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Sample records for adsorption resistant surface

  1. Protein adsorption resistance of PVP-modified polyurethane film prepared by surface-initiated atom transfer radical polymerization

    Energy Technology Data Exchange (ETDEWEB)

    Yuan, Huihui; Qian, Bin; Zhang, Wei [Shanghai Key Laboratory of Functional Materials Chemistry and Research Center of Analysis and Test, East China University of Science and Technology, Shanghai 200237 (China); Lan, Minbo, E-mail: minbolan@ecust.edu.cn [Shanghai Key Laboratory of Functional Materials Chemistry and Research Center of Analysis and Test, East China University of Science and Technology, Shanghai 200237 (China); State Key Laboratory of Bioreactor Engineering, East China University of Science and Technology, Shanghai 200237 (China)

    2016-02-15

    Highlights: • Antifouling PVP brushes were successfully grafted on PU films by SI-ATRP. • The effect of polymerization time on surface property and topography was studied. • Hydrophilicity and protein fouling resistance of PVP–PU films were greatly promoted. • Competitive adsorption of three proteins on PVP–PU films was evaluated. - Abstract: An anti-fouling surface of polyurethane (PU) film grafted with Poly(N-vinylpyrrolidone) (PVP) was prepared through surface-initiated atom transfer radical polymerization (SI-ATRP). And the polymerization time was investigated to obtain PU films with PVP brushes of different lengths. The surface properties and protein adsorption of modified PU films were evaluated. The results showed that the hydrophilicity of PU–PVP films were improved with the increase of polymerization time, which was not positive correlation with the surface roughness due to the brush structure. Additionally, the protein resistance performance was promoted when prolonging the polymerization time. The best antifouling PU–PVP (6.0 h) film reduced the adsoption level of bovine serum albumin (BSA), lysozyme (LYS), and brovin serum fibrinogen (BFG) by 93.4%, 68.3%, 85.6%, respectively, compared to the unmodified PU film. The competitive adsorption of three proteins indicated that LYS preferentially adsorbed on the modified PU film, while BFG had the lowest adsorption selectivity. And the amount of BFG on PU–PVP (6.0 h) film reduced greatly to 0.08 μg/cm{sup 2}, which was almost one-tenth of its adsorption from the single-protein system. Presented results suggested that both hydrophilicity and surface roughness might be the important factors in all cases of protein adsorption, and the competitive or selective adsorption might be related to the size of the proteins, especially on the non-charged films.

  2. The effect of electron-surface scattering and thiol adsorption on the electrical resistivity of gold ultrathin films

    International Nuclear Information System (INIS)

    Henriquez, Ricardo; Del Campo, Valeria; Gonzalez-Fuentes, Claudio; Correa-Puerta, Jonathan; Moraga, Luis; Flores, Marcos; Segura, Rodrigo; Donoso, Sebastián; Marín, Francisca; Bravo, Sergio; Häberle, Patricio

    2017-01-01

    Highlights: • We prepared ultra thin films (10 nm) on mica on top of a chromium seedlayer (<1 nm). • We prepared samples with different topographies controlling the substrate temperature. • We studied the contribution of the different scattering mechanims on the resistivity. • We developed a discernment method based on thiol adsorption. - Abstract: In order to study the effect of electron-surface scattering in gold ultrathin films (∼10 nm), we have prepared a set of Au samples on mica on top of a chromium seedlayer (<1 nm). Chromium is added as a metallic surfactant which enables surpassing the electric percolation threshold for substrate temperatures above room temperature. We prepared samples with the same thickness but different topographies setting different substrate temperatures. These modifications modulate the contributions of the different electronic scattering mechanisms to the film resistivity. A second set of gold thin films deposited on mica at room temperature, with different thicknesses between 8 and 100 nm, was also prepared to compare the resisitivities of both sets through Mayadas and Shatzkes theory. We found that in samples with thicknesses below 15 nm, the electron-surface scattering is indeed the dominant mechanism influencing the film resistivity. To obtain further evidence of this prevalence, we developed a discrimination method based on thiol adsorption. The film with the highest resistivity increase is the sample in which electron-surface scattering is dominant. With this method, we observed that a large enhancement of the electron-surface scattering not only occurs in samples with large diameters grains, but also if the film has a reduced surface roughness.​

  3. The effect of electron-surface scattering and thiol adsorption on the electrical resistivity of gold ultrathin films

    Energy Technology Data Exchange (ETDEWEB)

    Henriquez, Ricardo, E-mail: ricardo.henriquez@usm.cl [Departamento de Física, Universidad Técnica Federico Santa María, Av. España 1680, Valparaiso 2390123 (Chile); Del Campo, Valeria; Gonzalez-Fuentes, Claudio [Departamento de Física, Universidad Técnica Federico Santa María, Av. España 1680, Valparaiso 2390123 (Chile); Correa-Puerta, Jonathan [Instituto de Física, Pontificia Universidad Católica de Valparaíso, Av. Universidad 330, Curauma, Valparaíso (Chile); Moraga, Luis [Universidad Central de Chile, Toesca 1783, Santiago 8370178 (Chile); Flores, Marcos [Departamento de Física, Facultad de Ciencias Físicas y Matemáticas, Universidad de Chile, Av. Blanco Encalada 2008, Santiago (Chile); Segura, Rodrigo [Instituto de Química y Bioquímica, Facultad de Ciencias, Universidad de Valparaíso, Av. Gran Bretaña 1111, Valparaíso (Chile); Donoso, Sebastián; Marín, Francisca; Bravo, Sergio; Häberle, Patricio [Departamento de Física, Universidad Técnica Federico Santa María, Av. España 1680, Valparaiso 2390123 (Chile)

    2017-06-15

    Highlights: • We prepared ultra thin films (10 nm) on mica on top of a chromium seedlayer (<1 nm). • We prepared samples with different topographies controlling the substrate temperature. • We studied the contribution of the different scattering mechanims on the resistivity. • We developed a discernment method based on thiol adsorption. - Abstract: In order to study the effect of electron-surface scattering in gold ultrathin films (∼10 nm), we have prepared a set of Au samples on mica on top of a chromium seedlayer (<1 nm). Chromium is added as a metallic surfactant which enables surpassing the electric percolation threshold for substrate temperatures above room temperature. We prepared samples with the same thickness but different topographies setting different substrate temperatures. These modifications modulate the contributions of the different electronic scattering mechanisms to the film resistivity. A second set of gold thin films deposited on mica at room temperature, with different thicknesses between 8 and 100 nm, was also prepared to compare the resisitivities of both sets through Mayadas and Shatzkes theory. We found that in samples with thicknesses below 15 nm, the electron-surface scattering is indeed the dominant mechanism influencing the film resistivity. To obtain further evidence of this prevalence, we developed a discrimination method based on thiol adsorption. The film with the highest resistivity increase is the sample in which electron-surface scattering is dominant. With this method, we observed that a large enhancement of the electron-surface scattering not only occurs in samples with large diameters grains, but also if the film has a reduced surface roughness.​.

  4. Competitive Protein Adsorption - Multilayer Adsorption and Surface Induced Protein Aggregation

    DEFF Research Database (Denmark)

    Holmberg, Maria; Hou, Xiaolin

    2009-01-01

    and that the outcome of IgG adsorption is much more sensitive to surface characteristics than the outcome of albumin adsorption. Using high concentrations of protein solution and hydrophobic polymer surfaces during adsorption can induce IgG aggregation, which is observed as extremely high IgG adsorptions. Besides......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...

  5. From aggregative adsorption to surface depletion

    DEFF Research Database (Denmark)

    Rother, Gernot; Müter, Dirk; Bock, Henry

    2017-01-01

    Adsorption of a short-chain nonionic amphiphile (C6E3) at the surface of mesoporous silica glass (CPG) was studied by a combination of adsorption measurements and mesoscale simulations. Adsorption measurements covering a wide composition range of the C6E3 + water system show that no adsorption...... occurs up to the critical micelle concentration, at which a sharp increase of adsorption is observed that is attributed to ad-micelle formation at the pore walls. Intriguingly, as the concentration is increased further, the surface excess of the amphiphile begins to decrease and eventually becomes...... negative, which corresponds to preferential adsorption of water rather than amphiphile at high amphiphile concentrations. The existence of such a surface-azeotropic point has not previously been reported in the surfactant adsorption field. Dissipative particle dynamics simulations were performed to reveal...

  6. Adsorption of Hazardous Compounds to Mineral Surfaces

    National Research Council Canada - National Science Library

    Carron, Keith

    1997-01-01

    The project entitled 'Adsorption of Hazardous Compounds to Mineral Surfaces' involved five faculty members from the University of Wyoming's Departments of Chemistry, Geology, Soil Science, and Mathematics...

  7. Adsorption of gases on heterogeneous surfaces

    CERN Document Server

    Rudzinski, W

    1991-01-01

    All real solid surfaces are heterogeneous to a greater or lesser extent and this book provides a broad yet detailed survey of the present state of gas adsorption. Coverage is comprehensive and extends from basic principles to computer simulation of adsorption. Underlying concepts are clarified and the strengths and weaknesses of the various methods described are discussed.Key Features* Adsorption isotherm equations for various types of heterogeneous solid surfaces* Methods of determining the nature of surface heterogeneity and porosity from experimental data* Studies of pha

  8. Adsorption of Wine Constituents on Functionalized Surfaces.

    Science.gov (United States)

    Mierczynska-Vasilev, Agnieszka; Smith, Paul A

    2016-10-18

    The adsorption of macromolecules on solid surfaces is of great importance in the field of nanotechnology, biomaterials, biotechnological, and food processes. In the field of oenology adsorption of wine macromolecules such as polyphenols, polysaccharides, and proteins is much less desirable on membrane materials because of fouling and reduced filtering performance. On the other hand, adsorption of these molecules on processing aids is very beneficial for achieving wine clarity and stability. In this article, the effect of surface chemical functionalities on the adsorption of white, rosé, and red wine constituents was evaluated. Allylamine, acrylic acid, and ethanol were selected as precursors for plasma polymerization in order to generate coatings rich in amine, carboxyl, and hydroxyl chemical groups, respectively. The surface chemical functionalities were characterized by X-ray photoelectron spectroscopy (XPS) and the ability of different surface chemical functionalities to adsorb wine constituents were characterized by quartz crystal microbalance with dissipation (QCM-D) and atomic force microscopy (AFM). The results demonstrated that the amine and carboxyl modified surfaces encourage adsorption of constituents from white wine. The hydroxyl modified surfaces have the ability to preferentially adsorb rosé wine constituents, whereas red wine adsorbed to the highest extent on acrylic acid surface.

  9. Adsorption of Wine Constituents on Functionalized Surfaces

    Directory of Open Access Journals (Sweden)

    Agnieszka Mierczynska-Vasilev

    2016-10-01

    Full Text Available The adsorption of macromolecules on solid surfaces is of great importance in the field of nanotechnology, biomaterials, biotechnological, and food processes. In the field of oenology adsorption of wine macromolecules such as polyphenols, polysaccharides, and proteins is much less desirable on membrane materials because of fouling and reduced filtering performance. On the other hand, adsorption of these molecules on processing aids is very beneficial for achieving wine clarity and stability. In this article, the effect of surface chemical functionalities on the adsorption of white, rosé, and red wine constituents was evaluated. Allylamine, acrylic acid, and ethanol were selected as precursors for plasma polymerization in order to generate coatings rich in amine, carboxyl, and hydroxyl chemical groups, respectively. The surface chemical functionalities were characterized by X-ray photoelectron spectroscopy (XPS and the ability of different surface chemical functionalities to adsorb wine constituents were characterized by quartz crystal microbalance with dissipation (QCM-D and atomic force microscopy (AFM. The results demonstrated that the amine and carboxyl modified surfaces encourage adsorption of constituents from white wine. The hydroxyl modified surfaces have the ability to preferentially adsorb rosé wine constituents, whereas red wine adsorbed to the highest extent on acrylic acid surface.

  10. Chirality in adsorption on solid surfaces.

    Science.gov (United States)

    Zaera, Francisco

    2017-12-07

    In the present review we survey the main advances made in recent years on the understanding of chemical chirality at solid surfaces. Chirality is an important topic, made particularly relevant by the homochiral nature of the biochemistry of life on Earth, and many chiral chemical reactions involve solid surfaces. Here we start our discussion with a description of surface chirality and of the different ways that chirality can be bestowed on solid surfaces. We then expand on the studies carried out to date to understand the adsorption of chiral compounds at a molecular level. We summarize the work published on the adsorption of pure enantiomers, of enantiomeric mixtures, and of prochiral molecules on chiral and achiral model surfaces, especially on well-defined metal single crystals but also on other flat substrates such as highly ordered pyrolytic graphite. Several phenomena are identified, including surface reconstruction and chiral imprinting upon adsorption of chiral agents, and the enhancement or suppression of enantioselectivity seen in some cases upon adsorption of enantiomixtures of chiral compounds. The possibility of enhancing the enantiopurity of adsorbed layers upon the addition of chiral seeds and the so-called "sergeants and soldiers" phenomenon are presented. Examples are provided where the chiral behavior has been associated with either thermodynamic or kinetic driving forces. Two main approaches to the creation of enantioselective surface sites are discussed, namely, via the formation of supramolecular chiral ensembles made out of small chiral adsorbates, and by adsorption of more complex chiral molecules capable of providing suitable chiral environments for reactants by themselves, via the formation of individual adsorbate:modifier adducts on the surface. Finally, a discussion is offered on the additional effects generated by the presence of the liquid phase often required in practical applications such as enantioselective crystallization, chiral

  11. Albumin (BSA) adsorption onto graphite stepped surfaces

    Science.gov (United States)

    Rubio-Pereda, Pamela; Vilhena, J. G.; Takeuchi, Noboru; Serena, Pedro A.; Pérez, Rubén

    2017-06-01

    Nanomaterials are good candidates for the design of novel components with biomedical applications. For example, nano-patterned substrates may be used to immobilize protein molecules in order to integrate them in biosensing units. Here, we perform long MD simulations (up to 200 ns) using an explicit solvent and physiological ion concentrations to characterize the adsorption of bovine serum albumin (BSA) onto a nano-patterned graphite substrate. We have studied the effect of the orientation and step size on the protein adsorption and final conformation. Our results show that the protein is stable, with small changes in the protein secondary structure that are confined to the contact area and reveal the influence of nano-structuring on the spontaneous adsorption, protein-surface binding energies, and protein mobility. Although van der Waals (vdW) interactions play a dominant role, our simulations reveal the important role played by the hydrophobic lipid-binding sites of the BSA molecule in the adsorption process. The complex structure of these sites, that incorporate residues with different hydrophobic character, and their flexibility are crucial to understand the influence of the ion concentration and protein orientation in the different steps of the adsorption process. Our study provides useful information for the molecular engineering of components that require the immobilization of biomolecules and the preservation of their biological activity.

  12. Surface shear rheology of saponin adsorption layers.

    Science.gov (United States)

    Golemanov, Konstantin; Tcholakova, Slavka; Denkov, Nikolai; Pelan, Edward; Stoyanov, Simeon D

    2012-08-21

    Saponins are a wide class of natural surfactants, with molecules containing a rigid hydrophobic group (triterpenoid or steroid), connected via glycoside bonds to hydrophilic oligosaccharide chains. These surfactants are very good foam stabiliziers and emulsifiers, and show a range of nontrivial biological activities. The molecular mechanisms behind these unusual properties are unknown, and, therefore, the saponins have attracted significant research interest in recent years. In our previous study (Stanimirova et al. Langmuir 2011, 27, 12486-12498), we showed that the triterpenoid saponins extracted from Quillaja saponaria plant (Quillaja saponins) formed adsorption layers with unusually high surface dilatational elasticity, 280 ± 30 mN/m. In this Article, we study the shear rheological properties of the adsorption layers of Quillaja saponins. In addition, we study the surface shear rheological properties of Yucca saponins, which are of steroid type. The experimental results show that the adsorption layers of Yucca saponins exhibit purely viscous rheological response, even at the lowest shear stress applied, whereas the adsorption layers of Quillaja saponins behave like a viscoelastic two-dimensional body. For Quillaja saponins, a single master curve describes the data for the viscoelastic creep compliance versus deformation time, up to a certain critical value of the applied shear stress. Above this value, the layer compliance increases, and the adsorption layers eventually transform into viscous ones. The experimental creep-recovery curves for the viscoelastic layers are fitted very well by compound Voigt rheological model. The obtained results are discussed from the viewpoint of the layer structure and the possible molecular mechanisms, governing the rheological response of the saponin adsorption layers.

  13. Polymer adsorption on curved surfaces

    Science.gov (United States)

    Arkin, Handan; Janke, Wolfhard

    2017-12-01

    The conformational behavior of a coarse-grained finite polymer chain near an attractive spherical surface was investigated by means of multicanonical Monte Carlo computer simulations. In a detailed analysis of canonical equilibrium data over a wide range of sphere radius and temperature, we have constructed entire phase diagrams both for nongrafted and end-grafted polymers. For the identification of the conformational phases, we have calculated several energetic and structural observables such as gyration tensor based shape parameters and their fluctuations by canonical statistical analysis. Despite the simplicity of our model, it qualitatively represents in the considered parameter range real systems that are studied in experiments. The work discussed here could have experimental implications from protein-ligand interactions to designing nanosmart materials.

  14. Polymer adsorption on platinum: surface coverage determination using iodide-125

    International Nuclear Information System (INIS)

    Ellis, T.M.; Van de Mark, M.R.; mi, FL

    1981-01-01

    Adsorption of iodide-125, a γ emitter, was used as a quantitative methodology for polymer adsorption surface coverage analysis. Adsorption of I-125 on clean platinum produced surface elemental ratios of I:Pt of 1:4. The technique was applied to the adsorption of polyethylene glycol terephthalate from trifluoroacetic acid on platinum flags with a 2-cm 2 surface area. This polymer adsorption is approximated by a logarithmic relationship similar to the Temkin isotherm. Polymer coverage attained up to 99.6% of the surface

  15. Uranyl adsorption at clay mineral surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Roesch, N. [Technische Univ. Muenchen (Germany). Fachgebiet Theoretische Chemie

    2016-11-01

    This first systematic survey of actinide adsorption at complex clay mineral surfaces, which provided new insights at the atomic level, is currently being extended to neptunyl NpO{sub 2}{sup +} and more complex minerals, like iron-substituted phyllosilicates. In this way we examine if the concepts developed so far can be applied more generally to support the interpretation of pertinent experiments. A further facet of these studies is to account also for the dynamic nature of the mineral/water interface by means of exemplary dynamic simulations.

  16. Competitive protein adsorption to polymer surface from human serum

    DEFF Research Database (Denmark)

    Holmberg, Maria; Jensen, Karin Bagger Stibius; Larsen, Niels Bent

    2008-01-01

    Surface modification by "soft" plasma polymerisation to obtain a hydrophilic and non-fouling polymer surface has been validated using radioactive labelling. Adsorption to unmodified and modified polymer surfaces, from both single protein and human serum solutions, has been investigated. By using...... different radioisotopes, albumin and Immunoglobulin G (IgG) adsorption has been monitored simultaneously during competitive adsorption processes, which to our knowledge has not been reported in the literature before. Results show that albumin and IgG adsorption is dependent on adsorption time...

  17. "Hearing Loss" in QCM Measurement of Protein Adsorption to Protein Resistant Polymer Brush Layers.

    Science.gov (United States)

    Luan, Yafei; Li, Dan; Wei, Ting; Wang, Mengmeng; Tang, Zengchao; Brash, John L; Chen, Hong

    2017-04-04

    Accurate quantification of nonspecific protein adsorption on biomaterial surfaces is essential for evaluation of their antifouling properties. The quartz crystal microbalance (QCM) is an acoustic sensor widely used for the measurement of protein adsorption. However, although the QCM is highly sensitive, it does have performance limitations when working with surfaces modified with thick viscous layers. In the case of polymer brush surfaces, factors such as the thickness and viscosity of the brush may bring such limitations. In the present work, three types of antifouling molecules were used to explore the applicability of QCM for the evaluation of the protein resistance of hydrophilic polymer brush surfaces. Adsorption was also measured by surface plasmon resonance (SPR) as a reference. It was shown that the detection of adsorbed protein requires that protein be located within a critical distance from the QCM chip surface, determined by the viscosity of polymer brush. For larger proteins like fibrinogen, adsorption is expected to occur mainly "on top" of the polymer brush, and brush thickness determines whether protein is located in the "detectable zone". For smaller proteins like lysozyme, adsorption is expected to occur mainly at the chip surface and within the polymer brush layer and to be detectable by QCM. However, the quantity of adsorbed lysozyme may be underestimated when secondary adsorption also occurred. It is concluded that QCM data suggesting very low protein adsorption on polymer brush surfaces should take account of these considerations and should be treated generally with caution.

  18. Surface Adsorption in Nonpolarizable Atomic Models.

    Science.gov (United States)

    Whitmer, Jonathan K; Joshi, Abhijeet A; Carlton, Rebecca J; Abbott, Nicholas L; de Pablo, Juan J

    2014-12-09

    Many ionic solutions exhibit species-dependent properties, including surface tension and the salting-out of proteins. These effects may be loosely quantified in terms of the Hofmeister series, first identified in the context of protein solubility. Here, our interest is to develop atomistic models capable of capturing Hofmeister effects rigorously. Importantly, we aim to capture this dependence in computationally cheap "hard" ionic models, which do not exhibit dynamic polarization. To do this, we have performed an investigation detailing the effects of the water model on these properties. Though incredibly important, the role of water models in simulation of ionic solutions and biological systems is essentially unexplored. We quantify this via the ion-dependent surface attraction of the halide series (Cl, Br, I) and, in so doing, determine the relative importance of various hypothesized contributions to ionic surface free energies. Importantly, we demonstrate surface adsorption can result in hard ionic models combined with a thermodynamically accurate representation of the water molecule (TIP4Q). The effect observed in simulations of iodide is commensurate with previous calculations of the surface potential of mean force in rigid molecular dynamics and polarizable density-functional models. Our calculations are direct simulation evidence of the subtle but sensitive role of water thermodynamics in atomistic simulations.

  19. Monte Carlo Simulation of Protein Adsorption on Energetically Heterogeneous Surfaces

    OpenAIRE

    Danwanichakul, Panu

    2014-01-01

    The modified triangular-well potential model was applied to incorporate the effect of surface energy on the adsorption of particles or proteins on energetically heterogeneous surfaces. The method is convenient in simulating the adsorption on heterogeneous surface of which different region possesses different free energy. Spherical particles with attractive forces were added on the surface and underwent surface diffusion before they were quenched in place. It was seen that the ratio of surface...

  20. 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...

  1. Surfaces of Microparticles in Colloids: Structure and Molecular Adsorption Kinetics

    Science.gov (United States)

    Dai, Hai-Lung

    2002-03-01

    Surfaces of micron and sub-micron size particles in liquid solution are probed by second harmonic generation (SHG) facilitated with femtosecond laser pulses. The particles probed include inorganic objects such as carbon black and color pigments, polymeric species like polystyrene beads, and biological systems such as blood cells and ecoli. In the experiments, dye molecules are first adsorbed onto the particle surface to allow generation of second harmonics upon light irradiation. Competition for adsorption between these surface dye molecules and the molecules of interest in the solution is then monitored by the SHG signal to reveal the molecular adsorption kinetics and surface structure. Specifically, surfactant adsorption on polymer surfaces, the structure of carbon black surface, and protein adsorption on biological surfaces, monitored by this technique, will be discussed.

  2. Water adsorption on the stoichiometric and defected Fe(110) surfaces

    Science.gov (United States)

    Ossowski, Tomasz; Da Silva, Juarez L. F.; Kiejna, Adam

    2018-02-01

    The adsorption of water molecules on defect-free (called here as stoichiometric) and defected Fe(110) surfaces has been investigated using density functional theory (DFT) calculations. It is found that on the stoichiometric surface H2O molecules do not dissociate spontaneously and adsorbs flat on top of the surface Fe atom. By studying different orientations of the flat lying molecule in different adsorption sites it is found that some of them are degenerated in energy thus suggesting a possibility of molecule rotation around direction normal to the surface. At the vacancy defected surface the water molecule favors undercoordinated adsorption sites at or next to the vacancy edge - not the ones in the stoichiometric region of the surface. Moreover, similarly to the stoichiometric surface, at defected one some different configurations are degenerated in energy, making possible molecules circling around the vacancy. The influence of the van der Waals interactions on the adsorption properties of the system is also considered and discussed.

  3. Adsorption Properties of the Cu(115) Surface

    DEFF Research Database (Denmark)

    Godowski, P. J.; Groso, A.; Hoffmann, S. V.

    2010-01-01

    in context of substrate geometry and compared with the ones of other copper planes. There are no indications of dissociative adsorption of CO, only residual carbon and oxygen were found after adsorbate desorption around 220 K. CO molecules show a strong tendency to "on top" adsorption in sites far from...

  4. Surface Complexation Modeling of Fluoride Adsorption by Soil and the Role of Dissolved Aluminum on Adsorption

    Science.gov (United States)

    Padhi, S.; Tokunaga, T.

    2017-12-01

    Adsorption of fluoride (F) on soil can control the mobility of F and subsequent contamination of groundwater. Hence, accurate evaluation of adsorption equilibrium is a prerequisite for understanding transport and fate of F in the subsurface. While there have been studies for the adsorption behavior of F with respect to single mineral constituents based on surface complexation models (SCM), F adsorption to natural soil in the presence of complexing agents needs much investigation. We evaluated the adsorption processes of F on a natural granitic soil from Tsukuba, Japan, as a function of initial F concentration, ionic strength, and initial pH. A SCM was developed to model F adsorption behavior. Four possible surface complexation reactions were postulated with and without including dissolved aluminum (Al) and Al-F complex sorption. Decrease in F adsorption with the increase in initial pH was observed in between the initial pH range of 4 to 9, and a decrease in the rate of the reduction of adsorbed F with respect to the increase in the initial pH was observed in the initial pH range of 5 to 7. Ionic strength variation in the range of 0 to 100mM had insignificant effect on F removal. Changes in solution pH were observed by comparing the solution before and after F adsorption experiments. At acidic pH, the solution pH increased, whereas at alkaline pH, the solution pH decreased after equilibrium. The SCM including dissolved Al and the adsorption of Al-F complex can simulate the experimental results quite successfully. Also, including dissolved Al and the adsorption of Al-F complex to the model explained the change in solution pH after F adsorption.

  5. A theoretical investigation of water adsorption on titanium dioxide surfaces

    Science.gov (United States)

    Fahmi, Adil; Minot, Christian

    1994-03-01

    Water adsorption on various crystallographic faces of TiO 2 (anatase and rutile) are calculated using a periodic Hartree-Fock method. Titanium oxide is an amphoteric compound. Water adsorbs on the acidic site, the titanium atom, and then dissociates to give hydroxyl groups. The adsorption energy is larger on the (110) face of the rutile structure than on other faces and is correlated with its very acidic sites. The OH groups are oriented to maximize hydrogen bonding. Hydrogen bonding is particularly important for molecular adsorption on the (100) face of the rutile structure; in this case, the molecular adsorption becomes competitive with the dissociative one. The thermodynamics of water adsorption strongly favor dissociation when singly-coordinated oxygen atoms are present on the surface as it is in a perfectly truncated anatase surface.

  6. Characterizing adsorption of associating surfactants on carbonates surfaces.

    Science.gov (United States)

    Jian, Guoqing; Puerto, Maura; Wehowsky, Anna; Miller, Clarence; Hirasaki, George J; Biswal, Sibani L

    2018-03-01

    The adsorption of anionic surfactants onto positively charged carbonate minerals is typically high due to electrostatic interactions. By blending anionic surfactants with cationic or zwitterionic surfactants, which naturally form surfactant complexes, surfactant adsorption is expected to be influenced by a competition between surfactant complexes and surfactant-surface interactions. The adsorption behavior of surfactant blends known to form complexes was investigated. The surfactants probed include an anionic C 15-18 internal olefin sulfonate (IOS), a zwitterionic lauryl betaine (LB), and an anionic C 13 -alcohol polyethylene glycol ether carboxylic acid (L38). An analytical method based on high-performance liquid chromatography evaporative light scattering detector (HPLC-ELSD) was developed to measure three individual surfactant concentrations from a blended surfactant solution. The adsorption of the individual surfactants and surfactant blends were systematically investigated on different mineral surfaces using varying brine solutions. LB adsorption on calcite surfaces was found to be significantly increased when blended with IOS or L38 since it forms surfactant complexes that partition to the surface. However, the total adsorption of the LB-IOS-L38 solution on dolomite decreased from 3.09 mg/m 2 to 1.97 mg/m 2 when blended together compared to summing the adsorption values of individual surfactants, which highlights the importance of mixed surfactant association. Copyright © 2017 Elsevier Inc. All rights reserved.

