing hydrogen from natural gas at small scale including steam reforming, partial oxidation and autothermal reforming. (2) Case study of developing a hydrogen vehicle refueling infrastructure in Southern California. Many analysts suggest that the first widespread use of hydrogen energy is likely to be in zero emission vehicles in Southern California. Several hundred thousand zero emission automobiles are projected for the Los Angeles Basin alone by 2010, if mandated levels are implemented. Assuming that hydrogen vehicles capture a significant fraction of this market, a large demand for hydrogen fuel could evolve over the next few decades. Refueling a large number of hydrogen vehicles poses significant challenges. In this task the authors assess near term options for producing and delivering gaseous hydrogen transportation fuel to users in Southern California including: (1) hydrogen produced from natural gas in a large, centralized steam reforming plant, and delivered to refueling stations via liquid hydrogen truck or small scale hydrogen gas pipeline, (2) hydrogen produced at the refueling station via small scale steam reforming of natural gas, (3) hydrogen produced via small scale electrolysis at the refueling station, and (4) hydrogen from low cost chemical industry sources (e.g. excess capacity in refineries which have recently upgraded their hydrogen production capacity, etc.).

  8. Theoretical insights into the uranyl adsorption behavior on vanadium carbide MXene

    Science.gov (United States)

    Zhang, Yu-Juan; Zhou, Zhang-Jian; Lan, Jian-Hui; Ge, Chang-Chun; Chai, Zhi-Fang; Zhang, Peihong; Shi, Wei-Qun

    2017-12-01

    Remediation of the contamination by long-lived actinide wastes is extremely important but also challenging. Adsorption based techniques have attracted much research attention for their potential as low-cost and effective methods to reduce the radioactive waste from solution. In this work, we have investigated the adsorption behavior of uranyl species [with the general form UO2(L1)x(L2)y(L3)z, where L1, L2 and L3 stand for ligands H2O, OH and CO3, respectively] on hydroxylated vanadium carbide V2C(OH)2 MXene nanosheets using density functional theory based simulation methods We find that all studied uranyl species can stably bond to hydroxylated MXene with binding energies ranging from -3.3 to -4.6 eV, suggesting that MXenes could be effective adsorbers for uranyl ions. The strong adsorption is achieved by forming two Usbnd O bonds with the hydroxylated Mxene. In addition, the axial oxygen atoms from the uranyl ions form hydrogen bonds with the hydroxylated V2C, further strengthening the adsorption. We have also investigated the effects of F termination on the uranyl adsorption properties of V2C nanosheets. Usbnd F bonds are in general weaker than Usbnd O bonds on the adsorption site, suggesting that F terminated Mexne is less favorable for uranyl adsorption applications.

  9. Equilibrium and heat of adsorption of diethyl phthalate on heterogeneous adsorbents

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, W.M.; Xu, Z.W.; Pan, B.C.; Hong, C.H.; Jia, K.; Jiang, P.J.; Zhang, Q.J.; Pan, B.J. [Nanjing University, Nanjing (China)

    2008-09-15

    Removal of phthalate esters from water has been of considerable concern recently. In the present study, the adsorptive removal performance of diethyl phthalate (DEP) from water was investigated with the aminated polystyrene resin (NDA-101) and oxidized polystyrene resin (NDA-702). In addition, the commercial homogeneous polystyrene resin (XAD-4) and acrylic ester resin (Amberlite XAD-7) as well as coal-based granular activated carbon (AC-750) were chosen for comparison. The corresponding equilibrium isotherms are well described by the Freundlich equation and the adsorption capacities for DEP followed the order NDA-702 > NDA-101 > AC-750 > XAD-4 > XAD-7. Analysis of adsorption mechanisms suggested that these adsorbents spontaneously adsorb DEP molecules driven mainly by enthalpy change, and the adsorption process was derived by multiple adsorbent-adsorbate interactions such as hydrogen bonding, {pi}-{pi} stacking, and micropore filling. The information related to the adsorbent surface heterogeneity and the adsorbate-adsorbate interaction was obtained by Do's model. All the results indicate that heterogeneous resins NDA-702 and NDA-101 have excellent potential as an adsorption material for the removal of DEP from the contaminated water.

  10. Adsorption properties of thermally sputtered calcein film

    Science.gov (United States)

    Kruglenko, I.; Burlachenko, J.; Kravchenko, S.; Savchenko, A.; Slabkovska, M.; Shirshov, Yu.

    2014-05-01

    High humidity environments are often found in such areas as biotechnology, food chemistry, plant physiology etc. The controlling of parameters of such ambiences is vitally important. Thermally deposited calcein films have extremely high adsorptivity at exposure to water vapor of high concentration. This feature makes calcein a promising material for humidity sensing applications. The aim of this work is to explain high sensitivity and selectivity of calcein film to high humidity. Quartz crystal microbalance sensor, AFM and ellipsometry were used for calcein film characterization and adsorption properties investigation. The proposed model takes into account both the molecular properties of calcein (the presence of several functional groups capable of forming hydrogen bonds, and their arrangement) and the features of structure of thermally deposited calcein film (film restructuring due to the switching of bonds "calcein-calcein" to "calcein-water" in the course of water adsorption).

  11. Adsorption of ionizable organic contaminants on multi-walled carbon nanotubes with different oxygen contents

    International Nuclear Information System (INIS)

    Li Xiaona; Zhao Huimin; Quan Xie; Chen Shuo; Zhang Yaobin; Yu Hongtao

    2011-01-01

    Multi-walled carbon nanotubes (MWNTs), which are considered to be promising candidates for the adsorption of toxic organics, are released into aqueous environment with their increasing production and application. In this study, the adsorption behaviors of five structurally related ionizable organic contaminants namely perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorooctanesulfonamide (PFOSA), 2,4-dichlorophenoxyacetic acid (2,4-D) and 4-n-nonylphenol (4-NP) onto MWNTs with different oxygen contents (3.84-22.85%) were investigated. The adsorption kinetics was investigated and simulated with pseudo-second-order model. The adsorption isotherms were found to be fitted with Freundlich model and influenced by both the properties of organic chemicals and the oxygen contents of MWNTs. As adsorption capacity decreases dramatically with the increasing of oxygen contents, the MWNTs with the lowest oxygen contents possess the highest adsorption capacity among four MWNTs. For the MWNTs with the oxygen contents of 3.84%, the adsorption affinity related with hydrophobic interaction and π-electron polarizability decreased in the order of 4-NP > PFOSA > PFOS > 2,4-D > PFOA. Furthermore, the adsorption characters of five contaminants were affected by solution pH and solute pK a considering electrostatic repulse force and hydrogen bonding, which showed the adsorption of MWNTs with lower oxygen content is much sensitive to solution chemistry.

  12. Nitrotyrosine adsorption on carbon nanotube: a density functional theory study

    Science.gov (United States)

    Majidi, R.; Karami, A. R.

    2014-05-01

    We have studied the effect of nitrotyrosine on electronic properties of different single-wall carbon nanotubes by density functional theory. Optimal adsorption configurations of nitrotyrosine adsorbed on carbon nanotube have been determined by calculation of adsorption energy. Adsorption energies indicate that nitrotyrosine is chemisorbed on carbon nanotubes. It is found that the nitrotyrosine adsorption modifies the electronic properties of the semiconducting carbon nanotubes significantly and these nanotubes become n-type semiconductors, while the effect of nitrotyrosine on metallic carbon nanotubes is not considerable and these nanotubes remain metallic. Results clarify sensitivity of carbon nanotubes to nitrotyrosine adsorption and suggest the possibility of using carbon nanotubes as biosensor for nitrotyrosine detection.

  13. Theoretical study of adsorption of lithium atom on carbon nanotube

    OpenAIRE

    Senami, Masato; Ikeda, Yuji; Fukushima, Akinori; Tachibana, Akitomo

    2011-01-01

    We investigate the adsorption of lithium atoms on the surface of the (12, 0) single wall carbon nanotube (SWCNT) by using ab initio quantum chemical calculations. The adsorption of one lithium atom on the inside of this SWCNT is favored compared to the outside. We check this feature by charge transfer and regional chemical potential density. The adsorption of multiple lithium atoms on the interior of the SWCNT is studied in terms of adsorption energy and charge transfer. We show that repulsiv...

  14. A SANS study of the adsorption of guar gum on talc surfaces

    International Nuclear Information System (INIS)

    Cram, S.L.; Knott, R.; Hanley, H.

    2002-01-01

    Reagents based on guar gum are commonly used as 'gangue' depressants in the flotation of sulphides from ores containing naturally floating layer silicate minerals such as talc. Nickel sulphide ores processed by WMC Resources Ltd. at the Leinster Nickel Operations in Western Australia typically contain 1-2 % talc. Guar gum, added to the flotation cell, depresses the talc by adsorbing onto its surface, thereby reducing its hydrophobic nature. Guar gum is a long chain polysaccharide containing many hydroxyl functional groups along the length of its chain. The ratio of chain length to the number of hydroxyl and carboxyl groups causes the guar gum to be selective in depressing talc rather than nickel sulphide minerals. Small angle neutron scattering (SANS) it is an excellent tool for probing structures in the nano length scale. Unlike X-rays, neutrons are sensitive to low atomic weight elements, especially hydrogen and therefore organics. Using SANS it is possible to contrast different parts of a composite sample to get information on spatial arrangements. These qualities make SANS an obvious choice for studying the adsorption of guar gum on the surface of talc in aqueous solutions. Complimentary SANS experiments were carried out in Australia at the Australian Nuclear Science and Technology Organisation (ANSTO) and in the United States at the National Institute of Standards and Technology (NIST). Initially talc samples were studied 'as supplied', however as experiments proceeded attempts to reduce the particle size and distribution were carried out by milling and centrifuging procedures. Contrast matching techniques were used to observed the scattering behaviour of talc with and without the presence of guar gum and vice versa, over a total q range of 0.002 - 0.1 Angstroms -1 . The size of the talc particles appears to affect the scattering behaviour not only of talc but also of guar gum in the same solutions. This implies that the structure of the guar gum is strongly

  15. Interfacial adsorption of insulin - Conformational changes and reversibility of adsorption

    NARCIS (Netherlands)

    Mollmann, SH; Jorgensen, L; Bukrinsky, JT; Elofsson, U; Norde, W; Frokjaer, S

    The adsorption of human insulin to Teflon particles was studied with respect to conformational changes and the reversibility of adsorption was examined by total internal reflection fluorescence (TIRF). Adsorption isotherms for the adsorption of human insulin indicated high affinity adsorption, even

  16. Adsorption of sulfonamides to demineralized pine wood biochars prepared under different thermochemical conditions

    International Nuclear Information System (INIS)

    Xie, Mengxing; Chen, Wei; Xu, Zhaoyi; Zheng, Shourong; Zhu, Dongqiang

    2014-01-01

    The main objective of this study was to understand the key factors and mechanisms controlling adsorption of sulfonamides to biochars. Batch adsorption experiments were performed for sulfamethoxazole and sulfapyridine to three pine-wood biochars prepared under different thermochemical conditions: pyrolysis at 400 °C (C400) and 500 °C (C500), and pyrolysis at 500 °C followed with hydrogenation (C500-H). For both sulfonamides, the adsorbent surface area-normalized adsorption was stronger to C500 than to C400. This is attributable to the enhanced π–π electron-donor–acceptor interaction with the carbon surface of C500 due to the higher degree of graphitization. Despite the relatively large difference in surface O-functionality content between C500 (12.2%) and C500-H (6.6%), the two biochars exhibited nearly identical adsorbent surface area-normalized adsorption, indicating negligible role of surface O-functionalities in the adsorption to these adsorbents. Effects of solution chemistry conditions (pH, Cu 2+ , and dissolved soil humic acid) on adsorption were examined. -- Highlights: • Adsorption to biochars is dominated by π–π electron-donor–acceptor (EDA) interaction. • Graphitic surfaces of biochars are predominant adsorption sites. • Surface O-functionalities of biochars play minor roles in adsorption. • Adsorption affinities are markedly affected by Cu ions and humic acids. -- Adsorption of sulfonamides to biochars is dominated by π–π electron-donor–acceptor (EDA) interaction with the graphitic surface

  17. Effect of heat treatment and rotor steels composition on hydrogen solubility

    International Nuclear Information System (INIS)

    Ivanov, A.I.; Samojlenko, L.V.; Gorovaya, O.N.; Najdovskij, A.G.; Bilik, I.; Kret, Ya.

    1988-01-01

    Measurements of equilibrium hydrogen adsorption in samples of 27KhN3MFA and 25Kh2NMFA steels were conducted. Carbide inclusions and doping additions, typical for rotor steels, don't produce noticeable effect on hydrogen solubility in

  18. DFT Studies of Adsorption of Cu7-atom Nanoclusters on TiO2 Surfaces and Application to Methanol Steam Reforming Reactions

    Science.gov (United States)

    Taft, Michael J., Sr.

    Alcohol conversion to hydrogen, via steam reforming, is an alternative energy process that is promising for the future of clean energy economies. With advancements in fuel cell technologies, on-board hydrogen reforming could leverage already existing automotive designs and fuel infrastructure. The design of catalytic materials with tunable properties requires a level of insight that has yet to be achieved experimentally. The central objective of this project is to develop a working model of metal-oxide surface mediated copper clusters, since such catalytic beds have a wide-range of applications. More specifically, we investigate the catalytic framework of this process with theoretical models of the active metal (Cu) and metal­oxide support (TiO2). We employ a Density Functional Theory (DFT)-Generalized Gradient Approximation (GGA) approach for the quantum level electronic structure calculations of Cu, TiO2 and CH3OH. Additionally, we have generated anatase (A(001), A(101)) and rutile (R(100), R(110)) surface morphologies and 7­atom copper cluster complexes with those planes. To examine the possible influence of TiO2 on the adsorption properties of our active metal, Cu7, we have carried out adsorption studies with CH3OH. Our final data and observations predict that the Cu7 cluster adopts a symmetric pentagonal bipyramidal geometry with D5h symmetry. We find that the anatase morphology has a greater overall stability than rutile. The adsorption strength of the Cu7 cluster has been predicted in this study to be according to the following order: A(001) > A(101)> R(110). Indeed, the R(100) surface appears to be an unfavorable surface for metal cluster binding. Our data indicates that copper cluster stabilization on the metal-oxide surface depends on the nature of the crystal face. Again, we studied the adsorption properties of methanol on nascent Cu7 cluster, Cu7-TiO 2 complex and on pure TiO2-surface in A(001) polymorphic form. The calculations revealed that methanol

  19. Trends in the exchange current for hydrogen evolution

    DEFF Research Database (Denmark)

    Nørskov, Jens Kehlet; Bligaard, Thomas; Logadottir, Ashildur

    2005-01-01

    A density functional theory database of hydrogen chemisorption energies on close packed surfaces of a number of transition and noble metals is presented. The bond energies are used to understand the trends in the exchange current for hydrogen evolution. A volcano curve is obtained when measured...... exchange currents are plotted as a function of the calculated hydrogen adsorption energies and a simple kinetic model is developed to understand the origin of the volcano. The volcano curve is also consistent with Pt being the most efficient electrocatalyst for hydrogen evolution. (c) 2005...

  20. Hydrogen generation utilizing integrated CO2 removal with steam reforming

    Science.gov (United States)

    Duraiswamy, Kandaswamy; Chellappa, Anand S

    2013-07-23

    A steam reformer may comprise fluid inlet and outlet connections and have a substantially cylindrical geometry divided into reforming segments and reforming compartments extending longitudinally within the reformer, each being in fluid communication. With the fluid inlets and outlets. Further, methods for generating hydrogen may comprise steam reformation and material adsorption in one operation followed by regeneration of adsorbers in another operation. Cathode off-gas from a fuel cell may be used to regenerate and sweep the adsorbers, and the operations may cycle among a plurality of adsorption enhanced reformers to provide a continuous flow of hydrogen.

  1. Calcium decorated and doped phosphorene for gas adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Lalitha, Murugan; Nataraj, Yuvarani; Lakshmipathi, Senthilkumar, E-mail: lsenthilkumar@buc.edu.in

    2016-07-30

    Highlights: • Phosphorene exhibits n-type/p-type nature on decorating/doping calcium respectively. • Gas molecules (CH{sub 4}, CO{sub 2}, H{sub 2} and NH{sub 3}) are physisorbed on phosphorene. • Ca decorated Phosphorene is recommended for high density hydrogen storage applications. • Calcium doping on zigzag and armchair sites makes phosphorene more reactive. • CH{sub 4}, CO{sub 2}, H{sub 2} prefer Ca-doped on zigzag1 site, whereas ammonia prefers Ca-doped on armchair. - Abstract: In this paper, we present the results from first-principles study based on the electronic structure and adsorption characteristics of CH{sub 4}, CO{sub 2}, H{sub 2} and NH{sub 3} adsorbed on Ca decorated/doped phosphorene. Our study finds that phosphorene exhibits n-type behaviour on decorating calcium, and p-type on doping calcium. Gas molecules are physisorbed on both pristine and calcium-mediated phosphorene, visible through their lower binding energy and charge transfer values. Ca decorated phosphorene is suitable for hydrogen storage due to its higher binding energy for H{sub 2}. Ca doped structures shows increased binding affinity towards CH{sub 4} and NH{sub 3} in zigzag1 direction and armchair directions respectively. The extracts of our study implies that Ca doped phosphorene possess increased binding affinity towards gas molecules, and the results are highly helpful for gas adsorption and to design gas sensors based on calcium doped or decorated phosphorene.

  2. Sc-Decorated Porous Graphene for High-Capacity Hydrogen Storage: First-Principles Calculations

    Directory of Open Access Journals (Sweden)

    Yuhong Chen

    2017-08-01

    Full Text Available The generalized gradient approximation (GGA function based on density functional theory is adopted to investigate the optimized geometrical structure, electron structure and hydrogen storage performance of Sc modified porous graphene (PG. It is found that the carbon ring center is the most stable adsorbed position for a single Sc atom on PG, and the maximum number of adsorbed H2 molecules is four with the average adsorption energy of −0.429 eV/H2. By adding a second Sc atom on the other side of the system, the hydrogen storage capacity of the system can be improved effectively. Two Sc atoms located on opposite sides of the PG carbon ring center hole is the most suitable hydrogen storage structure, and the hydrogen storage capacity reach a maximum 9.09 wt % at the average adsorption energy of −0.296 eV/H2. The adsorption of H2 molecules in the PG system is mainly attributed to orbital hybridization among H, Sc, and C atoms, and Coulomb attraction between negatively charged H2 molecules and positively charged Sc atoms.