  7. Influence of surface charge on lysozyme adsorption to ceria nanoparticles

    International Nuclear Information System (INIS)

    Wang Binghui; Wu Peng; Yokel, Robert A.; Grulke, Eric A.

    2012-01-01

    Understanding mechanisms for forming protein coronas on nanomaterial surfaces is essential to designing drug delivery systems and designing and interpreting the results of nanomaterial toxicity tests. The study reports the adsorption behavior of a positively charged protein, lysozyme, on cerium dioxide (ceria) nanoparticles with three different surface charges. Adsorption isotherms were modeled with the Toth and Sips equations. Isotherm loading levels were compared to monolayer coverage estimate for ‘side-on’ and ‘end-on’ lysozyme orientations as well as random packing (jamming) and maximum packing limits. Evaluation of adsorption site energy distributions (generated using the model coefficients) suggested that the negatively charged ceria surface had a very broad site energy distribution and that its surface heterogeneity controls the adsorption process. By contrast, the adsorption of lysozyme on the positively charged nanoparticles appears to be influenced by lateral effects from adsorbed protein species. The results illustrate the importance of nanoparticle surface chemistry to protein adsorption. The modeling and site energy distribution evaluations may be useful for interpreting the formation of protein coronas on nanoparticles.

  8. Adsorption of T4 bacteriophages on planar indium tin oxide surface via controlled surface tailoring.

    Science.gov (United States)

    Liana, Ayu Ekajayanthi; Chia, Ed Win; Marquis, Christopher P; Gunawan, Cindy; Gooding, J Justin; Amal, Rose

    2016-04-15

    The work investigates the influence of surface physicochemical properties of planar indium tin oxide (ITO) as a model substrate on T4 bacteriophage adsorption. A comparative T4 bacteriophage adsorption study shows a significant difference in bacteriophage adsorption observed on chemically modified planar ITO when compared to similarly modified particulate ITO, which infers that trends observed in virus-particle interaction studies are not necessarily transferrable to predict virus-planar surface adsorption behaviour. We also found that ITO surfaces modified with methyl groups, (resulting in increased surface roughness and hydrophobicity) remained capable of adsorbing T4 bacteriophage. The adsorption of T4 onto bare, amine and carboxylic functionalised planar ITO suggests the presence of a unique binding behaviour involving specific functional groups on planar ITO surface beyond the non-specific electrostatic interactions that dominate phage to particle interactions. The paper demonstrates the significance of physicochemical properties of surfaces on bacteriophage-surface interactions. Copyright © 2016 Elsevier Inc. All rights reserved.

  9. Adsorption of amino acids on hydrophilic surfaces

    International Nuclear Information System (INIS)

    Paszti, Z; Keszthelyi, T; Hakkel, O; Guczi, L

    2008-01-01

    Sum frequency generation vibrational spectroscopy (SFG) is a powerful tool for in situ investigation of adsorption processes at biologically important solid-liquid interfaces. In this work adsorption of selected amino acids on fused silica, calcium fluoride and titanium dioxide substrates was studied by this technique. SFG spectra taken at the amino acid solution-fused SiO 2 interface revealed the lack of formation of any ordered adsorbate layer, regardless of whether acidic or other, e.g. aromatic, amino acids were used. Ex situ spectra (measured after drying the substrate) showed the formation and gradual growth of amino acid crystallites. In the case of CaF 2 , growth of randomly oriented aspartic acid crystallites was observed even at the solution-substrate interface. Finally, on the TiO 2 substrate, acidic amino acids formed a stable, uniform, more or less ordered coating, which remained unchanged even after drying the sample. On the other hand, non-acidic amino acids like phenylalanine showed very little affinity towards TiO 2 , emphasizing the role of the acidic side chain in the bonding to the substrate. The fact that formation of an amino acid overlayer was observed only on titanium dioxide is probably related to its biocompatibility property

  10. Nitrogen adsorption on Fe(111), (100), and (110) surfaces

    DEFF Research Database (Denmark)

    Mortensen, Jens Jørgen; Ganduglia-Pirovano, Veronica; Hansen, Lars Bruno

    1999-01-01

    Adsorption energies and structures for N atoms on three low-index surfaces of Fe have been calculated using density functional theory (DFT) and the generalized gradient approximation (GGA). At low N coverage the adsorption energy on Fe(100) is found to be similar to 0.7 eV higher than on the (111......) and (110) surfaces - particularly the c(2 x 2)-N/Fe(100) structure with the N atoms in four-fold sites is very stable. We attribute the differences in adsorption energy to the lack of four-fold sites on the (111) and (110) surfaces, We suggest that at higher N coverages, islands with a structure similar...

  11. Adsorption of plasma proteins : adsorption behaviour on apolar surfaces and effect on colloid stability

    NARCIS (Netherlands)

    van der Scheer, Albert

    1978-01-01

    In this thesis the adsorption of some plasma proteins (human albumin (HSA) and fibrinogen (HFb)) on non polar surfaces is studied, together with the influence of these proteins on the stability of polystyrene latices. The aim of these investigations is a better understanding of the processes

  12. Studies of surface adsorption on LiAlO2

    International Nuclear Information System (INIS)

    Fischer, A.K.; Johnson, C.E.; McDaniel, J.A.

    1986-01-01

    Computational and experimental approaches are being taken to understanding surface adsorption/desorption effects on tritium inventory and release. The computational survey integrates a thermodynamic treatment of surface adsorption and bulk phase effects such as solubility and gas phase composition. The system T 2 O:T 2 :LiAlO 2 was examined. The calculations indicate that surface adsorption can be expected to contribute most to tritium inventory under the conditions of lower temperatures and higher oxygen activities. Higher temperature and lower oxygen activity favor lower surface inventory. In the experimental work, a high temperature gas chromatograph was constructed in order to measure the H 2 O:H 2 surface adsorption isotherms and the solubility of hydroxide in LiAlO 2 . Preliminary data indicate that at 478 K approximately 15% of the surface is coverred for a partial pressure of H 2 O of approximately 52 Pa. Calculated values can be obtained that are in reasonable agreement with this. (orig.)

  13. Modulating Protein Adsorption on Oxygen Plasma Modified Polysiloxane Surfaces

    International Nuclear Information System (INIS)

    Marletta, G.

    2006-01-01

    In the present paper we report the study on the adsorption behaviour of three model globular proteins, Human Serum Albumin, Lactoferrin and Egg Chicken Lysozyme onto both unmodified surfaces of a silicon-based polymer and the corresponding plasma treated surfaces. In particular, thin films of hydrophobic polysiloxane (about 90 degree of static water contact angle, WCA) were converted by oxygen plasma treatment at reduced pressure into very hydrophilic phases of SiOx (WCA less than 5 degree). The kinetics of protein adsorption processes were investigated by QCM-D technique, while the chemical structure and topography of the protein adlayer have been studied by Angular resolved-XPS and AFM respectively. It turned out that Albumin and Lysozyme exhibited the opposite preferential adsorption respectively onto the hydrophobic and hydrophilic surfaces, while Lactoferrin did not exhibit significant differences. The observed protein behaviour are discussed both in terms of surface-dependent parameters, including surface free energy and chemical structure, and in terms of protein-dependent parameters, including charge as well as the average molecular orientation in the adlayers. Finally, some examples of differential adsorption behaviour of the investigated proteins are reported onto nanopatterned polysiloxane surfaces consisting of hydrophobic nanopores surrounded by hydrophilic (plasma-treated) matrix and the reverse

  14. Probing the selectivity of a nanostructured surface by xenon adsorption.

    Science.gov (United States)

    Widmer, Roland; Passerone, Daniele; Mattle, Thomas; Sachdev, Hermann; Gröning, Oliver

    2010-04-01

    Surface-supported molecular self-assembly with the goal to produce highly ordered, functional supramolecular nanostructures are often realized using nanopatterned surfaces, which exhibit long range - ideally periodic - modulations of the molecule adsorption properties. To elucidate the physical origins of the site-specific adsorption properties of such a nanopatterned substrate, we investigated the temperature-dependent microscopic structure and the dynamics of adsorbed Xe at different temperatures on single-sheet h-BN on a Rh(111) nanomesh. In combination with molecular dynamics simulations we show that the site-specific adsorption arises from two different interactions of similar magnitude with respect to their lateral variations. The first can be attributed to a van der Waals type interaction, whereas the second originates from lateral variation of the electrostatic surface potential and is of polarization type. Both types lead to an adsorption energy minimum at the rim of the nanomesh pore and are therefore responsible for stabilizing dynamic and static Xe rings in these pores. The insight into this interplay of interactions should pave the way to gain a more general knowledge on such site-specific adsorption processes.

  15. Water and Carbon Dioxide Adsorption at Olivine Surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Kerisit, Sebastien N.; Bylaska, Eric J.; Felmy, Andrew R.

    2013-11-14

    Plane-wave density functional theory (DFT) calculations were performed to simulate water and carbon dioxide adsorption at the (010) surface of five olivine minerals, namely, forsterite (Mg2SiO4), calcio-olivine (Ca2SiO4), tephroite (Mn2SiO4), fayalite (Fe2SiO4), and Co-olivine (Co2SiO4). Adsorption energies per water molecule obtained from energy minimizations varied from -78 kJ mol-1 for fayalite to -128 kJ mol-1 for calcio-olivine at sub-monolayer coverage and became less exothermic as coverage increased. In contrast, carbon dioxide adsorption energies at sub-monolayer coverage ranged from -20 kJ mol-1 for fayalite to -59 kJ mol-1 for calcio-olivine. Therefore, the DFT calculations show a strong driving force for carbon dioxide displacement by water at the surface of all olivine minerals in a competitive adsorption scenario. Additionally, adsorption energies for both water and carbon dioxide were found to be more exothermic for the alkaline-earth (AE) olivines than for the transition-metal (TM) olivines and to not correlate with the solvation enthalpies of the corresponding divalent cations. However, a correlation was obtained with the charge of the surface divalent cation indicating that the more ionic character of the AE cations in the olivine structure relative to the TM cations leads to greater interactions with adsorbed water and carbon dioxide molecules at the surface and thus more exothermic adsorption energies for the AE olivines. For calcio-olivine, which exhibits the highest divalent cation charge of the five olivines, ab initio molecular dynamics simulations showed that this effect leads both water and carbon dioxide to react with the surface and form hydroxyl groups and a carbonate-like species, respectively.

  16. Corrosion-resistant metal surfaces

    Science.gov (United States)

    Sugama, Toshifumi [Wading River, NY

    2009-03-24

    The present invention relates to metal surfaces having thereon an ultrathin (e.g., less than ten nanometer thickness) corrosion-resistant film, thereby rendering the metal surfaces corrosion-resistant. The corrosion-resistant film includes an at least partially crosslinked amido-functionalized silanol component in combination with rare-earth metal oxide nanoparticles. The invention also relates to methods for producing such corrosion-resistant films.

  17. Zwitterionic polymers exhibiting high resistance to nonspecific protein adsorption from human serum and plasma.

    Science.gov (United States)

    Ladd, Jon; Zhang, Zheng; Chen, Shengfu; Hower, Jason C; Jiang, Shaoyi

    2008-05-01

    This study examined six different polymer and self-assembled monolayer (SAM) surface modifications for their interactions with human serum and plasma. It was demonstrated that zwitterionic polymer surfaces are viable alternatives to more traditional surfaces based on poly(ethylene glycol) (PEG) as nonfouling surfaces. All polymer surfaces were formed using atom transfer radical polymerization (ATRP) and they showed an increased resistance to nonspecific protein adsorption compared to SAMs. This improvement is due to an increase in the surface packing density of nonfouling groups on the surface, as well as a steric repulsion from the flexible polymer brush surfaces. The zwitterionic polymer surface based on carboxybetaine methacrylate (CBMA) also incorporates functional groups for protein immobilization in the nonfouling background, making it a strong candidate for many applications such as in diagnostics and drug delivery.

  18. Transient Convection, Diffusion, and Adsorption in Surface-Based Biosensors

    DEFF Research Database (Denmark)

    Hansen, Rasmus; Bruus, Henrik; Callisen, Thomas H.

    2012-01-01

    This paper presents a theoretical and computational investigation of convection, diffusion, and adsorption in surface-based biosensors. In particular, we study the transport dynamics in a model geometry of a surface plasmon resonance (SPR) sensor. The work, however, is equally relevant for other...... microfluidic surface-based biosensors, operating under flow conditions. A widely adopted approximate quasi-steady theory to capture convective and diffusive mass transport is reviewed, and an analytical solution is presented. An expression of the Damköhler number is derived in terms of the nondimensional...... concentration to the maximum surface capacity is critical for reliable use of the quasi-steady theory. Finally, our results provide users of surface-based biosensors with a tool for correcting experimentally obtained adsorption rate constants....

  19. Surface-complexation modelling for describing adsorption of ...

    African Journals Online (AJOL)

    2013-06-08

    Jun 8, 2013 ... Adsorption of dissolved phosphate onto synthetic hydrous ferric oxide (HFO) was measured in the laboratory as a function of pH, ionic strength, and phosphate relative concentration. Experimental data were used to constrain optimal values of surface complexation reactions using a geochemical modeling ...

  20. Adsorption mechanisms of carboxymethyl cellulose on mineral surfaces.

    NARCIS (Netherlands)

    Hoogendam, C.W.; Keizer, de A.; Cohen Stuart, M.A.; Bijsterbosch, B.H.; Batelaan, J.G.; Horst, van der P.M.

    1998-01-01

    The adsorption behavior of carboxymethyl cellulose (CMC) on inorganic surfaces (TiO2 and -Fe2O3) in aqueous solution has been studied systematically. The general trends are that the adsorbed amount decreases with increasing pH, whereas increasing the electrolyte (NaCl) concentration causes the

  1. Adsorption of methylene blue from aqueous solution on the surface ...

    African Journals Online (AJOL)

    Adsorption of dye methylene blue from aqueous solution on the surface of sheep wool and cotton fibers was accomplished under the optimize conditions of temperature, concentration, pH, stay time duration and quantity of adsorbent. Spectrometric technique was used for the measurements of concentration of dye before ...

  2. Surface adsorption technique for the treatment of textile wastewaters ...

    African Journals Online (AJOL)

    Reductions in color and pH variation of the effluent were monitored through absorbance and pH measurements throughout the process. Concentration levels of Ni2+ in the wastewater ranged ... for treated samples to be employed for domestic purposes. Key Words: Effluents Treatment, Nickel, Chromium, Surface adsorption ...

  3. Plasma proteins adsorption mechanism on polyethylene-grafted poly(ethylene glycol) surface by quartz crystal microbalance with dissipation.

    Science.gov (United States)

    Jin, Jing; Jiang, Wei; Yin, Jinghua; Ji, Xiangling; Stagnaro, Paola

    2013-06-04

    Protein adsorption has a vital role in biomaterial surface science because it is directly related to the hemocompatibility of blood-contacting materials. In this study, monomethoxy poly(ethylene glycol) (mPEG) with two different molecular weights was grafted on polyethylene as a model to elucidate the adsorption mechanisms of plasma protein through quartz crystal microbalance with dissipation (QCM-D). Combined with data from platelet adhesion, whole blood clotting time, and hemolysis rate, the blood compatibility of PE-g-mPEG film was found to have significantly improved. Two adsorption schemes were developed for real-time monitoring of protein adsorption. Results showed that the preadsorbed bovine serum albumin (BSA) on the surfaces of PE-g-mPEG films could effectively inhibit subsequent adsorption of fibrinogen (Fib). Nonspecific protein adsorption of BSA was determined by surface coverage, not by the chain length of PEG. Dense PEG brush could release more trapped water molecules to resist BSA adsorption. Moreover, the preadsorbed Fib could be gradually displaced by high-concentration BSA. However, the adsorption and displacement of Fib was determined by surface hydrophilicity.

  4. Effect of surface strain on oxygen adsorption on Zr (0001) surface

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Xing [Univ. of Wisconsin-Madison, Madison, WI (United States). Dept. of Engineering Physics; Khafizov, Marat [Idaho National Laboratory (INL), Idaho Falls, ID (United States); Szlufarska, Izabela [Univ. of Wisconsin-Madison, Madison, WI (United States). Dept. of Engineering Physics; Univ. of Wisconsin-Madison, Madison, WI (United States). Dept. of Materials Science and Engineering

    2014-02-01

    The effect of surface strain on oxygen adsorption on Zr (0 0 0 1) surface is investigated by density functional theory (DFT) calculations. It is demonstrated that both surface strain and interactions between oxygen adsorbates influence the adsorption process. Oxygen binding to zirconium becomes stronger as the strain changes from compressive to tensile. When oxygen coverage is low and the oxygen interactions are negligible, surface face-centered cubic sites are the most stable for O binding. At high coverage and under compression, octahedral sites between second and third Zr layers become most favorable because the interactions between adsorbates are weakened by positive charge screening. Calculations with both single-layer adsorption model and multiple-layer adsorption model demonstrate that compressive strain at the Zr/oxide interface will provide a thermodynamic driving force for oxygen to incorporate from the surface into the bulk of Zr, while binding oxygen to the Zr surface will be easier when tensile strain is applied.

  5. Biological Surface Adsorption Index of Nanomaterials: Modelling Surface Interactions of Nanomaterials with Biomolecules.

    Science.gov (United States)

    Chen, Ran; Riviere, Jim E

    2017-01-01

    Quantitative analysis of the interactions between nanomaterials and their surrounding environment is crucial for safety evaluation in the application of nanotechnology as well as its development and standardization. In this chapter, we demonstrate the importance of the adsorption of surrounding molecules onto the surface of nanomaterials by forming biocorona and thus impact the bio-identity and fate of those materials. We illustrate the key factors including various physical forces in determining the interaction happening at bio-nano interfaces. We further discuss the mathematical endeavors in explaining and predicting the adsorption phenomena, and propose a new statistics-based surface adsorption model, the Biological Surface Adsorption Index (BSAI), to quantitatively analyze the interaction profile of surface adsorption of a large group of small organic molecules onto nanomaterials with varying surface physicochemical properties, first employing five descriptors representing the surface energy profile of the nanomaterials, then further incorporating traditional semi-empirical adsorption models to address concentration effects of solutes. These Advancements in surface adsorption modelling showed a promising development in the application of quantitative predictive models in biological applications, nanomedicine, and environmental safety assessment of nanomaterials.

  6. Surface free energy analysis of adsorbents used for radioiodine adsorption

    Energy Technology Data Exchange (ETDEWEB)

    González-García, C.M. [Departamento de Física Aplicada, Universidad de Extremadura, Avda. Elvas s/n, 06006 Badajoz (Spain); Román, S., E-mail: sroman@unex.es [Departamento de Física Aplicada, Universidad de Extremadura, Avda. Elvas s/n, 06006 Badajoz (Spain); González, J.F.; Sabio, E. [Departamento de Física Aplicada, Universidad de Extremadura, Avda. Elvas s/n, 06006 Badajoz (Spain); Ledesma, B. [Departamento de Ingeniería Mecánica, Energética y de los Materiales, Universidad de Extremadura, Avda. Elvas s/n, 06006 Badajoz (Spain)

    2013-10-01

    In this work, the surface free energy of biomass-based activated carbons, both fresh and impregnated with triethylenediamine, has been evaluated. The contribution of Lifshitz van der Waals components was determined by the model proposed by van Oss et al. The results obtained allowed predicting the most probable configurations of the impregnant onto the carbon surface and its influence on the subsequent adsorption of radioactive methyl iodide.

  7. Fibrinogen adsorption on blocked surface of albumin

    DEFF Research Database (Denmark)

    Holmberg, Maria; Hou, Xiaolin

    2011-01-01

    biological samples, including protein solutions. It is based on the assumption that proteins adsorbs as a monolayer on surfaces and that proteins do not adsorb on top of each other. By labelling albumin and fibrinogen with two different radioactive iodine isotopes that emit gamma radiation with different...

  8. Electrochemical analysis of the adsorption and desorption behaviors of carboxylic acid and anhydride monomers onto zinc surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Taheri, P. [Materials innovation institute (M2i), Mekelweg 2, 2628 CD Delft (Netherlands); Delft University of Technology, Department of Materials Science and Engineering, Mekelweg 2, 2628 CD Delft (Netherlands); Hauffman, T. [Vrije Universiteit Brussel, Department of Electrochemical and Surface Engineering, Pleinlaan 2, B-1050 Brussels (Belgium); Mol, J.M.C. [Delft University of Technology, Department of Materials Science and Engineering, Mekelweg 2, 2628 CD Delft (Netherlands); Flores, J.R.; Hannour, F. [Tata Steel Research, Development and Technology, PO Box 10.000, 1970 CA IJmuiden (Netherlands); Wit, J.H.W. de [Materials innovation institute (M2i), Mekelweg 2, 2628 CD Delft (Netherlands); Delft University of Technology, Department of Materials Science and Engineering, Mekelweg 2, 2628 CD Delft (Netherlands); Terryn, H., E-mail: hterryn@irexchange.vub.ac.b [Materials innovation institute (M2i), Mekelweg 2, 2628 CD Delft (Netherlands); Vrije Universiteit Brussel, Department of Electrochemical and Surface Engineering, Pleinlaan 2, B-1050 Brussels (Belgium)

    2011-10-30

    The interfacial bondings formed between succinic acid and myristic acid, as well as succinic anhydride molecules with a set of differently treated zinc substrates have been investigated using infrared reflection absorption spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The compounds were selected to model typically used carboxylic-based adhesives and coatings. Moreover, the adsorption kinetic has been evaluated by means of chronoamperometry (CA) and chronovoltammetry measurements. XPS results showed a relation between the amount of carboxylates formed by adsorption of succinic acid/myristic acid and the hydroxyl fraction presented on the surfaces as proved by a higher electron transfer in CA. On the other hand a set of oxidative/reductive interactions was detected during the adsorption of succinic anhydride, in turn proving a spontaneous ring opening and adsorption mechanism. A clear relationship between the amount of adsorbents and surface hydroxyls/carbonates was detected for the adsorption of succinic anhydride. The extent to which the formed carboxylates resisted negative potentials was also investigated by cyclic voltammetry (CV) in an aqueous solution. The coordinative bonding of a bifunctional carboxylic acid group to the oxide surface was found to be not stable in the presence of a negative potential, while a monofunctional carboxylic acid group could resist displacement by water for a prolonged period of time. On the other hand, a low double layer capacitance was obtained after the adsorption of succinic anhydride, which was related to a change in potential of zero charge (PZC) upon the adsorption.

  9. Dynamics of fibronectin adsorption on TiO2 surfaces.

    Science.gov (United States)

    Sousa, S R; Brás, M Manuela; Moradas-Ferreira, P; Barbosa, M A

    2007-06-19

    In the present work we analyze the dynamics of fibronectin (FN) adsorption on two different stable titanium oxides, with varied surface roughness, and chemically similar to those used in clinical practice. The two types of titanium oxide surfaces used were TiO2 sputtered on Si (TiO2 sp) and TiO2 formed on commercially pure titanium after immersion in H2O2 (TiO2 cp). Surface characterization was previously carried out using different techniques (Sousa, S. R.; Moradas-Ferreira, P.; Melo, L. V.; Saramago, B.; Barbosa, M. A. Langmuir 2004, 20 (22), 9745-9754). Imaging and roughness analysis before and after FN adsorption used atomic force microscopy (AFM) in tapping mode, in air, and in magnetic alternating current mode, in liquid (water). FN adsorption as a function of time was followed by X-ray photoelectron spectroscopy (XPS), by radiolabeling of FN with 125I (125I-FN), and by ellipsometry. Exchangeability studies were performed using FN and HSA. AFM roughness analysis revealed that, before FN adsorption, both TiO2 surfaces exhibited a lower root-mean-square (Rq) and maximum peak with the depth of the maximum valley (Rmax) roughness in air than in water, due to TiO2 hydration. After protein adsorption, the same behavior was observed for the TiO2 sp substrate, while Rq and Rmax roughness values in air and in water were similar in the case of the TiO2 cp substrate, for the higher FN concentration used. Surface roughness was always significantly higher on the TiO2 cp surfaces. AFM led to direct visualization of adsorbed FN on both surfaces tested, indicating that after 10 min of FN incubation the TiO2 sp surface was partially covered by FN. The adsorbed protein seems to form globular aggregates or ellipsoids, and FN aggregates coalesce, forming clusters as the time of adsorption and the concentration increase. Radiolabeling of FN revealed that a rapid adsorption occurs on both surfaces and the amount adsorbed increased with time, reaching a maximum after 60 min of

  10. Iodide adsorption on the surface of chemically pretreated clinoptilolite

    International Nuclear Information System (INIS)

    Chmielewska-Horvatova, E.; Lesny, J.

    1995-01-01

    The possibility to use the monoionic Ag +- form (eventually Hg +- and Hg 2+ -forms) of clinoptilolite of domestic origin for radioactive iodide elimination from waters has been studied. The capacity of the monoforms of clinoptilolite towards iodide exceeds many times that of the capacity of clinoptilolite in natural form. Due to the low solubility product of AgI, Hg 2 I 2 and HgI 2 iodides generate precipitates on the zeolite surface. Rtg analyses of the silver form of clinoptilolite after sorption of iodide demonstrate the formation of new crystals on the zeolite surface. The influence of interfering anions on the adsorption capacity of silver clinoptilolite towards iodide was investigated, too. Kinetic curves of iodide desorption from the surface of silver and mercury clinoptilolite were compared. Simultaneously, adsorption isotherms for the systems aqueous iodide solution/Ag-, Hg-clinoptilolite were determined. (author) 6 refs.; 7 figs.; 4 tabs

  11. Molecular dynamics simulation of uranium compound adsorption on solid surface

    International Nuclear Information System (INIS)

    Omori, Yuki; Takizawa, Yuji; Okamoto, Tsuyoshi

    2010-01-01

    Particles mixed in the UF6 gas have the property of accumulating on the inside of piping or units. This type of accumulation will cause material unaccounted for (MUF) in the UF6 gas processing facilities. Development of a calculation model for estimating the accumulation rate of uranium compounds has been expected. And predicting possible part of the units where uranium compounds adsorb will contribute to design an effective detection system. The purpose of this study is to take the basic knowledge of the particle's adsorption mechanism from the microscopic point of view. In simulation analysis, UF5 model particle is produced, then two types of solid surfaces are prepared; one is a solid surface at rest and the other is a moving solid surface. The result obtained by the code 'PABS' showed that when the solid surface moves at a lower velocity, the particle's adsorption process dominates over the particle's breakup one. Besides the velocity of the solid surface, other principal factors affecting an adsorption ratio were also discussed. (author)

  12. Arginine inhibits adsorption of proteins on polystyrene surface.

    Directory of Open Access Journals (Sweden)

    Yui Shikiya

    Full Text Available Nonspecific adsorption of protein on solid surfaces causes a reduction of concentration as well as enzyme inactivation during purification and storage. However, there are no versatile inhibitors of the adsorption between proteins and solid surfaces at low concentrations. Therefore, we examined additives for the prevention of protein adsorption on polystyrene particles (PS particles as a commonly-used material for vessels such as disposable test tubes and microtubes. A protein solution was mixed with PS particles, and then adsorption of protein was monitored by the concentration and activity of protein in the supernatant after centrifugation. Five different proteins bound to PS particles through electrostatic, hydrophobic, and aromatic interactions, causing a decrease in protein concentration and loss of enzyme activity in the supernatant. Among the additives, including arginine hydrochloride (Arg, lysine hydrochloride, guanidine hydrochloride, NaCl, glycine, and glucose, Arg was most effective in preventing the binding of proteins to PS particles as well as activity loss. Moreover, even after the mixing of protein and PS particles, the addition of Arg caused desorption of the bound protein from PS particles. This study demonstrated a new function of Arg, which expands the potential for application of Arg to proteins.

  13. Adsorption of water, sulfates and chloride on arsenopyrite surface

    Science.gov (United States)

    Silva, Juliana C. M.; dos Santos, Egon C.; de Oliveira, Aline; Heine, Thomas; De Abreu, Heitor A.; Duarte, Hélio A.

    2018-03-01

    Arsenopyrite is one of the sulfide minerals responsible for acid rock drainage (ARD) and is one of the most hazardous in regions affected by mining activities. This phenomenon involves complex reaction mechanism. Although it is intensely investigated, there is a lack of consensus concerning the reaction mechanisms and more information is still necessary. In this work, the adsorption of water, hydrochloric acid, and sulfuric acid on arsenopyrite (001) surface was investigated by means of Density Functional calculations and the results compared to other sulfides aiming to understand the mineral/water interface. The interaction of the chemical species with the (001) FeAsS surface is the first step to understand the intricate oxidation mechanism of arsenopyrite. Molecular water adsorption on (001) FeAsS is more favored than the adsorption of sulfate favoring the dissolution of sulfates and enhancing its oxidation. The estimated adsorption energies of water, sulfates and chloride on other sulfide minerals are compared with the estimated values for arsenopyrite and the chemical reactivity differences discussed in detail.

  14. DFT study of water adsorption on lignite molecule surface.

    Science.gov (United States)

    Gao, Zhengyang; Ding, Yi; Yang, Weijie; Han, Wentao

    2017-01-01

    High moisture content is a main characteristic of low-rank coal, such as lignite. Numerous oxygen containing functional groups in lignite make it represent some special properties, and these functional groups affect the adsorption mechanisms of water molecules on lignite surface. This study reports some typical water · · · lignite conformations, along with a detailed analysis of the geometry, electrostatic potential distribution, reduced density gradient of interaction, and interaction energy decomposition. The results show that water molecules tend to aggregate around functional groups, and hydrogen bonds play a dominant role in the interaction. The adsorption energy of water cluster on lignite surface is larger than that of isolated water molecule, a good linear relationship between the interaction distance and adsorption energy of layers has been found. Since water is a polar molecule, the local minima and maxima of electrostatic potential in conformations increase along with more water adsorbing on lignite surface. Reduced density gradient analysis shows that H-bonds, van der Waals interaction, and a little steric make up the interaction between water cluster and lignite molecule. In these studied conformations which mainly are H-bond complexes, electrostatic and exchange repulsion play a dominant role, whereas polarization and dispersion make relatively small contribution to the interaction. Attractive and repulsive interaction both affect the stability of water · · · lignite conformations.

  15. Adsorption of phospholipid bilayers onto pullulan-modified cellulose surfaces

    Science.gov (United States)

    Choi, Heejun; Liu, Zelin; Esker, Alan

    2009-03-01

    1,2-Dimyristoyl-sn-glycero-3-phosphocholine (DMPC) vesicle adsorption onto regenerated cellulose and pullulan 4-bromocinnamate (P4BC) modified cellulose surfaces was investigated via surface plasmon resonance (SPR) spectroscopy and quartz crystal microbalance with dissipation monitoring (QCM-D). P4BC with a degree of substitution (DS) of 0.061 ± 0.002 from UV measurements and 0.058 from ^1H NMR was synthesized from pullulan and 4-bromocinnamic acid to yield P4BC. The deduced thicknesses from SPR for DMPC layers were ˜3.7 nm (bilayer) on regenerated cellulose surfaces and ˜2.1 nm (monolayer) on P4BC modified cellulose surfaces. Qualitative analysis of the QCM-D data also indicated that the DMPC layers on P4BC modified cellulose surfaces were thinner than on regenerated cellulose surfaces.

  16. Polymer Adsorption on Graphite and CVD Graphene Surfaces Studied by Surface-Specific Vibrational Spectroscopy.

    Science.gov (United States)

    Su, Yudan; Han, Hui-Ling; Cai, Qun; Wu, Qiong; Xie, Mingxiu; Chen, Daoyong; Geng, Baisong; Zhang, Yuanbo; Wang, Feng; Shen, Y R; Tian, Chuanshan

    2015-10-14

    Sum-frequency vibrational spectroscopy was employed to probe polymer contaminants on chemical vapor deposition (CVD) graphene and to study alkane and polyethylene (PE) adsorption on graphite. In comparing the spectra from the two surfaces, it was found that the contaminants on CVD graphene must be long-chain alkane or PE-like molecules. PE adsorption from solution on the honeycomb surface results in a self-assembled ordered monolayer with the C-C skeleton plane perpendicular to the surface and an adsorption free energy of ∼42 kJ/mol for PE(H(CH2CH2)nH) with n ≈ 60. Such large adsorption energy is responsible for the easy contamination of CVD graphene by impurity in the polymer during standard transfer processes. Contamination can be minimized with the use of purified polymers free of PE-like impurities.

  17. Adsorption of surface functionalized silica nanoparticles onto mineral surfaces and decane/water interface

    International Nuclear Information System (INIS)

    Metin, Cigdem O.; Baran, Jimmie R.; Nguyen, Quoc P.

    2012-01-01

    The adsorption of silica nanoparticles onto representative mineral surfaces and at the decane/water interface was studied. The effects of particle size (the mean diameters from 5 to 75 nm), concentration and surface type on the adsorption were studied in detail. Silica nanoparticles with four different surfaces [unmodified, surface modified with anionic (sulfonate), cationic (quaternary ammonium (quat)) or nonionic (polyethylene glycol (PEG)) surfactant] were used. The zeta potential of these silica nanoparticles ranges from −79.8 to 15.3 mV. The shape of silica particles examined by a Hitachi-S5500 scanning transmission electron microscope (STEM) is quite spherical. The adsorption of all the nanoparticles (unmodified or surface modified) on quartz and calcite surfaces was found to be insignificant. We used interfacial tension (IFT) measurements to investigate the adsorption of silica nanoparticles at the decane/water interface. Unmodified nanoparticles or surface modified ones with sulfonate or quat do not significantly affect the IFT of the decane/water interface. It also does not appear that the particle size or concentration influences the IFT. However, the presence of PEG as a surface modifying material significantly reduces the IFT. The PEG surface modifier alone in an aqueous solution, without the nanoparticles, yields the same IFT reduction for an equivalent PEG concentration as that used for modifying the surface of nanoparticles. Contact angle measurements of a decane droplet on quartz or calcite plate immersed in water (or aqueous nanoparticle dispersion) showed a slight change in the contact angle in the presence of the studied nanoparticles. The results of contact angle measurements are in good agreement with experiments of adsorption of nanoparticles on mineral surfaces or decane/water interface. This study brings new insights into the understanding and modeling of the adsorption of surface-modified silica nanoparticles onto mineral surfaces and

  18. Controlled adsorption of cytochrome c to nanostructured gold surfaces

    International Nuclear Information System (INIS)

    Gomes, Inês; Feio, Maria J.; Santos, Nuno C.; Eaton, Peter; Serro, Ana Paula; Saramago, Benilde; Pereira, Eulália; Franco, Ricardo

    2012-01-01

    Controlled electrostatic physisorption of horse heart cytochrome c (Cyt c) onto nanostructured gold surfaces was investigated using Quartz-Crystal Microbalance measurements in planar gold surfaces with or without functionalization using a self-assembled monolayer (SAM) of the alkanethiol mercaptoundecanoic acid (MUA). MUA is a useful functionalization ligand for gold surfaces, shedding adsorbed biomolecules from the excessive electron density of the metal. A parallel analysis was conducted in the corresponding curved surfaces of 15 nm gold nanoparticles (AuNPs), using zeta-potential and UV– visible spectroscopy. Atomic Force Microscopy of both types of functionalized gold surfaces with a MUA SAM, allowed for visualization of Cyt c deposits on the nanostructured gold surface. The amount of Cyt c adsorbed onto the gold surface could be controlled by the solution pH. For the assays conducted at pH 4.5, when MUA SAM- functionalized planar gold surfaces are positive or neutral, and Cyt c has a positive net charge, only 13 % of the planar gold surface area was coated with protein. In contrast, at pH 7.4, when MUA SAM-functionalized planar gold surfaces and Cyt c have opposite charges, a protein coverage of 28 % could be observed implying an adsorption process strongly governed by electrostatic forces. Cyt c adsorption on planar and curved gold surfaces are found to be greatly favored by the presence of a MUA-capping layer. In particular, on the AuNPs, the binding constant is three times larger than the binding constant obtained for the original citrate-capped AuNPs.

  19. Controlled adsorption of cytochrome c to nanostructured gold surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Gomes, Ines [Faculdade de Ciencias e Tecnologia, Universidade Nova de Lisboa, REQUIMTE, Departamento de Quimica (Portugal); Feio, Maria J. [Faculdade de Ciencias da Universidade do Porto, REQUIMTE, Departamento de Quimica e Bioquimica (Portugal); Santos, Nuno C. [Faculdade de Medicina da Universidade de Lisboa, Instituto de Medicina Molecular (Portugal); Eaton, Peter [Faculdade de Ciencias da Universidade do Porto, REQUIMTE, Departamento de Quimica e Bioquimica (Portugal); Serro, Ana Paula; Saramago, Benilde [Centro de Quimica Estrutural, Instituto Superior Tecnico (Portugal); Pereira, Eulalia [Faculdade de Ciencias da Universidade do Porto, REQUIMTE, Departamento de Quimica e Bioquimica (Portugal); Franco, Ricardo, E-mail: ricardo.franco@fct.unl.pt [Faculdade de Ciencias e Tecnologia, Universidade Nova de Lisboa, REQUIMTE, Departamento de Quimica (Portugal)

    2012-12-15

    Controlled electrostatic physisorption of horse heart cytochrome c (Cyt c) onto nanostructured gold surfaces was investigated using Quartz-Crystal Microbalance measurements in planar gold surfaces with or without functionalization using a self-assembled monolayer (SAM) of the alkanethiol mercaptoundecanoic acid (MUA). MUA is a useful functionalization ligand for gold surfaces, shedding adsorbed biomolecules from the excessive electron density of the metal. A parallel analysis was conducted in the corresponding curved surfaces of 15 nm gold nanoparticles (AuNPs), using zeta-potential and UV- visible spectroscopy. Atomic Force Microscopy of both types of functionalized gold surfaces with a MUA SAM, allowed for visualization of Cyt c deposits on the nanostructured gold surface. The amount of Cyt c adsorbed onto the gold surface could be controlled by the solution pH. For the assays conducted at pH 4.5, when MUA SAM- functionalized planar gold surfaces are positive or neutral, and Cyt c has a positive net charge, only 13 % of the planar gold surface area was coated with protein. In contrast, at pH 7.4, when MUA SAM-functionalized planar gold surfaces and Cyt c have opposite charges, a protein coverage of 28 % could be observed implying an adsorption process strongly governed by electrostatic forces. Cyt c adsorption on planar and curved gold surfaces are found to be greatly favored by the presence of a MUA-capping layer. In particular, on the AuNPs, the binding constant is three times larger than the binding constant obtained for the original citrate-capped AuNPs.

  20. 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

  1. 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.

  2. Non-equilibrium dynamics of single polymer adsorption to solid surfaces

    NARCIS (Netherlands)

    Panja, D.; Barkema, G.T.; Kolomeisky, A.B.

    2009-01-01

    The adsorption of polymers to surfaces is crucial for understanding many fundamental processes in nature. Recent experimental studies indicate that the adsorption dynamics is dominated by non-equilibrium effects. We investigate the adsorption of a single polymer of length N to a planar solid surface

  3. SiO adsorption on a p(2 × 2) reconstructed Si(1 0 0) surface

    NARCIS (Netherlands)

    Violanda, M.|info:eu-repo/dai/nl/304840262; Rudolph, H.|info:eu-repo/dai/nl/304830496

    2009-01-01

    We have investigated the adsorption mechanism of SiO molecule incident on a clean Si(1 0 0) p(2 × 2) reconstructed surface using density functional theory based methods. Stable adsorption geometries of SiO on Si surface, as well as their corresponding activation and adsorption energies are

  4. Adsorption of trace gases to ice surfaces: surface, bulk and co-adsorbate effects

    Science.gov (United States)

    Kerbrat, Michael; Bartels-Rausch, Thorsten; Huthwelker, Thomas; Schneebeli, Martin; Pinzer, Bernd; Ammann, Markus

    2010-05-01

    Atmospheric ices frequently interact with trace gases and aerosol making them an important storage, transport or reaction medium in the global ecosystem. Further, this also alters the physical properties of the ice particles with potential consequences for the global irradiation balance and for the relative humidity of surrounding air masses. We present recent results from a set of laboratory experiments of atmospheric relevance to investigate the nature of the uptake processes. The focus of this talk will be placed on the partitioning of acidic acid and nitrous acid on ice surfaces.The presented results span from very simple reversible adsorption experiments of a single trace gas onto ice surfaces to more complex, but well controlled, experimental procedures that successfully allowed us to - Disentangle surface adsorption and uptake into the ice matrix using radioactive labelled trace gases. - Show that simultaneous adsorption of acetic acid and nitrous acid to an ice surface is consistent with the Langmuir co-adsorption model. The experiments were done in a packed ice bed flow tube at atmospheric pressure and at temperatures between 213 and 253 K. The HONO gas phase mixing ratio was between 0.4 and 137 ppbv, the mixing ratio of acetic acid between 5 and 160 ppbv . The use of the radioactive labelled nitrous acid molecules for these experiments enabled in situ monitoring of the migration of trace gas in the flow tube. The measurements showed that the interactions do not only occur through adsorption but also via diffusion into polycrystalline ice. A method is suggested to disentangle the bulk and the surface processes. The co-adsorption of acetic and nitrous acids was also investigated. The measurements are well reproduced by a competitive Langmuir adsorption model.

  5. Bovine serum albumin adsorption on functionalized porous silicon surfaces

    Science.gov (United States)

    Tay, Li-Lin; Rowell, Nelson L.; Lockwood, David J.; Boukherroub, Rabah

    2004-10-01

    The large surface area within porous Si (pSi) and its strong room temperature photoluminescence (PL) make it an ideal host for biological sensors. In particular, the development of pSi-based optical sensors for DNA, enzyme and other biochemical molecules have become of great interest. Here, we demonstrate that the in-situ monitoring of the pSi PL behaviour can be used as a positive identification of bovine serum albumin (BSA) protein adsorption inside the porous matrix. Electrochemically prepared pSi films were first functionalized with undecylenic acid to produce an organic monolayer covalently attached to the porous silicon surfaces. The acid terminal group also provided favourable BSA binding sites on the pSi matrix sidewalls. In-situ PL spectra showed a gradual red shift (up to 12 meV) in the PL peak energy due to the protein incorporation into the porous matrix. The PL then exhibited a continuous blue shift after saturation of the protein molecules in the pores. This blue shift of the PL peak frequency and a steady increase in the PL intensity is evidence of surface oxidation. Comparing the specular reflectance obtained by Fourier transform infrared spectroscopy (FTIR) before and after BSA incubation confirmed the adsorption of protein in the pSi matrix.

  6. Nickel adsorption by wild type and nickel resistant isolate of chlorella sp

    International Nuclear Information System (INIS)

    Shakya, P.R.

    2007-01-01

    Use of unicellular green microalgae has several advantages over conventional methods for removing heavy metals from contaminated sites. Here, a comparative study was made to investigate nickel detoxification mechanisms between a wild type(WT) Chlorella sp. and a nickel resistant, EMS-5 cell line isolated from the same species by EMS (Ethyl Methane Sulphonate) mutagenesis. Results showed that the growth rate of the tested algal cells was inhibited with increasing nickel concentrations in the liquid growth medium. Higher ID/sub 50/ value of EMS-5 compared to the WT revealed some degree of resistance to nickel. Removal and adsorption of Ni/sub 2+/ were found rapid during the first few hours in both the algal cultures when exposed to 50 microM Ni/sub 2+/. However, kinetic experiments showed significantly higher removal and adsorption of Ni by EMS-5 compared to the WT throughout the treatment hours. Besides, the total nickel accumulation, surface bound and intracellular nickel in EMS-5 was significantly higher to that of the WT. Hence the EMS-5 appeared more resistant to nickel. (author)

  7. Adsorption configuration of magnesium on wurtzite gallium nitride surface using first-principles calculations

    International Nuclear Information System (INIS)

    Yan Han; Gan Zhiyin; Song Xiaohui; Chen Zhaohui; Xu Jingping; Liu Sheng

    2009-01-01

    First-principles calculations of magnesium adsorption at the Ga-terminated and N-terminated {0 0 0 1} basal plane wurtzite gallium nitride surfaces have been carried out to explain the atomic-scale insight into the initial adsorption processes of magnesium doping in gallium nitride. The results reveal that magnesium adsorption on N-terminated surfaces is preferred than that on Ga-terminated surfaces. Furthermore, the surface diffusivity of magnesium atom on the N-terminated surface is much lower than that on the Ga-terminated surface, which is due to both the larger average adsorption energies and the lower adsorption distance on N-terminated surface than that on Ga-terminated surface. The results indicate that the p-type doping on the Ga-terminated surface will be better distributed than that on the N-terminated surface.

  8. A first principles investigation of the oxygen adsorption on Zr(0001) surface using cluster expansions

    Science.gov (United States)

    Samin, Adib J.; Taylor, Christopher D.

    2017-11-01

    The design of corrosion resistant zircalloys is important for a variety of technological applications ranging from medicine to the nuclear industry. Since corrosion resistance is mainly attributed to the formation of a surface oxide layer, developing a detailed understanding of this process may assist in future corrosion resistance design. In this work, we conduct a systematic multi-scale investigation of the early stages of oxide formation. This was accomplished by first using a database of fully relaxed DFT calculations to build a cluster-expansion description of the potential function. The developed potential was reasonably good at predicting DFT energies as evidenced by the cross-validation score of 4.4 meV/site. The effective cluster expansion parameters were indicative of repulsive adsorbate interactions in the adlayer in agreement with the literature. The potential then allowed for a systematic investigation of the oxygen configurations on the Zr(0001) surface via Monte Carlo simulations. The adsorption energy was recorded as a function of coverage and an increasing trend was observed in agreement with DFT predictions and the repulsive nature of interactions in the adlayer. The convex hull diagram was recorded indicating the most stable configuration to occur around a coverage of 0.6 ML. The adsorption isotherm was also recorded and contrasted for two temperatures relevant for different applications.

  9. Optimization of lead adsorption of mordenite by response surface methodology: characterization and modification

    OpenAIRE

    Turkyilmaz, Havva; Kartal, Tolga; Yigitarslan Yildiz, Sibel

    2014-01-01

    Background In order to remove heavy metals, water treatment by adsorption of zeolite is gaining momentum due to low cost and good performance. In this research, the natural mordenite was used as an adsorbent to remove lead ions in an aqueous solution. Methods The effects of adsorption temperature, time and initial concentration of lead on the adsorption yield were investigated. Response surface methodology based on Box-Behnken design was applied for optimization. Adsorption data were analyzed...

  10. Effects of Surface Treatment of Activated Carbon on Its Surface and Cr(VI) Adsorption Characteristics

    Energy Technology Data Exchange (ETDEWEB)

    Park, Soo Jin; Jang, Yu Sin [Advanced Materials Division., Korea Research Institute of Chimical Technology, Taejon (Korea)

    2001-04-01

    In this work, the effect of surface treatments on activated carbons (ACs) has been studied in the context of gas and liquid adsorption behaviors. The chemical solutions used in this experiment were 35% sodium hydroxide, and these were used for the acidic and basic treatments, respectively. The surface properties have been determined by pH, acid-base values, and FT-IR. The adsorption isotherms of Cr(VI) ion on activated carbons have been studied with the 5 mg/l concentration at ambient temperature. N{sub 2} adsorption isotherm characteristics, which include the specific surface area, micro pore volume, and microporosity, were determined by BET and Boer's-plot methods. In case of the acidic treatment of activated carbons, it was observed that the adsorption of Cr(VI) ion was more effective due to the increase acid value (or acidic functional group) of activated carbon surfaces. However, the basic treatment on activated carbons was caused no significant effects, probably due to the decreased specific surface area and total pore volume. 27 refs., 7 figs., 4 tabs.

  11. Competitive Protein Adsorption of Albumin and Immunoglobulin G from Human Serum onto Polymer Surfaces

    DEFF Research Database (Denmark)

    Holmberg, Maria; Hou, Xiaolin

    2010-01-01

    Competitive protein adsorption from human serum onto unmodified polyethylene terephthalate (PET) surfaces and plasma-polymerized PET surfaces, using the monomer diethylene glycol vinyl ether (DEGVE), has been investigated using radioactive labeling. Albumin and immunoglobulin G (IgG) labeled...... with two different iodine isotopes have been added to human serum solutions of different concentrations, and adsorption has been performed using adsorption times from approximately 5 s to 24 h. DEGVE surfaces showed indications of being nonfouling regarding albumin and IgG adsorption during competitive...... protein adsorption from diluted human serum solutions with relatively low protein concentrations, but the nonfouling character was weakened when less diluted human serum solutions with higher protein concentrations were used. The observed adsorption trend is independent of adsorption time, indicating...

  12. Adsorption of Dyes in Studying the Surface Chemistry of Ultradispersed Diamond

    Science.gov (United States)

    Khokhlova, T. D.; Yunusova, G. R.; Lanin, S. N.

    2018-05-01

    The effect the surface chemistry of ultradispersed diamond (UDD) has on the adsorption of watersoluble dyes is considered. A comparison is made to adsorption on graphitized thermal carbon black (GTCB), which has a homogeneous and nonporous surface. The adsorption isotherms of dyes and the dependence of the adsorption on the pH of solutions are measured. It is found that UDD adsorbs acid (anionic) dyes—acid orange (AO) and acid anthraquinone blue (AAB)—but barely adsorbs a basic (cationic) dye, methylene blue (MB), because of the predominance of positively charged basic groups on the surface of UDD. The maximum adsorption of AO is much lower on UDD than on GTCB, while the maximum adsorption of AAB is similar for both surfaces. The adsorption of AO on UDD depends strongly on the pH of the solution, while the adsorption of AAB is independent of this parameter. It is suggested that the adsorption of AAB is determined not only by ionic and hydrophobic interactions but also by coordination interactions with impurity metal ions on a UDD surface. It is concluded that the adsorption of dyes characterizes the chemistry of a UDD surface with high sensitivity.

  13. Sputter deposited bioceramic coatings: surface characterisation and initial protein adsorption studies using surface-MALDI-MS

    DEFF Research Database (Denmark)

    Boyd, A. R.; Burke, G. A.; Duffy, H.

    2011-01-01

    Protein adsorption onto calcium phosphate (Ca–P) bioceramics utilised in hard tissue implant applications has been highlighted as one of the key events that influences the subsequent biological response, in vivo. This work reports on the use of surface-matrix assisted laser desorption ionisation ...

  14. Response surface modeling of boron adsorption from aqueous solution by vermiculite using different adsorption agents: Box-Behnken experimental design.

    Science.gov (United States)

    Demirçivi, Pelin; Saygılı, Gülhayat Nasün

    2017-07-01

    In this study, a different method was applied for boron removal by using vermiculite as the adsorbent. Vermiculite, which was used in the experiments, was not modified with adsorption agents before boron adsorption using a separate process. Hexadecyltrimethylammonium bromide (HDTMA) and Gallic acid (GA) were used as adsorption agents for vermiculite by maintaining the solid/liquid ratio at 12.5 g/L. HDTMA/GA concentration, contact time, pH, initial boron concentration, inert electrolyte and temperature effects on boron adsorption were analyzed. A three-factor, three-level Box-Behnken design model combined with response surface method (RSM) was employed to examine and optimize process variables for boron adsorption from aqueous solution by vermiculite using HDTMA and GA. Solution pH (2-12), temperature (25-60 °C) and initial boron concentration (50-8,000 mg/L) were chosen as independent variables and coded x 1 , x 2 and x 3 at three levels (-1, 0 and 1). Analysis of variance was used to test the significance of variables and their interactions with 95% confidence limit (α = 0.05). According to the regression coefficients, a second-order empirical equation was evaluated between the adsorption capacity (q i ) and the coded variables tested (x i ). Optimum values of the variables were also evaluated for maximum boron adsorption by vermiculite-HDTMA (HDTMA-Verm) and vermiculite-GA (GA-Verm).

  15. Adsorption of lysozyme unto silica and polystyrene surfaces in ...

    African Journals Online (AJOL)

    The adsorption capacity of lysozyme (chicken egg white) from aqueous solutions unto silica and polystyrene interfaces was studied at varying lysozyme concentrations and ionic strength. The studies revealed an increase in adsorption capacity with increase in concentration and with maximum adsorption densities of 1.34 ...

  16. Computational study of ethanol adsorption and reaction over rutile TiO2 (110) surfaces

    KAUST Repository

    Muir, J. N.

    2012-01-01

    Studies of the modes of adsorption and the associated changes in electronic structures of renewable organic compounds are needed in order to understand the fundamentals behind surface reactions of catalysts for future energies. Using planewave density functional theory (DFT) calculations, the adsorption of ethanol on perfect and O-defected TiO 2 rutile (110) surfaces was examined. On both surfaces the dissociative adsorption mode on five-fold coordinated Ti cations (Ti 4+ 5c) was found to be more favourable than the molecular adsorption mode. On the stoichiometric surface E ads was found to be equal to 0.85 eV for the ethoxide mode and equal to 0.76 eV for the molecular mode. These energies slightly increased when adsorption occurred on the Ti 4+ 5c closest to the O-defected site. However, both considerably increased when adsorption occurred at the removed bridging surface O; interacting with Ti 3+ cations. In this case the dissociative adsorption becomes strongly favoured (E ads = 1.28 eV for molecular adsorption and 2.27 eV for dissociative adsorption). Geometry and electronic structures of adsorbed ethanol were analysed in detail on the stoichiometric surface. Ethanol does not undergo major changes in its structure upon adsorption with its C-O bond rotating nearly freely on the surface. Bonding to surface Ti atoms is a σ type transfer from the O2p of the ethanol-ethoxide species. Both ethanol and ethoxide present potential hole traps on O lone pairs. Charge density and work function analyses also suggest charge transfer from the adsorbate to the surface, in which the dissociative adsorptions show a larger charge transfer than the molecular adsorption mode. This journal is © 2012 the Owner Societies.

  17. Computational study of ethanol adsorption and reaction over rutile TiO2 (110) surfaces.

    Science.gov (United States)

    Muir, J M R; Muir, J N; Choi, Y; Idriss, H

    2012-09-14

    Studies of the modes of adsorption and the associated changes in electronic structures of renewable organic compounds are needed in order to understand the fundamentals behind surface reactions of catalysts for future energies. Using planewave density functional theory (DFT) calculations, the adsorption of ethanol on perfect and O-defected TiO(2) rutile (110) surfaces was examined. On both surfaces the dissociative adsorption mode on five-fold coordinated Ti cations (Ti(4+)(5c)) was found to be more favourable than the molecular adsorption mode. On the stoichiometric surface E(ads) was found to be equal to 0.85 eV for the ethoxide mode and equal to 0.76 eV for the molecular mode. These energies slightly increased when adsorption occurred on the Ti(4+)(5c) closest to the O-defected site. However, both considerably increased when adsorption occurred at the removed bridging surface O; interacting with Ti(3+) cations. In this case the dissociative adsorption becomes strongly favoured (E(ads) = 1.28 eV for molecular adsorption and 2.27 eV for dissociative adsorption). Geometry and electronic structures of adsorbed ethanol were analysed in detail on the stoichiometric surface. Ethanol does not undergo major changes in its structure upon adsorption with its C-O bond rotating nearly freely on the surface. Bonding to surface Ti atoms is a σ type transfer from the O2p of the ethanol-ethoxide species. Both ethanol and ethoxide present potential hole traps on O lone pairs. Charge density and work function analyses also suggest charge transfer from the adsorbate to the surface, in which the dissociative adsorptions show a larger charge transfer than the molecular adsorption mode.

  18. Surface Modification Effects on CNTs Adsorption of Methylene Blue and Phenol

    Directory of Open Access Journals (Sweden)

    A. H. Norzilah

    2011-01-01

    Full Text Available This study compares the adsorption capacity of modified CNTs using acid and heat treatment. The CNTs were synthesized from acetone and ethanol as carbon sources, using floating catalyst chemical vapor deposition (FC-CVD method. energy-dispersive X-ray spectroscopy (EDX and Boehm method revealed the existence of oxygen functional group on the surface of CNTs. Heat modification increases the adsorption capacity of as-synthesized CNTs for methylene blue (MB and phenol by approximately 76% and 50%, respectively. However, acid modification decreases the adsorption capacity. The equilibrium adsorption data fitted the Redlich-Peterson isotherm. For the adsorption kinetic study, the experimental data obeyed the pseudo-second-order model. Both modifications methods reduced the surface area and pore volume. The studies show that the adsorption of MB and phenol onto modified CNTs is much more influenced by their surface functional group than their surface area and pore volume.

  19. Surface electrical resistivity of insulators

    International Nuclear Information System (INIS)

    Senn, B. C.; Liesegang, J.

    1996-01-01

    A method is presented here for measuring surface charge decay, and theory has been developed so as to produce determinations of resistivity in the surface region of insulator films or wafers. This method incorporates the use of a coaxial cylindrical capacitor arrangement and an electrometer interfaced to a PC. The charge transport theory given here is based on Mott-Gurney diffusion, and allows easy interpretation of the experimental data, especially for the initial phase of surface charge decay. Resistivity measurements are presented for glass, mica, perspex and polyethylene, covering a range of 10 9 to 10 18 Ωm, as an illustration of the useful range of the instrument for static and antistatic materials, particularly in film or sheet form. Values for the surface charge diffusion constants of the materials are also presented. The charge transport theory has also been extended to allow the experimental and computational theoretical comparison of surface charge decay not only over the initial phase of charge decay, but also over longer times. The theoretical predictions show excellent agreement with experiment using the values for the diffusion constants referred to above

  20. The effect of surface structure on Ag atom adsorption over CuO(111) surfaces: A first principles study

    Science.gov (United States)

    Hu, Riming; Zhou, Xiaolong; Yu, Jie

    2017-12-01

    The interactions of Ag atom with different types of CuO(111) surface, including the perfect, oxygen-vacancy and precovered oxygen surfaces, have been systematically investigated using density functional theory (DFT) calculations to examine the effect of surface structures on Ag atom adsorption. The calculated results indicate that the Cu1-Cu1 bridge site and the oxygen-vacancy site are the active centres for atomic Ag adsorption on the perfect surface and the oxygen-vacancy surface respectively, while atomic Ag preferentially adsorbs at the Op site on the precovered oxygen surface. The activity of the CuO(111) surface for atomic Ag adsorption can be improved both on the perfect and oxygen-vacancy surfaces, while the activity of the CuO(111) surface for atomic Ag adsorption will be suppressed on precovered oxygen surfaces. Furthermore, the adsorption of NO on different CuO(111) surfaces with Ag adsorption was investigated, and the calculation results show that the adsorption of NO on an Ag-loaded CuO(111) surface is greater than that on the pure CuO(111) surface.