  3. Adsorption study of Ammonia Nitrogen by watermelon rind

    Science.gov (United States)

    Ibrahim, A.; Yusof, L.; Beddu, N. S.; Galasin, N.; Lee, P. Y.; Lee, R. N. S.; Zahrim, A. Y.

    2016-06-01

    The utilization of fruit waste for low-cost adsorbents as a replacement for costly conventional methods of removing ammonia nitrogen from wastewater has been reviewed. The adsorption studies were conducted as a function of contact time and adsorbent dosage and it were carried out on four different adsorbents; fresh watermelon rind and modified watermelon rind with sodium hydroxide (NaOH), potassium hydroxide (KOH) and sulphuric acid (H2SO4). Adsorbents were tested for characterization by using zeta potential test and all samples shows negative values thus makes it favourable for the adsorption process. The batch experimental result showed that adsorption process is rapid and equilibrium was established within 40 minutes of contact time. The ammonia nitrogen removal rate amounted in range of 96% to 99%, and the adsorption capacities were in range of 1.21 to 1.24 mg/g for all four different types of adsorbents used.

  4. Model studies of secondary hydrogenation in Fischer-Tropsch synthesis studied by cobalt catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Aaserud, Christian

    2003-07-01

    of propene hydrogenation (g/g{sub Co(surface)}, h) increased with increasing surface area of the alumina support. Promoting the cobalt catalyst with rhenium increased the cobalt dispersion, but it did not affect the rate of propene hydrogenation. CO hydrogenation on the same alumina supported catalysts at FT conditions (210 {sup o}C, 20 bar and H{sub 2}/CO = 2.1) has shown that the C{sub 5+} selectivity increased with decreasing surface area of the alumina support. Decreased importance of hydrogenation of olefins will result in increased selectivity of C{sub 5+} due to increased probability for readsorption and further chain growth of olefins. Decreased propene hydrogenation on catalysts with low surface area fits very well with increased C{sub 5+} selectivity in FT synthesis for these catalysts. The effect of water on the activity for propene hydrogenation on the same catalysts as used for the propene hydrogenation study has also been studied in a fixed bed microreactor at 120 {sup o}C, 1.8 bar, H{sub 2}/C{sub 3}H{sub 6} = 6 and H{sub 2}O/H{sub 2} = 0.8. Cobalt FT catalysts on various alumina supports, on silica support, on titania support and also unsupported cobalt catalysts were all decreasing their activity for propene hydrogenation sharply when water was added to the feed. Inhibition of propene hydrogenation during water addition was reversible for all catalysts. Reversibility of the propene hydrogenation activity indicates that no deactivation of the catalyst occurred during water addition. It is suggested that the decreased activity of propene hydrogenation during water addition is due to competitive adsorption of water on the cobalt surface. Decreased importance of secondary hydrogenation of olefins will result in an improved selectivity of C{sub 5} and higher hydrocarbons. By adding water during FT synthesis it has been observed that the C{sub 5+} selectivity increased. Improved C{sub 5+} selectivity is therefore in line with the observed inhibition of

  5. Synthesis and Thermodynamic Studies of Physisorptive Energy Storage Materials

    Science.gov (United States)

    Stadie, Nicholas

    Physical adsorption of hydrogen or other chemical fuels on the surface of carbonaceous materials offers a promising avenue for energy storage applications. The addition of a well-chosen sorbent material to a compressed gas tank increases the volumetric energy density of the system while still permitting fast refueling, simplicity of design, complete reversibility, high cyclability, and low overall cost of materials. While physical adsorption is most effective at temperatures below ambient, effective storage technologies are possible at room temperature and modestly high pressure. A volumetric Sieverts apparatus was designed, constructed, and commissioned to accurately measure adsorption uptake at high pressures and an appropriate thermodynamic treatment of the experimental data is presented. In Chapter 1, the problem of energy storage is introduced in the context of hydrogen as an ideal alternative fuel for future mobile vehicle applications, and with methane in mind as a near-term solution. The theory of physical adsorption that is relevant to this work is covered in Chapter 2. In-depth studies of two classes of materials are presented in the final chapters. Chapter 3 presents a study of the dissociative "hydrogen spillover" effect in the context of its viability as a practical hydrogen storage solution at room temperature. Chapters 4-5 deal with zeolite-templated carbon, an extremely high surface-area material which shows promise for hydrogen and methane storage applications. Studies of hydrogen adsorption at high pressure (Chapter 4) and anomalous thermodynamic properties of methane adsorption (Chapter 5) on ZTCs are presented. The concluding chapter discusses the impact of and possible future directions for this work.

  6. Adsorptive removal of Auramine-O: Kinetic and equilibrium study

    International Nuclear Information System (INIS)

    Mall, Indra Deo; Srivastava, Vimal Chandra; Agarwal, Nitin Kumar

    2007-01-01

    Present study deals with the adsorption of Auramine-O (AO) dye by bagasse fly ash (BFA) and activated carbon-commercial grade (ACC) and laboratory grade (ACL). BFA is a solid waste obtained from the particulate collection equipment attached to the flue gas line of the bagasse fired boilers of cane sugar mills. Batch studies were performed to evaluate the influences of various experimental parameters like initial pH (pH 0 ), contact time, adsorbent dose and initial concentration (C 0 ) for the removal of AO. Optimum conditions for AO removal were found to be pH 0 ∼ 7.0 and equilibrium time ∼30 min for BFA and ∼120 min for activated carbons. Optimum BFA, ACC and ACL dosages were found to be 1, 20 and 2 g/l, respectively. Adsorption of AO followed pseudo-second order kinetics with the initial sorption rate for adsorption on BFA being the highest followed by those on ACL and ACC. The sorption process was found to be controlled by both film and pore diffusion with film diffusion at the earlier stages followed by pore diffusion at the later stages. Equilibrium isotherms for the adsorption of AO on BFA, ACC and ACL were analyzed by Freundlich, Langmuir, Dubinin-Radushkevich, and Temkin isotherm equations using linear correlation coefficient. Langmuir isotherm gave the best correlation of adsorption for all the adsorbents studied. Thermodynamic study showed that adsorption of AO on ACC (with a more negative Gibbs free energy value) is more favoured. BFA which was used without any pretreatment showed high surface area, pore volume and pore size exhibiting its potential to be used as an adsorbent for the removal of AO

  7. Molecular structure-adsorption study on current textile dyes.

    Science.gov (United States)

    Örücü, E; Tugcu, G; Saçan, M T

    2014-01-01

    This study was performed to investigate the adsorption of a diverse set of textile dyes onto granulated activated carbon (GAC). The adsorption experiments were carried out in a batch system. The Langmuir and Freundlich isotherm models were applied to experimental data and the isotherm constants were calculated for 33 anthraquinone and azo dyes. The adsorption equilibrium data fitted more adequately to the Langmuir isotherm model than the Freundlich isotherm model. Added to a qualitative analysis of experimental results, multiple linear regression (MLR), support vector regression (SVR) and back propagation neural network (BPNN) methods were used to develop quantitative structure-property relationship (QSPR) models with the novel adsorption data. The data were divided randomly into training and test sets. The predictive ability of all models was evaluated using the test set. Descriptors were selected with a genetic algorithm (GA) using QSARINS software. Results related to QSPR models on the adsorption capacity of GAC showed that molecular structure of dyes was represented by ionization potential based on two-dimensional topological distances, chromophoric features and a property filter index. Comparison of the performance of the models demonstrated the superiority of the BPNN over GA-MLR and SVR models.

  8. Hydrogen isotope in erbium oxide: Adsorption, penetration, diffusion, and vacancy trapping

    International Nuclear Information System (INIS)

    Mao, Wei; Chikada, Takumi; Suzuki, Akihiro; Terai, Takayuki; Matsuzaki, Hiroyuki

    2015-01-01

    Highlights: • H adsorption on cubic Er 2 O 3 surface results in electron transfer from H to the surface. • The H penetration energy of at least 1.6 eV is required for cubic Er 2 O 3 surface. • The dominated mechanisms of H diffusion in bulk Er 2 O 3 are elucidated. • H diffusion near or at vacancies in Er 2 O 3 is an exothermic reaction. - Abstract: In this study, we report results using first-principles density functional theory calculations for four critical aspects of the interaction: H adsorption on Er 2 O 3 surface, surface-to-subsurface penetration of H into Er 2 O 3 , bulk diffusion of H in Er 2 O 3 , and trapping of H at vacancies. We identify surface stable adsorption positions and find that H prefers to transfer electrons to the surfaces and form covalent bonds with the nearest neighboring four oxygen atoms. For low surface coverage of H as in our case (0.89 × 10 14 H/cm 2 ), a penetration energy of at least 1.60 eV is required for cubic Er 2 O 3 surfaces. Further, the H diffusion barrier between the planes defined by Er 2 O 3 units along the favorable <1 1 1> direction is found to be very small – 0.16 eV – whereas higher barriers of 0.41 eV and 1.64 eV are required for diffusion across the planes, somewhat higher than the diffusion energy barrier of 0.20 eV observed experimentally at 873 K. In addition, we predict that interstitial H is exothermically trapped when it approaches a vacancy with the vacancy defect behaving as an electron trap since the H-vacancy defect is found to be more stable than the intrinsic defect

  9. Effects of an electron beam on adsorption and desorption of ammonia on ruthenium (0001)

    International Nuclear Information System (INIS)

    Danielson, L.R.; Dresser, M.J.; Donaldson, E.E.; Sandstrom, D.R.

    1978-01-01

    The effects of an electron beam on ammonia adsorption and desorption on Ru(0001) have been investigated by Auger electron spectroscopy, low-energy electron diffraction, and thermal flash desorption. Appreciable adsorption at room temperature occurred only on the area of the Ru crystal which had been bombarded by an electron beam during dosing. The adsorption rate was a function of beam current density and ammonia pressure, and an apparent (2x2) diffraction pattern appeared in the area bombarded by the electron beam. Electron bombardment of the molecular γ states of ammonia followed by flash desorption showed that less ammonia and more hydrogen and nitrogen were desorbed as the bombardment time increased. An analysis of this process based on electron-induced dissociation of the ammonia molecule yielded an effective initial dissociation cross section of 3x10 -6 cm 2 . Hydrogen flash desorption spectra after bombardment of the γ states obeying first order kinetics with desorption energies of 0.78 and 1.0 eV. Electron bombardment of the γ states for short times produced the same effects on the ammonia flash desorption spectra as preadsorption of hydrogen. (Auth.)

  10. Study of neon adsorption on carbon nanocones using molecular dynamics simulation

    International Nuclear Information System (INIS)

    Majidi, R.; Ghafoori Tabrizi, K.

    2010-01-01

    We have used molecular dynamics simulation to study Ne adsorption on carbon nanocones. Adsorption isotherms were obtained at several temperatures between 22.67 and 49.82 K. Adsorption coverage, isosteric heat, and binding energy were calculated. Adsorption was observed both inside and outside of an individual carbon nanocone. The results indicate that the saturation coverage and saturation pressure depend on temperature. At saturation conditions, the maximum values of interior and exterior coverages are 0.17 and 0.39 neon per carbon, respectively. The results are compared to Ne adsorption on open-ended single-walled carbon nanotubes. It is found that adsorption coverages on carbon nanocones are greater than those on carbon nanotubes. The isosteric heat and binding energy of neon adsorption on nanocones indicate that nanocones and nanotubes have highly desirable characteristics as an adsorbent.

  11. Study of neon adsorption on carbon nanocones using molecular dynamics simulation

    Energy Technology Data Exchange (ETDEWEB)

    Majidi, R. [Department of Physics, Shahid Beheshti University, G.C., Evin, Tehran 19839-63113 (Iran, Islamic Republic of); Ghafoori Tabrizi, K., E-mail: k-tabrizi@sbu.ac.i [Department of Physics, Shahid Beheshti University, G.C., Evin, Tehran 19839-63113 (Iran, Islamic Republic of)

    2010-04-15

    We have used molecular dynamics simulation to study Ne adsorption on carbon nanocones. Adsorption isotherms were obtained at several temperatures between 22.67 and 49.82 K. Adsorption coverage, isosteric heat, and binding energy were calculated. Adsorption was observed both inside and outside of an individual carbon nanocone. The results indicate that the saturation coverage and saturation pressure depend on temperature. At saturation conditions, the maximum values of interior and exterior coverages are 0.17 and 0.39 neon per carbon, respectively. The results are compared to Ne adsorption on open-ended single-walled carbon nanotubes. It is found that adsorption coverages on carbon nanocones are greater than those on carbon nanotubes. The isosteric heat and binding energy of neon adsorption on nanocones indicate that nanocones and nanotubes have highly desirable characteristics as an adsorbent.

  12. Adsorption of metal adatoms on single-layer phosphorene.

    Science.gov (United States)

    Kulish, Vadym V; Malyi, Oleksandr I; Persson, Clas; Wu, Ping

    2015-01-14

    Single- or few-layer phosphorene is a novel two-dimensional direct-bandgap nanomaterial. Based on first-principles calculations, we present a systematic study on the binding energy, geometry, magnetic moment and electronic structure of 20 different adatoms adsorbed on phosphorene. The adatoms cover a wide range of valences, including s and p valence metals, 3d transition metals, noble metals, semiconductors, hydrogen and oxygen. We find that adsorbed adatoms produce a rich diversity of structural, electronic and magnetic properties. Our work demonstrates that phosphorene forms strong bonds with all studied adatoms while still preserving its structural integrity. The adsorption energies of adatoms on phosphorene are more than twice higher than on graphene, while the largest distortions of phosphorene are only ∼0.1-0.2 Å. The charge carrier type in phosphorene can be widely tuned by adatom adsorption. The unique combination of high reactivity with good structural stability is very promising for potential applications of phosphorene.

  13. Adsorption studies of iron(III)

    Indian Academy of Sciences (India)

    Adsorption of ferric ions by chitin was studied by the batch equilibration method. The influence of particle size and dosage of the adsorbant, contact time, initial concentration of the adsorbate and temperature were experimentally verified. The effect of anions like chloride, nitrate and sulphate and also of cations like zinc, ...

  14. Adsorption properties of CO, H{sub 2} and CH{sub 4} over Pd/γ-Al{sub 2}O{sub 3} catalyst: A density functional study

    Energy Technology Data Exchange (ETDEWEB)

    Song, Zijian; Wang, Ben, E-mail: benwang@hust.edu.cn; Yu, Jie; Ma, Chuan; Qu, Qinggong; Zeng, Zhao; Xiang, Jun; Hu, Song; Sun, Lushi, E-mail: sunlushi@hust.edu.cn

    2016-11-30

    Highlights: • Model of dimer Pd supported on γ-Al{sub 2}O{sub 3} (1 1 0) surface was established. • CO, H{sub 2} and CH{sub 4} adsorption on clean γ-Al{sub 2}O{sub 3} and on Pd/γ-Al{sub 2}O{sub 3} surface was studied by DFT calculations. • CO, H{sub 2} and CH{sub 4} adsorptions are energetically more favorable in the presence of dimer Pd. • Mechanism of CO, H{sub 2} and CH{sub 4} adsorption on Pd/γ-Al{sub 2}O{sub 3} (1 1 0) surface was explained. - Abstract: Density functional theory (DFT) calculations were employed to investigate the adsorption characteristics of carbon monoxide (CO), hydrogen (H{sub 2}), and methane (CH{sub 4}) on the surface of clean γ-Al{sub 2}O{sub 3} and Pd supported γ-Al{sub 2}O{sub 3}, which is of significant for catalytic combustion. The adsorption intensities of the three gas molecules in pure γ-Al{sub 2}O{sub 3} (1 1 0) and Pd/γ-Al{sub 2}O{sub 3} (1 1 0) were in the order of CO > H{sub 2} > CH{sub 4}. The corresponding adsorption energies on the Pd/γ-Al{sub 2}O{sub 3} (1 1 0) surface were at least three times higher than those on γ-Al{sub 2}O{sub 3} (1 1 0). Anlysis of Mulliken population and partial density of states (PDOS) showed that the adsorption mechanisms were as follow: (a) CO stably adsorbed on the bridge site of dimer Pd with two C−Pd bonds because of charges transfer from the surface to CO, and the triple bond (C≡O) was broken to a double bond (C=O); (b) H{sub 2} was dissociated into hydrogen atoms on the dimer Pd and produced a stable planar configuration; and (c) the tetrahedral structure of CH{sub 4} was destroyed on the surface and formed a −CH{sub 3} species bonded to the Pd atom, which contributes to the orbital hybridization between C and Pd atoms.

  15. A density functional theory study of the TMG adsorption on the GaN surface

    Energy Technology Data Exchange (ETDEWEB)

    Ptasinska, Maria; Soltys, Jakub; Piechota, Jacek [Interdisciplinary Centre for Materials Modelling, University of Warsaw, ul. Pawinskiego 5a, 02-106 Warszawa (Poland); Krukowski, Stanislaw [Interdisciplinary Centre for Materials Modelling, University of Warsaw, ul. Pawinskiego 5a, 02-106 Warszawa (Poland); Institute of High Pressure Physics, Polish Academy of Sciences, ul. Sokolowska 29/37, 01-142 Warsaw (Poland)

    2011-07-01

    TMG (trimetylogallium) and NH{sub 3} (ammonia) are widely used reactants in the metal organic chemical vapor deposition (MOCVD) technique used in the growth of the GaN thin films. We have recently examined theoretically, with the help of the density functional theory (DFT), TMG adsorption on the GaN(0001) surface in order to study formation of bonds between Ga and N. Dangling bonds on the GaN(0001) surface were saturated with the hydrogen atoms. The slab polarization, which is due to the dangling bonds present on the GaN(0001) surface, and energy of the system in the vicinity of TMG was computed for different distances between the surface atoms and TMG. We also studied TMG diffusion on the GaN surface. As a result, the energy path for diffusion from Top N to Hollow was obtained.