  1. Wear resistance of hydrophobic surfaces

    Science.gov (United States)

    Martinez, MA; Abenojar, J.; Pantoja, M.; López de Armentia, S.

    2017-05-01

    Nature has been an inspiration source to develop artificial hydrophobic surfaces. During the latest years the development of hydrophobic surfaces has been widely researched due to their numerous ranges of industrial applications. Industrially the use of hydrophobic surfaces is being highly demanded. This is why many companies develop hydrophobic products to repel water, in order to be used as coatings. Moreover, these coating should have the appropriated mechanical properties and wear resistance. In this work wear study of a hydrophobic coating on glass is carried out. Hydrophobic product used was Sika Crystal Dry by Sika S.A.U. (Alcobendas, Spain). This product is currently used on car windshield. To calculate wear resistance, pin-on-disk tests were carried out in dry and water conditions. The test parameters were rate, load and sliding distance, which were fixed to 60 rpm, 5 N and 1000 m respectively. A chamois was used as pin. It allows to simulate a real use. The friction coefficient and loss weight were compared to determinate coating resistance

  2. Structure of adsorption layers and conformation transformations of ethylhydroxyethylcellulose on surfaces of titanium and iron oxides

    Science.gov (United States)

    Bulychev, N. A.; Fomin, V. N.; Malyukova, E. B.; Ur'ev, N. B.

    2011-01-01

    Regularities of the adsorption of ethylhydroxyethylcellulose (EHEC) hydrophilic polymer on a surface of inorganic pigments of TiO2 and Fe2O3 were investigated by infrared spectroscopy. It was found that the adsorption interaction between EHEC and a surface of oxides is accompanied by conformation transformations of the adsorbed molecules of EHEC. The means by which macromolecules bind with active centers on a surface of metal oxides and the influence of the oxides' nature on the EHEC macromolecule conformation transformations determining the structure of the adsorption layer upon adsorption were established.

  3. Albumin adsorption onto surfaces of urine collection and analysis containers.

    Science.gov (United States)

    Robinson, Mary K; Caudill, Samuel P; Koch, David D; Ritchie, James; Hortin, Glen; Eckfeldt, John H; Sandberg, Sverre; Williams, Desmond; Myers, Gary; Miller, W Greg

    2014-04-20

    Adsorption of albumin onto urine collection and analysis containers may cause falsely low concentrations. We added (125)I-labeled human serum albumin to urine and to phosphate buffered solutions, incubated them with 22 plastic container materials and measured adsorption by liquid scintillation counting. Adsorption of urine albumin (UA) at 5-6 mg/l was containers, and to instrument sample cups and showed <1% change in concentration at 5 mg/l and <0.5% change at 20 mg/l or higher concentrations. Adsorption of albumin from phosphate buffered solutions (2-28%) was larger than that from urine. Albumin adsorption differed among urine samples and plastic materials, but the total influence of adsorption was <1% for all materials and urine samples tested. Adsorption of albumin from phosphate buffered solutions was larger than that from urine and could be a limitation for preparations used as calibrators. Copyright © 2014 Elsevier B.V. All rights reserved.

  4. Modeling adsorption and reactions of organic molecules at metal surfaces.

    Science.gov (United States)

    Liu, Wei; Tkatchenko, Alexandre; Scheffler, Matthias

    2014-11-18

    CONSPECTUS: The understanding of adsorption and reactions of (large) organic molecules at metal surfaces plays an increasingly important role in modern surface science and technology. Such hybrid inorganic/organic systems (HIOS) are relevant for many applications in catalysis, light-emitting diodes, single-molecule junctions, molecular sensors and switches, and photovoltaics. Obviously, the predictive modeling and understanding of the structure and stability of such hybrid systems is an essential prerequisite for tuning their electronic properties and functions. At present, density-functional theory (DFT) is the most promising approach to study the structure, stability, and electronic properties of complex systems, because it can be applied to both molecules and solids comprising thousands of atoms. However, state-of-the-art approximations to DFT do not provide a consistent and reliable description for HIOS, which is largely due to two issues: (i) the self-interaction of the electrons with themselves arising from the Hartree term of the total energy that is not fully compensated in approximate exchange-correlation functionals, and (ii) the lack of long-range part of the ubiquitous van der Waals (vdW) interactions. The self-interaction errors sometimes lead to incorrect description of charge transfer and electronic level alignment in HIOS, although for molecules adsorbed on metals these effects will often cancel out in total energy differences. Regarding vdW interactions, several promising vdW-inclusive DFT-based methods have been recently demonstrated to yield remarkable accuracy for intermolecular interactions in the gas phase. However, the majority of these approaches neglect the nonlocal collective electron response in the vdW energy tail, an effect that is particularly strong in condensed phases and at interfaces between different materials. Here we show that the recently developed DFT+vdW(surf) method that accurately accounts for the collective electronic

  5. External surface adsorption on silicalite-1 zeolite studied by molecular simulation

    NARCIS (Netherlands)

    Garcia-Perez, E.; Schnell, S.K.; Castillo, J.M.; Calero, S.; Kjelstrup, S.; Dubbeldam, D.; Vlugt, T.J.H.

    2011-01-01

    We have studied the adsorption of ethane, propane, and their mixtures on the external surface of silicalite-1 zeolite by molecular simulation using a classical force field. The ideal adsorbed solution theory (IAST) was successfully used to describe mixture adsorption, both on the external surface

  6. Surface stoichiometry of zinc sulfide and its effect on the adsorption behaviors of xanthate

    Directory of Open Access Journals (Sweden)

    Wang Meng

    2011-11-01

    Full Text Available Abstract In this paper, the surface stoichiometry, acid-base properties as well as the adsorption of xanthate at ZnS surfaces were studied by means of potentiometric titration, adsorption and solution speciation modeling. The surface proton binding site was determined by using Gran plot to evaluate the potentiometric titration data. Testing results implied that for stoichiometric surfaces of zinc sulfide, the proton and hydroxide determine the surface charge. For the nonstoichiometric surfaces, the surface charge is controlled by proton, hydroxide, zinc and sulfide ions depending on specific conditions. The xanthate adsorption decreases with increasing solution pH, which indicates an ion exchange reaction at the surfaces. Based on experimental results, the surface protonation, deprotonation, stoichiometry and xanthate adsorption mechanism were discussed.

  7. Adsorption of cations onto positively charged surface mesopores.

    Science.gov (United States)

    Neue, Uwe; Iraneta, Pamela; Gritti, Fabrice; Guiochon, Georges

    2013-11-29

    Uwe Neue developed a theoretical treatment to account for the adsorption of ions on mesopores of packing materials the walls of which are bonded to ionic ligands but left this work unfinished. We elaborated upon this treatment and refined it, based on the equivalence that he suggested between charged surface particles and a membrane that separates two ionic solutions but is impermeable to one specification. He had written that the electro-chemical potentials in both ionic solutions are equal (Donnan equilibrium). The equilibrium between the surface and the pore concentrations is accounted for by an homogeneous electrostatically modified Langmuir (EML) isotherm model. The theoretical results are presented for four different charge surface concentrations σ0=0, 0.001, 0.002, and 0.003C/m(2), using a phosphate buffer (W(S)pH=2.65) of ionic strength I=10mM. The average pore size, the specific surface area, and the specific pore volume of the stationary phase were Dp=140Å, Sp=182m(2)/g, and Vp=0.70cm(3)/g, respectively. The theoretical results provide the quantitative difference between the ionic strength, the pH, and the concentrations of all the ions in the pores and in the bulk eluent. The theory predicts (1) that the retention times of cations under linear conditions is lower and (2) that their band widths under overloaded conditions for a given retention factor shrinks when the surface charge density σ0 is increased. These theoretical results are in good agreement with experimental results published previously and explain them. Copyright © 2013 Elsevier B.V. All rights reserved.

  8. Surface complexation models for uranium adsorption in the sub-surface environment

    International Nuclear Information System (INIS)

    Payne, T.E.

    2007-01-01

    Adsorption experiments with soil component minerals under a range of conditions are being used to develop models of uranium(VI) uptake in the sub-surface environment. The results show that adsorption of U on iron oxides and clay minerals is influenced by chemical factors including the pH, partial pressure of CO 2 , and the presence of ligands such as phosphate. Surface complexation models (SCMs) can be used to simulate U adsorption on these minerals. The SCMs are based on plausible mechanistic assumptions and describe the experimental data more adequately than Kd values or sorption isotherms. It is conceptually possible to simulate U sorption data on complex natural samples by combining SCMs for individual component minerals. This approach was used to develop a SCM for U adsorption to mineral assemblages from Koongarra (Australia), and produced a reasonable description of U uptake. In order to assess the applicability of experimental data to the field situation, in-situ measurements of U distributions between solid and liquid phases were undertaken at the Koongarra U deposit. This field partitioning data showed a satisfactory agreement with laboratory sorption data obtained under comparable conditions. (author)

  9. The Effect of Nano-ZnO Surface Wettability on Modulating Protein Adsorption

    Science.gov (United States)

    Hu, Qian; Ding, Yadan; Shao, Hong; Cong, Tie; Yang, Xiaoguang; Hong, Xia

    2017-07-01

    Although surface wettability plays a major role in regulating protein adsorption and nanostructured ZnO has shown great potential in various biomedical fields, few reports have examined the influence of nano-ZnO surface wettability on protein adsorption. Herein, we explored the adsorption behavior of bovine serum albumin (BSA) on the superhydrophilic, hydrophilic, hydrophobic and superhydrophobic nano-ZnO surfaces. The adsorption amount of BSA increased with increase of hydrophilicity because of increased adsorption sites on the hydrophilic surface. The protein adsorption was proved to occur along with the desorption and conformational changes by well-fitted kinetic adsorption curves with the Spreading Particle Model and Fourier transformation infrared spectral analysis. The rates of BSA adsorption and desorption increased with hydrophobicity of the ZnO surfaces, which was considered to be related with the energy barrier created by water bound to the ZnO surfaces via hydrogen bonding. The rate of conformational change varied in a complex way, which might be influenced by the surface wettability of ZnO and some other factors. The present work may open up a new avenue to design nano-bio interfacial materials for advanced biological study and clinical applications.

  10. Competitive Adsorption of Plasma Proteins on Polysaccharide-Modified Silicon Surfaces

    National Research Council Canada - National Science Library

    Ombelli, Michela; Costello, Lauren B; Meng, Qing C; Composto, Russell J; Eckmann, David M

    2005-01-01

    .... Competitive protein adsorption plays a key role in the hemocompatibility of the surface. The synthesis of nonfouling surfaces is therefore one of the major prerequisites for devices for biomedical applications...

  11. A new theoretical approach to adsorption desorption behavior of Ga on GaAs surfaces

    Science.gov (United States)

    Kangawa, Y.; Ito, T.; Taguchi, A.; Shiraishi, K.; Ohachi, T.

    2001-11-01

    We propose a new theoretical approach for studying adsorption-desorption behavior of atoms on semiconductor surfaces. The new theoretical approach based on the ab initio calculations incorporates the free energy of gas phase; therefore we can calculate how adsorption and desorption depends on growth temperature and beam equivalent pressure (BEP). The versatility of the new theoretical approach was confirmed by the calculation of Ga adsorption-desorption transition temperatures and transition BEPs on the GaAs(0 0 1)-(4×2)β2 Ga-rich surface. This new approach is feasible to predict how adsorption and desorption depend on the growth conditions.

  12. Surface Charge Transfer Doping of Monolayer Phosphorene via Molecular Adsorption.

    Science.gov (United States)

    He, Yuanyuan; Xia, Feifei; Shao, Zhibin; Zhao, Jianwei; Jie, Jiansheng

    2015-12-03

    Monolayer phosphorene has attracted much attention owing to its extraordinary electronic, optical, and structural properties. Rationally tuning the electrical transport characteristics of monolayer phosphorene is essential to its applications in electronic and optoelectronic devices. Herein, we study the electronic transport behaviors of monolayer phosphorene with surface charge transfer doping of electrophilic molecules, including 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ), NO2, and MoO3, using density functional theory combined with the nonequilibrium Green's function formalism. F4TCNQ shows optimal performance in enhancing the p-type conductance of monolayer phosphorene. Static electronic properties indicate that the enhancement is originated from the charge transfer between adsorbed molecule and phosphorene layer. Dynamic transport behaviors demonstrate that additional channels for hole transport in host monolayer phosphorene were generated upon the adsorption of molecule. Our work unveils the great potential of surface charge transfer doping in tuning the electronic properties of monolayer phosphorene and is of significance to its application in high-performance devices.

  13. Americium adsorption on the surface of macrophytic algae

    Energy Technology Data Exchange (ETDEWEB)

    Carvalho, F.P.; Fowler, S.W.

    1985-01-01

    Data are presented on the rates at which americium (Am) deposits upon blade surfaces of three benthic algal species (Ulva rigida, Fucus vesiculosus and Gigartina stellata) following short-term exposures (1-6 h). Am is taken up in direct proportion to the ambient radionuclide concentration in sea water. Uptake by the green alga was 3 to 5 times greater than that for the brown and red species. Experimental evidence indicated that Am accumulation is a passive process and that adsorption takes place mainly on the thin outer organic coating of the seaweed. The Am transport coefficients are quite similar to that previously found for the naturally occurring ..cap alpha..-emitter /sup 210/Po, but are an order of magnitude lower than a plutonium transport coefficient reported in the literature. Release of labelled extracellular products associated with the algal surface coating is considered to be responsible for the rapid loss of Am observed previously in macroalgae and may in fact serve as a mechanism for transferring Am to filter feeding zooplankton. (author).

  14. Americium adsorption on the surface of macrophytic algae

    International Nuclear Information System (INIS)

    Carvalho, F.P.; Fowler, S.W.

    1985-01-01

    Data are presented on the rates at which americium (Am) deposits upon blade surfaces of three benthic algal species (Ulva rigida, Fucus vesiculosus and Gigartina stellata) following short-term exposures (1-6 h). Am is taken up in direct proportion to the ambient radionuclide concentration in sea water. Uptake by the green alga was 3 to 5 times greater than that for the brown and red species. Experimental evidence indicated that Am accumulation is a passive process and that adsorption takes place mainly on the thin outer organic coating of the seaweed. The Am transport coefficients are quite similar to that previously found for the naturally occurring α-emitter 210 Po, but are an order of magnitude lower than a plutonium transport coefficient reported in the literature. Release of labelled extracellular products associated with the algal surface coating is considered to be responsible for the rapid loss of Am observed previously in macroalgae and may in fact serve as a mechanism for transferring Am to filter feeding zooplankton. (author)

  15. Competitive Adsorption between Nanoparticles and Surface Active Ions for the Oil-Water Interface.

    Science.gov (United States)

    Hua, Xiaoqing; Bevan, Michael A; Frechette, Joelle

    2018-04-16

    Nanoparticles (NPs) can add functionality (e.g., catalytic, optical, rheological) to an oil-water interface. Adsorption of ∼10 nm NPs can be reversible; however, the mechanisms for adsorption and its effects on surface pressure remain poorly understood. Here we demonstrate how the competitive reversible adsorption of NPs and surfactants at fluid interfaces can lead to independent control of both the adsorbed amount and surface pressure. In contrast to prior work, both species investigated (NPs and surfactants) interact reversibly with the interface and without the surface active species binding to NPs. Independent measurements of the adsorption and surface pressure isotherms allow determination of the equation of state (EOS) of the interface under conditions where the NPs and surfactants are both in dynamic equilibrium with the bulk phase. The adsorption and surface pressure measurements are performed with gold NPs of two different sizes (5 and 10 nm), at two pH values, and across a wide concentration range of surfactant (tetrapentylammonium, TPeA + ) and NPs. We show that free surface active ions compete with NPs for the interface and give rise to larger surface pressures upon the adsorption of NPs. Through a competitive adsorption model, we decouple the contributions of NPs wetting at the interface and their surface activity on the measured surface pressure. We also demonstrate reversible control of adsorbed amount via changes in the surfactant concentration or the aqueous phase pH.

  16. Oxygen adsorption on the Al₉Co₂(001) surface: first-principles and STM study.

    Science.gov (United States)

    Villaseca, S Alarcón; Loli, L N Serkovic; Ledieu, J; Fournée, V; Gille, P; Dubois, J-M; Gaudry, E

    2013-09-04

    Atomic oxygen adsorption on a pure aluminum terminated Al9Co2(001) surface is studied by first-principle calculations coupled with STM measurements. Relative adsorption energies of oxygen atoms have been calculated on different surface sites along with the associated STM images. The local electronic structure of the most favourable adsorption site is described. The preferential adsorption site is identified as a 'bridge' type site between the cluster entities exposed at the (001) surface termination. The Al-O bonding between the adsorbate and the substrate presents a covalent character, with s-p hybridization occurring between the states of the adsorbed oxygen atom and the aluminum atoms of the surface. The simulated STM image of the preferential adsorption site is in agreement with experimental observations. This work shows that oxygen adsorption generates important atomic relaxations of the topmost surface layer and that sub-surface cobalt atoms strongly influence the values of the adsorption energies. The calculated Al-O distances are in agreement with those reported in Al2O and Al2O3 oxides and for oxygen adsorption on Al(111).

  17. Study of lysozyme mobility and binding free energy during adsorption on a graphene surface

    International Nuclear Information System (INIS)

    Nakano, C. Masato; Ma, Heng; Wei, Tao

    2015-01-01

    Understanding protein adsorption is a key to the development of biosensors and anti-biofouling materials. Hydration essentially controls the adsorption process on hydrophobic surfaces, but its effect is complicated by various factors. Here, we present an ideal model system to isolate hydration effects—lysozyme adsorption on a flat hydrophobic graphene surface. Our all-atom molecular dynamics and molecular-mechanics/Poisson-Boltzmann surface area computation study reveal that lysozyme on graphene displays much larger diffusivity than in bulk water. Protein's hydration free energy within the first hydration shell is dominated by the protein-water electrostatic interactions and acts as an energy barrier for protein adsorption. On the other hand, the surface tension, especially that from the hydrophobic graphene, can effectively weaken the barrier to promote adsorption

  18. Study of lysozyme mobility and binding free energy during adsorption on a graphene surface

    Energy Technology Data Exchange (ETDEWEB)

    Nakano, C. Masato [Flintridge Preparatory School, La Canada Flintridge, California 91011 (United States); Ma, Heng; Wei, Tao, E-mail: twei@lamar.edu [Dan F. Smith Department of Chemical Engineering, Lamar University, Beaumont, Texas 77710 (United States)

    2015-04-13

    Understanding protein adsorption is a key to the development of biosensors and anti-biofouling materials. Hydration essentially controls the adsorption process on hydrophobic surfaces, but its effect is complicated by various factors. Here, we present an ideal model system to isolate hydration effects—lysozyme adsorption on a flat hydrophobic graphene surface. Our all-atom molecular dynamics and molecular-mechanics/Poisson-Boltzmann surface area computation study reveal that lysozyme on graphene displays much larger diffusivity than in bulk water. Protein's hydration free energy within the first hydration shell is dominated by the protein-water electrostatic interactions and acts as an energy barrier for protein adsorption. On the other hand, the surface tension, especially that from the hydrophobic graphene, can effectively weaken the barrier to promote adsorption.

  19. Adsorption Mechanisms of NH3 on Chlorinated Si(100)-2 x 1 Surface

    International Nuclear Information System (INIS)

    Lee, Hee Soon; Choi, Cheol Ho

    2012-01-01

    The potential energy surfaces of ammonia molecule adsorptions on the symmetrically chlorinated Si(100)- 2 x 1 surface were explored with SIMOMM:MP2/6-31G(d). It was found that the initial nucleophilic attack by ammonia nitrogen to the surface Si forms a S N 2 type transition state, which eventually leads to an HCl molecular desorption. The second ammonia molecule adsorption requires much less reaction barrier, which can be rationalized by the surface cooperative effect. In general, it was shown that the surface Si-Cl bonds can be easily subjected to the substitution reactions by ammonia molecules yielding symmetric surface Si-NH 2 bonds, which can be a good initial template for subsequent surface chemical modifications. The ammonia adsorptions are in general more facile than the corresponding water adsorption, since ammonia is better nucleophile

  20. Adsorption of sugars on Al- and Ga-doped boron nitride surfaces: A computational study

    Energy Technology Data Exchange (ETDEWEB)

    Darwish, Ahmed A. [Center for Nanotechnology, Zewail City of Science and Technology, Giza 12588 (Egypt); Department of Nuclear and Radiation Engineering, Faculty of Engineering, Alexandria University, Alexandria (Egypt); Fadlallah, Mohamed M. [Center for Fundamental Physics, Zewail City of Science and Technology, Giza 12588 (Egypt); Department of Physics, Faculty of Science, Benha University, Benha (Egypt); Badawi, Ashraf [Center for Nanotechnology, Zewail City of Science and Technology, Giza 12588 (Egypt); Maarouf, Ahmed A., E-mail: ahmed.maarouf@egnc.gov.eg [Center for Fundamental Physics, Zewail City of Science and Technology, Giza 12588 (Egypt); Egypt Nanotechnology Center & Department of Physics, Faculty of Science, Cairo University, Giza 12613 (Egypt)

    2016-07-30

    Highlights: • Doping boron nitride sheets with aluminum or gallium atoms significantly enhances their molecular adsorption properties. • Adsorption of glucose or glucosamine on Al- and Ga-doped boron nitride sheets changes the band gap. • Doping concentration changes the bad gap, but has a minor effect on the adsorption energy. - Abstract: Molecular adsorption on surfaces is a key element for many applications, including sensing and catalysis. Non-invasive sugar sensing has been an active area of research due to its importance to diabetes care. The adsorption of sugars on a template surface study is at the heart of matter. Here, we study doped hexagonal boron nitride sheets (h-BNNs) as adsorbing and sensing template for glucose and glucosamine. Using first principles calculations, we find that the adsorption of glucose and glucosamine on h-BNNs is significantly enhanced by the substitutional doping of the sheet with Al and Ga. Including long range van der Waals corrections gives adsorption energies of about 2 eV. In addition to the charge transfer occurring between glucose and the Al/Ga-doped BN sheets, the adsorption alters the size of the band gap, allowing for optical detection of adsorption. We also find that Al-doped boron nitride sheet is better than Ga-doped boron nitride sheet to enhance the adsorption energy of glucose and glucosamine. The results of our work can be potentially utilized when designing support templates for glucose and glucosamine.

  1. Phosphate adsorption on aluminum-coordinated functionalized macroporous–mesoporous silica: Surface structure and adsorption behavior

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Weiya [Department of Chemistry, Jinan University, Guangzhou 510632 (China); Department of Materials Science and Engineering, Taizhou University, Linhai 317000 (China); Li, Dan [Environmetal Engineering, School of Engineering and Information Technology, Murdoch University, Murdoch, Western Australia 6150 (Australia); Zhu, Yi; Xu, Kai; Li, Jianqiang [Department of Chemistry, Jinan University, Guangzhou 510632 (China); Han, Boping [Institute of Hydrobiology, Jinan University, Guangzhou 510460 (China); Zhang, Yuanming, E-mail: tzhangym@jnu.edu.cn [Department of Chemistry, Jinan University, Guangzhou 510632 (China)

    2013-12-15

    Graphical abstract: - Highlights: • Al-coordinated functionalized macroporous–mesoporous silica for phosphate removal. • It had the maximum adsorption capacity of 23.59 mg P/g. • Over 95% of the final adsorption capacity reached in the first 1 min. - Abstract: In this study, Al(III)-coordinated diamino-functionalized macroporous–mesoporous silica was synthesized and characterized by X-ray diffraction, N{sub 2} adsorption–desorption, Fourier transform infrared spectroscopy, scanning and transmission electron microscopy. Because of well-defined and interconnecting macroporous–mesoporous networks, the resulting adsorbent (MM-SBA) exhibited a significantly better phosphate adsorption performance and faster removal rate, as compared with the mesoporous adsorbent (M-SBA). Based on the Freundlich and Langmuir models, the phosphate adsorption capacity and the maximum adsorption capacity of MM-SBA were 7.99 mg P/g and 23.59 mg P/g, respectively. In the kinetic study of MM-SBA, over 95% of its final adsorption capacity reached in the first 1 min; whereas that of M-SBA was less than 79%.

  2. Surface complexation modeling of uranyl adsorption on corrensite from the Waste Isolation Pilot Plant Site

    International Nuclear Information System (INIS)

    Park, Sang-Won; Leckie, J.O.; Siegel, M.D.

    1995-09-01

    Corrensite is the dominant clay mineral in the Culebra Dolomite at the Waste Isolation Pilot Plant. The surface characteristics of corrensite, a mixed chlorite/smectite clay mineral, have been studied. Zeta potential measurements and titration experiments suggest that the corrensite surface contains a mixture of permanent charge sites on the basal plane and SiOH and AlOH sites with a net pH-dependent charge at the edge of the clay platelets. Triple-layer model parameters were determined by the double extrapolation technique for use in chemical speciation calculations of adsorption reactions using the computer program HYDRAQL. Batch adsorption studies showed that corrensite is an effective adsorbent for uranyl. The pH-dependent adsorption behavior indicates that adsorption occurs at the edge sites. Adsorption studies were also conducted in the presence of competing cations and complexing ligands. The cations did not affect uranyl adsorption in the range studied. This observation lends support to the hypothesis that uranyl adsorption occurs at the edge sites. Uranyl adsorption was significantly hindered by carbonate. It is proposed that the formation of carbonate uranyl complexes inhibits uranyl adsorption and that only the carbonate-free species adsorb to the corrensite surface. The presence of the organic complexing agents EDTA and oxine also inhibits uranyl sorption

  3. Adsorption

    Directory of Open Access Journals (Sweden)

    Sushmita Banerjee

    2017-05-01

    Full Text Available Application of saw dust for the removal of an anionic dye, tartrazine, from aqueous solutions has been investigated. The experiments were carried out in batch mode. Effect of the parameters such as pH, initial dye concentration and temperature on the removal of the dye was studied. Equilibrium was achieved in 70 min. Maximum adsorption of dye was achieved at pH 3. Removal percent was found to be dependent on the initial concentration of dye solution, and maximum removal was found to be 97% at 1 mg/L of tartrazine. The removal increases from 71% to 97% when the initial concentration of dye solution decreases from 15 mg/L to 1 mg/L. The equilibrium adsorption data were analyzed by Langmuir, Freundlich, Temkin and Dubinin–Radushkevich isotherm models. The (Langmuir adsorption capacity of the adsorbent is found to be 4.71 mg/g at 318 K. Kinetic modeling of the process of removal was carried out and the process of removal was found to follow a pseudo second order model and the value of rate constant for adsorption process was calculated as 2.7 × 10−3 g mg−1 min−1 at 318 K. The thermodynamic parameters such as change in free energy (ΔG°, enthalpy (ΔH° and entropy (ΔS° were determined and the negative values of ΔG° indicated that the process of removal was spontaneous at all values of temperatures. Further, the values of ΔH° indicated the endothermic nature of the process of removal.

  4. Influence of activated carbon characteristics on toluene and hexane adsorption: Application of surface response methodology

    Science.gov (United States)

    Izquierdo, Mª Teresa; de Yuso, Alicia Martínez; Valenciano, Raquel; Rubio, Begoña; Pino, Mª Rosa

    2013-01-01

    The objective of this study was to evaluate the adsorption capacity of toluene and hexane over activated carbons prepared according an experimental design, considering as variables the activation temperature, the impregnation ratio and the activation time. The response surface methodology was applied to optimize the adsorption capacity of the carbons regarding the preparation conditions that determine the physicochemical characteristics of the activated carbons. The methodology of preparation produced activated carbons with surface areas and micropore volumes as high as 1128 m2/g and 0.52 cm3/g, respectively. Moreover, the activated carbons exhibit mesoporosity, ranging from 64.6% to 89.1% the percentage of microporosity. The surface chemistry was characterized by TPD, FTIR and acid-base titration obtaining different values of surface groups from the different techniques because the limitation of each technique, but obtaining similar trends for the activated carbons studied. The exhaustive characterization of the activated carbons allows to state that the measured surface area does not explain the adsorption capacity for either toluene or n-hexane. On the other hand, the surface chemistry does not explain the adsorption results either. A compromise between physical and chemical characteristics can be obtained from the appropriate activation conditions, and the response surface methodology gives the optimal activated carbon to maximize adsorption capacity. Low activation temperature, intermediate impregnation ratio lead to high toluene and n-hexane adsorption capacities depending on the activation time, which a determining factor to maximize toluene adsorption.

  5. Adsorption of lysozyme on base metal surfaces in the presence of an external electric potential.

    Science.gov (United States)

    Ei Ei, Htwe; Nakama, Yuhi; Tanaka, Hiroshi; Imanaka, Hiroyuki; Ishida, Naoyuki; Imamura, Koreyoshi

    2016-11-01

    The impact of external electric potential on the adsorption of a protein to base metal surfaces was examined. Hen egg white lysozyme (LSZ) and six types of base metal plates (stainless steel SUS316L (St), Ti, Ta, Zr, Cr, or Ni) were used as the protein and adsorption surface, respectively. LSZ was allowed to adsorb on the surface under different conditions (surface potential, pH, electrolyte type and concentration, surface material), which was monitored using an ellipsometer. LSZ adsorption was minimized in the potential range above a certain threshold and, in the surface potential range below the threshold, decreasing the surface potential increased the amount of protein adsorbed. The threshold potential for LSZ adsorption was shifted toward a positive value with increasing pH and was lower for Ta and Zr than for the others. A divalent anion salt (K2SO4) as an electrolyte exhibited the adsorption of LSZ in the positive potential range while a monovalent salt (KCl) did not. A comprehensive consideration of the obtained results suggests that two modes of interactions, namely the electric force by an external electric field and electrostatic interactions with ionized surface hydroxyl groups, act on the LSZ molecules and determine the extent of suppression of LSZ adsorption. All these findings appear to support the view that a base metal surface can be controlled for the affinity to a protein by manipulating the surface electric potential as has been reported on some electrode materials. Copyright © 2016 Elsevier B.V. All rights reserved.

  6. Methyl Butanoate Adsorption on MoS2 Surface: A Density Functional Theory Investigation

    Directory of Open Access Journals (Sweden)

    Prabowo Wahyu Aji Eko

    2018-01-01

    Full Text Available Methyl butanoate is one of the compound which is obtained from triglyceride molecule. It has hydrocarbon components and hence may produce hydrocarbon through hydrodeoxygenation (HDO or decarbonylation (DCO processes. The first step to uncover the underlying mechanism of HDO or DCO is to find the active site of methyl butanoate adsorption over the catalyst. This study attempts to investigate the active site of methyl butanoate adsorption on MoS2 surface. Stable bonding configuration for methyl butanoate adsorption on MoS2 is investigated by using density functional theory (DFT. This investigation consists of geometry optimisation and adsorption energy calculations. The stable configuration of methyl butanoate adsorption on MoS2 surface is found to be on top of Mo atom in Mo-edge surface.

  7. Study of the processes of adsorption of amine-containing surface-active substance on the surface of Aluminum powder

    Directory of Open Access Journals (Sweden)

    Antonina Dyuryagina

    2012-03-01

    Full Text Available Equilibrium characteristics of adsorption on a surface of a pigment depending on concentration factors and temperature of the dispersive environment are defined. Kinetic laws of superficial activity of binary, threefold homogeneous and heterogeneous modeling systems are studied. The estimation of mechanisms of process of adsorption is carried out.

  8. One-step polymer surface modification for minimizing drug, protein, and DNA adsorption in microanalytical systems

    DEFF Research Database (Denmark)

    Larsen, Esben Kjær Unmack; Larsen, Niels Bent

    2013-01-01

    The non-specific adsorption of dissolved analytes strongly reduces the sensitivity and reliability in polymer microanalytical systems. Here, a one-step aqueous phase procedure modifies polymer material surfaces to strongly reduce their non-specific adsorption of a broad range of organic analytes ...... systems, including polystyrene (PS), cyclic olefin copolymer (COC), liquid crystalline polymer (LCP), and polyimide (PI)....

  9. Preventing protein adsorption from a range of surfaces using an aqueous fish protein extract

    DEFF Research Database (Denmark)

    Pillai, Saju; Arpanaei, Ayyoob; Meyer, Rikke L.

    2009-01-01

    We utilize an aqueous extract of fish proteins (FPs) as a coating for minimizing the adsorption of fibrinogen (Fg) and human serum albumin (HSA). The surfaces include stainless steel (SS), gold (Au), silicon dioxide (SiO2), and poly(styrene) (PS). The adsorption processes (kinetics and adsorbed...

  10. Scaling relationships for adsorption energies of C2 hydrocarbons on transition metal surfaces

    DEFF Research Database (Denmark)

    Jones, Glenn; Studt, Felix; Abild-Pedersen, Frank

    2011-01-01

    Using density functional theory calculations we show that the adsorption energies for C2Hx-type adsorbates on transition metal surfaces scale with each other according to a simple bond order conservation model. This observation generalizes some recently recognized adsorption energy scaling laws...

  11. Specific surface area effect on adsorption of chlorpyrifos and TCP by soils and modeling

    Science.gov (United States)

    The adsorption of chlorpyrifos and TCP (3,5,6, trichloro-2-pyridinol) was determined in four soils (Mollisol, Inceptisol, Entisol, Alfisol) having different specific surface areas (19–84 m2/g) but rather similar organic matter content (2.4–3.5%). Adsorption isotherms were derived from batch equilibr...

  12. Adsorption of croconate dyes on TiO2 anatase (101) surface: A ...

    Indian Academy of Sciences (India)

    Abstract. The adsorption of model croconate dyes on the stoichiometric TiO2 anatase (101) surface has been studied by means of periodic density functional calculations to understand the adsorption of the diketo. (-COCO-) groups. Past experimental and theoretical results have shown the strong binding ability of the acid.

  13. Infrared spectroscopic study of radiation-induced adsorption of n-hexane on a beryllium surface

    Science.gov (United States)

    Gadzhieva, N. N.

    2017-07-01

    Radiation-stimulated adsorption on a beryllium surface is studied by IR reflection-absorption spectroscopy. It is found that γ-irradiation at room temperature leads to the appearance of n-hexane adsorption centers on a beryllium surface according to molecular and dissociation mechanisms. The kinetics of n-hexane adsorption in a Be- n-hexane system is studied; activated dissociative chemisorption accompanied by formation of beryllium alkyls and surface hydrides is observed at absorbed doses 15 kGy ≤ Vγ ≤ 35 kGy. A possible mechanism of this process is suggested.

  14. Effect of grain size on uranium(VI) surface complexation kinetics and adsorption additivity.

    Science.gov (United States)

    Shang, Jianying; Liu, Chongxuan; Wang, Zheming; Zachara, John M

    2011-07-15

    The contribution of variable grain sizes to uranium adsorption/desorption was studied using a sediment from the US DOE Hanford site. The sediment was wet sieved into four size fractions: coarse sand (1-2 mm), medium sand (0.2-1 mm), fine sand (0.053-0.2 mm), and clay/silt fraction (effects of size-specific adsorption site concentration and kinetic rate constants. The larger-size fraction had a larger mass percentage in the sediment but with a smaller adsorption site concentration and generally a slower uranium adsorption/desorption rate. The same equilibrium surface complexation reaction and reaction constant could describe uranium adsorption isotherms for all size fractions and the composite after accounting for the effect of adsorption site concentration. Mass-weighted, linear additivity was observed for both uranium adsorption isotherms and adsorption/desorption kinetics in the composite. One important implication of this study is that grain-size distribution may be used to estimate uranium adsorption site and adsorption/desorption kinetic rates in heterogeneous sediments from a common location.

  15. High coverage water adsorption on the CuO(111) surface

    Science.gov (United States)

    Yu, Xiaohu; Zhang, Xuemei; Wang, Hongtao; Feng, Gang

    2017-12-01

    Water adsorption on the CuO(111) surface at different coverage has been systematically studied by spin-polarized density functional theory calculations (GGA+U) and atomic thermodynamics. Both molecular and dissociative adsorptions are studied. It is found that H2O molecule can chirally adsorb on CuO(111) surface which maybe play an important role in catalysis field. Molecular H2O adsorption is preferred for one H2O molecule, while mixed molecular and dissociative coadsorption is preferred on CuO(111) surface for two, three and four H2O molecules. Molecular and dissociative H2O adsorption can coexist at high temperature by using Boltzmann statistics. The phase diagram shows that only three surface configurations are stable thermodynamically: clean CuO(111) surface, two H2O and four H2O adsorption. The surface uncoordinated copper and oxygen atoms, and hydrogen bonding contribute to the adsorption energies. H2O adsorption mechanism has been analyzed by projected density of states (PDOS).

  16. Theoretical analysis of adsorption thermodynamics for hydrophobic peptide residues on SAM surfaces of varying functionality.

    Science.gov (United States)

    Latour, Robert A; Rini, Christopher J

    2002-06-15

    At a fundamental level, protein adsorption to a synthetic surface must be strongly influenced by the interaction between the peptide residues presented by the protein's surface (primary protein structure) and the functional groups presented by the synthetic surface. In this study, semi-empirical molecular modeling was used along with experimental wetting data to theoretically approach protein adsorption at this primary structural level. Changes in enthalpy, entropy, and Gibbs free energy were calculated as a function of residue-surface separation distance for the adsorption of individual hydrophobic peptide residues (valine, leucine, phenylalanine) on alkanethiol self-assembled monolayers on gold [Au-S(CH(2))(15)-X; X = CH(3), OH, NH(3)(+), COO(-)]. The results predict that the adsorption of each type of hydrophobic residue is energetically favorable and entropy dominated on a methyl-terminated hydrophobic surface, energetically unfavorable and enthalpy dominated on a hydroxyl-terminated neutral hydrophilic surface, and very slightly favorable to unfavorable and enthalpy dominated on charged surfaces. These theoretical results provide a basis for understanding some of the fundamental effects governing protein adsorption to synthetic surfaces. This level of understanding is needed for the proactive design of surfaces to control protein adsorption and subsequent cellular response for both implant and tissue engineering applications. Copyright 2002 Wiley Periodicals, Inc. J Biomed Mater Res 60: 564-577, 2002

  17. Fast Adsorption of Soft Hydrogel Microspheres on Solid Surfaces in Aqueous Solution.

    Science.gov (United States)

    Matsui, Shusuke; Kureha, Takuma; Hiroshige, Seina; Shibata, Mikihiro; Uchihashi, Takayuki; Suzuki, Daisuke

    2017-09-25

    The real-time adsorption behavior of polymeric colloidal microspheres onto solid surfaces in aqueous solution was visualized for the first time using high-speed atomic force microscopy (HS-AFM) to reveal how the softness of the microspheres affects their dynamic adsorption. Studies that focus on the deformability of microspheres upon dynamic adsorption have not yet been reported, most likely on account of a lack of techniques that appropriately depict the dynamic adsorption and deformation behavior of individual microspheres at the nanoscale in real time. In this study, the deformability of microspheres plays a crucial role on the adsorption kinetics, that is, soft hydrogel microspheres adsorb faster than harder elastomeric or rigid microspheres. These results should provide insight towards development of new colloidal nanomaterials that exhibit effective adsorption on specific sites in aqueous solution. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  18. Selective adsorption of toluene-3,4-dithiol on Si(553)-Au surfaces

    Science.gov (United States)

    Suchkova, Svetlana; Hogan, Conor; Bechstedt, Friedhelm; Speiser, Eugen; Esser, Norbert

    2018-01-01

    The adsorption of small organic molecules onto vicinal Au-stabilized Si(111) surfaces is shown to be a versatile route towards controlled growth of ordered organic-metal hybrid one-dimensional nanostructures. Density functional theory is used to investigate the site-specific adsorption of toluene-3,4-dithiol (TDT) molecules onto the clean Si(553)-Au surface and onto a co-doped surface whose steps are passivated by hydrogen. We find that the most reactive sites involve bonding to silicon at the step edge or on the terraces, while gold sites are relatively unfavored. H passivation and TDT adsorption both induce a controlled charge redistribution within the surface layer, causing the surface metallicity, electronic structure, and chemical reactivity of individual adsorption sites to be substantially altered.

  19. Theoretical and Experimental Analysis of Adsorption in Surface-based Biosensors

    DEFF Research Database (Denmark)

    Hansen, Rasmus

    The present Ph.D. dissertation concerns the application of surface plasmon resonance (SPR) spectroscopy, which is a surface-based biosensor technology, for studies of adsorption dynamics. The thesis contains both experimental and theoretical work. In the theoretical part we develop the theory...... for convection, diffusion, and adsorption in surface-based biosensors in general. In particular, we study the transport dynamics in a model geometry of a Biacore SPR sensor. An approximate quasi-steady theory, which has been widely adopted in the SPR literature to capture convective and diffusive mass transport...... is critical for reliable use of the quasi-steady theory. Our theoretical results provide users of surface-based biosensors with a tool of correcting experimentally obtained adsorption rate constants, based on the quasisteady theory. Finally, the consequence of adsorption on all surfaces present in the flow...

  20. 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.)

  1. Optimization of lead adsorption of mordenite by response surface methodology: characterization and modification.

    Science.gov (United States)

    Turkyilmaz, Havva; Kartal, Tolga; Yigitarslan Yildiz, Sibel

    2014-01-06

    In order to remove heavy metals, water treatment by adsorption of zeolite is gaining momentum due to low cost and good performance. In this research, the natural mordenite was used as an adsorbent to remove lead ions in an aqueous solution. The effects of adsorption temperature, time and initial concentration of lead on the adsorption yield were investigated. Response surface methodology based on Box-Behnken design was applied for optimization. Adsorption data were analyzed by isotherm models. The process was investigated by batch experiments; kinetic and thermodynamic studies were carried out. Adsorption yields of natural and hexadecyltrimethylammonium-bromide-modified mordenite were compared. The optimum conditions of maximum adsorption (nearly 84 percent) were found as follows: adsorption time of 85-90 min, adsorption temperature of 50°C, and initial lead concentration of 10 mg/L. At the same optimum conditions, modification of mordenite produced 97 percent adsorption yield. The most appropriate isotherm for the process was the Freundlich. Adsorption rate was found as 4.4. Thermodynamic calculations showed that the adsorption was a spontaneous and an exothermic process. Quadratic model and reduced cubic model were developed to correlate the variables with the adsorption yield of mordenite. From the analysis of variance, the most influential factor was identified as initial lead concentration. At the optimum conditions modification increased the adsorption yield up to nearly 100 percent. Mordenite was found an applicable adsorbent for lead ions especially in dilute solutions and may also be applicable in more concentrated ones with lower yields.

  2. Adsorption Mechanism of Inhibitor and Guest Molecules on the Surface of Gas Hydrates.

    Science.gov (United States)

    Yagasaki, Takuma; Matsumoto, Masakazu; Tanaka, Hideki

    2015-09-23

    The adsorption of guest and kinetic inhibitor molecules on the surface of methane hydrate is investigated by using molecular dynamics simulations. We calculate the free energy profile for transferring a solute molecule from bulk water to the hydrate surface for various molecules. Spherical solutes with a diameter of ∼0.5 nm are significantly stabilized at the hydrate surface, whereas smaller and larger solutes exhibit lower adsorption affinity than the solutes of intermediate size. The range of the attractive force is subnanoscale, implying that this force has no effect on the macroscopic mass transfer of guest molecules in crystal growth processes of gas hydrates. We also examine the adsorption mechanism of a kinetic hydrate inhibitor. It is found that a monomer of the kinetic hydrate inhibitor is strongly adsorbed on the hydrate surface. However, the hydrogen bonding between the amide group of the inhibitor and water molecules on the hydrate surface, which was believed to be the driving force for the adsorption, makes no contribution to the adsorption affinity. The preferential adsorption of both the kinetic inhibitor and the spherical molecules to the surface is mainly due to the entropic stabilization arising from the presence of cavities at the hydrate surface. The dependence of surface affinity on the size of adsorbed molecules is also explained by this mechanism.

  3. Inter-row Adsorption Configuration and Stability of Threonine Adsorbed on the Ge(100) Surfaces

    International Nuclear Information System (INIS)

    Lee, Myungjin; Park, Youngchan; Jeong, Hyuk; Lee, Hangil

    2013-01-01

    The adsorption structures of threonine on the Ge(100) surface were investigated using core-level photoemission spectroscopy (CLPES) in conjunction with density functional theory (DFT) calculations. CLPES measurements were performed to identify the experimentally preferred adsorption structure. The preferred structure indicated the relative reactivities of the carboxyl and hydroxymethyl groups as electron donors to the Ge(100) surface during adsorption. The core-level C 1s, N 1s, and O 1s CLPES spectra indicated that the carboxyl oxygen competed more strongly with the hydroxymethyl oxygen during the adsorption reaction. Three among six possible adsorption structures were identified as energetically favorable using DFT calculation methods that considered the inter- and intra-bonding configurations upon adsorption onto the Ge(100) surface. These structures were O-H dissociated N dative inter bonding, O-H dissociated N dative intra bonding, O-H dissociation bonding. One of the adsorption structures: O-H dissociated N dative inter bonding was predicted to be stable in light of the transition state energies. We thus confirmed that the most favorable adsorption structure is the O-H dissociated N dative-inter bonding structure using CLPES and DFT calculation

  4. An experimental-computer modeling study of inorganic phosphates surface adsorption on hydroxyapatite particles.

    Science.gov (United States)

    Rivas, Manuel; Casanovas, Jordi; del Valle, Luis J; Bertran, Oscar; Revilla-López, Guillermo; Turon, Pau; Puiggalí, Jordi; Alemán, Carlos

    2015-06-07

    The adsorption of orthophosphate, pyrophosphate, triphosphate and a trisphosphonate onto hydroxyapatite has been examined using experiments and quantum mechanical calculations. Adsorption studies with FTIR and X-ray photoelectron spectroscopies have been performed considering both crystalline hydroxyapatite (HAp) and amorphous calcium phosphate particles, which were specifically prepared and characterized for this purpose. Density functional theory (DFT) calculations have been carried out considering the (100) and (001) surfaces of HAp, which were represented using 1 × 2 × 2 and 3 × 3 × 1 slab models, respectively. The adsorption of phosphate onto the two crystallographic surfaces is very much favored from an energetic point of view, which is fully consistent with current interpretations of the HAp growing process. The structures calculated for the adsorption of pyrophosphate and triphosphate evidence that this process is easier for the latter than for the former. Thus, the adsorption of pyrophosphate is severely limited by the surface geometry while the flexibility of triphosphate allows transforming repulsive electrostatic interactions into molecular strain. On the other hand, calculations predict that the trisphosphonate only adsorbs onto the (001) surface of HAp. Theoretical predictions are fully consistent with experimental data. Thus, comparison of DFT results and spectroscopic data suggests that the experimental conditions used to prepare HAp particles promote the predominance of the (100) surface. Accordingly, experimental identification of the adsorption of trisphosphonate onto such crystalline particles is unclear while the adsorption of pyrophosphate and triphosphate is clearly observed.

  5. A combined QCM and XPS investigation of asphaltene adsorption on metal surfaces.

    Science.gov (United States)

    Rudrake, Amit; Karan, Kunal; Horton, J Hugh

    2009-04-01

    To investigate asphaltene-metal interactions, a combined quartz crystal microbalance (QCM) and X-ray photoelectron spectroscopy (XPS) study of asphaltene adsorption on a gold surface was conducted. Adsorption experiments were conducted at 25 degrees C with solutions of asphaltenes in toluene at concentrations ranging from 50 to 1500 ppm. QCM measurements yielded information on the kinetics of adsorption and further assessment of the data allowed the estimation of equilibrium adsorption levels. XPS analysis of adsorbed and bulk asphaltene demonstrated the presence of carboxylic, thiophenic, sulfide, pyridinic and pyrrolic type functional groups. The intensity of the main carbon (C-H) peak was related to surface coverage of adsorbed asphaltene as a function of asphaltene concentration by a simple mathematical model. The mass adsorption data from the QCM experiments also allowed estimation of the surface coverage, which was compared to those from XPS analyses. Surface coverage estimates as a function of asphaltene concentration could be described by a Langmuir (type-I) isotherm. The free energy of asphaltene adsorption was estimated to be -26.8+/-0.1 and -27.3+/-0.1 kJ/mol from QCM and XPS data, respectively assuming asphaltene molar mass of 750 g/gmol. QCM and XPS data was also analyzed to estimate adsorbed layer thickness after accounting for surface coverage. The thickness of the adsorbed asphaltene estimated from both XPS and QCM data analyses ranged from 6-8 nm over the entire range of adsorption concentrations investigated.

  6. Nanometer polymer surface features: the influence on surface energy, protein adsorption and endothelial cell adhesion

    Science.gov (United States)

    Carpenter, Joseph; Khang, Dongwoo; Webster, Thomas J.

    2008-12-01

    Current small diameter (lactic-co-glycolic acid) (PLGA) surfaces elevated endothelial cell adhesion, proliferation, and extracellular matrix synthesis when compared to nanosmooth surfaces. Nonetheless, these studies failed to address the importance of lateral and vertical surface feature dimensionality coupled with surface free energy; nor did such studies elicit an optimum specific surface feature size for promoting endothelial cell adhesion. In this study, a series of highly ordered nanometer to submicron structured PLGA surfaces of identical chemistry were created using a technique employing polystyrene nanobeads and poly(dimethylsiloxane) (PDMS) molds. Results demonstrated increased endothelial cell adhesion on PLGA surfaces with vertical surface features of size less than 18.87 nm but greater than 0 nm due to increased surface energy and subsequently protein (fibronectin and collagen type IV) adsorption. Furthermore, this study provided evidence that the vertical dimension of nanometer surface features, rather than the lateral dimension, is largely responsible for these increases. In this manner, this study provides key design parameters that may promote vascular graft efficacy.

  7. Effect of the selective adsorption on the reactive scattering process of molecular beams from stepped surfaces

    International Nuclear Information System (INIS)

    Garcia, N.

    1977-01-01

    An indicative proposal which may explain the diffusion of incident atomic beams scattered by a crystal surface is made in terms of the selective adsorption mechanism. In this sense, the stepped metallic surfaces present characteristics which enhance the displacements and the lifetimes of the beams on the surface. This may be important for increasing the exchange reactive scattering of molecules from crystal surfaces

  8. Competitive adsorption of monoclonal antibodies and nonionic surfactants at solid hydrophobic surfaces

    DEFF Research Database (Denmark)

    Kapp, Sebastian J; Larsson, Iben; van de Weert, Marco

    2015-01-01

    , such as infusion bags and i.v. lines. Total internal reflection fluorescence and quartz crystal microbalance with dissipation monitoring were used to follow and quantify this. Furthermore, the influence of the nonionic surfactant polysorbate 80 (PS80) on the adsorption process of these two antibodies...... was investigated. Despite belonging to two different IgG subclasses, both antibodies displayed comparable adsorption behavior. Both antibodies readily adsorbed in the absence of PS80, whereas adsorption was reduced in the presence of 30 mg/L surfactant. The sequence of exposure of the surfactant and protein...... to the surface was found to have a major influence on the extent of protein adsorption. Although only a fraction of adsorbed protein could be removed by rinsing with 30 mg/L surfactant solution, adsorption was entirely prevented when surfaces were pre-exposed to PS80. © 2014 Wiley Periodicals, Inc...

  9. Surface alloy formation by adsorption of holmium on Ag/Mo(112) bimetallic surfaces

    Science.gov (United States)

    Kołaczkiewicz, Jan; Oleksy, Czesław

    2018-03-01

    Work function change measurements, low energy electron diffraction (LEED) and density functional theory (DFT) are used to determine the structures formed on Ag/Mo(112) bimetallic surfaces upon deposition of 0.5 monolayer (ML) of holmium. As the bimetallic surfaces, we have chosen the Mo(112) substrate covered with 1 or 2 ML of Ag. Such surfaces have the same symmetry as the Mo(112) face but different electronic properties. LEED experiment indicates that the c(2 × 2) structure is formed on (1 ML Ag)/Mo(112) bimetallic surface upon deposition of 0.5 ML of Ho. DFT calculations show that a type of Ag-Ho surface alloy is formed, with Ho atoms 0.6 Å below the distorted layer of Ag. This is neither a substitutional nor a subsurface alloy. It is found that the adsorption structure formed on the (2 ML Ag)/Mo(112) bimetallic surface depends on the annealing temperature. After deposition of 0.5 ML of Ho at 300 K, the LEED pattern of p(2 × 2) symmetry is observed. Annealing of the overlayer at 640 K irreversibly changes the p(2 × 2) pattern into a pattern of c(2 × 2) type. The results of DFT computations show that the c(2 × 2) structure of the Ag-Ho surface alloy is energetically most favorable. In this structure, 0.5 ML of Ho is between the two monolayers of Ag, and the symmetry of the topmost layer is changed. The work function change calculated for the c(2 × 2) structure is in a good agreement with the measured value (0.22 eV). The results show that adsorption of Ho on the Ag/Mo(112) bimetallic surfaces is substantially different than on the clean Mo(112).

  10. Stability of Fluorosurfactant Adsorption on Mineral Surface for Water Removal in Tight Gas Reservoirs

    Directory of Open Access Journals (Sweden)

    Lijun You

    2015-01-01

    Full Text Available Long-term effectiveness of rock wettability alteration for water removal during gas production from tight reservoir depends on the surfactant adsorption on the pore surface of a reservoir. This paper selected typical cationic fluorosurfactant FW-134 as an example and took advantage of Fourier transform infrared spectroscopy (FTIR, X-ray photoelectron spectroscopy (XPS, and atomic force microscope (AFM to investigate its adsorption stability on the rock mineral surface under the oscillation condition at high temperature for a long time. The experimental results indicate that the F element content on the sample surface increases obviously, the surface structure of fluorine-carbonization also undergoes a significant change, and the fluorine surfactant exhibits a good interfacial modification and wettability alteration ability due to its adsorption on the pore surface transforming the chemical structure of the original surface. The adsorption increases indistinctly with the concentration of over 0.05% due to a single layer adsorption structure and is mainly electrostatic adsorption because the chemical bonding between the fluorosurfactant and the rock mineral surface, the hydrogen bonding, is weak and inconspicuous.

  11. Prediction of iodide adsorption on oxides by surface complexation modeling with spectroscopic confirmation.

    Science.gov (United States)

    Nagata, Takahiro; Fukushi, Keisuke; Takahashi, Yoshio

    2009-04-15

    A deficiency in environmental iodine can cause a number of health problems. Understanding how iodine is sequestered by materials is helpful for evaluating and developing methods for minimizing human health effects related to iodine. In addition, (129)I is considered to be strategically important for safety assessment of underground radioactive waste disposal. To assess the long-term stability of disposed radioactive waste, an understanding of (129)I adsorption on geologic materials is essential. Therefore, the adsorption of I(-) on naturally occurring oxides is of environmental concern. The surface charges of hydrous ferric oxide (HFO) in NaI electrolyte solutions were measured by potentiometric acid-base titration. The surface charge data were analyzed by means of an extended triple-layer model (ETLM) for surface complexation modeling to obtain the I(-) adsorption reaction and its equilibrium constant. The adsorption of I(-) was determined to be an outer-sphere process from ETLM analysis, which was consistent with independent X-ray absorption near-edge structure (XANES) observation of I(-) adsorbed on HFO. The adsorption equilibrium constants for I(-) on beta-TiO(2) and gamma-Al(2)O(3) were also evaluated by analyzing the surface charge data of these oxides in NaI solution as reported in the literature. Comparison of these adsorption equilibrium constants for HFO, beta-TiO(2), and gamma-Al(2)O(3) based on site-occupancy standard states permitted prediction of I(-) adsorption equilibrium constants for all oxides by means of the Born solvation theory. The batch adsorption data for I(-) on HFO and amorphous aluminum oxide were reasonably reproduced by ETLM with the predicted equilibrium constants, confirming the validity of the present approach. Using the predicted adsorption equilibrium constants, we calculated distribution coefficient (K(d)) values for I(-) adsorption on common soil minerals as a function of pH and ionic strength.