  16. Kinetics and the mass transfer mechanism of hydrogen sulfide removal by biochar derived from rice hull.

    Science.gov (United States)

    Shang, Guofeng; Liu, Liang; Chen, Ping; Shen, Guoqing; Li, Qiwu

    2016-05-01

    The biochar derived from rice hull was evaluated for its abilities to remove hydrogen sulfide (H2S) from gas phase. The surface area and pH of the biochar were compared. The biochar derived from rice hull was evaluated for its abilities to remove hydrogen sulfide (H2S) from gas phase. The surface area and pH of the biochar were compared. The different pyrolysis temperature has great influence on the adsorption of H2S. At the different pyrolysis temperature, the H2S removal efficiency of rice hull-derived biochar was different. The adsorption capacities of biochar were 2.09 mg·g(-1), 2.65 mg·g(-1), 16.30 mg·g(-1), 20.80 mg·g(-1), and 382.70 mg·g(-1), which their pyrolysis temperatures were 100 °C, 200 °C, 300 °C, 400 °C and 500 °C respectively. Based on the Yoon-Nelson model, it analyzed the mass transfer mechanism of hydrogen sulfide adsorption by biochar. The paper focuses on the biochar derived from rice hull-removed hydrogen sulfide (H2S) from gas phase. The surface area and pH of the biochar were compared. The different pyrolysis temperatures have great influence on the adsorption of H2S. At the different pyrolysis temperatures, the H2S removal efficiency of rice hull-derived biohar was different. The adsorption capacities of biochar were 2.09, 2.65, 16.30, 20.80, and 382.70 mg·g(-1), and their pyrolysis temperatures were 100, 200, 300, 400, and 500 °C, respectively. Based on the Yoon-Nelson model, the mass transfer mechanism of hydrogen sulfide adsorption by biochar was analyzed.

  17. Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces

    DEFF Research Database (Denmark)

    Abild-Pedersen, Frank; Greeley, Jeffrey Philip; Studt, Felix

    2007-01-01

    Density functional theory calculations are presented for CHx, x=0,1,2,3, NHx, x=0,1,2, OHx, x=0,1, and SHx, x=0,1 adsorption on a range of close-packed and stepped transition-metal surfaces. We find that the adsorption energy of any of the molecules considered scales approximately with the adsorp...

  18. Experimental study of adsorption chiller driven by variable heat source

    Energy Technology Data Exchange (ETDEWEB)

    Wang, D.C.; Wang, Y.J.; Zhang, J.P.; Tian, X.L. [College of Electromechanical Engineering, Qingdao University, Qingdao 266071 (China); Wu, J.Y. [Institute of Refrigeration and Cryogenics, Shanghai Jiao Tong University, Shanghai 200030 (China)

    2008-05-15

    A silica gel-water adsorption chiller has been developed in recent years and has been applied in an air conditioning system driven by solar energy. The heat source used to drive the adsorption chiller is variable at any moment because the solar radiation intensity or the waste heat from engines varies frequently. An adsorption cooling system may be badly impacted by a variable heat source with temperature variations in a large range. In this work, a silica gel-water adsorption chiller driven by a variable heat source is experimentally studied. The influences of the variable heat source on the performance of the chiller are analyzed, especially for a continuous temperature increase process and a continuous temperature decrease process of the heat source. As an example, the dynamic characteristics of the heat source are also analyzed when solar energy is taken as the heat source of the adsorption chiller. According to the experimental results for the adsorption chiller and the characteristics of the heat source from solar energy, control strategies of the adsorption chiller driven by solar energy are proposed. (author)

  19. Experimental study of adsorption chiller driven by variable heat source

    International Nuclear Information System (INIS)

    Wang, D.C.; Wang, Y.J.; Zhang, J.P.; Tian, X.L.; Wu, J.Y.

    2008-01-01

    A silica gel-water adsorption chiller has been developed in recent years and has been applied in an air conditioning system driven by solar energy. The heat source used to drive the adsorption chiller is variable at any moment because the solar radiation intensity or the waste heat from engines varies frequently. An adsorption cooling system may be badly impacted by a variable heat source with temperature variations in a large range. In this work, a silica gel-water adsorption chiller driven by a variable heat source is experimentally studied. The influences of the variable heat source on the performance of the chiller are analyzed, especially for a continuous temperature increase process and a continuous temperature decrease process of the heat source. As an example, the dynamic characteristics of the heat source are also analyzed when solar energy is taken as the heat source of the adsorption chiller. According to the experimental results for the adsorption chiller and the characteristics of the heat source from solar energy, control strategies of the adsorption chiller driven by solar energy are proposed

  20. Modeling of hydrogen desorption from tungsten surface

    Energy Technology Data Exchange (ETDEWEB)

    Guterl, J., E-mail: jguterl@ucsd.edu [University of California, San Diego, La Jolla, CA 92093 (United States); Smirnov, R.D. [University of California, San Diego, La Jolla, CA 92093 (United States); Krasheninnikov, S.I. [University of California, San Diego, La Jolla, CA 92093 (United States); Nuclear Research National University MEPhI, Moscow 115409 (Russian Federation); Uberuaga, B.; Voter, A.F.; Perez, D. [Los Alamos National Laboratory, Los Alamos, NM 8754 (United States)

    2015-08-15

    Hydrogen retention in metallic plasma-facing components is among key-issues for future fusion devices. For tungsten, which has been chosen as divertor material in ITER, hydrogen desorption parameters experimentally measured for fusion-related conditions show large discrepancies. In this paper, we therefore investigate hydrogen recombination and desorption on tungsten surfaces using molecular dynamics simulations and accelerated molecular dynamics simulations to analyze adsorption states, diffusion, hydrogen recombination into molecules, and clustering of hydrogen on tungsten surfaces. The quality of tungsten hydrogen interatomic potential is discussed in the light of MD simulations results, showing that three body interactions in current interatomic potential do not allow to reproduce hydrogen molecular recombination and desorption. Effects of surface hydrogen clustering on hydrogen desorption are analyzed by introducing a kinetic model describing the competition between surface diffusion, clustering and recombination. Different desorption regimes are identified and reproduce some aspects of desorption regimes experimentally observed.

  1. Correlation between the Microstructure of Porous Materials and the Adsorption Properties of H2 and D2

    International Nuclear Information System (INIS)

    Krkljus, Ivana Biljana

    2011-01-01

    One of the most challenging tasks toward the full implementation of the hydrogen based economy is the reversible storage of hydrogen for portable applications. Three main approaches have been investigated to store the hydrogen, storage as a compressed gas or a liquid, or through a direct chemical bond between the hydrogen atom and the material. The alternative approach, the most recently investigated, is the storage of hydrogen at cryogenic conditions. Storage by physisorption within porous adsorbents has particular advantages of complete reversibility, the fast refueling time, the low heat evolution, and above all increased safety. The nature of interaction of hydrogen, deuterium, and gas mixtures with porous adsorbents was exploited by performing thermal desorption spectroscopy (TDS) measurements. This sensitive experimental technique gives qualitative information about the different adsorption sites, which show different desorption temperatures depending on the interaction energy. After an appropriate calibration the amount of gas desorbed may be quantified. To gain a more fundamental insight into the available adsorption sites multiple TDS spectra were recorded, corresponding to different surface coverages (in the pressure range of 1 to 700 mbar), and different heating regimes. Different kind of porous adsorbents, conventional carbon-based materials and novel Metal Organic Framework Materials (MOFs), were used to investigate the hydrogen/deuterium physisorption mechanism. For carbon materials an increase in the hydrogen interaction potential was observed for adsorbents with narrow pore size. The confined geometry, where hydrogen simultaneously interacts with all the surrounding adsorbent walls, strengthens the interaction potential with the adsorbate molecule, thus, maximizing the total van der Waals force on the adsorbate. Crystalline MOFs are a new class of porous materials assembled from discrete metal centers, which act as framework nodes, and organic

  2. Adsorption of surfactants and polymers at interfaces

    Science.gov (United States)

    Rojas, Orlando Jose

    Surface tension and high-resolution laser light scattering experiments were used to investigate the adsorption of isomeric sugar-based surfactants at the air/liquid interface in terms of surfactant surface packing and rheology. Soluble monolayers of submicellar surfactant solutions exhibited a relatively viscous behavior. It was also proved that light scattering of high-frequency thermally-induced capillary waves can be utilized to study surfactant exchange between the surface and the bulk solution. Such analysis revealed the existence of a diffusional relaxation mechanism. A procedure based on XPS was developed for quantification, on an absolute basis, of polymer adsorption on mica and Langmuir-Blodgett cellulose films. The adsorption of cationic polyelectrolytes on negatively-charged solid surfaces was highly dependent on the polymer ionicity. It was found that the adsorption process is driven by electrostatic mechanisms. Charge overcompensation (or charge reversal) of mica occurred after adsorption of polyelectrolytes of ca. 50% charge density, or higher. It was demonstrated that low-charge-density polyelectrolytes adsorb on solid surfaces with an extended configuration dominated by loops and tails. In this case the extent of adsorption is limited by steric constraints. The conformation of the polyelectrolyte in the adsorbed layer is dramatically affected by the presence of salts or surfactants in aqueous solution. The phenomena which occur upon increasing the ionic strength are consistent with the screening of the electrostatic attraction between polyelectrolyte segments and solid surface. This situation leads to polyelectrolyte desorption accompanied by both an increase in the layer thickness and the range of the steric force. Adsorbed polyelectrolytes and oppositely charged surfactants readily associate at the solid/liquid interface. Such association induces polyelectrolyte desorption at a surfactant concentration which depends on the polyelectrolyte charge

  3. Membrane adsorption and binding, cellular uptake and cytotoxicity of cell-penetrating peptidomimetics with α-peptide/β-peptoid backbone

    DEFF Research Database (Denmark)

    Jing, Xiaona; Yang, Mingjun; Kasimova, Marina Robertovna

    2012-01-01

    to evaluate the effect of α-chirality in the β-peptoid residues and the presence of guanidinium groups in the α-amino acid residues on membrane interaction. The molecular properties of the peptidomimetics in solution (surface and intramolecular hydrogen bonding, aqueous diffusion rate and molecular size) were...... studied along with their adsorption to lipid bilayers, cellular uptake, and toxicity. The surface hydrogen bonding ability of the peptidomimetics reflected their adsorbed amounts onto lipid bilayers as well as with their cellular uptake, indicating the importance of hydrogen bonding for their membrane...

  4. Low-cost metal oxide activated carbon prepared and modified by microwave heating method for hydrogen storage

    Energy Technology Data Exchange (ETDEWEB)

    Moradi, S. E. [Islamic Azad University, Sari (Iran, Islamic Republic of)

    2014-09-15

    Novel microporous activated carbon (MAC) with high surface area and pore volume has been synthesized by microwave heating. Iron oxide nanoparticles were loaded into MAC by using Fe(NO{sub 3}){sub 3}·9H{sub 2}O followed by microwave irradiation for up to five minutes. The surface modified microporous activated carbon was characterized by BET, XRD, SEM and thermogravimetric examinations. Adsorption data of H{sub 2} on the unmodified and modified MACs were collected with PCT method for a pressure range up to 120 bar at 303 K. Greater hydrogen adsorption was observed on the carbon adsorbents doped with 1.45 wt% of iron oxide nanoparticle loaded due to the joint properties of hydrogen adsorption on the carbon surface and the spill-over of hydrogen molecules into carbon structures.

  5. Multi-level computational chemistry study on hydrogen recombination catalyst of off-gas treatment system

    International Nuclear Information System (INIS)

    Hatakeyama, Nozomu; Ise, Mariko; Inaba, Kenji

    2011-01-01

    In order to reveal the deactivation mechanism of the hydrogen recombination catalyst of off-gas treatment system, we investigate by using multi-level computational chemistry simulation methods. The recombiner apparatus is modeled by the numerical mesh system in the axial coordinates, and unsteady, advection and reaction rate equations are solved by using a finite difference method. The chemical reactions are formulated to represent adsorption-desorption of hydrogen and oxygen on Pt catalyst, and time developments of the coverage factors of Pt are solved numerically. The computational simulations successfully reproduce the very similar behaviors observed by experiments, such as increasing of the inversion rates of H 2 to H 2 O, the temperatures distributions along the flow direction, dependencies of experimental condition, and so on. Thus Pt poisoning is considered to cause the deactivation of the hydrogen recombination catalyst. To clarify the poisoning mechanism, the molecular level simulation is applied to the system of Pt on boehmite attacked by a cyclic siloxane which has been detected by experiments and considered as one of poisoning spices. The simulation shows ring-opening reaction of the cyclic siloxane on Pt, then attachment of two ends of the chain-like siloxane to Pt and boehmite, respectively, and that finally the recombination reaction is prevented. This may be the first study to find out the detailed dynamical mechanism of hydrogen recombination catalyst poisoning with cyclic siloxane. (author)

  6. Theoretical study of adsorption of lithium atom on carbon nanotube

    Directory of Open Access Journals (Sweden)

    Masato Senami

    2011-12-01

    Full Text Available We investigate the adsorption of lithium atoms on the surface of the (12,0 single wall carbon nanotube (SWCNT by using ab initio quantum chemical calculations. The adsorption of one lithium atom on the inside of this SWCNT is favored compared to the outside. We check this feature by charge transfer and regional chemical potential density. The adsorption of multiple lithium atoms on the interior of the SWCNT is studied in terms of adsorption energy and charge transfer. We show that repulsive force between lithium atoms destabilizes a system for the large number of lithium atoms.

  7. Surface charge effects in protein adsorption on nanodiamonds.

    Science.gov (United States)

    Aramesh, M; Shimoni, O; Ostrikov, K; Prawer, S; Cervenka, J

    2015-03-19

    Understanding the interaction of proteins with charged diamond nanoparticles is of fundamental importance for diverse biomedical applications. Here we present a thorough study of protein binding, adsorption kinetics and structure on strongly positively (hydrogen-terminated) and negatively (oxygen-terminated) charged nanodiamond particles using a quartz crystal microbalance by dissipation and infrared spectroscopy. By using two model proteins (bovine serum albumin and lysozyme) of different properties (charge, molecular weight and rigidity), the main driving mechanism responsible for the protein binding to the charged nanoparticles was identified. Electrostatic interactions were found to dominate the protein adsorption dynamics, attachment and conformation. We developed a simple electrostatic model that can qualitatively explain the observed adsorption behaviour based on charge-induced pH modifications near the charged nanoparticle surfaces. Under neutral conditions, the local pH around the positively and negatively charged nanodiamonds becomes very high (11-12) and low (1-3) respectively, which has a profound impact on the protein charge, hydration and affinity to the nanodiamonds. Small proteins (lysozyme) were found to form multilayers with significant conformational changes to screen the surface charge, while larger proteins (albumin) formed monolayers with minor conformational changes. The findings of this study provide a step forward toward understanding and eventually predicting nanoparticle interactions with biofluids.

  8. Feasibility study on the application of a heat-pipe type adsorption chiller

    Energy Technology Data Exchange (ETDEWEB)

    Ahn, Sang Hyeok; Chung, Jae Dong [Dept. of Mechanical Engineering, Sejong University, Seoul (Korea, Republic of); Kwon, Oh Kyung [Energy System R and D Group, Korea Institute of Industrial Technology, Cheonan (Korea, Republic of)

    2017-01-15

    A parametric study on a heat-pipe type adsorption chiller with SWS-1L (mesoporous silica gel impregnated with CaCl{sub 2}) and water pair was conducted using a numerical method in this research. A heat pipe that is in direct contact with the adsorbent is applied to the adsorption chiller to improve the heat transfer capacity of the adsorption bed. A feasibility study was performed on the heat-pipe type adsorption bed with a single layer. The Coefficient of performance (COP) and the Specific cooling power (SCP) were 0.231 and 844.8 W/kg, respectively. These values are lower than the system performance values of the existing fin-tube type adsorption bed. However, when the number of bed layers was increased to seven, the COP and SCP of the heat-pipe type adsorption bed were 0.520 and 752.4 W/kg, respectively. These values are 5.25 % and 39.8 % higher than the COP and SCP, respectively, of the fin-tube type adsorption bed. These findings indicate that the heat-pipe type adsorption bed can potentially address the disadvantage caused by the system size of the adsorption chiller. A parametric study was also conducted for six design parameters, namely, number of layers, heat pipe pitch, heat pipe radius, fin width, fin spacing, and hot water temperature.

  9. Feasibility study on the application of a heat-pipe type adsorption chiller

    International Nuclear Information System (INIS)

    Ahn, Sang Hyeok; Chung, Jae Dong; Kwon, Oh Kyung

    2017-01-01

    A parametric study on a heat-pipe type adsorption chiller with SWS-1L (mesoporous silica gel impregnated with CaCl_2) and water pair was conducted using a numerical method in this research. A heat pipe that is in direct contact with the adsorbent is applied to the adsorption chiller to improve the heat transfer capacity of the adsorption bed. A feasibility study was performed on the heat-pipe type adsorption bed with a single layer. The Coefficient of performance (COP) and the Specific cooling power (SCP) were 0.231 and 844.8 W/kg, respectively. These values are lower than the system performance values of the existing fin-tube type adsorption bed. However, when the number of bed layers was increased to seven, the COP and SCP of the heat-pipe type adsorption bed were 0.520 and 752.4 W/kg, respectively. These values are 5.25 % and 39.8 % higher than the COP and SCP, respectively, of the fin-tube type adsorption bed. These findings indicate that the heat-pipe type adsorption bed can potentially address the disadvantage caused by the system size of the adsorption chiller. A parametric study was also conducted for six design parameters, namely, number of layers, heat pipe pitch, heat pipe radius, fin width, fin spacing, and hot water temperature

  10. Effect of Li Adsorption on the Electronic and Hydrogen Storage Properties of Acenes: A Dispersion-Corrected TAO-DFT Study

    Science.gov (United States)

    Seenithurai, Sonai; Chai, Jeng-Da

    2016-01-01

    Due to the presence of strong static correlation effects and noncovalent interactions, accurate prediction of the electronic and hydrogen storage properties of Li-adsorbed acenes with n linearly fused benzene rings (n = 3–8) has been very challenging for conventional electronic structure methods. To meet the challenge, we study these properties using our recently developed thermally-assisted-occupation density functional theory (TAO-DFT) with dispersion corrections. In contrast to pure acenes, the binding energies of H2 molecules on Li-adsorbed acenes are in the ideal binding energy range (about 20 to 40 kJ/mol per H2). Besides, the H2 gravimetric storage capacities of Li-adsorbed acenes are in the range of 9.9 to 10.7 wt%, satisfying the United States Department of Energy (USDOE) ultimate target of 7.5 wt%. On the basis of our results, Li-adsorbed acenes can be high-capacity hydrogen storage materials for reversible hydrogen uptake and release at ambient conditions. PMID:27609626

  11. Hydrogen production from hydrocarbons

    Energy Technology Data Exchange (ETDEWEB)

    Docekal, J

    1986-01-01

    Hydrogen is an important feed stock for chemical and petroleum industries, in addition to being considered as the energy carrier of the future. At the present time the feed stock hydrogen is mainly manufactured from hydrocarbons using steam reforming. In steam reforming two processes are employed, the conventional process and PSA (pressure swing adsorption) process. These two processes are described and compared. The results show that the total costs and the maintenance costs are lower for the PSA process, the capital outlay is lower for the conventional process, and the operating costs are similar for the two processes.