  12. Combined DFT and XPS investigation of iodine anions adsorption on the sulfur terminated (001) chalcopyrite surface

    Energy Technology Data Exchange (ETDEWEB)

    Li, Kui, E-mail: likui9606@stu.xjtu.edu.cn [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049 (China); Zhao, Yaolin, E-mail: zhaoyaolin@mail.xjtu.edu.cn [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049 (China); Zhang, Peng, E-mail: zp32@qq.com [Sino Shaanxi Nuclear Industry Group, Xi’an 710100 (China); He, Chaohui, E-mail: hechaohui@mail.xjtu.edu.cn [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049 (China); Deng, Jia, E-mail: djkokocase@stu.xjtu.edu.cn [School of Nuclear Science and Technology, Xi’an Jiaotong University, Xi’an 710049 (China); Ding, Shujiang, E-mail: dingsj@mail.xjtu.edu.cn [Department of Applied Chemistry, School of Science, Xi’an Jiaotong University, Xi’an 710049 (China); Shi, Weiqun, E-mail: shiwq@ihep.ac.cn [Key Laboratory of Nuclear Radiation and Nuclear Energy Technology and Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049 (China)

    2016-12-30

    Highlights: • Metal surface sites of (001)-S surface of chalcopyrite show significant chemical affinity to iodide and iodate. • The energetically favorable active site is copper for iodide adsorption and iron for iodate adsorption, respectively. • Iodate undergoes a dissociative adsorption on the copper site of chalcopyrite surface. - Abstract: The adsorption of iodine anions (iodide and iodate) on the sulfur terminated (001) chalcopyrite surface has been systematically investigated combining first-principles calculations based on density functional theory (DFT) with X-ray photoelectron spectroscopy (XPS) measurements. Based on the total energy calculations and geometric optimization, the thermodynamically preferred site was copper atom for iodide adsorption and iron atom for iodate adsorption, respectively. In the case of Cu site mode, the iodate underwent a dissociative adsorption, where one I−O bond of iodate ion was broken and the dissociative oxygen atom adsorbed on the adjacent sulphur site. Projected density of states (PDOS) analysis further clarified the interaction mechanism between active sites of chalcopyrite surface and adsorbates. In addition, full-range XPS spectra qualitatively revealed the presence of iodine on chalcopyrite surface. High resolution XPS spectra of the I 3d peaks after adsorption verified the chemical environment of iodine. The binding energies of 618.8 eV and 623.5 eV for I 3d{sub 5/2} peaks unveiled that the adsorption of iodide and iodate ions on copper-iron sulfide minerals was the result of formation of low solubility metal iodides precipitate. Also two I 3d peaks with low intensity around 618 eV and 630 eV might be related to the inorganic reduction of iodate to iodide by reducing S{sup 2−} ion of chalcopyrite.

  13. Combined quantum chemistry and Monte Carlo simulation of competitive adsorption of O{sub 2} and OH on Pt surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Li, Rui, E-mail: ruililcu@gmail.com [Department of Chemistry, Liaocheng University, Liaocheng 252059 (China); Li, Haibo; Xu, Shuling [Department of Chemistry, Liaocheng University, Liaocheng 252059 (China); Liu, Jifeng, E-mail: liujifeng111@gmail.com [Key Laboratory of Food Nutrition and Safety, Ministry of Education of China, Tianjin University of Science and Technology, Tianjin 300457 (China)

    2017-07-15

    Highlights: • Competitive adsorption of O{sub 2} and OH on different Pt surfaces was theoretically studied. • The adsorption energies of O{sub 2} and OH depend on the Pt surfaces and the adsorption sites. • The order of O{sub 2} adsorption efficiency was characterized. - Abstract: To obtain a microscopic explanation on the difference of oxygen reduction reaction activity on different Pt low index surfaces, we simulated competitive adsorptions of O{sub 2} and OH on four Pt low index surfaces. Firstly, all possible chemical adsorption configurations of the O{sub 2} and OH molecules on the three surfaces were acquired through density functional theory. The distribution of these configurations on the different surfaces was collected from Monte Carlo simulations. Our results demonstrated that the adsorption energy order of O{sub 2} on different surfaces was (110)(1 × 2) > (110) > (100) > (111) and that the adsorption energy order of the OH molecules on Pt surfaces was the same. Considering the competitive adsorption of O{sub 2} and OH on Pt surfaces, the final O{sub 2} adsorption efficiencies order of three surfaces was (111) > (110) > (100) > (110)(1 × 2), which was consistent with the experimental activities of oxygen reduction. Our study provided theoretical references for previous experimental studies and had important significance for the understanding of oxygen adsorption on Pt surfaces.

  14. Influence of preadsorbed oxygen on the sign and magnitude of the chemisorption-induced resistance change for H2 adsorption onto Fe films

    Science.gov (United States)

    Shanabarger, M. R.

    1986-01-01

    Measurements have been made of the chemisorption-induced resistance change for H2 adsorbed onto Fe film substrates predosed with fixed coverages of chemisorbed oxygen. The measurements were made at temperatures from 295 to 340 K and for estimated oxygen coverages of less than 0.1 monolayers. Two distinct resistance change components were observed in both the adsorption kinetics and the equilibrium isotherms: a positive component which is associated with the adsorption of H2 onto a clean Fe surface, and a negative component which was correlated with the presence of the chemisorbed oxygen. The resistance change isotherms can be fit with a model which assumes that each of the resistance change components result from dissociative chemisorbed hydrogen. Possible mechanisms for the chemisorbed-oxygen-induced negative resistance change are discussed.

  15. Effects of chemical functional groups on elemental mercury adsorption on carbonaceous surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Liu Jing, E-mail: liujing27@mail.hust.edu.cn [State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074 (China); Cheney, Marcos A. [Department of Natural Sciences, University of Maryland Eastern Shore, Princess Anne, MD 21853 (United States); Wu Fan; Li Meng [State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074 (China)

    2011-02-15

    A systematic theoretical study using density functional theory is performed to provide molecular-level understanding of the effects of chemical functional groups on mercury adsorption on carbonaceous surfaces. The zigzag and armchair edges were used in modeling the carbonaceous surfaces to simulate different adsorption sites. The edge atoms on the upper side of the models are unsaturated to simulate active sites. All calculations (optimizations, energies, and frequencies) were made at B3PW91 density functional theory level, using RCEP60VDZ basis set for mercury and 6-31G(d) pople basis set for other atoms. The results indicate that the embedding of halogen atom can increase the activity of its neighboring site which in turn increases the adsorption capacity of the carbonaceous surface for Hg{sup 0}. The adsorption belongs to chemisorptions, which is in good agreement with the experimental results. For the effects of oxygen functional groups, lactone, carbonyl and semiquinone favor Hg{sup 0} adsorption because they increase the neighboring site's activity for mercury adsorption. On the contrary, phenol and carboxyl functional groups show a physisorption of Hg{sup 0}, and reduce Hg capture. This result can explain the seemingly conflicting experimental results reported in the literature concerning the influence of oxygen functional groups on mercury adsorption on carbonaceous surface.

  16. The surface characteristics of hyperbranched polyamide modified corncob and its adsorption property for Cr(VI)

    Energy Technology Data Exchange (ETDEWEB)

    Lin, Hai, E-mail: linhai@ces.ustb.edu.cn [School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083 (China); Beijing Key Laboratory on Resource-oriented Treatment of Industrial Pollutants, Beijing 100083 (China); Han, Shaoke; Dong, Yingbo; He, Yinhai [School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083 (China); Beijing Key Laboratory on Resource-oriented Treatment of Industrial Pollutants, Beijing 100083 (China)

    2017-08-01

    Highlights: • An anion adsorbent was synthesized by hyperbranched polyamide modified corncob (HPMC). • The surface characteristics of samples (RCC, HPMC, HPMC-Cr) were studied. • Langmuir isotherm provided more fit and maximum adsorption capacity was 131.6 mg/g. • The adsorption process was chemisorption, controlled by intra-particle diffusion and film diffusion. • Adsorption is fast, stable, spontaneous and endothermic. - Abstract: A low-cost anion adsorbent for Cr(VI) effectively removing was synthesized by hyperbranched polyamide modified corncob (HPMC). Samples were characterized by Brunauer–Emmett–Teller (BET) surface area analysis, field-emission scanning electron microscopy (FE-SEM) with energy-dispersive X-ray spectroscopy, Fourier transform infrared (FTIR) and zeta potential analysis. Kinetics, isotherms and thermodynamics studies of HPMC for Cr(VI) adsorption were investigated in batch static experiments, in the temperature range of 25–45 °C, pH = 2.0. Results showed that the adsorption was rapid and stable, with the uptake capacity higher than 80% after 30 min. Adsorption behavior and rate-controlling mechanisms were analyzed using three kinetic models (pseudo-first order, pseudo-second order, intra-particle kinetic model). Kinetic studies showed that the adsorption of HPMC to Cr(VI) relied the pseudo-second-order model, and controlled both by the intra-particle diffusion and film diffusion. Equilibrium data was tested by Langmuir and Freundlich adsorption isotherm models. Langmuir model was more suitable to indicate a homogeneous distribution of active sites on HPMC and monolayer adsorption. The maximum adsorption capacity from the Langmuir model, q{sub max}, was 131.6 mg/g at pH 2.0 and 45 °C for HPMC. Thermodynamic parameters revealed spontaneous and endothermic nature of the Cr(VI) adsorption onto HPMC.

  17. Surface chemistry of ferrihydrite: Part 2. Kinetics of arsenate adsorption and coprecipitation

    Science.gov (United States)

    Fuller, C.C.; Dadis, J.A.; Waychunas, G.A.

    1993-01-01

    The kinetics of As(V) adsorption by ferrihydrite was investigated in coprecipitation and postsynthesis adsorption experiments conducted in the pH range 7.5-9.0. In coprecipitation experiments, As(V) was present in solution during the hydrolysis and precipitation of iron. In adsorption experiments, a period of rapid (kinetics of As(V) desorption after an increase in pH were also consistent with diffusion as a rate-limiting process. Aging of pure ferrihydrite prior to As(V) adsorption caused a decrease in adsorption sites on the precipitate owing to crystallite growth. In coprecipitation experiments, the initial As(V) uptake was significantly greater than in post-synthesis adsorption experiments, and the rate of uptake was not diffusion limited because As(V) was coordinated by surface sites before crystallite growth and coagulation processes could proceed. After the initial adsorption, As(V) was slowly released from coprecipitates for at least one month, as crystallite growth caused desorption of As(V). Adsorption densities as high as 0.7 mole As(V) per mole of Fe were measured in coprecipitates, in comparison to 0.25 mole As(V) per mole of Fe in post-synthesis adsorption experiments. Despite the high Concentration of As(V) in the precipitates, EXAFS spectroscopy (Waychunas et al., 1993) showed that neither ferric arsenate nor any other As-bearing surface precipitate or solid solution was formed. The high adsorption densities are possible because the ferrihydrite particles are extremely small, approaching the size of small dioctahedral chains at the highest As(V) adsorption density. The results suggest that the solid solution model proposed by Fox (1989, 1992) for control of arsenate and phosphate concentrations in natural waters may be invalid. ?? 1993.

  18. [Surface properties and adsorption characteristics for fluoride of goethite, kaolinite and their association].

    Science.gov (United States)

    Wei, Shi-Yong; Yang, Xiao-Hong

    2010-09-01

    The basic properties of goethite, kaolinite and their association were characterized using X-ray diffraction (XRD) , scanning electron microscopes (SEM), Fourier transform infrared spectroscopy (FT-IR), potentiometric titrations, specific surface area (SSA) and micropore analysis. Moreover, the adsorption capacity and adsorption models of fluoride by the investigated samples were studied. Results show that when kaolinite and goethite presented simultaneously in the same suspension system, goethite was apt to coat the surface of kaolinite and the interactions between them could occur rapidly. As a result, the binary association containing kaolinite and goethite was formed. The binary association possessed the pore diameter of 0.42 nm and 0.61 nm, specific surface area of 34.08 m2/g, surface fractal dimension of D = 2.726 and the pH(PZNPC) (pH of point of zero net proton charge) in the range of 5.50-6.50. At the initial pH 6. 00, the maximum adsorption capacity (q(max) of goethite, kaolinite and association was 4.506, 0.608 and 3.520 mg/g respectively. The adsorption of fluoride by the single kaolinite or goethite could be attributed to monolayer adsorption and the data of isotherm adsorption could be well fitted by Langmuir model (R2 = 0.991 and R2 = 0.964 respectively). The Freundlich model was suitable for describing the adsorption of fluoride by the binary association (R2 = 0.995), which indicated that the surface of the binary association is heterogeneous and is probably provided with multilayer adsorption sites. The adsorption mechanisms for fluoride by the investigated samples include anion ligand exchange, surface coordination and electrostatic attraction. In addition, F acting as a bond bridge between the surfaces of kaolinite and goethite contributed to the adsorption of fluoride too. Compared to the single goethite or kaolinite, the binary association exhibited the higher specific surface area, surface fractal dimension and adsorption capacity for fluoride

  19. 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.

  20. Hydrophilic crosslinked-polymeric surface capable of effective suppression of protein adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Kamon, Yuri; Inoue, Naoko; Mihara, Erika; Kitayama, Yukiya; Ooya, Tooru; Takeuchi, Toshifumi, E-mail: takeuchi@gold.kobe-u.ac.jp

    2016-08-15

    Highlights: • Three hydrophilic crosslinked polymers were examined for protein adsorption. • All polymers showed low nonspecific adsorption of negatively charged proteins. • Poly(MMPC) showed the lowest adsorption for positively charged proteins. • Poly(MMPC) is able to reduce nonspecific adsorption of a wide range of proteins. - Abstract: We investigated the nonspecific adsorption of proteins towards three hydrophilic crosslinked-polymeric thin layers prepared by surface-initiated atom transfer radical polymerization using N,N′-methylenebisacrylamide, 2-(methacryloyloxy)ethyl-[N-(2-methacryloyloxy)ethyl]phosphorylcholine (MMPC), or 6,6′-diacryloyl-trehalose crosslinkers. Protein binding experiments were performed by surface plasmon resonance with six proteins of different pI values including α-lactalbumin, bovine serum albumin (BSA), myoglobin, ribonuclease A, cytochrome C, and lysozyme in buffer solution at pH 7.4. All of the obtained crosslinked-polymeric thin layers showed low nonspecific adsorption of negatively charged proteins at pH 7.4 such as α-lactalbumin, BSA, and myoglobin. Nonspecific adsorption of positively charged proteins including ribonuclease A, cytochrome C, and lysozyme was the lowest for poly(MMPC). These results suggest poly(MMPC) can effectively reduce nonspecific adsorption of a wide range of proteins that are negatively or positively charged at pH 7.4. MMPC is a promising crosslinker for a wide range of polymeric materials requiring low nonspecific protein binding.

  1. Adsorption of atomic nitrogen and oxygen on [Formula: see text] surface: a density functional theory study.

    Science.gov (United States)

    Breedon, M; Spencer, M J S; Yarovsky, I

    2009-04-08

    The adsorption of atomic nitrogen and oxygen on the ([Formula: see text]) crystal face of zinc oxide (ZnO) was studied. Binding energies, workfunction changes, vibrational frequencies, charge density differences and electron localization functions were calculated. It was elucidated that atomic oxygen binds more strongly than nitrogen, with the most stable [Formula: see text] structure exhibiting a binding energy of -2.47 eV, indicating chemisorption onto the surface. Surface reconstructions were observed for the most stable minima of both atomic species. Positive workfunction changes were calculated for both adsorbed oxygen and nitrogen if the adsorbate interacted with zinc atoms. Negative workfunction changes were calculated when the adsorbate interacted with both surface oxygen and zinc atoms. Interactions between the adsorbate and the surface zinc atoms resulted in ionic-type bonding, whereas interactions with oxygen atoms were more likely to result in the formation of covalent-type bonding. The positive workfunction changes correlate with an experimentally observed increase in resistance of ZnO conductometric sensor devices.

  2. Adsorption of tetracycline on kaolinite with pH-dependent surface charges.

    Science.gov (United States)

    Li, Zhaohui; Schulz, Laura; Ackley, Caren; Fenske, Nancy

    2010-11-01

    Kaolinite is a major type of clay minerals in soils of warm and humid climate. Although it has a much lower cation exchange capacity (CEC) and specific surface area compared to swelling clays, its ubiquitous existence as well as its pH-dependent surface charge makes it an important component to study the interactions between contaminants and soils. Tetracycline (TC) is a group of broad spectrum antibiotics used extensively in human and veterinary medicine. It has a high aqueous solubility and a long environmental half-life. In this study, the interactions between TC and kaolinite in aqueous solution were investigated in batch tests and supplemented by FTIR analyses. The adsorption of TC on kaolinite was mainly on the external surfaces via cation exchange as confirmed by stoichiometric desorption of exchangeable cations and simultaneous adsorption of H(+) rather than due to complexation. Under acidic conditions, a reduction in surface charge, thus the CEC, resulted in more desorption of exchangeable cations compared to TC adsorption. Fitting of the experimental data to the adsorption of different species revealed that TC(+) accounted for 4/5 of the total TC adsorbed with the remaining by zwitterion TC(0), possible via hydrogen bonding. At higher temperature, the pKa2 and pKa3 values seem to shift a pH unit lower. Due to its pH-dependent charge of kaolinite, TC adsorption is more pH dependent. The TC adsorption capacity on kaolinite was much lower compared to that on swelling clays. However, the adsorption rate constant was faster than that on swelling clays owing to surface adsorption instead of intercalation. Despite its low TC adsorption capacity, the ubiquitous existence of kaolinite in soils of warm climate may play a vital role in the fate and transport of TC in these soils. Copyright 2010 Elsevier Inc. All rights reserved.

  3. Surface and subsurface hydrogen: adsorption properties on transition metals and near-surface alloys.

    Science.gov (United States)

    Greeley, Jeff; Mavrikakis, Manos

    2005-03-03

    Periodic, self-consistent DFT-GGA calculations are used to study the thermochemical properties of both surface and subsurface atomic hydrogen on a variety of pure metals and near-surface alloys (NSAs). For surface hydrogen on pure metals, calculated site preferences, adsorption geometries, vibrational frequencies, and binding energies are reported and are found to be in good agreement with available experimental data. On NSAs, defined as alloys wherein a solute is present near the surface of a host metal in a composition different from the bulk composition, surface hydrogen generally binds more weakly than it binds to the pure-metal components composing the alloys. Some of the NSAs even possess the unusual property of binding hydrogen as weakly as the noble metals while, at the same time, dissociating H(2) much more easily. On both NSAs and pure metals, formation of surface hydrogen is generally exothermic with respect to H(2)(g). In contrast, formation of subsurface hydrogen is typically endothermic with respect to gas-phase H(2) (the only exception to this general statement is found for pure Pd). As with surface H, subsurface H typically binds more weakly to NSAs than to the corresponding pure-metal components of the alloys. The diffusion barrier for hydrogen from surface to subsurface sites, however, is usually lower on NSAs compared to the pure-metal components, suggesting that population of subsurface sites may occur more rapidly on NSAs.

  4. Surface-water interface induces conformational changes critical for protein adsorption: Implications for monolayer formation of EAS hydrophobin

    Directory of Open Access Journals (Sweden)

    Kamron eLey

    2015-11-01

    Full Text Available The class I hydrophobin EAS is part of a family of small, amphiphilic fungal proteins best known for their ability to self-assemble into stable monolayers that modify the hydrophobicity of a surface to facilitate further microbial growth. These proteins have attracted increasing attention for industrial and biomedical applications, with the aim of designing surfaces that have the potential to maintain their clean state by resisting non-specific protein binding. To gain a better understanding of this process, we have employed all-atom molecular dynamics to study initial stages of the spontaneous adsorption of monomeric EAS hydrophobin on fully hydroxylated silica, a commonly used industrial and biomedical substrate. Particular interest has been paid to the Cys3-Cys4 loop, which has been shown to exhibit disruptive behavior in solution, and the Cys7-Cys8 loop, which is believed to be involved in the aggregation of EAS hydrophobin at interfaces. Specific and water mediated interactions with the surface were also analyzed. We have identified two possible binding motifs, one which allows unfolding of the Cys7-Cys8 loop due to the surfactant-like behavior of the Cys3-Cys4 loop, and another which has limited unfolding due to the Cys3-Cys4 loop remaining disordered in solution. We have also identified intermittent interactions with water which mediate the protein adsorption to the surface, as well as longer lasting interactions which control the diffusion of water around the adsorption site. These results have shown that EAS behaves in a similar way at the air-water and surface-water interfaces, and have also highlighted the need for hydrophilic ligand functionalization of the silica surface in order to prevent the adsorption of EAS hydrophobin.

  5. Role of the oxidation state of cerium on the ceria surfaces for silicate adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Seo, Jihoon [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of); Moon, Jinok [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of); Clean/CMP Technology Team, Memory, Samsung Electronics, Hwaseong (Korea, Republic of); Kim, Joo Hyun; Lee, Kangchun [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of); Hwang, Junha [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of); Materials R& D Center, K.C.Tech, Anseong (Korea, Republic of); Yoon, Heesung [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of); Yi, Dong Kee, E-mail: vitalis@mju.ac.kr [Department of Chemistry, Myongji University, Yongin (Korea, Republic of); Paik, Ungyu, E-mail: upaik@hanyang.ac.kr [WCD Department of Energy Engineering, Hanyang University, Seoul (Korea, Republic of)

    2016-12-15

    Highlights: • We investigated the role of Ce oxidation state (Ce{sup 3+}/Ce{sup 4+}) on the CeO{sub 2} surfaces for the silicate adsorption. • As the Ce{sup 3+} concentration increased from 19.3 to 27.6%, the surface density of −OH group increased from 0.34 to 0.72 OH/nm{sup 2}. • The Freundlich constant for the relative adsorption capacity (K{sub F}) and adsorption intensity (1/n) indicated that CeO{sub 2} NPs with high Ce{sup 3+} concentration show higher adsorption affinity with silicate ions. - Abstract: In this study, we have investigated the role of the Ce oxidation state (Ce{sup 3+}/Ce{sup 4+}) on the CeO{sub 2} surfaces for silicate adsorption. In aqueous medium, the Ce{sup 3+} sites lead to the formation of −OH groups at the CeO{sub 2} surface through H{sub 2}O dissociation. Silicate ions can adsorb onto the CeO{sub 2} surface through interaction with the −OH groups (−Ce−OH− + −Si−O{sup −} ↔ −Ce−O−Si− + OH{sup −}). As the Ce{sup 3+} concentration increased from 19.3 to 27.6%, the surface density of −OH group increased from 0.34 to 0.72 OH/nm{sup 2}. To evaluate the adsorption behaviors of silicate ions onto CeO{sub 2} NPs, we carried out an adsorption isothermal analysis, and the adsorption isotherm data followed the Freundlich model. The Freundlich constant for the relative adsorption capacity (K{sub F}) and adsorption intensity (1/n) indicated that CeO{sub 2} NPs with high Ce{sup 3+} concentration show higher adsorption affinity with silicate ions. As a result, we have demonstrated that the Ce oxidation state (Ce{sup 3+}/Ce{sup 4+}) on the CeO{sub 2} surface can have a significant influence on the silicate adsorption.

  6. Adsorption of lysozyme unto silica and polystyrene surfaces in ...

    African Journals Online (AJOL)

    user

    2011-04-11

    Apr 11, 2011 ... polystyrene interfaces was studied at varying lysozyme concentrations and ionic strength. The studies revealed an ... adsorption densities of 1.34 x10-6 mol g-1 and 1.57 x10-6 mol g-1 obtained for silica and polystyrene respectively at the ..... Differential scanning calometry and FTIR analysis. J. Colloid.

  7. Dynamics of competitive polymer adsorption onto planar surfaces in good solvent.

    Science.gov (United States)

    Källrot, Niklas; Linse, Per

    2010-03-25

    Adsorption of mixed polymer solutions in good solvent containing polymers of different chain length has been studied by applying simulation techniques on a coarse-grained bead-spring polymer model. Fully flexible polymers at varying bead-surface interaction strength and different combinations of flexible, semiflexible, and stiff polymers at a single bead-surface interaction strength have been examined. Monte Carlo simulation techniques have been employed to investigate static equilibrium properties and Brownian dynamic simulations to follow the dynamics of the adsorption process. The properties examined comprise the adsorbed number of polymers, adsorbed number of beads, bead density profiles, components of the polymer radius of gyration, tail, loop, and train configurations, and nematic bond order of adsorbed beads. The adsorption involves an initially independent adsorption of the two polymer types followed by competitive adsorption. The competitive adsorption is characterized by a maximum of the adsorbed amount and a desorption of the polymer with the smallest surface affinity and a continued, but reduced, growth of the adsorbed amount of the polymer with the largest surface affinity. The surface affinity difference between the two polymer types of different length increased with increasing bead-surface interaction. Furthermore, the surface affinity of a polymer initially decreased but then largely increased at increasing stiffness. As a consequence, a stiff short polymer was found to displace a 4-fold longer flexible polymer. The spatial extension of adsorbed polymers as characterized by the radius of gyration parallel and perpendicular to the surface of a polymer of a given flexibility was independent of the flexibility of the other polymer type. The fraction of beads in tails was increased and in trains reduced as the surface affinity of the dissimilar polymer type was raised. Finally, the adsorption layer of a stiff polymer possesses a nematic bond order. In

  8. Effect of the surface oxygen groups on methane adsorption on coals

    Energy Technology Data Exchange (ETDEWEB)

    Hao Shixiong [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Department of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000 (China); Wen Jie [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Yu Xiaopeng [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Department of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000 (China); Chu Wei, E-mail: chuwei1965_scu@yahoo.com [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China)

    2013-01-01

    Highlights: Black-Right-Pointing-Pointer We modified one coal with H{sub 2}O{sub 2}, (NH{sub 4}){sub 2}S{sub 2}O{sub 8} and HNO{sub 3} respectively, to prepare coal samples with different surface properties. Black-Right-Pointing-Pointer The oxygen groups on coal surface were characterized by XPS. Black-Right-Pointing-Pointer The textures of the coal samples were investigated by N{sub 2} adsorption at 77 K. Black-Right-Pointing-Pointer The adsorption behaviors were measured by volumetric method. Black-Right-Pointing-Pointer There was a negative correlation between methane saturated adsorption capacity and the O{sub total}/C{sub total}. - Abstract: To investigate the influence of surface oxygen groups on methane adsorption on coals, one bituminous coal was modified with H{sub 2}O{sub 2}, (NH{sub 4}){sub 2}S{sub 2}O{sub 8} and HNO{sub 3} respectively, to prepare coal samples with different surface properties. The oxygen groups on coal surface were characterized by X-ray photoelectron spectroscopy (XPS). The textures of the coal samples were investigated by N{sub 2} adsorption at 77 K. Their surface morphologies were analyzed by scanning electron microscopy (SEM). The methane adsorption behaviors of these coal samples were measured at 303 K in pressure range of 0-5.3 MPa by volumetric method. The adsorption data of methane were fitted to the Langmuir model and Dubinin-Astakhov (D-A) model. The fitting results showed that the D-A model fitted the isotherm data better than the Langmuir model. It was observed that there was, in general, a positive correlation between the methane saturated adsorption capacity and the micropore volume of coals while a negative correlation between methane saturated adsorption capacity and the O{sub total}/C{sub total}. The methane adsorption capacity was determined by the coal surface chemistry when the microporosity parameters of two samples were similar. Coal with a higher amount of oxygen surface groups, and consequently with a less

  9. Methane adsorption on the surface of a model of shale: A density functional theory study

    International Nuclear Information System (INIS)

    Zhu, Yuan-qiang; Su, Hong; Jing, Ya; Guo, Jianchun; Tang, Junlei

    2016-01-01

    Highlights: • The adsorption of methane on kerogen was investigated by DFT method with D3 dispersion correction. • Methane prefers to be adsorbed on the sites directly above the carbon atoms of the kerogen. • The interaction energy with BSSE corrections is around 14 kJ mol −1 . • RDG gradient isosurface depicted the van der Waals interactions between methane and kerogen. • The adsorption of methane on kerogen slightly depends upon the adsorption sites on kerogen as well as the orientations of methane. - Abstract: As a model of shale, one part of polycyclic aromatic ring was used to represent the kerogen surface with the structural heterogeneity. The adsorption mechanisms of methane on the surface of the kerogen were investigated by M06-2× functional with D3 dispersion correction. Nine stable adsorption sites and the orientations of methane (CH 4 ) on the surface of the kerogen were systematically considered. Information from different methods lead to the same conclusion that methane prefers to be adsorbed on the sites directly above the carbon atoms of the kerogen rather than above the center of the six-membered rings. The interactions between methane and the surface of the kerogen are the van der Waals interactions. The interaction energies with the basis set superposition error (BSSE) corrections are around 14 kJ mol −1 at the M06-2×-D3/Jun-cc-pVDZ level. The RDG scatter graphs and the RDG gradient isosurface further illustrate that the interactions between methane and the surface of the kerogen belong to the van der Waals interactions. The weak interactions indicate that the adsorption of methane on the surface of the kerogen is physical adsorption and it slightly depends upon the adsorption sites on kerogen as well as the orientations of methane. These results are helpful for the understanding of the microcosmic mechanism of methane–shale interactions and for the exploitation of shale gas.

  10. SERS, XPS, and DFT Study of Adenine Adsorption on Silver and Gold Surfaces.

    Science.gov (United States)

    Pagliai, Marco; Caporali, Stefano; Muniz-Miranda, Maurizio; Pratesi, Giovanni; Schettino, Vincenzo

    2012-01-19

    The adsorption of adenine on silver and gold surfaces has been investigated combining density functional theory calculations with surface-enhanced Raman scattering and angle-resolved X-ray photoelectron spectroscopy measurements, obtaining useful insight into the orientation and interaction of the nucleobase with the metal surfaces.

  11. Probing adsorption phenomena on a single crystal Pt-alloy surface under oxygen reduction reaction conditions

    DEFF Research Database (Denmark)

    Bondarenko, Alexander S.; Stephens, Ifan E.L.; Bech, Lone

    2012-01-01

    The adsorption dynamics of *OH and *O species at Pt(111) and Cu/Pt(111) near-surface alloy (NSA) surfaces in oxygen-free and O2-saturated 0.1M HClO4 was investigated. Subsurface Cu modifies the electronic structure at the Pt(111) surface resulting in weaker bonding to adsorbates like *OH, *H or *...

  12. Selective adsorption of bovine hemoglobin on functional TiO2 nano-adsorbents: surface physic-chemical properties determined adsorption activity

    Science.gov (United States)

    Guo, Shiguang; Zhang, Jianghua; Shao, Mingxue; Zhang, Xia; Liu, Yufeng; Xu, Junli; Meng, Hao; Han, Yide

    2015-04-01

    Surface functionalized nanoparticles are efficient adsorbents which have shown good potential for protein separation. In this work, we chose two different types of organic molecules, oleic acid (OA) and 3-glycidoxypropyltrimethoxy silane (GPTMS), to functionalize the surface of TiO2 nanoparticles, and we studied the effects of this modification on their surface physicochemical properties in correlation with their selective adsorption of proteins. The results showed that the surface zeta potential and the surface water wettability of the modified TiO2 were significantly changed in comparison with the original TiO2 nanoparticles. The adsorption activities of bovine hemoglobin (BHb) and bovine serum albumin (BSA) on these functionalized TiO2 samples were investigated under different conditions, including pH values, contact time, ion strength, and initial protein concentration. In comparison with the non-specific adsorption of original TiO2, however, both the OA-TiO2 and GPTMS-TiO2 exhibited increased BHb adsorption and decreased BSA adsorption at the same time. Using a binary protein mixture as the adsorption object, a higher separation factor (SF) was obtained for OA-TiO2 under optimum conditions. The different adsorption activities of BHb and BSA on the modified TiO2 were correlated with different interactions at the protein/solid interface, and the chemical force as well as the electrostatic force played an important role in the selective adsorption process.

  13. 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.

  14. Density functional theory calculations and molecular dynamics simulations of the adsorption of biomolecules on graphene surfaces.

    Science.gov (United States)

    Qin, Wu; Li, Xin; Bian, Wen-Wen; Fan, Xiu-Juan; Qi, Jing-Yao

    2010-02-01

    There is increasing attention in the unique biological and medical properties of graphene, and it is expected that biomaterials incorporating graphene will be developed for the graphene-based drug delivery systems and biomedical devices. Despite the importance of biomolecules-graphene interactions, a detailed understanding of the adsorption mechanism and features of biomolecules onto the surfaces of graphene is lacking. To address this, we have performed density functional theory (DFT) and molecular dynamics (MD) methods exploring the adsorption geometries, adsorption energies, electronic band structures, adsorption isotherms, and adsorption dynamics of l-leucine (model biomolecule)/graphene composite system. DFT calculations confirmed the energetic stability of adsorption model and revealed that electronic structure of graphene can be controlled by the adsorption direction of l-leucine. MD simulations further investigate the potential energy and van der Waals energy for the interaction processes of l-leucine/graphene system at different temperatures and pressures. We find that the van der Waals interaction between the l-leucine and the graphene play a dominant role in the adsorption process under a certain range of temperature and pressure, and the l-leucine molecule could be adsorbed onto graphene spontaneously in aqueous solution.

  15. Competitive adsorptions of nitrile hydratase and amidase on polyacrylonitrile and its effect on surface modification.

    Science.gov (United States)

    Babu, Vikash; Choudhury, Bijan

    2012-01-01

    In this study, enzymatic surface modification of polyacrylonitrile was studied using nitrile metabolizing enzyme of Amycolatopsis sp. IITR 215. During enzymatic treatment of polyacrylonitrile at pH of 5.8 and 7, it was observed that the conversion of cyano group to carboxylic acid at pH 5.8 was three times higher than at pH 7. This difference in enzymatic treatment efficiency was explained by studying the differences in adsorption profiles of nitrile hydratase and amidase on polyacrylonitrile at pH of 5.8 and 7. Adsorption profiles were determined by monitoring the unbound activities of these two enzymes in the supernatant. From the specific activity profiles of bound nitrile hydratase and amidase it was concluded that more specific binding of nitrile hydratase was observed at pH 5.8 as compared to pH 7. In case of amidase, optimum adsorption was obtained at pH 5.8 within 5h whereas in case of pH 7 it was obtained within 20 h. Thus at pH 7, sequential adsorption of nitrile hydratase and amidase was observed and this adsorption profile was similar to the Vroman effect reported during plasma protein adsorption at solid-liquid interface. Ideally, specific nitrile hydratase adsorption followed by sequential adsorption of amidase may enhance higher conversion of cyano group to carboxylic acid. Copyright © 2011 Elsevier B.V. All rights reserved.

  16. A semiflexible alternating copolymer chain adsorption on a flat and a fluctuating surface.

    Science.gov (United States)

    Mishra, Pramod Kumar

    2010-04-21

    A lattice model of a directed self-avoiding walk is used to investigate adsorption properties of a semiflexible alternating copolymer chain on an impenetrable flat and fluctuating surface in two (square, hexagonal and rectangular lattice) and three dimensions (cubic lattice). In the cubic lattice case the surface is two-dimensional impenetrable flat and in two dimensions the surface is a fluctuating impenetrable line (hexagonal lattice) and also flat impenetrable line (square and rectangular lattice). Walks of the copolymer chains are directed perpendicular to the plane of the surface and at a suitable value of monomer surface attraction, the copolymer chain gets adsorbed on the surface. To calculate the exact value of the monomer surface attraction, the directed walk model has been solved analytically using the generating function method to discuss results when one type of monomer of the copolymer chain has attractive, repulsive or no interaction with the surface. Results obtained in the flat surface case show that, for a stiffer copolymer chain, adsorption transition occurs at a smaller value of monomer surface attraction than a flexible copolymer chain while in the case of a fluctuating surface, the adsorption transition point is independent of bending energy of the copolymer chain. These features are similar to that of a semiflexible homopolymer chain adsorption.

  17. A semiflexible alternating copolymer chain adsorption on a flat and a fluctuating surface

    International Nuclear Information System (INIS)

    Mishra, Pramod Kumar

    2010-01-01

    A lattice model of a directed self-avoiding walk is used to investigate adsorption properties of a semiflexible alternating copolymer chain on an impenetrable flat and fluctuating surface in two (square, hexagonal and rectangular lattice) and three dimensions (cubic lattice). In the cubic lattice case the surface is two-dimensional impenetrable flat and in two dimensions the surface is a fluctuating impenetrable line (hexagonal lattice) and also flat impenetrable line (square and rectangular lattice). Walks of the copolymer chains are directed perpendicular to the plane of the surface and at a suitable value of monomer surface attraction, the copolymer chain gets adsorbed on the surface. To calculate the exact value of the monomer surface attraction, the directed walk model has been solved analytically using the generating function method to discuss results when one type of monomer of the copolymer chain has attractive, repulsive or no interaction with the surface. Results obtained in the flat surface case show that, for a stiffer copolymer chain, adsorption transition occurs at a smaller value of monomer surface attraction than a flexible copolymer chain while in the case of a fluctuating surface, the adsorption transition point is independent of bending energy of the copolymer chain. These features are similar to that of a semiflexible homopolymer chain adsorption.

  18. Surface Characterization and in situ Protein Adsorption Studies on Carbene-Modified Polymers.

    Science.gov (United States)

    Nelson, Geoffrey W; Parker, Emily M; Singh, Kulveer; Blanford, Christopher F; Moloney, Mark G; Foord, John S

    2015-10-13

    Polystyrene thin films were functionalized using a facile two-step chemical protocol involving carbene insertion followed by azo-coupling, permitting the introduction of a range of chemical functional groups, including aniline, hexyl, amine, carboxyl, phenyl, phosphonate diester, and ethylene glycol. X-ray photoelectron spectroscopy (XPS) confirmed the success of the two-step chemical modification with a grafting density of at least 1/10th of the typical loading density (10(14)-10(15)) of a self-assembled monolayer (SAM). In situ, real-time quartz crystal microbalance with dissipation (QCM-D) studies show that the dynamics of binding of bovine serum albumin (BSA) are different at each modified surface. Mass, viscoelastic, and kinetic data were analyzed, and compared to cheminformatic descriptors (i.e., c log P, polar surface area) typically used for drug discovery. Results show that functionalities may either resist or adsorb BSA, and uniquely influence its adsorption dynamics. It is concluded that carbene-based surface modification can usefully influence BSA binding dynamics in a manner consistent with, and more robust than, traditional systems based on SAM chemistry.

  19. Effect of solution chemistry on the adsorption of perfluorooctane sulfonate onto mineral surfaces.

    Science.gov (United States)

    Tang, Chuyang Y; Shiang Fu, Q; Gao, Dawen; Criddle, Craig S; Leckie, James O

    2010-04-01

    Perfluorooctane sulfonate (PFOS) is an emergent contaminant of substantial environmental concerns, yet very limited information has been available on PFOS adsorption onto mineral surfaces. PFOS adsorption onto goethite and silica was investigated by batch adsorption experiments under various solution compositions. Adsorption onto silica was only marginally affected by pH, ionic strength, and calcium concentration, likely due to the dominance of non-electrostatic interactions. In contrast, PFOS uptake by goethite increased significantly at high [H+] and [Ca2+], which was likely due to enhanced electrostatic attraction between the negatively charged PFOS molecules and positively charged goethite surface. The effect of pH was less significant at high ionic strength, likely due to electrical double layer compression. PFOS uptake was reduced at higher ionic strength for a strongly positively charged goethite surface (pH 3), while it increased for a weakly charged surface (pH 7 and 9), which could be attributed to the competition between PFOS-surface electrostatic attraction and PFOS-PFOS electrostatic repulsion. A conceptual model that captures PFOS-surface and PFOS-PFOS electrostatic interactions as well as non-electrostatic interaction was also formulated to understand the effect of solution chemistry on PFOS adsorption onto goethite and silica surfaces. Copyright (c) 2010 Elsevier Ltd. All rights reserved.

  20. [Preparation of surface molecularly imprinted polymers for penicilloic acid, and its adsorption properties].

    Science.gov (United States)

    Zheng, Penglei; Luo, Zhimin; Chang, Ruimiao; Ge, Yanhui; Du, Wei; Chang, Chun; Fu, Qiang

    2015-09-01

    On account of the specificity and reproducibility for the determination of penicilloic acid in penicillin, this study aims to prepare penicilloic acid imprinted polymers (PEOA-MIPs) by surface polymerization method at the surface of modified silica particles by using penicilloic acid (PEOA) as the template molecule, methacrylic acid (MAA) as the functional monomer, ethylene glycol dimethacrylate ( EGDMA) as the cross linker, and methanol/acetonitrile as the solvents. The synthesis conditions were optimized, and PEOA-MIPs had the best adsorption capacity when the molar ratio of template molecule/functional monomer was 1 :4, cross linking degree was 85% and the solvent ratio of methanol/acetonitrile was 1 :1 (v/v). The adsorption properties were evaluated by adsorption experiments, including the adsorption isotherms, kinetics and selectivity. The adsorption process between PEOA-MIPs and PEOA fitted the Langmuir adsorption isotherm with the maximum adsorption capacity of 122. 78 mg/g and the pseudo-second-order reaction kinetics with fast adsorption kinetics (the equilibrium time of 45 min). The as-synthesized PEOA-MIPs were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), and thermal gravimetric analysis (TGA). The results indicated that the MIPs layer has been successfully grafted on the surface of SiO2 microparticles and the PEOA-MIPs had the excellent thermal stability. The PEOA-MIPs showed the highest selective recognition for PEOA. The PEOA-MIPs possess a high adsorption capacity, rapid mass-transfer rate and high selectivity to PEOA when compared with non-imprinted polymers (PEOA-NIPs). The PEOA-MIPs was expected to be used as the solid phase extraction medium and this study provides the potential applications for fast recognition and analysis of the penicilloic acid in penicillin.

  1. The influence of the surface properties of silicon-fluorine hydrogel on protein adsorption.

    Science.gov (United States)

    Xie, Haijiao; Zhao, Zhengbai; An, Shuangshuang; Jiang, Yong

    2015-12-01

    A range of fluorinated hydrogels were synthesized using the copolymerization of 1, 1, 1, 3, 3, 3-hexafluoroisopropyl methacrylate (HFMA) or 1H, 1H, 7H-dodecafluoroheptyl methacrylate (DFMA) with hydrophilic monomers. Bovine serum albumin (BSA) and Lysozyme (LZM) were chosen as model proteins to investigate the performance of protein adsorption on the surface of these fluorinated hydrogels. It was found that the performance of the fluorinated hydrogels toward protein adsorption was different for different proteins; simultaneously, the amount of protein adsorption was related to but not linear with the fluorine content on the hydrogel surface. With increasing HFMA content, the mass of BSA adsorption increased in the first stage and then decreased, meanwhile the mass of LZM adsorption exhibited an upward trend in general. In addition, the amount of protein adsorption was also related to the type and length of the fluorinated groups. The hydrogels made from DFMA behaved better than HFMA hydrogels in terms of reducing protein adsorption. This study might provide further reference in choosing fluorine monomer to prepare protein-repelling hydrogels. Copyright © 2015 Elsevier B.V. All rights reserved.

  2. Selective Adsorption of Nano-bio materials and nanostructure fabrication on Molecular Resists Modified by proton beam irradiation

    International Nuclear Information System (INIS)

    Lee, H. W.; Kim, H. S.; Kim, S. M.

    2008-04-01

    The purpose of this research is the fabrication of nanostructures on silicon substrate using proton beam and selectively adsorption of bio-nano materials on the patterned substrate. Recently, the miniaturization of the integrated devices with fine functional structures was intensively investigated, based on combination of nanotechnology (NT), biotechnology (BT) and information technology (IT). Because of the inherent limitation in optical lithography, large variety of novel patterning technologies were evolved to construct nano-structures onto a substrate. Atomic force microscope-based nanolithography has readily formed sub-50 nm patterns by the local modification of a substrate using a probe with a curvature of 10 nm. The surface property was regarded as one of the most important factors for AFM-based nanolithography as well as for other novel nanolithographies. The molecular thin films such as a self-assembled monolayer or a polymer resist layer have been used as an alternative to modifying the surface property. Although proton or ion beam irradiation has been used as an efficient tool to modify the physical, chemical and electrical properties of a surface, the nano-patterning on the substrate or the molecular film modified with the beam irradiation has hardly been studied at both home and abroad. The selective adsorption of nano-bio materials such as carbon nanotubes and proteins on the patterns would contribute to developing the integrated devices. The polystyrene nanoparticles (400 nm) were arrayed on al silicon surface using nanosphere lithography and the various nanopatterns were fabricated by proton beam irradiation on the polystyrene nanoparticles arrayed silicon surface. We obtained the two different nanopatterns such as polymer nanoring patterns and silicon oxide patterns on the same silicon substrate. The polymer nanoring patterns formed by the crosslinkage of polystyrene when proton beam was irradiated at the triangular void spaces that are enclosed by

  3. ADSORPTION OF ASSOCIATING FLUIDS AT ACTIVE SURFACES: A DENSITY FUNCTIONAL THEORY

    Directory of Open Access Journals (Sweden)

    S.Tripathi

    2003-01-01

    Full Text Available We present a density functional theory (DFT to describe adsorption in systems where molecules of associating fluids can bond (or associate with discrete, localized functional groups attached to the surfaces, in addition to other fluid molecules. For such systems as water adsorbing on activated carbon, silica, clay minerals etc. this is a realistic model to account for surface heterogeneity rather than using a continuous smeared surface-fluid potential employed in most of the theoretical works on adsorption on heterogeneous surfaces. Association is modelled within the framework of first order thermodynamic perturbation theory (TPT1. The new theory accurately predicts the distribution of bonded and non-bonded species and adsorption behavior under various conditions of bulk pressure, surface-fluid and fluid-fluid association strengths. Competition between the surface-fluid and fluid-fluid association is analyzed for fluids with multiple association sites and its impact on adsorption is discussed. The theory, supported by simulations demonstrates that the extent and the nature of adsorption (e.g. monolayer vary with the number of association sites on the fluid molecules.

  4. MONTE CARLO SIMULATIONS OF THE ADSORPTION OF DIMERS ON STRUCTURED HETEROGENEOUS SURFACES

    Directory of Open Access Journals (Sweden)

    Abreu C.R.A.

    2001-01-01

    Full Text Available The effect of surface topography upon the adsorption of dimer molecules is analyzed by means of grand canonical ensemble Monte Carlo simulations. Heterogeneous surfaces were assumed to consist of a square lattice containing active sites with two different energies. These were distributed in three different configurations: a random distribution of isolated sites; a random distribution of grains with four high-energy sites; and a random distribution of grains with nine high-energy sites. For the random distribution of isolated sites, the results are in good agreement with the molecular simulations performed by Nitta et al. (1997. In general, the comparison with theoretical models shows that the Nitta et al. (1984 isotherm presents good predictions of dimer adsorption both on homogeneous and heterogeneous surfaces with sites having small differences in characteristic energies. The molecular simulation results also show that the energy topology of the solid surfaces plays an important role in the adsorption of dimers on solids with large differences in site energies. For these cases, the Nitta et al. model does not describe well the data on dimer adsorption on random heterogeneous surfaces (grains with one acid site, but does describe reasonably well the adsorption of dimers on more patchwise heterogeneous surfaces (grains with nine acid sites.

  5. Influence of surface modification by sulfuric acid on coking coal's adsorption of coking wastewater.

    Science.gov (United States)

    Gao, Lihui; Wen, Hong; Tian, Quanzhi; Wang, Yongtian; Li, Guosheng

    2017-07-01

    Coking coal, the raw material of a coke plant, was applied to the adsorption of coking wastewater. In this study, coking coal was directly treated with sulfuric acid to improve its surface properties and adsorption ability. Acid treatment was carried out at various concentrations, by varying from 0.001 to 1 mol/L. The samples were characterized by ash content analysis, scanning electron microscope (SEM), N 2 adsorption-desorption analysis, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), wettability analysis, and zeta potential analysis. These results demonstrated that H + could react with inorganic minerals, which resulted in a significant variation of the chemical composition and the structure of coal surface. Furthermore, both the ash content and the surface content of O = C-O, C = O and C-O groups declined gradually as the concentration of sulfuric acid increased, while the surface area and pore volume of micropore, the lipophilic and hydrophobic properties, and zeta potential magnitude increased, resulting in enhanced hydrophobic and Van der Waals' forces between the fine coal and organic pollutants. Characterization modification showed a better performance in adsorption, the removal rate enhanced from 23% to 42% after treated by 1 mol/L sulfuric acid. It was concluded that the acid activation modified the lipophilic and hydrophobic properties, the surface charge properties, surface area and pore volume, the content of oxygen functional groups, all of which could be potentially useful in wastewater adsorption.

  6. Assessment of caffeine adsorption onto mild steel surface as an eco-friendly corrosion inhibitor

    OpenAIRE

    Souza, Fernando S. de; Gonçalves, Reinaldo S.; Spinelli, Almir

    2014-01-01

    The adsorption and corrosion-inhibition properties of caffeine as an eco-friendly corrosion inhibitor for mild steel in acid medium were investigated by electrochemical and spectroscopic techniques. Polarization experiments indicated that caffeine behaves as a cathodic-type inhibitor. Impedance data showed that surface coverage increased with caffeine concentration in the range of 1.0 to 10.0 mmol L-1. The maximum inhibition efficiency obtained was 92.4%. The adsorption of the corrosion inhib...

  7. Adsorption of surfactants on sand surface in enhanced oil recovery: Isotherms, kinetics and thermodynamic studies

    Energy Technology Data Exchange (ETDEWEB)

    Bera, Achinta; Kumar, T.; Ojha, Keka; Mandal, Ajay, E-mail: mandal_ajay@hotmail.com

    2013-11-01

    Adsorption of surfactants onto reservoir rock surface may result in the loss and reduction of their concentrations in surfactant flooding, which may render them less efficient or ineffective in practical applications of enhanced oil recovery (EOR) techniques. Surfactant flooding for EOR received attraction due to its ability to increase the displacement efficiency by lowering the interfacial tension between oil and water and mobilizing the residual oil. This article highlights the adsorption of surfactants onto sand surface with variation of different influencing factors. It has been experimentally found that adsorption of cationic surfactant on sand surface is more and less for anionic surfactant, while non-ionic surfactant shows intermediate behaviour. X-ray diffraction (XRD) study of clean sand particles has been made to determine the main component present in the sand particles. The interaction between sand particles and surfactant has been studied by Fourier Transform Infrared (FTIR) Spectroscopy of the sand particles before and after aging with surfactant. Salinity plays an important role in adsorption of anionic surfactant. Batch experiments were also performed to understand the effects of pH and adsorbent dose on the sorption efficiency. The sand particles exhibited high adsorption efficiency at low pH for anionic and nonionic surfactants. But opposite trend was found for cationic surfactant. Adsorption data were analyzed by fitting with Langmuir, Freundlich, Redlich-Peterson, and Sips isotherm models. Results show that the Langmuir isotherm and pseudo-second order kinetics models suit the equilibrium and kinetics of adsorption on sand surface. Thermodynamics feasibility of the adsorption process was also studied to verify the spontaneity of the process.

  8. Surface modification of poly (styrene-b-(ethylene-co-butylene)-b-styrene) elastomer and its plasma protein adsorption by QCM-D

    International Nuclear Information System (INIS)

    Li, Rui; Jin, Jing; Sun, Yingchun

    2014-01-01

    Graphical abstract: - Highlights: • Grafting concentration of PEG was defined by the peak-area ratio of [C–O]/[C]. • Quantitatively investigated the adsorption processes of BSA and fibrinogen using QCM-D. • The inactivated BSA on SEBS surface could induce the subsequent fibrinogen adsorption. • SEBS-g-PEG with graft concentration of 0.207 has excellent protein resistance. - Abstract: Protein adsorption is a dynamic process and plays a major role in determining the hemocompatibility of biomaterials. We have obtained different poly (ethylene glycol) (PEG) graft concentrations of SEBS-g-PEG and the surface chemical compositions are confirmed by X-ray photoelectron spectroscopy (XPS). Graft concentration is defined by peak-area ratio of [C-O]/[C] on modified SEBS surface. With increasing graft concentration, water contact angles of the modified SEBS have significantly decreased. The platelet adhesion and static protein adsorption demonstrate that the hemocompatibility of copolymers films are improved effectively and SEBS-g-PEG-2 with larger graft concentration has more superior anticoagulation than that of SEBS-g-PEG-1. Moreover, we have quantitatively investigated the adsorption process of bovine serum albumin (BSA) and fibrinogen (Fib) on the surfaces of pristine SEBS and modified SEBS using quartz crystal microbalance with dissipation (QCM-D) in real time. The results indicate that the inactivated BSA on the pristine SEBS can continuously induce the subsequent Fib adsorption. The hemocompatibility of SEBS-g-PEG-2 with the graft concentration of 0.207 has excellent anti-protein property and the bio-inert BSA layer on the film can resist the subsequent Fib adsorption

  9. Surface modification of poly (styrene-b-(ethylene-co-butylene)-b-styrene) elastomer and its plasma protein adsorption by QCM-D

    Energy Technology Data Exchange (ETDEWEB)

    Li, Rui [Northeast Normal University, School of Physics, Changchun 130022 (China); Jin, Jing, E-mail: jjin@ciac.ac.cn [State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022 (China); Sun, Yingchun, E-mail: sunyc149@nenu.edu.cn [Northeast Normal University, School of Physics, Changchun 130022 (China)

    2014-05-01

    Graphical abstract: - Highlights: • Grafting concentration of PEG was defined by the peak-area ratio of [C–O]/[C]. • Quantitatively investigated the adsorption processes of BSA and fibrinogen using QCM-D. • The inactivated BSA on SEBS surface could induce the subsequent fibrinogen adsorption. • SEBS-g-PEG with graft concentration of 0.207 has excellent protein resistance. - Abstract: Protein adsorption is a dynamic process and plays a major role in determining the hemocompatibility of biomaterials. We have obtained different poly (ethylene glycol) (PEG) graft concentrations of SEBS-g-PEG and the surface chemical compositions are confirmed by X-ray photoelectron spectroscopy (XPS). Graft concentration is defined by peak-area ratio of [C-O]/[C] on modified SEBS surface. With increasing graft concentration, water contact angles of the modified SEBS have significantly decreased. The platelet adhesion and static protein adsorption demonstrate that the hemocompatibility of copolymers films are improved effectively and SEBS-g-PEG-2 with larger graft concentration has more superior anticoagulation than that of SEBS-g-PEG-1. Moreover, we have quantitatively investigated the adsorption process of bovine serum albumin (BSA) and fibrinogen (Fib) on the surfaces of pristine SEBS and modified SEBS using quartz crystal microbalance with dissipation (QCM-D) in real time. The results indicate that the inactivated BSA on the pristine SEBS can continuously induce the subsequent Fib adsorption. The hemocompatibility of SEBS-g-PEG-2 with the graft concentration of 0.207 has excellent anti-protein property and the bio-inert BSA layer on the film can resist the subsequent Fib adsorption.

  10. Adsorption of oxygen atom on MoSi{sub 2} (110) surface

    Energy Technology Data Exchange (ETDEWEB)

    Sun, S.P., E-mail: sunshunping@jsut.edu.cn [School of Materials Engineering, Jiangsu University of Technology, Changzhou 213001 (China); Li, X.P.; Wang, H.J. [School of Materials Engineering, Jiangsu University of Technology, Changzhou 213001 (China); Jiang, Y., E-mail: yjiang@csu.edu.cn [School of Materials Science and Engineering, and Key Laboratory for Non-ferrous Materials of Ministry of Education, Central South University, Changsha 410083 (China); Yi, D.Q. [School of Materials Science and Engineering, and Key Laboratory for Non-ferrous Materials of Ministry of Education, Central South University, Changsha 410083 (China)

    2016-09-30

    Highlights: • The adsorption of oxygen atom on MoSi{sub 2} (110) surface was studied systematically. • The stability of MoSi{sub 2} low-index surfaces was also investigated. • The preference adsorption site of MoSi{sub 2} (110) surface for oxygen atom was H site. - Abstract: The adsorption energy, structural relaxation and electronic properties of oxygen atom on MoSi{sub 2} (110) surface have been investigated by first-principles calculations. The energetic stability of MoSi{sub 2} low-index surfaces was analyzed, and the results suggested that MoSi{sub 2} (110) surface had energetically stability. The site of oxygen atom adsorbed on MoSi{sub 2} (110) surface were discussed, and the results indicated that the preference adsorption site of MoSi{sub 2} (110) surface for oxygen atom was H site (hollow position). Our calculated work should help to understand further the interaction between oxygen atoms and MoSi{sub 2} surfaces.

  11. Theoretical study of adsorption of nitrogen-containing environmental contaminants on kaolinite surfaces.

    Science.gov (United States)

    Scott, Andrea Michalkova; Burns, Elizabeth A; Hill, Frances C

    2014-08-01

    The adsorption of nitrogen-containing compounds (NCCs) including 2,4,6-trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), 2,4-dinitroanisole (DNAN), and 3-nitro-1,2,4-triazol-5-one (NTO) on kaolinite surfaces was investigated. The M06-2X and M06-2X-D3 density functionals were applied with the cluster approximation. Several different positions of NCCs relative to the adsorption sites of kaolinite were examined, including NCCs in perpendicular and parallel orientation toward both surface models of kaolinite. The binding between the target molecules and kaolinite surfaces was analyzed and bond energies were calculated applying the atoms in molecules (AIM) method. All NCCs were found to prefer a parallel orientation toward both kaolinite surfaces, and were bound more strongly to the octahedral than to the tetrahedral site. TNT exhibited the strongest interaction with the octahedral surface and DNAN with the tetrahedral surface of kaolinite. Hydrogen bonding was shown to be the dominant non-covalent interaction for NCCs interacting with the octahedral surface of kaolinite with a small stabilizing effect of dispersion interactions. In the case of adsorption on the tetrahedral surface, kaolonite-NCC binding was shown to be governed by the balance between hydrogen bonds and dispersion forces. The presence of water as a solvent leads to a significant decrease in the adsorption strength for all studied NCCs interacting with both kaolinite surfaces.