  12. Adsorption of diuron and dichlobenil on multiwalled carbon nanotubes as affected by lead.

    Science.gov (United States)

    Chen, Guang-Cai; Shan, Xiao-Quan; Pei, Zhi-Guo; Wang, Huanhua; Zheng, Li-Rong; Zhang, Jing; Xie, Ya-Ning

    2011-04-15

    The effect of lead on the adsorption of diuron and dichlobenil on multiwalled carbon nanotubes (MWCNTs) was investigated to explore the possible application of MWCNTs for removal of both herbicides from contaminated water. The adsorption of diuron and dichlobenil on MWCNTs at pH 6 was nonlinear and fit the Polanyi-Manes model well. The adsorption of diuron and dichlobenil was closely correlated with specific surface areas and micropore volumes of MWCNTs. An increase in oxygen content of MWCNTs with same diameters and similar surface areas decreased the adsorption of diuron and dichlobenil, while increased the adsorption of lead. Micro-Fourier transform infrared spectroscopic study indicated that hydrogen bonding is a main mechanism responsible for the adsorption of diuron or dichlobenil onto MWCNTs-O. Oxygen containing groups, mainly carboxylic groups, significantly increased the adsorption of lead through the formations of outer-sphere and inner-sphere complexes, which are verified by X-ray absorption spectroscopic measurements. Oxygen containing groups and the presence of lead diminished the adsorption of diuron and dichlobenil. The suppression mechanisms of lead were ascribed to hydration and complexation of lead with carboxylic groups, which may occupy part of surface of MWCNTs-O. The large hydration shell of lead cations may intrude or shield hydrophobic and hydrophilic sites, resulting in a decreased adsorption of diuron and dichlobenil at the lead-complexed moieties. Copyright © 2011 Elsevier B.V. All rights reserved.

  13. Substituent effects in heterogeneous catalysis--5. The steric hindrance of bulky alkyl substituents in cyclohexanone hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Chihara, T; Tanaka, K

    1979-02-01

    The steric hindrance of bulky alkyl substituents in cyclohexanone hydrogenation was demonstrated by the reactivities of 2-isopropyl and 2-tert.-butyl cyclohexanone relative to cyclohexanone in individual and competitive hydrogenation at 30/sup 0/C over alumina-supported ruthenium, rhodium, and platinum catalysts. The results indicate that the ketone adsorption onto the catalyst is sterically hindered by the alkyl substitution significantly more than the surface reaction which follows the adsorption.

  14. Adsorption mechanism of alkyl polyglucoside (APG) on calcite nanoparticles in aqueous medium at varying pH

    Science.gov (United States)

    Suh, Seokjin; Choi, Kyeong-Ok; Yang, Seung-Chul; Kim, Yeong Eun; Ko, Sanghoon

    2017-07-01

    In this study, adsorption mechanism of alkyl polyglucoside (APG) on calcium carbonate (CaCO3) nanoparticles (CCNPs) in aqueous medium at varying pH was identified. An initial adsorption of APG on CCNP surface seemed to be occurred due to the van der Waals force. An initial surface charge influenced determination of a major driving force, which resulted in hydrogen bonds (pH 7) and the hydrophobic interaction (pH 10) as a main sources of adsorption of APG on the CCNP surface. Even if the initial surface charge of CCNPs had little effect on a quantitative adsorption of APG on CCNPs, eventually, it influence on the definitive adsorption structure between APG and CCNPs and improvement of dispersion stability of CCNPs in water. In conclusion, it was revealed that 0.39% APG aqueous solution was most appropriate to improve the dispersion stability of CCNPs, which is postulated to be used effectively in food and pharmaceutical fields.

  15. Adsorption of Xyloglucan onto Cellulose Surfaces of Different Morphologies: An Entropy-Driven Process.

    Science.gov (United States)

    Benselfelt, Tobias; Cranston, Emily D; Ondaral, Sedat; Johansson, Erik; Brumer, Harry; Rutland, Mark W; Wågberg, Lars

    2016-09-12

    The temperature-dependence of xyloglucan (XG) adsorption onto smooth cellulose model films regenerated from N-methylmorpholine N-oxide (NMMO) was investigated using surface plasmon resonance spectroscopy, and it was found that the adsorbed amount increased with increasing temperature. This implies that the adsorption of XG to NMMO-regenerated cellulose is endothermic and supports the hypothesis that the adsorption of XG onto cellulose is an entropy-driven process. We suggest that XG adsorption is mainly driven by the release of water molecules from the highly hydrated cellulose surfaces and from the XG molecules, rather than through hydrogen bonding and van der Waals forces as previously suggested. To test this hypothesis, the adsorption of XG onto cellulose was studied using cellulose films with different morphologies prepared from cellulose nanocrystals (CNC), semicrystalline NMMO-regenerated cellulose, and amorphous cellulose regenerated from lithium chloride/dimethylacetamide. The total amount of high molecular weight xyloglucan (XGHMW) adsorbed was studied by quartz crystal microbalance and reflectometry measurements, and it was found that the adsorption was greatest on the amorphous cellulose followed by the CNC and NMMO-regenerated cellulose films. There was a significant correlation between the cellulose dry film thickness and the adsorbed XG amount, indicating that XG penetrated into the films. There was also a correlation between the swelling of the films and the adsorbed amounts and conformation of XG, which further strengthened the conclusion that the water content and the subsequent release of the water upon adsorption are important components of the adsorption process.

  16. Process, including PSA and membrane separation, for separating hydrogen from hydrocarbons

    Science.gov (United States)

    Baker, Richard W.; Lokhandwala, Kaaeid A.; He, Zhenjie; Pinnau, Ingo

    2001-01-01

    An improved process for separating hydrogen from hydrocarbons. The process includes a pressure swing adsorption step, a compression/cooling step and a membrane separation step. The membrane step relies on achieving a methane/hydrogen selectivity of at least about 2.5 under the conditions of the process.

  17. Preparation, microstructure and hydrogen sorption properties of nanoporous carbon aerogels under ambient drying

    Science.gov (United States)

    Tian, H. Y.; Buckley, C. E.; Mulè, S.; Paskevicius, M.; Dhal, B. B.

    2008-11-01

    Organic aerogels are prepared by the sol-gel method from polymerization of resorcinol with furfural. These aerogels are further carbonized in nitrogen in order to obtain their corresponding carbon aerogels (CA); a sample which was carbonized at 900 °C was also activated in a carbon dioxide atmosphere at 900 °C. The chemical reaction mechanism and optimum synthesis conditions are investigated by means of Fourier transform infrared spectroscopy and thermoanalyses (thermogravimetric/differential thermal analyses) with a focus on the sol-gel process. The carbon aerogels were investigated with respect to their microstructures, using small angle x-ray scattering (SAXS), transmission electron microscopy (TEM) and nitrogen adsorption measurements at 77 K. SAXS studies showed that micropores with a radius of gyration of adsorption showed that larger mesopores were also present. Hydrogen storage properties of the CA were also investigated. An activated sample with a Brunauer-Emmett-Teller surface area of 1539 ± 20 m2 g-1 displayed a reasonably high hydrogen uptake at 77 K with a maximum hydrogen sorption of 3.6 wt% at 2.5 MPa. These results suggest that CA are promising candidate hydrogen storage materials.

  18. Water structure and aqueous uranyl(VI) adsorption equilibria onto external surfaces of beidellite, montmorillonite, and pyrophyllite: results from molecular simulations.

    Science.gov (United States)

    Greathouse, Jeffery A; Cygan, Randall T

    2006-06-15

    Molecular dynamics simulations were performed to provide a systematic study of aqueous uranyl adsorption onto the external surface of 2:1 dioctahedral clays. Our understanding of this key process is critical in predicting the fate of radioactive contaminants in natural groundwaters. These simulations provide atomistic detail to help explain experimental trends in uranyl adsorption onto natural media containing smectite clays. Aqueous uranyl concentrations ranged from 0.027 to 0.162 M. Sodium ions and carbonate ions (0.027-0.243 M) were also present in the aqueous regions to more faithfully model a stream of uranyl-containing groundwater contacting a mineral system comprised of Na-smectite. No adsorption occurred near the pyrophyllite surface, and there was little difference in uranyl adsorption onto the beidellite and montmorillonite, despite the difference in location of clay layer charge between the two. At low uranyl concentration, the pentaaquouranyl complex dominates in solution and readily adsorbs to the clay basal plane. At higher uranyl (and carbonate) concentrations, the mono(carbonato) complex forms in solution, and uranyl adsorption decreases. Sodium adsorption onto beidellite occurred both as inner- and outer-sphere surface complexes, again with little effect on uranyl adsorption. Uranyl surface complexes consisted primarily of the pentaaquo cation (85%) and to a lesser extent the mono(carbonato) species (15%). Speciation diagrams of the aqueous region indicate that the mono(carbonato)uranyl complex is abundant at high ionic strength. Oligomeric uranyl complexes are observed at high ionic strength, particularly near the pyrophyllite and montmorillonite surfaces. Atomic density profiles of water oxygen and hydrogen atoms are nearly identical near the beidellite and montmorillonite surfaces. Water structure therefore appears to be governed by the presence of adsorbed ions and not by the location of layer charge associated with the substrate. The water

  19. Phosphate adsorption from wastewater using zirconium (IV) hydroxide: Kinetics, thermodynamics and membrane filtration adsorption hybrid system studies.

    Science.gov (United States)

    Johir, M A H; Pradhan, M; Loganathan, P; Kandasamy, J; Vigneswaran, S

    2016-02-01

    Excessive phosphate in wastewater should be removed to control eutrophication of water bodies. The potential of employing amorphous zirconium (Zr) hydroxide to remove phosphate from synthetic wastewater was studied in batch adsorption experiments and in a submerged membrane filtration adsorption hybrid (MFAH) reactor. The adsorption data satisfactorily fitted to Langmuir, pseudo-first order and pseudo-second order models. Langmuir adsorption maxima at 22 °C and pHs of 4.0, 7.1, and 10.0 were 30.40, 18.50, and 19.60 mg P/g, respectively. At pH 7.1 and temperatures of 40 °C and 60 °C, they were 43.80 and 54.60 mg P/g, respectively. The thermodynamic parameters, ΔG° and ΔS° were negative and ΔH° was positive. FTIR, zeta potential and competitive phosphate, sulphate and nitrate adsorption data showed that the mechanism of phosphate adsorption was inner-sphere complexation. In the submerged MFAH reactor experiment, when Zr hydroxide was added at doses of 1-5 g/L once only at the start of the experiment, the removal of phosphate from 3 L of wastewater containing 10 mg P/L declined after 5 h of operation. However, when Zr hydroxide was repeatedly added at 5 g/L dose every 24 h, satisfactory removal of phosphate was maintained for 3 days. Copyright © 2015 Elsevier Ltd. All rights reserved.

  20. Sum Frequency Generation Vibrational Spectroscopy and Kinetic Study of 2-Methylfuran and 2,5-Dimethylfuran Hydrogenation over 7 nm Platinum Cubic Nanoparticles

    KAUST Repository

    Aliaga, Cesar

    2011-04-28

    Sum frequency generation vibrational spectroscopy and kinetic measurements obtained from gas chromatography were used to study the adsorption and hydrogenation of 2-methylfuran (MF) and 2,5-dimethylfuran (DMF) over cubic Pt nanoparticles of 7 nm average size, synthesized by colloidal methods and cleaned by ultraviolet light and ozone treatment. Reactions carried out at atmospheric pressure in the temperature range of 20-120 °C produced dihydro and tetrahydro species, as well as ring-opening products (alcohols) and ring-cracking products, showing high selectivity toward ring opening throughout the entire temperature range. The aromatic rings (MF and DMF) adsorbed parallel to the nanoparticle surface. Results yield insight into various surface reaction intermediates and the reason for the significantly lower selectivity for ring cracking in DMF hydrogenation compared to MF hydrogenation. © 2011 American Chemical Society.

  1. Pore size distribution and supercritical hydrogen adsorption in activated carbon fibers

    Science.gov (United States)

    Purewal, J. J.; Kabbour, H.; Vajo, J. J.; Ahn, C. C.; Fultz, B.

    2009-05-01

    Pore size distributions (PSD) and supercritical H2 isotherms have been measured for two activated carbon fiber (ACF) samples. The surface area and the PSD both depend on the degree of activation to which the ACF has been exposed. The low-surface-area ACF has a narrow PSD centered at 0.5 nm, while the high-surface-area ACF has a broad distribution of pore widths between 0.5 and 2 nm. The H2 adsorption enthalpy in the zero-coverage limit depends on the relative abundance of the smallest pores relative to the larger pores. Measurements of the H2 isosteric adsorption enthalpy indicate the presence of energy heterogeneity in both ACF samples. Additional measurements on a microporous, coconut-derived activated carbon are presented for reference.

  2. Pore size distribution and supercritical hydrogen adsorption in activated carbon fibers

    International Nuclear Information System (INIS)

    Purewal, J J; Kabbour, H; Ahn, C C; Fultz, B; Vajo, J J

    2009-01-01

    Pore size distributions (PSD) and supercritical H 2 isotherms have been measured for two activated carbon fiber (ACF) samples. The surface area and the PSD both depend on the degree of activation to which the ACF has been exposed. The low-surface-area ACF has a narrow PSD centered at 0.5 nm, while the high-surface-area ACF has a broad distribution of pore widths between 0.5 and 2 nm. The H 2 adsorption enthalpy in the zero-coverage limit depends on the relative abundance of the smallest pores relative to the larger pores. Measurements of the H 2 isosteric adsorption enthalpy indicate the presence of energy heterogeneity in both ACF samples. Additional measurements on a microporous, coconut-derived activated carbon are presented for reference.

  3. Dynamics of dissociative adsorption of hydrogen on Ni(100)

    International Nuclear Information System (INIS)

    Hamza, A.V.; Madix, R.J.

    1985-01-01

    Nearly monoenergetic beams of hydrogen and deuterium were used to determine dissociative sticking probabilities for H 2 and D 2 on Ni(100) at various energies. Variation of the surface temperature between 90 and 300 K had no effect on the dissociative sticking probability of H 2 at 3.6 and 5.8 kJ/mol incident beam energy, indicating a direct mechanism of dissociation. A four fold increase in the initial dissociative sticking probability for H 2 from 0.2 to 0.8 was observed by increasing the translational kinetic energy from 0.7 to 7.0 kJ/mol. The initial dissociative sticking probability for D 2 was slightly lower, increasing from 0.15 to 0.75 with increasing translational kinetic energy from 1.3 to 10.5 kJ/mol. The form of the increase with kinetic energy was explained by tunnelling through a low activation barrier, accounting as well for the high dissociation probability at low kinetic energies. The dissociative sticking probability decreased with hydrogen or deuterium adatom coverage at all energies. The decline in sticking probability with hydrogen coverage was fit to a s(theta) = s 0 (1 - a theta)/sup n/ functional form. From this relationship it was deduced that hydrogen adatoms block only single sites and that four vacant sites are needed for dissociation. The dissociative sticking probability for H 2 declined precipitously from 0.77 to 0.16 with oxygen adatom coverage from 0 to 5% of a monolayer at a translational energy of 9.6 kJ.mol. 36 references, 8 figures

  4. Solid-State Gas Adsorption Studies with Discrete Palladium(II) [Pd2 (L)4 ]4+ Cages.

    Science.gov (United States)

    Preston, Dan; White, Keith F; Lewis, James E M; Vasdev, Roan A S; Abrahams, Brendan F; Crowley, James D

    2017-08-04

    The need for effective CO 2 capture systems remains high, and due to their tunability, metallosupramolecular architectures are an attractive option for gas sorption. While the use of extended metal organic frameworks for gas adsorption has been extensively explored, the exploitation of discrete metallocage architectures to bind gases remains in its infancy. Herein the solid state gas adsorption properties of a series of [Pd 2 (L) 4 ] 4+ lantern shaped coordination cages (L = variants of 2,6-bis(pyridin-3-ylethynyl)pyridine), which had solvent accessible internal cavities suitable for gas binding, have been investigated. The cages showed little interaction with dinitrogen gas but were able to take up CO 2 . The best performing cage reversibly sorbed 1.4 mol CO 2 per mol cage at 298 K, and 2.3 mol CO 2 per mol cage at 258 K (1 bar). The enthalpy of binding was calculated to be 25-35 kJ mol -1 , across the number of equivalents bound, while DFT calculations on the CO 2 binding in the cage gave ΔE for the cage-CO 2 interaction of 23-28 kJ mol -1 , across the same range. DFT modelling suggested that the binding mode is a hydrogen bond between the carbonyl oxygen of CO 2 and the internally directed hydrogen atoms of the cage. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  5. Evaluation of the Characteristics of the Adsorption of Fibrinogen ...

    African Journals Online (AJOL)

    ... with calcium and magnesium ions increased the amount of fibrinogen adsorbed onto it as against treatment with potassium ion (a monovalent ion). Electrostatic attraction on the surface of the treated HAP and hydrogen are responsible for the adsorption. The results are useful in fabricating bone and teeth implants that are ...

  6. Acetate and phosphate anion adsorption linear sweep voltammograms simulated using density functional theory

    KAUST Repository

    Savizi, Iman Shahidi Pour

    2011-04-01

    Specific adsorption of anions to electrode surfaces may alter the rates of electrocatalytic reactions. Density functional theory (DFT) methods are used to predict the adsorption free energy of acetate and phosphate anions as a function of Pt(1 1 1) electrode potential. Four models of the electrode potential are used including a simple vacuum slab model, an applied electric field model with and without the inclusion of a solvating water bi-layer, and the double reference model. The linear sweep voltammogram (LSV) due to anion adsorption is simulated using the DFT results. The inclusion of solvation at the electrochemical interface is necessary for accurately predicting the adsorption peak position. The Langmuir model is sufficient for predicting the adsorption peak shape, indicating coverage effects are minor in altering the LSV for acetate and phosphate adsorption. Anion adsorption peak positions are determined for solution phase anion concentrations present in microbial fuel cells and microbial electrolysis cells and discussion is provided as to the impact of anion adsorption on oxygen reduction and hydrogen evolution reaction rates in these devices. © 2011 Elsevier Ltd. All rights reserved.

  7. Kinetic and Thermodynamic Studies on Adsorption of Sulphate from ...

    African Journals Online (AJOL)

    DELL USER

    22, No. 1, 2017. 39. Kinetic and Thermodynamic Studies on Adsorption of Sulphate from Aqueous Solution by. Magnetite ... poison catalysts, and affect the .... C for 1 h in a stainless steel reactor placed in a furnace ... N2 gas for 30 min. 50 ml of ...... adsorption for designing and evaluating the ... is the equilibrium liquid-phase.

  8. Carbon nanotube materials for hydrogen storage

    Energy Technology Data Exchange (ETDEWEB)

    Dillon, A.C.; Parilla, P.A.; Jones, K.M.; Riker, G.; Heben, M.J. [National Renewable Energy Lab., Golden, CO (United States)

    1998-08-01

    Carbon single-wall nanotubes (SWNTs) are essentially elongated pores of molecular dimensions and are capable of adsorbing hydrogen at relatively high temperatures and low pressures. This behavior is unique to these materials and indicates that SWNTs are the ideal building block for constructing safe, efficient, and high energy density adsorbents for hydrogen storage applications. In past work the authors developed methods for preparing and opening SWNTs, discovered the unique adsorption properties of these new materials, confirmed that hydrogen is stabilized by physical rather than chemical interactions, measured the strength of interaction to be {approximately} 5 times higher than for adsorption on planar graphite, and performed infrared absorption spectroscopy to determine the chemical nature of the surface terminations before, during, and after oxidation. This year the authors have made significant advances in synthesis and characterization of SWNT materials so that they can now prepare gram quantities of high-purity SWNT samples and measure and control the diameter distribution of the tubes by varying key parameters during synthesis. They have also developed methods which purify nanotubes and cut nanotubes into shorter segments. These capabilities provide a means for opening the tubes which were unreactive to the oxidation methods that successfully opened tubes, and offer a path towards organizing nanotube segments to enable high volumetric hydrogen storage densities. They also performed temperature programmed desorption spectroscopy on high purity carbon nanotube material obtained from collaborator Prof. Patrick Bernier and finished construction of a high precision Seivert`s apparatus which will allow the hydrogen pressure-temperature-composition phase diagrams to be evaluated for SWNT materials.

  9. Materials for Hydrogen Storage in Nanocavities: Design criteria

    Energy Technology Data Exchange (ETDEWEB)

    Reguera, E. [Centro de Investigacion en Ciencia Aplicada y Tecnologia Avanzada del IPN, Unidad Legaria, Legaria 694, Col. Irrigacion (Mexico)

    2009-11-15

    The adsorption potential for a given adsorbate depends of both, material surface and adsorbate properties. In this contribution the possible guest-host interactions for H{sub 2} within a cavity or on a surface are discussed considering the molecule physical properties. Five different interactions contribute to the adsorption forces for this molecule: 1) quadrupole moment interaction with the local electric field gradient; 1) electron cloud polarization by a charge center; 3) dispersive forces (van der Waals); 4) quadrupole moment versus quadrupole moment between neighboring H{sub 2} molecules, and, 5) H{sub 2} coordination to a metal center. The relative importance of these five interactions for the hydrogen storage in nanocavities is discussed from experimental evidences in order to extract materials design criteria for molecular hydrogen storage. (author)

  10. Hydrogen isotope in erbium oxide: Adsorption, penetration, diffusion, and vacancy trapping

    Energy Technology Data Exchange (ETDEWEB)

    Mao, Wei, E-mail: mao@nuclear.jp [Department of Nuclear Engineering and Management, School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656 (Japan); The University Museum, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-0032 (Japan); Chikada, Takumi [Department of Chemistry, Graduate School of Science, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka 422-8529 (Japan); Suzuki, Akihiro [Nuclear Professional School, School of Engineering, The University of Tokyo, 2-22, Shirakata-shirane, Tokai, Naka 319-1188, Ibaraki (Japan); Terai, Takayuki [Department of Nuclear Engineering and Management, School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-8656 (Japan); Matsuzaki, Hiroyuki [The University Museum, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo 113-0032 (Japan)

    2015-03-15

    Highlights: • H adsorption on cubic Er{sub 2}O{sub 3} surface results in electron transfer from H to the surface. • The H penetration energy of at least 1.6 eV is required for cubic Er{sub 2}O{sub 3} surface. • The dominated mechanisms of H diffusion in bulk Er{sub 2}O{sub 3} are elucidated. • H diffusion near or at vacancies in Er{sub 2}O{sub 3} is an exothermic reaction. - Abstract: In this study, we report results using first-principles density functional theory calculations for four critical aspects of the interaction: H adsorption on Er{sub 2}O{sub 3} surface, surface-to-subsurface penetration of H into Er{sub 2}O{sub 3}, bulk diffusion of H in Er{sub 2}O{sub 3}, and trapping of H at vacancies. We identify surface stable adsorption positions and find that H prefers to transfer electrons to the surfaces and form covalent bonds with the nearest neighboring four oxygen atoms. For low surface coverage of H as in our case (0.89 × 10{sup 14} H/cm{sup 2}), a penetration energy of at least 1.60 eV is required for cubic Er{sub 2}O{sub 3} surfaces. Further, the H diffusion barrier between the planes defined by Er{sub 2}O{sub 3} units along the favorable <1 1 1> direction is found to be very small – 0.16 eV – whereas higher barriers of 0.41 eV and 1.64 eV are required for diffusion across the planes, somewhat higher than the diffusion energy barrier of 0.20 eV observed experimentally at 873 K. In addition, we predict that interstitial H is exothermically trapped when it approaches a vacancy with the vacancy defect behaving as an electron trap since the H-vacancy defect is found to be more stable than the intrinsic defect.

  11. Excellent performance of copper based metal organic framework in adsorptive removal of toxic sulfonamide antibiotics from wastewater.

    Science.gov (United States)

    Azhar, Muhammad Rizwan; Abid, Hussein Rasool; Sun, Hongqi; Periasamy, Vijay; Tadé, Moses O; Wang, Shaobin

    2016-09-15

    The increasing concerns on toxicity of sulfonamide antibiotics in water require a prompt action to establish efficient wastewater treatment processes for their removal. In this study, adsorptive removal of a model sulfonamide antibiotic, sulfachloropyridazine (SCP), from wastewater is presented for the first time using a metal organic framework (MOF). A high surface area and thermally stable MOF, HKUST-1, was synthesized by a facile method. Batch adsorption studies were systematically carried out using HKUST-1. The high surface area and unsaturated metal sites resulted in a significant adsorption capacity with faster kinetics. Most of the SCP was removed in 15min and the kinetic data were best fitted with the pseudo second order model. Moreover, isothermal data were best fitted with the Langmuir model. The thermodynamic results showed that the adsorption is a spontaneous and endothermic process. The adsorption capacity of HKUST-1 is 384mg/g at 298K which is the highest compared to most of the materials for the antibiotics. The high adsorption capacity is attributed mainly to π-π stacking, hydrogen bonding and electrostatic interactions. Copyright © 2016 Elsevier Inc. All rights reserved.

  12. Adsorption characteristics of water vapor on ferroaluminophosphate for desalination cycle

    KAUST Repository

    Kim, Youngdeuk

    2014-07-01

    The adsorption characteristics of microporous ferroaluminophosphate adsorbent (FAM-Z01, Mitsubishi Plastics) are evaluated for possible application in adsorption desalination and cooling (AD) cycles. A particular interest is its water vapor uptake behavior at assorted adsorption temperatures and pressures whilst comparing them to the commercial silica gels of AD plants. The surface characteristics are first carried out using N2 gas adsorption followed by the water vapor uptake analysis for temperature ranging from 20°C to 80°C. We propose a hybrid isotherm model, composing of the Henry and the Sips isotherms, which can be integrated to satisfactorily fit the experimental data of water adsorption on the FAM-Z01. The hybrid model is selected to fit the unusual isotherm shapes, that is, a low adsorption in the initial section and followed by a rapid vapor uptake leading to a likely micropore volume filling by hydrogen bonding and cooperative interaction in micropores. It is shown that the equilibrium adsorption capacity of FAM-Z01 can be up to 5 folds higher than that of conventional silica gels. Owing to the quantum increase in the adsorbate uptake, the FAM-Z01 has the potential to significantly reduce the footprint of an existing AD plant for the same output capacity. © 2014 Elsevier B.V.

  13. First-principles calculation of adsorption of shale gas on CaCO3 (100) surfaces.

    Science.gov (United States)

    Luo, Qiang; Pan, Yikun; Guo, Ping; Wang, Zhouhua; Wei, Na; Sun, Pengfei; Liu, Yuxiao

    2017-06-16

    To demonstrate the adsorption strength of shale gas to calcium carbonate in shale matrix, the adsorption of shale gas on CaCO3 (100) surfaces was studied using the first-principles method, which is based on the density functional theory (DFT). The structures and electronic properties of CH4, C2H6, CO2 and N2 molecules were calculated by the generalized gradient approximation (GGA), for a coverage of 1 monolayer (ML). Under the same conditions, the density of states (DOS) of CaCO3 (100) surfaces before and after the adsorption of shale gas molecules at high-symmetry adsorption sites were compared. The results showed that the adsorption energies of CH4, C2H6, CO2 and N2 on CaCO3 (100) surfaces were between 0.2683 eV and -0.7388 eV. When a CH4 molecule was adsorbed at a hollow site and its 2 hydrogen atoms were parallel to the long diagonal (H3) on the CaCO3 (100) surface, it had the most stable adsorption, and the adsorption energy was only -0.4160 eV. The change of adsorption energy of CH4 was no more than 0.0535 eV. Compared with the DOS distribution of CH4 before adsorption, it shifted to the left overall after adsorption. At the same time, the partial density of states (PDOS) curves of CaCO3 (100) surfaces before and after adsorption basically overlapped. This work showed that the adsorption effect of shale gas on calcium carbonate is very weak, and the adsorption is physisorption at the molecular level.

  14. Study on adsorption mechanism of ammonia nitrogen in wastewater by natural heulandite

    Directory of Open Access Journals (Sweden)

    Xuekai JIN

    2018-02-01

    Full Text Available In order to explore the adsorption mechanism and optimal regeneration method of natural heulandite to high ammonia nitrogen wastewater, the natural heulandite from Hebei Province is selected as the research object. The adsorption kinetics, adsorption isotherms and adsorption thermodynamics are studied by single factor test. The results show that the adsorption process of ammonia nitrogen on heulandite with particle size range of 50~600 μm complies with the quasi-second order kinetic equation with ammonia nitrogen concentration of 500 mg/L at temperature of 25 ℃. Particle diffusion and liquid film diffusion are the dominated process of the adsorption. The adsorption capacity of heulandite is 7.81 mg/g at temperature of 45 ℃. The adsorption isotherm of ammonia nitrogen on the experimental heulandite is fitted well with Freundlich model. Gibbs free energy ΔG is calculated to be less than zero, indicating that the adsorption of ammonia nitrogen on the experimental heulandite is a spontaneous endothermic reaction. Additionally, the adsorption capacity of heulandite increases with appropriate increaseing in temperature. The optimal regeneration solvent of the saturated heulandite is 0.1 mol/L of NaCl, with which the desorption rate increases to 79%, and the times of elution and regeneration are more than 5. The results of this study can improve the economic benefits and environmental value of heulandite in the treatment of ammonia nitrogen wastewater. It can be seen that heulandite in the industrial wastewater treatment has broad prospects for application.

  15. Albumin adsorption on oxide thin films studied by spectroscopic ellipsometry

    Energy Technology Data Exchange (ETDEWEB)

    Silva-Bermudez, P., E-mail: suriel21@yahoo.com [Instituto de Investigaciones en Materiales, Universidad Nacional Autonoma de Mexico, Circuito Exterior s/n, C.U., 04510, Mexico D.F. (Mexico); Unidad de Posgrado, Facultad de Odontologia, Universidad Nacional Autonoma de Mexico, CU, 04510, Mexico D.F. (Mexico); Rodil, S.E.; Muhl, S. [Instituto de Investigaciones en Materiales, Universidad Nacional Autonoma de Mexico, Circuito Exterior s/n, C.U., 04510, Mexico D.F. (Mexico)

    2011-12-15

    Thin films of tantalum, niobium, zirconium and titanium oxides were deposited by reactive magnetron sputtering and their wettability and surface energy, optical properties, roughness, chemical composition and microstructure were characterized using contact angle measurements, spectroscopic ellipsometry, profilometry, X-ray photoelectron spectroscopy and X-ray diffraction, respectively. The purpose of the work was to correlate the surface properties of the films to the Bovine Serum Albumin (BSA) adsorption, as a first step into the development of an initial in vitro test of the films biocompatibility, based on standardized protein adsorption essays. The films were immersed into BSA solutions with different protein concentrations and protein adsorption was monitored in situ by dynamic ellipsometry; the adsorption-rate was dependent on the solution concentration and the immersion time. The overall BSA adsorption was studied in situ using spectroscopic ellipsometry and it was found to be influenced by the wettability of the films; larger BSA adsorption occurred on the more hydrophobic surface, the ZrO{sub 2} film. On the Ta{sub 2}O{sub 5}, Nb{sub 2}O{sub 5} and TiO{sub 2} films, hydrophilic surfaces, the overall BSA adsorption increased with the surface roughness or the polar component of the surface energy.

  16. Hydrogen storage property of nanoporous carbon aerogels

    International Nuclear Information System (INIS)

    Shen Jun; Liu Nianping; Ouyang Ling; Zhou Bin; Wu Guangming; Ni Xingyuan; Zhang Zhihua

    2011-01-01

    Carbon aerogels were prepared from resorcinol and formaldehyde via sol-gel process, high temperature carbonization and atmospheric pressure drying technology with solvent replacement. By changing the resorcinol-sodium carbonate molar ratio and the mass fraction of the reactants,resorcinol and formaldehyde, the pore structure of carbon aerogels can be controlled and the palladium-doped carbon aerogels were prepared.By transmission electron microscopy (TEM), X-ray diffraction (XRD) spectra, it is confirmed that the Pd exists in the skeleton structure of carbon aerogels as a form of nano simple substance pellet. The specific surface area is successfully raised by 2 times, and palladium-doped carbon aerogels with a specific surface area of 1 273 m 2 /g have been obtained by carrying out the activation process as the post-processing to the doped carbon aerogels. The hydrogen adsorption results show that the saturated hydrogen storage mass fraction of the carbon aerogels with the specific surface area of 3 212 m 2 /g is 3% in the condition of 92 K, 3.5 MPa, and 0.84% in the condition of 303 K, 3.2 MPa. In addition, the hydrogen adsorption test of palladium-doped carbon aerogels at room temperature (303 K) shows that the total hydrogen storage capacity of doped carbon aerogels is declined due to the relative small specific surface, but the hydrogen storage of unit specific surface area is enhanced. (authors)

  17. Modeling of hydrogen/deuterium dynamics and heat generation on palladium nanoparticles for hydrogen storage and solid-state nuclear fusion.

    Science.gov (United States)

    Tanabe, Katsuaki

    2016-01-01

    We modeled the dynamics of hydrogen and deuterium adsorbed on palladium nanoparticles including the heat generation induced by the chemical adsorption and desorption, as well as palladium-catalyzed reactions. Our calculations based on the proposed model reproduce the experimental time-evolution of pressure and temperature with a single set of fitting parameters for hydrogen and deuterium injection. The model we generated with a highly generalized set of formulations can be applied for any combination of a gas species and a catalytic adsorbent/absorbent. Our model can be used as a basis for future research into hydrogen storage and solid-state nuclear fusion technologies.

  18. Active Edge Sites Engineering in Nickel Cobalt Selenide Solid Solutions for Highly Efficient Hydrogen Evolution

    KAUST Repository

    Xia, Chuan; Liang, Hanfeng; Zhu, Jiajie; Schwingenschlö gl, Udo; Alshareef, Husam N.

    2017-01-01

    free energy for atomic hydrogen adsorption in NiCoSe, identified by temperature-dependent conductivities and density functional theory calculations, the authors have achieved unprecedented fast hydrogen evolution kinetics, approaching that of Pt

  19. Kinetic and equilibrium study of adsorption of di-azo dyes on commercial activated carbon

    International Nuclear Information System (INIS)

    Hyali, E.A.S.A.; Abady, T.G.A.

    2013-01-01

    This research work is concerned with studying the adsorption of a number of di-azo dyes on commercial activated carbon (CAC). The synthesized dyes vary in their structures by the central parts. which are either ortho, meta or para phenvlene diamine. This variation affects the linearity of molecules, their spatial arrangement and electron movement throughout the molecule by resonance. Factors a fleeting adsorption process, such as the efiect of contact time, initial concentration, p1-I of the adsorption medium, adsorbent dose, effect of solvent and temperature were studied. The results indicated that, the adsorption process is fast in the first 10 mm, then gradually decreased with time and approaches maximum within 70-80 min for all the studied dyes. The increase of initial concentration and temperature decreased the adsorption efficiency. The results also shows that, the adsorption is found to be more efficient at low Ph value. The increase of the adsorbent dose increases the adsorption efficiency and decreases its capacity. The variation of solvent (ethanol-water ratio) indicates that the decrease of dielectric constant lowers the adsorption efficiency. The study included application of three adsorption isotherms, Freundlich, Langmuir and Tempkin on the experimental data of the studied systems. The results indicated that, Freundlich isotherm fits better the adsorption data. Kinetic analysis of the adsorption data was also conducted by employing 4 kinetic models; pseudo first order and pseudo second order, Elovich and intra particle diffusion equations. The results obtained conclude that, the studied systems follow the Pseudo second order model. (author)

  20. Hydrogen storage in Chabazite zeolite frameworks.

    Science.gov (United States)

    Regli, Laura; Zecchina, Adriano; Vitillo, Jenny G; Cocina, Donato; Spoto, Giuseppe; Lamberti, Carlo; Lillerud, Karl P; Olsbye, Unni; Bordiga, Silvia

    2005-09-07

    We have recently highlighted that H-SSZ-13, a highly siliceous zeolite (Si/Al = 11.6) with a chabazitic framework, is the most efficient zeolitic material for hydrogen storage [A. Zecchina, S. Bordiga, J. G. Vitillo, G. Ricchiardi, C. Lamberti, G. Spoto, M. Bjørgen and K. P. Lillerud, J. Am. Chem. Soc., 2005, 127, 6361]. The aim of this new study is thus to clarify both the role played by the acidic strength and by the density of the polarizing centers hosted in the same framework topology in the increase of the adsorptive capabilities of the chabazitic materials towards H2. To achieve this goal, the volumetric experiments of H2 uptake (performed at 77 K) and the transmission IR experiment of H2 adsorption at 15 K have been performed on H-SSZ-13, H-SAPO-34 (the isostructural silico-aluminophosphate material with the same Brønsted site density) and H-CHA (the standard chabazite zeolite: Si/Al = 2.1) materials. We have found that a H2 uptake improvement has been obtained by increasing the acidic strength of the Brønsted sites (moving from H-SAPO-34 to H-SSZ-13). Conversely, the important increase of the Brønsted sites density (moving from H-SSZ-13 to H-CHA) has played a negative role. This unexpected behavior has been explained as follows. The additional Brønsted sites are in mutual interaction via H-bonds inside the small cages of the chabazitic framework and for most of them the energetic cost needed to displace the adjacent OH ligand is higher than the adsorption enthalpy of the OH...H2 adduct. From our work it can be concluded that proton exchanged chabazitic frameworks represent, among zeolites, the most efficient materials for hydrogen storage. We have shown that a proper balance between available space (volume accessible to hydrogen), high contact surface, and specific interaction with strong and isolated polarizing centers are the necessary characteristics requested to design better materials for molecular H2 storage.

  1. Adsorption and desorption study of 14C-Chloropyrifos in two Malaysian agricultural soils

    International Nuclear Information System (INIS)

    Halimah Muhammad; Nashriyah Mat; Tan Yew Ai; Ismail, B.S.

    2004-01-01

    The adsorption equilibrium time and effects of pH and concentration of 14 C-labeled chloropyrifos 0,0-diethyl 0-(3, 5, 6 tricloro-2-pyridyl)-phosphorothiote in soil were investigated. Two types of Malaysian soil under oil palm were used in this study; namely clay loam and clay soil obtained from the Sungai Sedu and Kuala Lumpur International Airport (KLIA) Estates, respectively. Equilibrium studies of chloropyrifos between the agricultural soil and the pesticide solution were conducted. Adsorption equilibrium time was achieved within 6 and 24 hours for clay loam and clay soil, respectively. It was found that chloropyrifos adsorbed by the soil samples was characterized by an initial rapid adsorption after which adsorption remained approximately constant. The percentage of 14 C-labeled chloropyrifos adsorption on soil was found to be higher in clay loam than in clay soils. Results of the study demonstrated that pH affected the adsorption of chloropyrifos on both clay loam and clay soils. The adsorption of chloropyrifos on both types of soil was higher at low pH with the adsorption reduced as the pH increased. Results also suggest that chloropyrifos sorption by soil is concentration dependent. (Author)

  2. Adsorption of H2S molecule on TiO2/Au nanocomposites: A density functional theory study

    Directory of Open Access Journals (Sweden)

    Amirali Abbasi

    2017-01-01

    Full Text Available The adsorption of hydrogen sulfide molecule on undoped and N-doped TiO2/Au nanocomposites was investigated by density functional theory (DFT calculations. The results showed that the adsorption energies of H2S on the nanocomposites follow the order of 2N doped (Ti site>N-doped (Ti site>Undoped (Ti site. The structural properties including bond lengths, angles and adsorption energies and electronic properties in view of the projected density of states (PDOSs and molecular orbitals (MOs were analyzed in detail. The results indicated that the interaction between H2S molecule and N-doped TiO2/Au nanocomposite is stronger than that between H2S and undoped nanocomposite, suggesting that N-doping helps to strengthen the interaction of H2S with TiO2/Au nanocomposite. Mulliken population analysis was conducted to analyze the charge transfer between the nanocomposite and H2S molecule. Although H2S molecule has no significant interaction with undoped nanocomposite, it tends to be strongly adsorbed on the N-doped nanocomposite. The results also suggest that the two doped nitrogen atoms in TiO2 greatly strengthen the adsorption process, being a helpful procedure to help in the design and development of improved sensor devices for H2S detection.

  3. Rapid and tunable selective adsorption of dyes using thermally oxidized nanodiamond.

    Science.gov (United States)

    Molavi, Hossein; Shojaei, Akbar; Pourghaderi, Alireza

    2018-03-27

    In the present study, capability of nanodiamond (ND) for the adsorption of anionic (methyl orange, MO) and cationic (methylene blue, MB) dyes from aqueous solution was investigated. Employing fourier transform infrared (FTIR) spectroscopy, Boehm titration method and zeta potential, it was found that the simple thermal oxidation of ND at 425 °C, increased the content of carboxylic acid of ND and accordingly the zeta potential of ND decreased considerably. Therefore, a series of oxidized NDs (OND) at various oxidation times and as-received untreated ND (UND) was used as adsorbents of MO and MB. The adsorption experiments exhibited that UND had large adsorption capacity, very fast adsorption kinetics and excellent selectivity for MO over MB. These results suggested that the adsorption tendency of UND toward anionic MO dye followed not only by electrostatic interactions but also via the chemical interaction caused by the strong hydrogen bond between the sulfonate groups of MO and the oxygen containing groups on the surface of UND. In contrast, ONDs exhibited higher adsorption capacity for cationic MB whose tendency toward MB increased by increasing the thermal oxidation time due to the promotion of the negative charge on the surface of OND leading to the higher electrostatic attraction. The adsorption rate of MB on ONDs was also very high. Kinetics data was well fitted with the pseudo- second-order model for most of the adsorbents. The adsorption selectivity analysis revealed that ONDs displayed more adsorption capacity for MB compared with MO which was also attributed to high electrostatic interactions of cationic dye with negative charges of ONDs. Finally, the release behavior of NDs was also demonstrated after soaking in ethanol and acetone. Copyright © 2018 Elsevier Inc. All rights reserved.

  4. Enhanced adsorption of hydroxyl contained/anionic dyes on non functionalized Ni@SiO{sub 2} core–shell nanoparticles: Kinetic and thermodynamic profile

    Energy Technology Data Exchange (ETDEWEB)

    Jiang, Zhifeng, E-mail: ntjiangzf@sina.com; Xie, Jimin, E-mail: xiejm391@sohu.com; Jiang, Deli, E-mail: jiangdeli100@yahoo.com; Yan, Zaoxue, E-mail: yanzaoxue@163.com; Jing, Junjie, E-mail: jingjj1975@163.com; Liu, Dong, E-mail: 919457966@qq.com

    2014-02-15

    A green and low-cost adsorbent with both magnetic property and high adsorption capacity was prepared on the basis of nickel magnetic core with silica shell. The surface of the prepared Ni@SiO{sub 2} composite was not modified. The influence of different functional groups and different charged of the dyes on the adsorption process on the non functionalized Ni@SiO{sub 2} have been studied. The results indicated that synthesized adsorbent exhibited higher adsorption capacity for dyes with negative charge/hydroxyl groups as compared to dyes with positive charge/without hydroxyl groups due to the hydrogen bonding interaction and electrostatic interaction between the adsorbent and dyes. Adsorption kinetics and isotherms experiments were carried out and the results indicated that the adsorption process was fitted by pseudo second order kinetics and Freundlich model. The binding of these dyes with magnetic adsorbent surface mainly involves physical adsorption according to D–R model. Furthermore, the adsorption process is spontaneous and endothermic as studied from adsorption thermodynamics. The value of ΔH° and mean free energy further confirmed that physical adsorption is the major adsorption process. After regeneration, the adsorbent still shows high adsorption capacity even for 4 cycles of desorption–adsorption.

  5. Equilibrium, kinetic and thermodynamic studies on the adsorption of phenol onto graphene

    Energy Technology Data Exchange (ETDEWEB)

    Li, Yanhui, E-mail: liyanhui@tsinghua.org.cn [Laboratory of Fiber Materials and Modern Textile, The Growing Base for State Key Laboratory, College of Electromechanical Engineering, Qingdao University, 308 Ningxia Road, Qingdao 266071 (China); Du, Qiuju; Liu, Tonghao; Sun, Jiankun; Jiao, Yuqin [Laboratory of Fiber Materials and Modern Textile, The Growing Base for State Key Laboratory, College of Electromechanical Engineering, Qingdao University, 308 Ningxia Road, Qingdao 266071 (China); Xia, Yanzhi, E-mail: xiayzh@qdu.edu.cn [Laboratory of Fiber Materials and Modern Textile, The Growing Base for State Key Laboratory, College of Electromechanical Engineering, Qingdao University, 308 Ningxia Road, Qingdao 266071 (China); Xia, Linhua; Wang, Zonghua [Laboratory of Fiber Materials and Modern Textile, The Growing Base for State Key Laboratory, College of Electromechanical Engineering, Qingdao University, 308 Ningxia Road, Qingdao 266071 (China); Zhang, Wei; Wang, Kunlin; Zhu, Hongwei; Wu, Dehai [Key Laboratory for Advanced Manufacturing by Material Processing Technology, Department of Mechanical Engineering, Tsinghua University, Beijing 100084 (China)

    2012-08-15

    Graphical abstract: The effect of temperature on phenol adsorbed by graphene shows that the equilibrium adsorption capacity of phenol increases with the increase in temperature from 285 to 333 K. Increasing adsorption capacities with temperature indicates that the adsorption of phenol is controlled by an endothermic reaction. Highlights: ► The graphene has high phenol adsorption capacity. ► The graphene has a high specific surface area of 305 m{sup 2}/g. ► The adsorption capacity is high at acidic pH range. ► The graphene has rapid phenol adsorption rate. ► Phenol adsorption is a spontaneous and endothermic process. -- Abstract: Graphene, a new member of carbon family, has been prepared, characterized and used as adsorbent to remove phenol from aqueous solution. The effect parameters including pH, dosage, contact time, and temperature on the adsorption properties of phenol onto graphene were investigated. The results showed that the maximum adsorption capacity can reach 28.26 mg/g at the conditions of initial phenol concentration of 50 mg/L, pH 6.3 and 285 K. Adsorption data were well described by both Freundlich and Langmuir models. The kinetic study illustrated that the adsorption of phenol onto graphene fit the pseudo second-order model. The thermodynamic parameters indicated that the adsorption of phenol onto graphene was endothermic and spontaneous.

  6. Equilibrium, kinetic and thermodynamic studies on the adsorption of phenol onto graphene

    International Nuclear Information System (INIS)

    Li, Yanhui; Du, Qiuju; Liu, Tonghao; Sun, Jiankun; Jiao, Yuqin; Xia, Yanzhi; Xia, Linhua; Wang, Zonghua; Zhang, Wei; Wang, Kunlin; Zhu, Hongwei; Wu, Dehai

    2012-01-01

    Graphical abstract: The effect of temperature on phenol adsorbed by graphene shows that the equilibrium adsorption capacity of phenol increases with the increase in temperature from 285 to 333 K. Increasing adsorption capacities with temperature indicates that the adsorption of phenol is controlled by an endothermic reaction. Highlights: ► The graphene has high phenol adsorption capacity. ► The graphene has a high specific surface area of 305 m 2 /g. ► The adsorption capacity is high at acidic pH range. ► The graphene has rapid phenol adsorption rate. ► Phenol adsorption is a spontaneous and endothermic process. -- Abstract: Graphene, a new member of carbon family, has been prepared, characterized and used as adsorbent to remove phenol from aqueous solution. The effect parameters including pH, dosage, contact time, and temperature on the adsorption properties of phenol onto graphene were investigated. The results showed that the maximum adsorption capacity can reach 28.26 mg/g at the conditions of initial phenol concentration of 50 mg/L, pH 6.3 and 285 K. Adsorption data were well described by both Freundlich and Langmuir models. The kinetic study illustrated that the adsorption of phenol onto graphene fit the pseudo second-order model. The thermodynamic parameters indicated that the adsorption of phenol onto graphene was endothermic and spontaneous.

  7. Adsorption isotherm special study. Final report

    International Nuclear Information System (INIS)

    1993-05-01

    The study was designed to identify methods to determine adsorption applicable to Uranium Mill Tailings Remedial Action (UMTRA) Project sites, and to determine how changes in aquifer conditions affect metal adsorption, resulting retardation factors, and estimated contaminant migration rates. EPA and ASTM procedures were used to estimate sediment sorption of U, As, and Mo under varying groundwater geochemical conditions. Aquifer matrix materials from three distinct locations at the DOE UMTRA Project site in Rifle, CO, were used as the adsorbents under different pH conditions; these conditions stimulated geochemical environments under the tailings, near the tailings, and downgradient from the tailings. Grain size, total surface area, bulk and clay mineralogy, and petrography of the sediments were characterized. U and Mo yielded linear isotherms, while As had nonlinear ones. U and Mo were adsorbed strongly on sediments acidified to levels similar to tailings leachate. Changes in pH had much less effect on As adsorption. Mo was adsorbed very little at pH 7-7.3, U was weakly sorbed, and As was moderately sorbed. Velocities were estimated for metal transport at different pHs. Results show that the aquifer materials must be characterized to estimate metal transport velocities in aquifers and to develop groundwater restoration strategies for the UMTRA project

  8. Hydrogen adsorption on palladium and palladium hydride at 1 bar

    DEFF Research Database (Denmark)

    Johansson, Martin; Skulason, Egill; Nielsen, Gunver

    2010-01-01

    strongly to Pd hydride than to Pd. The activation barrier for desorption at a H coverage of one mono layer is slightly lower on Pd hydride, whereas the activation energy for adsorption is similar on Pd and Pd hydride. It is concluded that the higher sticking probability on Pd hydride is most likely caused...

  9. Study on the adsorption-desorption characteristics of 14C-pirimicarb in soils

    International Nuclear Information System (INIS)

    Guo Jiangfeng; Sun Jinhe; Li Xingming

    1995-01-01

    14 C-pirimicarb was used to study its adsorption-desorption behavior in 8 kinds of soils. The results indicated that there were significant differences in its adsorption with different kinds of soil. The lowest adsorption percentage was only 13.16% and the highest one was 87.75%. The amount of adsorption in the same kind of soil increased with the concentration of pesticide, but concentration had little influence on the adsorption within the certain range of concentrations. Multiple linear regression equation was developed for prediction of adsorption and determination of the relative importance of the soil parameters. It was significant that the key factors, soil pH and clay content were negatively and positively correlated with the adsorption respectively. The adsorption equilibrium of pirimicarb in soils could be well described by both the Freundlich isotherm and the Langmuir isotherm. The adsorbed 14 C-pirimicarb could disrobe from soil and its desorption was also influenced by soil properties described by multiple linear regression equation

  10. Promoting effect of oxygen for hydrogenation of butadiene over Ni/sub 2/P catalyst

    Energy Technology Data Exchange (ETDEWEB)

    Nozaki, F.; Kitoh, T.; Sodesawa, T.

    1980-04-01

    When 0-10 mm Hg of oxygen were added to the reaction of 75 mm Hg butadiene and 225 mm Hg hydrogen over dinickel phosphide in a closed circulation system at 40/sup 0/C, increasing amounts of oxygen caused increasing lengths of induction periods followed by hydrogenation at reaction rates which had a maximum at 3 mm Hg oxygen. This maximum rate was about six times higher than the rate without oxygen addition. Adsorption, temperature-programed desorption, IR spectroscopy, and the product distribution of butadiene deuteration showed that two types of oxygen adsorbed on the dinickel phosphide catalyst; molecular oxygen on nickel, which desorbed on evacuation below 50/sup 0/C and which could be displaced by butadiene, was responsible for the induction period; molecular oxygen on phosphorus atoms, which promoted hydrogen adsorption, was responsible for the increased hydrogenation rate.

  11. Effect of water on methane adsorption on the kaolinite (0 0 1) surface based on molecular simulations

    Science.gov (United States)

    Zhang, Bin; Kang, Jianting; Kang, Tianhe

    2018-05-01

    CH4 adsorption isotherms of kaolinite with moisture contents ranging from 0 to 5 wt% water, the effects of water on maximum adsorption capacity, kaolinite swelling, and radial distribution function were modelled by the implementing combined Monte Carlo (MC) and molecular dynamics (MD) simulations at 293.15 K (20 °C) and a pressure range of 1-20 MPa. The simulation results showed that the absolute adsorption of CH4 on both dry and moist kaolinite followed a Langmuir isotherm within the simulated pressure range, and both the adsorption capacity and the rate of CH4 adsorption decreased with the water content increases. The adsorption isosteric heats of CH4 on kaolinite decreased linearly with increasing water content, indicating that at higher water contents, the interaction energy between the CH4 and kaolinite was weaker. The interaction between kaolinite and water dominates and was the main contributing factor to kaolinite clay swelling. Water molecules were preferentially adsorbed onto oxygen and hydrogen atoms in kaolinite, while methane showed a tendency to be adsorbed only onto oxygen. The simulation results of our study provide the quantitative analysis of effect of water on CH4 adsorption capacity, adsorption rate, and interaction energy from a microscopic perspective. We hope that our study will contribute to the development of strategies for the further exploration of coal bed methane and shale gas.

  12. SeO{sub 2} adsorption on CaO surface: DFT study on the adsorption of a single SeO{sub 2} molecule

    Energy Technology Data Exchange (ETDEWEB)

    Fan, Yaming; Zhuo, Yuqun; Lou, Yu; Zhu, Zhenwu [Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Thermal Engineering, Tsinghua University, Beijing 100084 (China); Li, Liangliang [Key Laboratory of Advanced Materials, Department of Material Science and Engineering, Tsinghua University, Beijing 100084 (China)

    2017-08-15

    Highlights: • Adsorption mechanisms of SeO{sub 2} on CaO surface under O{sub 2} were firstly studied by DFT. • The adsorption energies, bond length and electron density maps were calculated. • The electronic structure changes upon adsorption were studied. - Abstract: Selenium is a hazardous element in coal. During coal combustion, most of the selenium will convert to SeO{sub 2} in the flue gas. Ca-based adsorbents, especially CaO, have been considered as a potential sorbent to adsorb SeO{sub 2} due to its low cost. In this paper, the adsorption mechanisms of single SeO{sub 2} on CaO surface were investigated by density functional theory (DFT) calculation. Both the physisorption and chemisorption structures were determined. It has been identified that the adsorption of SeO{sub 2} on CaO surface is primarily chemisorption, while physisorption takes effects at the initial stage of the process. Under O{sub 2} atmosphere, selenate is hard to form. Most of the adsorption products are selenite. Additionally, the electron density maps were obtained to reveal the surface active sites. The partial density of states (PDOS) was calculated for analyzing the electronic structural change of SeO{sub 2} and CaO surface during adsorption. The results provide fundamental information of the adsorption process, which could be meaningful for the development of new absorbents.

  13. The Study of Cr3+ Adsorption Wukirsari Pumice

    International Nuclear Information System (INIS)

    Samin; Susanna TS

    2002-01-01

    As an alternative to solve an environmental problem of Cr 3+ , the use of Wukirsari pumice has been studied. Before used as an adsorbent. 100-200 mesh of Wukirsari pumice was washed and calcinate. The elements composition of adsorbent was analyzed using Atomic Adsorption Spectrophotometer (AAS) method and presented as their oxides. After calcination, the pumice was saturated by NaCI and then converted to its ceramic. The mineral composition of pumice and its ceramic was determined using XRD method. Experimental results show optimum temperature for calcination was 500 o C and 5 hours duration of contact time was found from adsorption of Na + , with the value of 505 mg/g pumice. The other results show that pH of the solution influence the adsorption. The ion exchange between Na + and Cr 3+ did not follow ideal solution, and one ion Cr 3+ could replace only one ion Na + hence optimum adsorption of Cr 3+ was 1141.47 mg/g pumice. The data XRD shows that mineral composition of the pumice was magnetite, anorthite, and montmorilonite, while composition of its ceramic was feldspar and cristobalite. (author)

  14. Improved synthesis and hydrogen storage of a microporous metal-organic framework material

    International Nuclear Information System (INIS)

    Cheng Shaojuan; Liu Shaobing; Zhao Qiang; Li Jinping

    2009-01-01

    A microporous metal-organic framework MOF-5 [Zn 4 O(BDC) 3 , BDC = 1,4-benzenedicarboxylic] was synthesized with and without H 2 O 2 by improved methods based on the previous studies. The obtained materials were characterized by X-ray diffraction, scanning electron microscopy and nitrogen adsorption, and their hydrogen storage capacities were measured. The synthesis experiments showed that H 2 O 2 favored the growth of high quality sample, large pore volume and high specific surface area. The measurements of hydrogen storage indicated that the sample with higher specific surface area and large pore volume showed better hydrogen storage behavior than other samples. It was suggested that specific surface area and pore volume influenced the capacity of hydrogen storage for MOF-5 material.

  15. Low Pressure Adsorbent for Recovery & Storage Vented Hydrogen, Phase I

    Data.gov (United States)

    National Aeronautics and Space Administration — A high performance fullerene-based adsorbent is proposed for recovery and storage hydrogen and separating helium via pressure-swing-adsorption (PSA) process....

  16. Potential of AlN nanostructures as hydrogen storage materials.

    Science.gov (United States)

    Wang, Qian; Sun, Qiang; Jena, Puru; Kawazoe, Yoshiyuki

    2009-03-24

    The capability of AlN nanostructures (nanocages, nanocones, nanotubes, and nanowires) to store hydrogen has been studied using gradient-corrected density functional theory. In contrast to bulk AlN, which has the wurtzite structure and four-fold coordination, the Al sites in AlN nanostructures are unsaturated and have two- and three-fold coordination. Each Al atom is capable of binding one H(2) molecule in quasi-molecular form, leading to 4.7 wt % hydrogen, irrespective of the topology of the nanostructures. With the exception of AlN nanotubes, energetics does not support the adsorption of additional hydrogen. The binding energies of hydrogen to these unsaturated metal sites lie in the range of 0.1-0.2 eV/H(2) and are ideal for applications under ambient thermodynamic conditions. Furthermore, these materials do not suffer from the clustering problem that often plagues metal-coated carbon nanostructures.

  17. Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700 °C.

    Science.gov (United States)

    Yang, Kun; Jiang, Yuan; Yang, Jingjing; Lin, Daohui

    2018-02-01

    Knowledge of adsorption behavior of organic contaminants on high heat temperature treated biochars is essential for application of biochars as adsorbents in wastewater treatment and soil remediation. In this study, isotherms of 25 aromatic compounds adsorption on biochars pyrolyzed at 700 °C from biomass including wood chips, rice straw, bamboo chips, cellulose, lignin and chitin were investigated to establish correlations between adsorption behavior and physicochemical properties of biochars. Isotherms were well fitted by Polanyi theory-based Dubinin-Ashtakhov (DA) model with three parameters, i.e., adsorption capacity (Q 0 ) and adsorption affinity (E and b). Besides the negative correlation of Q 0 with molecular maximum cross-sectional areas (σ) of organic compounds, positive correlations of Q 0 with total pore volume (V total ) and average diameter of micropore (D) of biochars were observed, indicating that adsorption by biochars is captured by the pore-filling mechanism with molecular sieving effect in biochar pores. Linear solvation energy relationships (LSERs) of adsorption affinity (E) with solvatochromic parameters of organic compounds (i. e., α m and π ∗ ) were established, suggesting that hydrophobic effect, π-π interaction and hydrogen-bonding interaction are the main forces responsible for adsorption. The regression coefficient (π 1 ) and intercept (C) of obtained LSERs are correlated with biochar H/C and R micro , respectively, implying that biochars with higher aromaticity and more micropores have stronger π-π bonding potential and hydrophobic effect potential with aromatic molecule, respectively. However, hydrogen-bonding potential of biochars for organic molecules is not changed significantly with properties of biochars. A negative correlation of b with biochar H/C is also obtained. These correlations could be used to predict the adsorption behavior of organic compounds on high heat temperature treated biochars from various biomass for

  18. Adsorption of saturated fatty acid in urea complexation: Kinetics and equilibrium studies

    Science.gov (United States)

    Setyawardhani, Dwi Ardiana; Sulistyo, Hary; Sediawan, Wahyudi Budi; Fahrurrozi, Mohammad

    2018-02-01

    Urea complexation is fractionation process for concentrating poly-unsaturated fatty acids (PUFAs) from vegetable oil or animal fats. For process design and optimization in commercial industries, it is necessary to provide kinetics and equilibrium data. Urea inclusion compounds (UICs) as the product is a unique complex form which one molecule (guest) is enclosed within another molecule (host). In urea complexation, the guest-host bonding exists between saturated fatty acids (SFAs) and crystalline urea. This research studied the complexation is analogous to an adsorption process. The Batch adsorption process was developed to obtain the experimental data. The ethanolic urea solution was mixed with SFA in certain compositions and adsorption times. The mixture was heated until it formed homogenous and clear solution, then it cooled very slowly until the first numerous crystal appeared. Adsorption times for the kinetic data were determined since the crystal formed. The temperature was maintained constant at room temperature. Experimental sets of data were observed with adsorption kinetics and equilibrium models. High concentration of saturated fatty acid (SFA) was used to represent adsorption kinetics and equilibrium parameters. Kinetic data were examined with pseudo first-order, pseudo second-order and intra particle diffusion models. Linier, Freundlich and Langmuir isotherm were used to study the equilibrium model of this adsorption. The experimental data showed that SFA adsorption in urea crystal followed pseudo second-order model. The compatibility of the data with Langmuir isotherm showed that urea complexation was a monolayer adsorption.

  19. Catalytic Hydrogenation and Hydrodeoxygenation of Furfural over Pt(111): A Model System for the Rational Design and Operation of Practical Biomass Conversion Catalysts.

    Science.gov (United States)

    Taylor, Martin J; Jiang, Li; Reichert, Joachim; Papageorgiou, Anthoula C; Beaumont, Simon K; Wilson, Karen; Lee, Adam F; Barth, Johannes V; Kyriakou, Georgios

    2017-04-20

    Furfural is a key bioderived platform chemical whose reactivity under hydrogen atmospheres affords diverse chemical intermediates. Here, temperature-programmed reaction spectrometry and complementary scanning tunneling microscopy (STM) are employed to investigate furfural adsorption and reactivity over a Pt(111) model catalyst. Furfural decarbonylation to furan is highly sensitive to reaction conditions, in particular, surface crowding and associated changes in the adsorption geometry: furfural adopts a planar geometry on clean Pt(111) at low coverage, tilting at higher coverage to form a densely packed furfural adlayer. This switch in adsorption geometry strongly influences product selectivity. STM reveals the formation of hydrogen-bonded networks for planar furfural, which favor decarbonylation on clean Pt(111) and hydrogenolysis in the presence of coadsorbed hydrogen. Preadsorbed hydrogen promotes furfural hydrogenation to furfuryl alcohol and its subsequent hydrogenolysis to methyl furan, while suppressing residual surface carbon. Furfural chemistry over Pt is markedly different from that over Pd, with weaker adsorption over the former affording a simpler product distribution than the latter; Pd catalyzes a wider range of chemistry, including ring-opening to form propene. Insight into the role of molecular orientation in controlling product selectivity will guide the design and operation of more selective and stable Pt catalysts for furfural hydrogenation.

  20. Polyclotrimers of 1,4-Diethynylbenzene, 2,6-Diethynylnaphthalene, and 2,6-Diethynylanthracene: Preparation and Gas Adsorption Properties

    Czech Academy of Sciences Publication Activity Database

    Zukal, Arnošt; Slováková, E.; Balcar, Hynek; Sedláček, J.

    2013-01-01

    Roč. 214, č. 18 (2013), s. 2016-2026 ISSN 1022-1352 R&D Projects: GA ČR(CZ) GAP108/11/1661; GA ČR GA203/08/0604 Institutional support: RVO:61388955 Keywords : hydrogen adsorption capacity * microporous polymers * nitrogen adsorption irreversibility Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.451, year: 2013

  1. Thin layer joining by gas adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Taga, Yasunori, E-mail: y-taga@isc.chubu.ac.jp; Fukumura, Toshio

    2014-10-01

    Highlights: • We report thin layer molecular joining between glass and COP by gas adsorption. Thickness of joining layer is 1–2 nm and joining process was carried out at low temperature at about 100 °C. • Adhesion strength measured by 180 degree peel test revealed to be 1–10 N/25 mm and the joined stack showed high durability for practical use. - Abstract: Attempt has been made to join borosilicate glass and cycloolefin (COP) polymer film by using gas adsorption method. After corona plasma treat, COP was exposed to (3-glycidoxypropyl) trimethoxysilane (GPS) and glass to (3-aminopropyl) triethoxysilane (APS) both in air atmosphere, resulting in co-adsorption of water vapor in the atmosphere and organosilane gases. Surface characterization of plasma treated and gas adsorbed surfaces was carried out by X-ray photoelectron spectroscopy (XPS) using Mg Kα X-ray source. Joining was carried out by a roll laminator after contact of both surfaces at room temperature, followed by annealing at 130 °C for 10 min. Adhesion strength was evaluated by 180 degree peel test based on ASTM D-903 and durability was examined under the conditions of 60 °C and 95% RH. It was found that after plasma treatment, complex functional groups such as C-H, C-O, C=O, O-C=O and CO{sub 3} were found on COP and O-H on glass. Thickness of GPS gas adsorption layer on COP was evaluated by the XPS to be at least 1.1 nm by taking inelastic mean free path of Si{sub 2p} photoelectron into consideration. Joining force was found to be more than 5 N/25 mm corresponding to almost equal to COP bulk tensile strength. In addition, durability of this adhesion strength remained unchanged over 2000 h even after exposure to the durability test conditions of 60 °C and 95% RH. The results can be explained in terms of formation of H-H hydrogen bonding and Si-O covalent bonding via silanols will be made at the interface as a result of lamination and annealing processes. In conclusion, ultrathin joining method

  2. Hydrogen selective NH{sub 2}-MIL-53(Al) MOF membranes with high permeability

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Feng; Zou, Xiaoqin; Gao, Xue; Fan, Songjie; Sun, Fuxing; Ren, Hao; Zhu, Guangshan [State Key Laboratory of Inorganic, Synthesis and Preparative Chemistry, Jilin University, Changchun (China)

    2012-09-11

    Hydrogen-based energy is a promising renewable and clean resource. Thus, hydrogen selective microporous membranes with high performance and high stability are demanded. Novel NH{sub 2}-MIL-53(Al) membranes are evaluated for hydrogen separation for this goal. Continuous NH{sub 2}-MIL-53(Al) membranes have been prepared successfully on macroporous glass frit discs assisted with colloidal seeds. The gas sorption ability of NH{sub 2}-MIL-53(Al) materials is studied by gas adsorption measurement. The isosteric heats of adsorption in a sequence of CO{sub 2}> N{sub 2}> CH{sub 4}{approx} H{sub 2} indicates different interactions between NH{sub 2}-MIL-53(Al) framework and these gases. As-prepared membranes are measured by single and binary gas permeation at different temperatures. The results of singe gas permeation show a decreasing permeance in an order of H{sub 2}> CH{sub 4}> N{sub 2}> CO{sub 2}, suggesting that the diffusion and adsorption properties make significant contributions in the gas permeation through the membrane. In binary gas permeation, the NH{sub 2}-MIL-53(Al) membrane shows high selectivity for H{sub 2} with separation factors of 20.7, 23.9 and 30.9 at room temperature (288 K) for H{sub 2} over CH{sub 4}, N{sub 2} and CO{sub 2}, respectively. In comparison to single gas permeation, a slightly higher separation factor is obtained due to the competitive adsorption effect between the gases in the porous MOF membrane. Additionally, the NH{sub 2}-MIL-53(Al) membrane exhibits very high permeance for H{sub 2} in the mixtures separation (above 1.5 x 10{sup -6} mol m{sup -2} s{sup -1} Pa{sup -1}) due to its large cavity, resulting in a very high separation power. The details of the temperature effect on the permeances of H{sub 2} over other gases are investigated from 288 to 353 K. The supported NH{sub 2}-MIL-53(Al) membranes with high hydrogen separation power possess high stability, resistance to cracking, temperature cycling and show high reproducibility

  3. Hydrogen production using plasma processing

    International Nuclear Information System (INIS)

    Wagner, D.; Whidden, T.K.

    2006-01-01

    Plasma processing is a promising method of extracting hydrogen from natural gas while avoiding the greenhouse gas (GHG) production typical of other methods such as steam methane reforming. This presentation describes a plasma discharge process based that, in a single reactor pass, can yield hydrogen concentrations of up to 50 % by volume in the product gas mixture. The process is free of GHG's, does not require catalysts and is easily scalable. Chemical and morphological analyses of the gaseous and solid products of the process by gas-chromatography/mass-spectrometry, microscopic Raman analyses and electron microscopy respectively are reviewed. The direct production of hydrogen-enriched natural gas (HENG) as a fuel for low pollution internal combustion engines and its purification to high-purity hydrogen (99.99%) from the product gas by pressure swing adsorption (PSA) purifier beds are reviewed. The presentation reviews potential commercial applications for the technology

  4. Study of carbon dioxide adsorption on a Cu-nitroprusside polymorph

    International Nuclear Information System (INIS)

    Roque-Malherbe, R.; Lozano, C.; Polanco, R.; Marquez, F.; Lugo, F.; Hernandez-Maldonado, A.; Primera-Pedrozo, J.N.

    2011-01-01

    A careful structural characterization was carried out to unequivocally determine the structure of the synthesized material. The TGA, DRIFTS and a Pawley fitting of the XRD powder profiles indicate that the hydrated and in situ dehydrated polymorph crystallizes in the orthorhombic space group Pnma. Meanwhile, the CO 2 isosteric heat of adsorption appears to be independent of loading with an average value of 30 kJ/mol. This translates to a physisorption type interaction, where the adsorption energy corresponding to wall and lateral interactions are mutually compensated to produce, an apparently, homogeneous adsorption energy. The somewhat high adsorption energy is probably due to the confinement of the CO 2 molecules in the nitroprusside pores. Statistical Physics and the Dubinin theory for pore volume filling allowed model the CO 2 equilibrium adsorption process in Cu-nitroprusside. A DRIFTS test for the adsorbed CO 2 displayed a peak at about 2338 cm -1 that was assigned to a contribution due to physical adsorption of the molecule. Another peak found at 2362 cm -1 evidenced that this molecule interacts with the Cu 2+ , which appears to act as an electron accepting Lewis acid site. The aim of the present paper is to report a Pnma stable Cu-nitroprusside polymorph obtained by the precipitation method that can adsorb carbon dioxide. -- Graphical abstract: The adsorption space of a very well characterized Cu-nitroprusside polymorph, applying carbon dioxide as probe molecule, was studied. Display Omitted Highlights: → Accurate information about the geometry of the adsorption space was provided. → Truthful data about the interactions within the adsorption space was presented. → The structure of the tested Cu-NP polymorph was established. → Was evidenced adsorbed CO 2 molecules in the form of weakly bonded adducts. → Is proposed that adsorbed molecules could change the Cu-NP magnetic properties.

  5. Modification of single wall carbon nanotubes (SWNT) for hydrogen storage

    Energy Technology Data Exchange (ETDEWEB)

    Rashidi, A.M.; Nouralishahi, A.; Karimi, A.; Kashefi, K. [Nanotechnology Research Center, Research Institute of petroleum industry (RIPI), Tehran (Iran); Khodadadi, A.A.; Mortazavi, Y. [Chemical engineering Department, University of Tehran, Tehran (Iran)

    2010-09-15

    Due to unique structural, mechanical and electrical properties of single wall carbon nanotubes, SWNTs, they have been proposed as promising hydrogen storage materials especially in automotive industries. This research deals with investing of CNT's and some activated carbons hydrogen storage capacity. The CNT's were prepared through natural gas decomposition at a temperature of 900 C over cobalt-molybdenum nanoparticles supported by nanoporous magnesium oxide (Co-Mo/MgO) during a chemical vapor deposition (CVD) process. The effects of purity of CNT (80-95%wt.) on hydrogen storage were investigated here. The results showed an improvement in the hydrogen adsorption capacity with increasing the purity of CNT's. Maximum adsorption capacity was 0.8%wt. in case of CNT's with 95% purity and it may be raised up with some purification to 1%wt. which was far less than the target specified by DOE (6.5%wt.). Also some activated carbons were manufactured and the results compared to CNTs. There were no considerable H{sub 2}-storage for carbon nanotubes and activated carbons at room-temperature due to insufficient binding between H{sub 2} molecules carbon nanostructures. Therefore, hydrogen must be adsorbed via interaction of atomic hydrogen with the storage environment in order to achieve DOE target, because the H atoms have a very stronger interaction with carbon nanostructures. (author)

  6. Substrate-mediated enhanced activity of Ru nanoparticles in catalytic hydrogenation of benzene

    KAUST Repository

    Liu, Xin

    2012-01-01

    The impact of carbon substrate-Ru nanoparticle interactions on benzene and hydrogen adsorption that is directly related to the performance in catalytic hydrogenation of benzene has been investigated by first-principles based calculations. The stability of Ru 13 nanoparticles is enhanced by the defective graphene substrate due to the hybridization between the dsp states of the Ru 13 particle with the sp 2 dangling bonds at the defect sites. The local curvature formed at the interface will also raise the Ru atomic diffusion barrier, and prohibit the particle sintering. The strong interfacial interaction results in the shift of averaged d-band center of the deposited Ru nanoparticle, from -1.41 eV for a freestanding Ru 13 particle, to -1.17 eV for the Ru/Graphene composites, and to -1.54 eV on mesocellular foam carbon. Accordingly, the adsorption energies of benzene are increased from -2.53 eV for the Ru/mesocellular foam carbon composites, to -2.62 eV on freestanding Ru 13 particles, to -2.74 eV on Ru/graphene composites. A similar change in hydrogen adsorption is also observed, and all these can be correlated to the shift of the d-band center of the nanoparticle. Thus, Ru nanoparticles graphene composites are expected to exhibit both high stability and superior catalytic performance in hydrogenation of arenes. © 2012 The Royal Society of Chemistry.

  7. Thermodynamics of organic molecule adsorption on sorbents modified with 5-hydroxy-6-methyluracil by inverse gas chromatography.

    Science.gov (United States)

    Gus'kov, Vladimir Yu; Gainullina, Yulia Yu; Ivanov, Sergey P; Kudasheva, Florida Kh

    2014-08-22

    The thermodynamic features of organic molecule adsorption from the gaseous phase of sorbents modified with 5-hydroxy-6-methyluracil (HMU) were studied. Molar internal energy and entropy of adsorption variation analyses showed that with every type surface, except for silica gel, layers of supramolecular structure have cavities equal in size with the ones revealed in HMU crystals by X-ray diffraction. Adsorption thermodynamics on HMU-modified sorbents depended on the amount of impregnated HMU and on the polarity, but not the porosity, of the initial sorbent. Polarity of the modified surface increased as a function of HMU quantity and initial sorbent mean pore size, but become appreciably lower if the initial surface is capable of hydrogen bonding. Copyright © 2014 Elsevier B.V. All rights reserved.

  8. Adsorption mechanisms of removing heavy metals and dyes from aqueous solution using date pits solid adsorbent

    International Nuclear Information System (INIS)

    Al-Ghouti, Mohammad A.; Li, Juiki; Salamh, Yousef; Al-Laqtah, Nasir; Walker, Gavin; Ahmad, Mohammad N.M.

    2010-01-01

    A potential usefulness of raw date pits as an inexpensive solid adsorbent for methylene blue (MB), copper ion (Cu 2+ ), and cadmium ion (Cd 2+ ) has been demonstrated in this work. This work was conducted to provide fundamental information from the study of equilibrium adsorption isotherms and to investigate the adsorption mechanisms in the adsorption of MB, Cu 2+ , and Cd 2+ onto raw date pits. The fit of two models, namely Langmuir and Freundlich models, to experimental data obtained from the adsorption isotherms was checked. The adsorption capacities of the raw date pits towards MB and both Cu 2+ and Cd 2+ ions obtained from Langmuir and Freundlich models were found to be 277.8, 35.9, and 39.5 mg g -1 , respectively. Surface functional groups on the raw date pits surface substantially influence the adsorption characteristics of MB, Cu 2+ , and Cd 2+ onto the raw date pits. The Fourier transform infrared spectroscopy (FTIR) studies show clear differences in both absorbances and shapes of the bands and in their locations before and after solute adsorption. Two mechanisms were observed for MB adsorption, hydrogen bonding and electrostatic attraction, while other mechanisms were observed for Cu 2+ and Cd 2+ . For Cu 2+ , binding two cellulose/lignin units together is the predominant mechanism. For Cd 2+ , the predominant mechanism is by binding itself using two hydroxyl groups in the cellulose/lignin unit.

  9. Fugitive gas adsorption capacity of biomass and animal-manure derived biochars

    Science.gov (United States)

    This research characterized and investigated ammonia and hydrogen sulfide gas adsorption capacities of low- and high-temperature biochars made from wood shavings and chicken litter. The biochar samples were activated with steam or phosphoric acid. The specific surface areas and pore volumes of the a...

  10. Method and apparatus for the selective separation of gaseous coal gasification products by pressure swing adsorption

    Science.gov (United States)

    Ghate, M.R.; Yang, R.T.

    1985-10-03

    Bulk separation of the gaseous components of multi-component gases provided by the gasification of coal including hydrogen, carbon monoxide, methane, and acid gases (carbon dioxide plus hydrogen sulfide) are selectively adsorbed by a pressure swing adsorption technique using activated carbon zeolite or a combination thereof as the adsorbent. By charging a column containing the adsorbent with a gas mixture and pressurizing the column to a pressure sufficient to cause the adsorption of the gases and then reducing the partial pressure of the contents of the column, the gases are selectively and sequentially desorbed. Hydrogen, the least absorbable gas of the gaseous mixture, is the first gas to be desorbed and is removed from the column in a co-current direction followed by the carbon monoxide, hydrogen and methane. With the pressure in the column reduced to about atmospheric pressure the column is evacuated in a countercurrent direction to remove the acid gases from the column. The present invention is particularly advantageous as a producer of high purity hydrogen from gaseous products of coal gasification and as an acid gas scrubber. 2 figs., 2 tabs.

  11. Insights into the mechanism of acetic acid hydrogenation to ethanol on Cu(111) surface

    International Nuclear Information System (INIS)

    Zhang, Minhua; Yao, Rui; Jiang, Haoxi; Li, Guiming; Chen, Yifei

    2017-01-01

    Highlights: • The scission of C–OH bond of acetic acid is the rate-determined step in acetic acid hydrogenation to ethanol on Cu(111). • Acetic acid adsorption and reaction barrier of C–OH scission of acetic acid are factors related to acetic acid conversion. • Acetaldehyde adsorption and reaction barriers of O–H formation of C_2–oxygenates are factors related to ethanol selectivity. - Abstract: Density functional theory (DFT) calculations were employed to theoretically explain the reaction mechanism of acetic acid hydrogenation to ethanol on Cu catalyst. The activation barriers of key elementary steps and the adsorption configurations of key intermediates involved in acetic acid hydrogenation on Cu(111) surface were investigated. The results indicated that the direct dissociation of acetic acid to acetyl (CH_3COOH → CH_3CO + OH) is the rate-determined step. The activation barrier of acetic acid scission to acetyl and the adsorption energy of acetic acid are two descriptors which could determine the conversion of acetic acid. The descriptors might have effects on the ethanol selectivity including: the adsorption energy of acetaldehyde and the activation barriers for O−H bond formation of C_2-oxygenates (CH_3CO + H → CH_3COH, CH_3CHO + H → CH_3CHOH and CH_3CH_2O + H → CH_3CH_2OH). These proposed descriptors could be used as references to design new Cu-based catalysts that have excellent catalytic performance.

  12. Dynamic response of physisorbed hydrogen molecules on lanthanide-modified zirconia nanoparticles

    International Nuclear Information System (INIS)

    Loong, C.K.; Trouw, F.; Ozawa, Masakuni; Suzuki, Suguru

    1997-01-01

    Ultrafine lanthanide (Ln = Ce and Nd)-modified zirconia powders synthesized by a coprecipitation method exhibit high surface areas and adsorption sites that are essential for catalytic applications. We report a study of the surface chemistry of Ce 0.1 Zr 0.9 O 2 and Nd 0.1 Zr 0.9 O 1.95 powders. First, the specific surface area and porosity are characterized by nitrogen isotherm-adsorption measurements. Second, the motion of hydrogen molecules physisorbed on Ce- and Nd-doped zirconias is studied by inelastic neutron scattering. Nitrogen adsorption-desorption isotherm measurements yield a BET surface area (26.1 m 2 /g) and mesopore size (∼5 nm radius) in Ce 0.1 Zr 0.9 O 2 as compared to those (72.3 m 2 /g and ∼3 nm) in Nd 0.1 Zr 0.9 O 1.95 . The vibrational densities of states of H 2 on Ce 0.1 Zr 0.9 O 2 and Nd 0.1 Zr 0.9 O 1.95 were measured at 20 K over the 0-200 meV energy range for three hydrogen coverage. The spectra for both samples consist of two parts: a sharp peak at ∼14.5 meV and a broad component extending beyond 200 meV. The sharp peak corresponds to transitions from the J=0 to J=1 rotational states of bulk hydrogen molecules, and its intensity decreases with decreasing H 2 coverage. The broad component corresponds to overdamped motion of surface adsorbed hydrogen molecules. The major difference in the latter component between the Ce- and Nd-doped samples is an excess of intensities in the 5-14 meV region in Nd 0.1 Zr 0.9 O 1.95 . The confined motion of adsorbed H 2 on the different micropore and mesopore surfaces of Ce 0.1 Zr 0.9 O 2 and Nd 0.1 Zr 0.9 O 1.95 is discussed

  13. Chemisorption of a hydrogen adatom on metal doped α-Zr (0 0 0 1 surfaces in a vacuum and an implicit solvation environment

    Directory of Open Access Journals (Sweden)

    Cheng Zeng

    2017-12-01

    Full Text Available First-principles calculations have been carried out to investigate the adsorption of a hydrogen adatom on 24 metal doped α-Zr (0 0 0 1 surfaces in both a vacuum and an implicit solvation environment. The dopant are the elements in the 4th and 5th periods in the periodic table. Doping elements at the tail of the 4th and 5th periods can significantly reduce the hydrogen pickup in a vacuum environment. A weighted d-band center theory is used to analyze the doping effect. On the other hand, the hydrogen adsorption energies in water are relatively lower for all doped slabs and the surface adsorption of hydrogen adatom is stronger than that in a vacuum environment, especially, for the slabs with doping elements at the tail of the 4th and 5th periods. In the solvation environment, electronegativity difference affects the adsorption. Doping elements Ag, Ga, Ge, Sn, and Sb can reduce the hydrogen pickup in vacuum, while Ag and Cu can reduce the hydrogen pickup of the zirconium alloys in solvent environment.

  14. A Study on adsorption of Li from aqueous solution using various adsorbents

    Energy Technology Data Exchange (ETDEWEB)

    Ryoo, Keon Sang [Dept. of Applied Chemistry, Andong National University, Andon (Korea, Republic of); Kim, Dae Ik [School of Electrical, Electronic Communication, and Computer Engineering, Chonnam National University, Yeosu (Korea, Republic of)

    2015-04-15

    The aim of the present study is to explore the possibility of utilizing fly ash, loess and activated charcoal for the adsorption of Li in aqueous solution. Batch adsorption experiments were performed to evaluate the influences of various factors like initial concentration, contact time, and temperature. The adsorption data showed that fly ash and activated charcoal are not effective for the adsorption of Li. On the contrary, loess showed much higher adsorption capacity for Li. The adsorption of Li on loess was highly concentration dependent. It was found that the adsorption capacity of loess is favored at a lower Li concentration. At equilibrium, approximately 95% of adsorption was achieved by loess. The equilibrium data were fitted well to the Freundlich isotherm model. The pseudo-second-order kinetic model appeared to be the better-fitting model because it has higher R 2 compared to the pseudo-first-order kinetic models. The thermodynamic parameters such as free energy ΔG, the enthalpy ΔH, and the entropy ΔS were calculated.

  15. Optimization of the elaboration conditions of an adsorber for the hydrogen storage; Optimisation des conditions d'elaboration d'un adsorbant pour le stockage d'hydrogene

    Energy Technology Data Exchange (ETDEWEB)

    Fierro, V.; Mareche, J.F.; Furdin, G. [Nancy-1 Univ. Henri Poincare, UMR - CNRS 7555, Laboratoire de Chimie du Solide Mineral, 54 - Vandoeuvre-les-Nancy (France); Szczurek, A.; Albiniak, A. [Wroclaw Univ. of Technology, Laboratory for Lignites and Carbon Adsorbents, Institute of Chemistry and Technology of Petroleum and Coal (Poland); Latroche, M. [Chimie Metallurgique des Terres Rares, ICMPE, UMR 7182, CNRS, 94 - Thiais (France); Celzard, A. [Nancy-Univ., ENSTIB, Laboratoire de Chimie du Solide Mineral, UMR CNRS 7555, 88 - Epinal (France)

    2008-07-01

    The microporous carbon are very efficient adsorbents for the hydrogen storage, because of pores size under 2 nm. This study describes the optimization of the elaboration conditions for a carbon adsorbent for the hydrogen storage by adsorption. The storage capacity has been measured at 25 C for 20 MPa and also at 77 K for pressures between 6 and 9 MPa. the porous texture characterization has been realized by four molecule probes of increasing diameter: CO{sub 2}, N{sub 2}, C{sub 6}H{sub 6} and CCl{sub 4}. (A.L.B.)

  16. Equilibrium, kinetic and thermodynamic studies of adsorption of Th(IV) from aqueous solution onto kaolin

    International Nuclear Information System (INIS)

    Hongxia Zhang; Zhiwei Niu; Zhi Liu; Zhaodong Wen; Weiping Li; Xiaoyun Wang; Wangsuo Wu

    2015-01-01

    The kinetics and thermodynamics of the adsorption of Th(IV) on the kaolin were studied by using batch method. In addition, the experimental data were studied by dynamic and thermodynamic models. The results showed that the adsorption capacity of the adsorbent increased with increasing temperature and solid liquid ratio, but decreased with increasing initial Th(IV) ion concentration, and the best fit was obtained for the pseudo-second-order kinetics model. The calculated activation energy for adsorption was about 45 kJ/mol, which indicated the adsorption process to be chemisorption. The adsorption isotherm data could be well described by the Langmuir as well as Dubinin-Radushkevich model. The mean free energy (E) of adsorption was calculated to be about 15 kJ/mol. The thermodynamic data calculated showed that the adsorption was spontaneous and enhanced at higher temperature. Considering kinetics and equilibrium studies, the adsorption on the sites was the rate-limiting step and that adsorption was mainly a chemisorption process through cation exchange. (author)

  17. Spectroscopic studies of hydrogen collisions

    International Nuclear Information System (INIS)

    Kielkopf, J.

    1991-01-01

    Low energy collisions involving neutral excited states of hydrogen are being studied with vacuum ultraviolet spectroscopy. Atomic hydrogen is generated by focusing an energetic pulse of ArF, KrF, or YAG laser light into a cell of molecular hydrogen, where a plasma is created near the focal point. The H 2 molecules in and near this region are dissociated, and the cooling atomic hydrogen gas is examined with laser and dispersive optical spectroscopy. In related experiments, we are also investigating neutral H + O and H + metal - atom collisions in these laser-generated plasmas

  18. Probing adsorption of polyacrylamide-based polymers on anisotropic Basal planes of kaolinite using quartz crystal microbalance.

    Science.gov (United States)

    Alagha, Lana; Wang, Shengqun; Yan, Lujie; Xu, Zhenghe; Masliyah, Jacob

    2013-03-26

    Quartz crystal microbalance with dissipation (QCM-D) was applied to investigate the adsorption characteristics of polyacrylamide-based polymers (PAMs) on anisotropic basal planes of kaolinite. Kaolinite basal planes were differentiated by depositing kaolinite nanoparticles (KNPs) on silica and alumina sensors in solutions of controlled pH values. Adsorption of an in-house synthesized organic-inorganic Al(OH)3-PAM (Al-PAM) as an example of cationic hybrid PAM and a commercially available partially hydrolyzed polyacrylamide (MF1011) as an example of anionic PAM was studied. Cationic Al-PAM was found to adsorb irreversibly and preferentially on tetrahedral silica basal planes of kaolinite. In contrast, anionic MF1011 adsorbed strongly on aluminum-hydroxy basal planes, while its adsorption on tetrahedral silica basal planes was weak and reversible. Adsorption study revealed that both electrostatic attraction and hydrogen-bonding mechanisms contribute to adsorption of PAMs on kaolinite. The adsorbed Al-PAM layer was able to release trapped water overtime and became more compact, while MF1011 film became more dissipative as backbones stretched out from kaolinite surface with minimal overlapping. Experimental results obtained from this study provide clear insights into the phenomenon that governs flocculation-based solid-liquid separation processes using multicomponent flocculants of anionic and cationic nature.

  19. Double vacancy on BN layer: A natural trap for Hydrogen Molecule

    International Nuclear Information System (INIS)

    Arellano, J S

    2015-01-01

    A pair of vacancies, one of boron and other of nitrogen atom at a flat layer becomes a natural trap to capture a hydrogen molecule at the center of the cavity defined by the empty space left by the lack of a nitrogen and a boron atom at the perfect BN layer formed by 16 N atoms and 16 B atoms. The adsorption of the hydrogen molecule is compared with the equivalent graphene layer with a pair of carbon vacancies. The little increase in the BN cell parameter respect to the graphene cell parameter, besides the differences between N, B and C atoms helps to explain the easier adsorption on the defective BN layer

  20. Modeling of hydrogen/deuterium dynamics and heat generation on palladium nanoparticles for hydrogen storage and solid-state nuclear fusion

    Directory of Open Access Journals (Sweden)

    Katsuaki Tanabe

    2016-01-01

    Full Text Available We modeled the dynamics of hydrogen and deuterium adsorbed on palladium nanoparticles including the heat generation induced by the chemical adsorption and desorption, as well as palladium-catalyzed reactions. Our calculations based on the proposed model reproduce the experimental time-evolution of pressure and temperature with a single set of fitting parameters for hydrogen and deuterium injection. The model we generated with a highly generalized set of formulations can be applied for any combination of a gas species and a catalytic adsorbent/absorbent. Our model can be used as a basis for future research into hydrogen storage and solid-state nuclear fusion technologies.