  12. Effect of surface acidic oxides of activated carbon on adsorption of ammonia.

    Science.gov (United States)

    Huang, Chen-Chia; Li, Hong-Song; Chen, Chien-Hung

    2008-11-30

    The influence of surface acidity of activated carbon (AC) was experimentally studied on adsorption of ammonia (NH(3)). Coconut shell-based AC was modified by various acids at different concentrations. There were five different acids employed to modified AC, which included nitric acid, sulfuric acid, hydrochloric acid, phosphoric acid, and acetic acid. Acidic functional groups on the surface of ACs were determined by a Fourier transform infrared spectrograph (FTIR) and by the Boehm titration method. Specific surface area and pore volume of the ACs were measured by a nitrogen adsorption apparatus. Adsorption amounts of NH(3) onto the ACs were measured by a dynamic adsorption system at room temperature according to the principle of the ASTM standard test method. The concentration of NH(3) in the effluent stream was monitored by a gas-detecting tube technique. Experimental results showed that adsorption amounts of NH(3) on the modified ACs were all enhanced. The ammonia adsorption amounts on various activated carbons modified by different acids are in the following order: nitric acid>sulfuric acid>acetic acid approximately phosphoric acid>hydrochloric acid. It is worth to note that the breakthrough capacity of NH(3) is linearly proportional to the amount of acidic functional groups of the ACs.

  13. First principles study of NH3 molecular adsorption on LiH (100) surfaces

    International Nuclear Information System (INIS)

    Lu Xiaoxia; Chen Yuhong; Dong Xiao

    2012-01-01

    The adsorption of NH 3 on LiH (100) crystal surfaces was studied by first principles method. The preferred adsorption sites, adsorption energy, dissociation energy and electronic structure of the LiH (100)/NH 3 systems were calculated separately. It is found that chemical adsorption happened mainly when NH 3 molecules are on the LiH (100) crystal surfaces. When NH 3 is adsorbed on the Li top site, NH 2 is formed on the LiH (100) crystal surfaces after loss of H atom, the calculated adsorption energy, 0.511 eV, belongs to strong chemical adsorption, then the interaction is strongest. The interaction between NH 2 and the neighboring Li, H are ionic. The covalent bonds are formed between N and H atoms in NH 2 . One H 2 molecule is formed by another H atom in NH 3 and H atom from LiH (100) crystal sur- faces. The covalent bonds are formed between H and H atoms in H 2 . (authors)

  14. Evaluation of protein adsorption onto a polyurethane nanofiber surface having different segment distributions

    Energy Technology Data Exchange (ETDEWEB)

    Morita, Yuko; Koizumi, Gaku [Frontier Fiber Technology and Science, Graduate School of Engineering, University of Fukui (Japan); Sakamoto, Hiroaki, E-mail: hi-saka@u-fukui.ac.jp [Tenure-Track Program for Innovative Research, University of Fukui (Japan); Suye, Shin-ichiro [Frontier Fiber Technology and Science, Graduate School of Engineering, University of Fukui (Japan)

    2017-02-01

    Electrospinning is well known to be an effective method for fabricating polymeric nanofibers with a diameter of several hundred nanometers. Recently, the molecular-level orientation within nanofibers has attracted particular attention. Previously, we used atomic force microscopy to visualize the phase separation between soft and hard segments of a polyurethane (PU) nanofiber surface prepared by electrospinning. The unstretched PU nanofibers exhibited irregularly distributed hard segments, whereas hard segments of stretched nanofibers prepared with a high-speed collector exhibited periodic structures along the long-axis direction. PU was originally used to inhibit protein adsorption, but because the surface segment distribution was changed in the stretched nanofiber, here, we hypothesized that the protein adsorption property on the stretched nanofiber might be affected. We investigated protein adsorption onto PU nanofibers to elucidate the effects of segment distribution on the surface properties of PU nanofibers. The amount of adsorbed protein on stretched PU nanofibers was increased compared with that of unstretched nanofibers. These results indicate that the hard segment alignment on stretched PU nanofibers mediated protein adsorption. It is therefore expected that the amount of protein adsorption can be controlled by rotation of the collector. - Highlights: • The hard segments of stretched PU nanofibers exhibit periodic structures. • The adsorbed protein on stretched PU nanofibers was increased compared with PU film. • The hard segment alignment on stretched PU nanofibers mediated protein adsorption.

  15. Optimization of CO2 adsorption capacity and cyclical adsorption/desorption on tetraethylenepentamine-supported surface-modified hydrotalcite.

    Science.gov (United States)

    Thouchprasitchai, Nutthavich; Pintuyothin, Nuthapol; Pongstabodee, Sangobtip

    2018-03-01

    The objective of this research was to investigate CO 2 adsorption capacity of tetraethylenepentamine-functionalized basic-modified calcined hydrotalcite (TEPA/b-cHT) sorbents at atmospheric pressure formed under varying TEPA loading levels, temperatures, sorbent weight to total gaseous flow rate (W/F) ratios and CO 2 concentrations in the influent gas. The TEPA/b-cHT sorbents were characterized by means of X-ray diffraction (XRD), Fourier transform infrared spectrometry (FT-IR), thermal gravimetric analysis (TGA), Brunauer-Emmet-Teller (BET) analysis of nitrogen (N 2 ) adsorption/desorption and carbon-hydrogen-nitrogen (CHN) elemental analysis. Moreover, a full 2 4 factorial design with three central points at a 95% confidence interval was used to screen important factor(s) on the CO 2 adsorption capacity. It revealed that 85.0% variation in the capacity came from the influence of four main factors and the 15.0% one was from their interactions. A face-centered central composite design response surface method (FCCCD-RSM) was then employed to optimize the condition, the maximal capacity of 5.5-6.1mmol/g was achieved when operating with a TEPA loading level of 39%-49% (W/W), temperature of 76-90°C, W/F ratio of 1.7-2.60(g·sec)/cm 3 and CO 2 concentration of 27%-41% (V/V). The model fitted sufficiently the experimental data with an error range of ±1.5%. From cyclical adsorption/desorption and selectivity at the optimal condition, the 40%TEPA/b-cHT still expressed its effective performance after eight cycles. Copyright © 2017. Published by Elsevier B.V.

  16. Adsorption of phthalocyanines on noble metal surfaces; Adsorption von Phthalocyaninen auf Edelmetalloberflaechen

    Energy Technology Data Exchange (ETDEWEB)

    Kroeger, Ingo

    2011-05-20

    In this thesis the adsorbate systems CuPc/Ag(111), CuPc/Au(111), CuPc/Cu(111), H2Pc and TiOPc/Ag(111) were investigated and characterized in great detail using complementary methods. The focus of the experiments was the determination of lateral geometric structures with spot-profile-analysis low energy electron diffraction (SPA-LEED) and scanning tunneling microscopy (STM), as well as the measurement of adsorption heights using the method of normal incidence X-ray standing waves (NIXSW). High resolution electron energy loss spectroscopy (HREELS) was used to characterize the vibronic properties of the molecule and the interface dynamical charge transfer (IDCT). The electronic structure and the charge transfer into the molecule were investigated with ultraviolet photoelectron spectroscopy (UPS). The most important results of this work are related with the interplay between adsorbate-substrate and adsorbate-adsorbate interaction of Phthalocyanines in the submonolayer regime. (orig.)

  17. 4He adsorption and third-sound propagation on rough CaF2 surfaces

    International Nuclear Information System (INIS)

    Herrmann, J.C.; Hallock, R.B.

    2003-01-01

    We have investigated the propagation of third sound on well characterized rough CaF 2 surfaces as a function of 4 He film thickness. In addition we have measured the adsorption of 4 He to the CaF 2 surfaces using quartz crystal microbalances. We report values for the superfluid depletion thickness D for the three surfaces examined here. A model for the reduction of the third-sound speed due to the increased helium adsorption on rough CaF 2 is explored

  18. 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

  19. First principles study of dissolved oxygen water adsorption on Fe (001 surfaces

    Directory of Open Access Journals (Sweden)

    Dong ZHANG

    2018-02-01

    Full Text Available In order to study the mechanism of dissolved oxygen content on the surface corrosion behavior of Fe-based heat transfer, the first principle is used to study the adsorption of O2 monomolecular, H2O monolayer and dissolved oxygen system on Fe-based heat transfer surface. The GGA/PBE approximation is used to calculate the adsorption energy, state density and population change during the adsorption process. Calculations prove that when the dissolved oxygen is adsorbed on the Fe-based surface, the water molecule tends to adsorb at the top sites, and the oxygen molecule tends to adsorb at Griffiths. When the H2O molecule adsorbs and interacts on the Fe (001 surface, the charge distribution of the interfacial double electric layer changes to cause the Fe atoms to lose electrons, resulting in the change of the surface potential. When the O2 molecule adsorbs on the Fe (001 crystal surfaces, the electrons on the Fe (001 surface are lost and the surface potential increases. O2 molecule and the surface of the Fe atoms are prone to electron transfer, in which O atom's 2p orbit for the adsorption of O2 molecule on Fe (001 crystal surface play a major role. With the increase of the proportion of O2 molecule in the dissolved oxygen water, the absolute value of the adsorption energy increases, and the interaction of the Fe-based heat transfer surface is stronger. This study explores the influence law of different dissolved oxygen on the Fe base heat exchange surface corrosion, and the base metal corrosion mechanism for experimental study provides a theoretical reference.

  20. The role of van der Waals interactions in the adsorption of noble gases on metal surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Chen, De-Li; Al-Saidi, W A; Johnson, J Karl

    2012-10-03

    Adsorption of noble gases on metal surfaces is determined by weak interactions. We applied two versions of the nonlocal van der Waals density functional (vdW-DF) to compute adsorption energies of Ar, Kr, and Xe on Pt(111), Pd(111), Cu(111), and Cu(110) metal surfaces. We have compared our results with data obtained using other density functional approaches, including the semiempirical vdW corrected DFT-D2. The vdW-DF results show considerable improvements in the description of adsorption energies and equilibrium distances over other DFTbased methods, giving good agreement with experiments. We have also calculated perpendicular vibrational energies for noble gases on the metal surfaces using vdWDF data and found excellent agreement with available experimental results. Our vdW-DF calculations show that adsorption of noble gases on low-coordination sites is energetically favored over high-coordination sites, but only by a few meV. Analysis of the 2-dimensional potential energy surface shows that the high-coordination sites are local maxima on the 2-dimensional potential energy surface and therefore unlikely to be observed in experiments, which provides an explanation of the experimental observations. The DFT-D2 approach with the standard parameterization was found to overestimate the dispersion interactions, and to give the wrong adsorption site preference for four of the nine systems we studied.

  1. Use of cellulose derivatives on gold surfaces for reduced nonspecific adsorption of immunoglobulin G.

    Science.gov (United States)

    Volden, Sondre; Zhu, Kaizheng; Nyström, Bo; Glomm, Wilhelm R

    2009-09-01

    This study addresses the design of protein-repellent gold surfaces using hydroxyethyl- and ethyl(hydroxyethyl) cellulose (HEC and EHEC) and hydrophobically modified analogues of these polymers (HM-HEC and HM-EHEC). Adsorption behavior of the protein immunoglobulin G (IgG) onto pure gold and gold surfaces coated with cellulose polymers was investigated and described by quartz crystal microbalance with dissipation monitoring (QCM-D), atomic force microscopy (AFM) and contact angle measurements (CAM). Surfaces coated with the hydrophobically modified cellulose derivatives were found to significantly outperform a reference poly(ethylene glycol) (PEG) coating, which in turn prevented 90% of non-specific protein adsorption as compared to adsorption onto pure gold. HEC and EHEC prevented around 30% and 60% of the IgG adsorption observed on pure gold, while HM-HEC and HM-EHEC were both found to completely hinder biofouling when deposited on the gold substrates. Adsorption behavior of IgG has been discussed in terms of polymer surface coverage and roughness of the applied surfaces, together with hydrophobic interactions between protein and gold, and also polymer-protein interactions.

  2. Anisotropic surface chemistry properties and adsorption behavior of silicate mineral crystals.

    Science.gov (United States)

    Xu, Longhua; Tian, Jia; Wu, Houqin; Fang, Shuai; Lu, Zhongyuan; Ma, Caifeng; Sun, Wei; Hu, Yuehua

    2018-03-07

    Anisotropic surface properties of minerals play an important role in a variety of fields. With a focus on the two most intensively investigated silicate minerals (i.e., phyllosilicate minerals and pegmatite aluminosilicate minerals), this review highlights the research on their anisotropic surface properties based on their crystal structures. Four surface features comprise the anisotropic surface chemistry of minerals: broken bonds, energy, wettability, and charge. Analysis of surface broken bond and energy anisotropy helps to explain the cleavage and growth properties of mineral crystals, and understanding surface wettability and charge anisotropy is critical to the analysis of minerals' solution behavior, such as their flotation performance and rheological properties. In a specific reaction, the anisotropic surface properties of minerals are reflected in the adsorption strengths of reagents on different mineral surfaces. Combined with the knowledge of mineral crushing and grinding, a thorough understanding of the anisotropic surface chemistry properties and the anisotropic adsorption behavior of minerals will lead to the development of effective relational models comprising their crystal structure, surface chemistry properties, and targeted reagent adsorption. Overall, such a comprehensive approach is expected to firmly establish the connection between selective cleavage of mineral crystals for desired surfaces and designing novel reagents selectively adsorbed on the mineral surfaces. As tools to characterize the anisotropic surface chemistry properties of minerals, DLVO theory, atomic force microscopy (AFM), and molecular dynamics (MD) simulations are also reviewed. Copyright © 2017 Elsevier B.V. All rights reserved.

  3. Spectroscopic link between adsorption site occupation and local surface chemical reactivity

    DEFF Research Database (Denmark)

    Baraldi, A.; Lizzit, S.; Comelli, G.

    2004-01-01

    rules, from which adsorption sites are directly determined. Theoretical calculations rationalize the results for transition metal surfaces in terms of the energy shift of the d-band center of mass and this proves that adsorbate-induced SCL shifts provide a spectroscopic measure of local surface...

  4. Ion effects in the adsorption of carboxylate on oxide surfaces, studied with quartz crystal microbalance

    NARCIS (Netherlands)

    Wang, Lei; Sîretanu, Igor; Duits, Michael H.G.; Cohen Stuart, Martinus Abraham; Mugele, Friedrich Gunther

    2016-01-01

    We chose water-soluble sodium hexanoate as a model organic molecule to study the role of salt ions (Ca2+, Na+, Cl−) in the adsorption of carboxylates to mineral surfaces (silica, alumina, gibbsite) of variable surface charge and chemistry. Quartz crystal microbalance (QCM-D) measurements reveal a

  5. Impacts of Surface Site Coordination on Arsenate Adsorption: Macroscopic Uptake and Binding Mechanisms on Aluminum Hydroxide Surfaces.

    Science.gov (United States)

    Xu, Tingying; Catalano, Jeffrey G

    2016-12-13

    Aluminum hydroxides play important roles in regulating the fate and transport of contaminants and nutrients in soils and aquatic systems. Like many metal oxides, these minerals display surface functional groups in a series of coordination states, each of which may differ in its affinity for adsorbates. The distribution of functional group types varies among distinct surfaces of aluminum hydroxides, and we thus hypothesize that the adsorption behavior and mechanisms will show a dependence on particle morphology. To test this hypothesis, we investigate arsenate adsorption on two aluminum hydroxide polymorphs with distinct particle morphologies, gibbsite [γ-Al(OH) 3 ] and bayerite [α-Al(OH) 3 ], at pH 4 and 7. Synthetic gibbsite platelets expose large (001) basal surfaces predicted to be terminated by doubly coordinated functional groups (>Al 2 OH). In contrast, synthetic bayerite microrods display mainly edge surfaces (parallel to the c axis) containing abundant singly coordinated functional groups (>AlOH 2 ). Macroscopic adsorption studies show that gibbsite adsorbs less arsenate per unit surface area than bayerite at both pH values and suggest that two surface complexes form on each material. Similar electrokinetic behavior is displayed at the same relative coverages of arsenate, suggesting that similar reactive surface groups (>AlOH 2 ) control the surface charging on both particles. EXAFS spectroscopy shows that there is no variation in arsenate surface speciation on a given mineral with surface coverage or pH. Whereas bidentate binuclear inner-sphere species are the dominant complexes present, the EXAFS result suggest that outer-sphere species also occur on both minerals, with a greater abundance on gibbsite. This binding mode likely involves adsorption to >Al 2 OH sites, which have a slow ligand exchange rate that inhibits inner-sphere binding. These results demonstrate that adsorption mechanisms and capacity, even when normalized for specific surface area

  6. 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)

  7. Surface structure and adsorption properties of ultrafine porous carbon fibers

    International Nuclear Information System (INIS)

    Song Xiaofeng; Wang Ce; Zhang Dejiang

    2009-01-01

    Ultrafine porous carbon fibers (UPCFs) were successfully synthesized by chemical activation of electrospun polyacrylonitrile fibers. In the current approach, potassium hydroxide was adopted as activation reagent. UPCFs were systematically evaluated by scanning electron microscope and nitrogen adsorption. The mass ratio of potassium hydroxide to preoxidized fibers, activation temperature and activation time are crucial for producing high quality UPCFs. The relationships between porous structure and process parameters are explored. UPCFs were applied as adsorbent for nitrogen monoxide to be compared with commercial porous carbon fibers.

  8. Surface modification influencing adsorption of red wine constituents: The role of functional groups

    Energy Technology Data Exchange (ETDEWEB)

    Mierczynska-Vasilev, Agnieszka, E-mail: agnieszka.mierczynska-vasilev@awri.com.au; Smith, Paul A., E-mail: paul.smith@awri.com.au

    2016-11-15

    Highlights: • Chemical surface composition affects behaviour of wine adsorption. • SO{sub 3}H and COOH groups adsorb more of the wine nitrogen-containing compounds. • NH{sub 2} and NR{sub 3} groups encourage carbon-containing compounds adsorption. • Red wine constituents after filtration adsorbed more on NR{sub 3} and CHO surfaces. - Abstract: The adsorption of wine constituents at solid surfaces is important in applications such as filtration and membrane fouling, binding to tanks and fittings and interactions with processing aids such as bentonite. The interaction of wine constituents with surfaces is mediated through adsorbed wine components, where the type of constituents, amount, orientation, and conformation are of consequence for the surface response. This study examines the effect of surface chemical functionalities on the adsorption of red wine constituents. Plasma-polymerized films rich in amine, carboxyl, hydroxyl, formyl and methyl functional groups were generated on solid substrates whereas, glycidyltrimethylammonium chloride was covalently attached to allylamine plasma-polymer modified surface and poly(sodium styrenesulfonate) was electrostatically adsorbed to an amine plasma-polymerized surface. The surface chemical functionalities were characterized by X-ray photoelectron spectroscopy. The ability of different substrates to adsorb red wine constituents was evaluated by quartz crystal microbalance and atomic force microscopy. The results showed that substrates modified with −SO{sub 3}H and –COOH groups can adsorb more of the wine nitrogen-containing compounds whereas −NH{sub 2} and −NR{sub 3} groups encourage carbon-containing compounds adsorption. Red wine constituents after filtration were adsorbed in higher extend on −NR{sub 3} and –CHO surfaces. The –OH modified surfaces had the lowest ability to absorb wine components.

  9. Surface modification influencing adsorption of red wine constituents: The role of functional groups

    International Nuclear Information System (INIS)

    Mierczynska-Vasilev, Agnieszka; Smith, Paul A.

    2016-01-01

    Highlights: • Chemical surface composition affects behaviour of wine adsorption. • SO 3 H and COOH groups adsorb more of the wine nitrogen-containing compounds. • NH 2 and NR 3 groups encourage carbon-containing compounds adsorption. • Red wine constituents after filtration adsorbed more on NR 3 and CHO surfaces. - Abstract: The adsorption of wine constituents at solid surfaces is important in applications such as filtration and membrane fouling, binding to tanks and fittings and interactions with processing aids such as bentonite. The interaction of wine constituents with surfaces is mediated through adsorbed wine components, where the type of constituents, amount, orientation, and conformation are of consequence for the surface response. This study examines the effect of surface chemical functionalities on the adsorption of red wine constituents. Plasma-polymerized films rich in amine, carboxyl, hydroxyl, formyl and methyl functional groups were generated on solid substrates whereas, glycidyltrimethylammonium chloride was covalently attached to allylamine plasma-polymer modified surface and poly(sodium styrenesulfonate) was electrostatically adsorbed to an amine plasma-polymerized surface. The surface chemical functionalities were characterized by X-ray photoelectron spectroscopy. The ability of different substrates to adsorb red wine constituents was evaluated by quartz crystal microbalance and atomic force microscopy. The results showed that substrates modified with −SO 3 H and –COOH groups can adsorb more of the wine nitrogen-containing compounds whereas −NH 2 and −NR 3 groups encourage carbon-containing compounds adsorption. Red wine constituents after filtration were adsorbed in higher extend on −NR 3 and –CHO surfaces. The –OH modified surfaces had the lowest ability to absorb wine components.

  10. Surface-Controlled Metal Oxide Resistive Memory

    KAUST Repository

    Ke, Jr-Jian

    2015-10-28

    To explore the surface effect on resistive random-access memory (ReRAM), the impact of surface roughness on the characteristics of ZnO ReRAM were studied. The thickness-independent resistance and the higher switching probability of ZnO ReRAM with rough surfaces indicate the importance of surface oxygen chemisorption on the switching process. Furthermore, the improvements in switching probability, switching voltage and resistance distribution observed for ReRAM with rough surfaces can be attributed to the stable oxygen adatoms under various ambience conditions. The findings validate the surface-controlled stability and uniformity of ReRAM and can serve as the guideline for developing practical device applications.

  11. An affinity adsorption media that mimics heparan sulfate proteoglycans for the treatment of drug-resistant bacteremia

    Science.gov (United States)

    McCrea, Keith R.; Ward, Robert S.

    2016-06-01

    Removal of several drug-resistant bacteria from blood by affinity adsorption onto a heparin-functional media is reported. Heparin is a chemical analogue of heparan sulfate (HS) proteoglycans, found on transmembrane proteins of endothelial cells. Many blood-borne human pathogens, including bacteria, viruses, parasites, and fungi have been reported to target HS as an initial step in their pathogenesis. Here, we demonstrate the binding and removal of Methicillin-resistant Staphylococcus aureus (MRSA), Extended-Spectrum Betalactamase Klebsiella pneumoniae (ESBL), and two Carbapenem-resistant Enterobacteriaceae (both CRE Escherichia coli and CRE K. pneumoniae) using 300 μm polyethylene beads surface modified with end-point-attached heparin. Depending on the specific bacteria, the amount removed ranged between 39% (ESBL) and 99.9% (CRE). The total amount of bacteria adsorbed ranged between 2.8 × 105 and 8.6 × 105 colony forming units (CFU) per gram of adsorption media. Based on a polymicrobial challenge which showed no competitive binding, MRSA and CRE apparently utilize different binding sequences on the immobilized heparin ligand. Since the total circulating bacterial load during bacteremia seldom exceeds 5 × 105 CFUs, it appears possible to significantly reduce bacterial concentration in infected patients by multi-pass recirculation of their blood through a small extracorporeal affinity filter containing the heparin-functional adsorption media. This 'dialysis-like therapy' is expected to improve patient outcomes and reduce the cost of care, particularly when there are no anti-infective drugs available to treat the infection.

  12. Adsorption Mechanism of Cu-Doped SnO2 (110 Surface toward H2 Dissolved in Power Transformer

    Directory of Open Access Journals (Sweden)

    Feng Wang

    2016-01-01

    Full Text Available The content of hydrogen is a key quantity in condition assessment and fault diagnosis of power transformer. Based on the density functional theory (DFT, the adsorption mechanism of Cu-doped SnO2 surface toward H2 has been systematically studied in this work. Firstly, the relaxation, the bond length, and overlap population of both the pure and Cu-doped SnO2 are computed. To determine the optimal doping position, the formation energies of four potential sites (i.e., Sn5c, Sn6c, Sn5c-s, and Sn6c-s are then compared with each other. The adsorption energy and the electronic structure of SnO2 surface are analysed and discussed in detail. Furthermore, to estimate the partial atomic charges and the electrical conductance, the Mulliken population analysis is also performed. It has been found that the bridge oxygen is the most favourable position. The partial density of states of H2 after adsorption is broadened and shifted close to the Fermi level. A large amount of charges would be transferred and then released back into its conduction band, leading to the reduction of resistance and the enhancement of sensitivity toward H2. The results of this work provide references for SnO2-based sensor design.

  13. Adsorption of uranium by amidoximated chitosan-grafted polyacrylonitrile, using response surface methodology.

    Science.gov (United States)

    Xu, Chao; Wang, Jingjing; Yang, Tilong; Chen, Xia; Liu, Xunyue; Ding, Xingcheng

    2015-05-05

    The amidoximated chitosan-grafted polyacrylonitrile (CTS-g-PAO) was prepared for the adsorption of uranium from water. The effects of pH, concentration of uranium and the solid-liquid ratio on the adsorption of uranium by CTS-g-PAO were optimized using Doehlert design of response surface methodology (RSM). The adsorption capacity and removal efficiency achieved 312.06 mg/g and 86.02%, respectively. The adsorption process attained equilibrium only in 120 min. More than 80% of the absorbed uranium could be desorbed by 0.1 mol/l HCl or EDTA-Na, and CTS-g-PAO could be reused at least 3 times. The CTS-g-PAO and U(VI) ions formed a chelate complex due to FTIR spectral analysis. The surface morphology of CTS-g-PAO was also investigated by SEM. The adsorption process was better described by Langmuir isotherm and pseudo second order kinetic model. Results obtained indicated that CTS-g-PAO was very promising in adsorption of uranium from water. Copyright © 2014 Elsevier Ltd. All rights reserved.

  14. Adsorption of naphthalene onto a high-surface-area carbon from waste ion exchange resin.

    Science.gov (United States)

    Shi, Qianqian; Li, Aimin; Zhu, Zhaolian; Liu, Bing

    2013-01-01

    A high-surface-area carbon (KC-1) was prepared from waste polystyrene-based ion exchange resin by KOH activation and used for naphthalene adsorption. The carbon exhibited a good hydrophobic nature with developed porous structure, favoring the adsorption of organic compounds. The Brunauer-Emmett-Teller surface area and total pore volume of KC-1 were 3442.2 and 1.68 cm3/g, respectively, which can be compared with those of KOH-activated carbons prepared from other precursors. Batch experiments were carried out to investigate the adsorption of naphthalene onto KC-1. The equilibrium data were analyzed by the Langmuir, Freundlich, and Polanyi-Manes isotherms and agreed with the Polanyi-Manes Model. The adsorption of naphthalene depended greatly on the porosity of the carbon, and the dispersive interactions between naphthalene and carbon could be relatively weak. The pH variation in aqueous solution had little effect on the adsorption process. The equilibrium time for 0.04 g/L of carbon dose was around 5 hr. Different models were used to evaluate the kinetic data and the pseudo second-order model was suitable to describe the kinetic process of naphthalene adsorption onto KC-1. Regeneration of spent carbon could be carried out effectively by alcohol treatment. The results indicated that KC-1 was a promising adsorbent for the removal of polycyclic aromatic hydrocarbons from aqueous solutions.

  15. Adsorption of thiophene on transition metal surfaces with the inclusion of van der Waals effects

    Science.gov (United States)

    Malone, Walter; Matos, Jeronimo; Kara, Abdelkader

    2018-03-01

    We use density functional theory with the inclusion of the van der Waals interaction to study the adsorption of thiophene, C4H4S, on Pt, Rh, Pd, Au, and Ag (100) surfaces. The five van der Waals (vdW) inclusive functionals we employ are optB86b-vdW, optB88-vdW, optPBE-vdW, revPBE-vdW, and rPW86-vdW2. For comparison we also run calculations with the GGA- Perdew Burke and Ernzerhof (PBE) functional. We examine several adsorption sites with the plane of the molecule parallel or perpendicular to the surface. The most stable configuration on all metals was the site where the center of the thiophene lies over a 4-fold hollow site with the sulfur atom lying close to a top site. Furthermore, we examine several electronic and geometric properties of the adsorbate including charge transfer, modification of the d-band, adsorption energy, tilt angle, and adsorption height. For the coinage metals PBE gives the lowest adsorption energy. For reactive transition metal substrates, revPBE-vdW and rPW86-vdW2 give lower adsorption energies than PBE.

  16. A DFT study of adsorption of glycine onto the surface of BC2N nanotube

    International Nuclear Information System (INIS)

    Soltani, Alireza; Azmoodeh, Zivar; Javan, Masoud Bezi; Lemeski, E. Tazikeh; Karami, Leila

    2016-01-01

    Highlights: • Glycine adsorption over the pristine BC 2 N nanotubes is investigated by DFT calculations. • Adsorption of glycine in its zwitterionic form is stronger in comparison with the radical form. • Adsorption of glycine from its amine head on adsorbent leads to a significant decrease in the electronic properties. - Abstract: A theoretical study of structure and the energy interaction of amino acid glycine (NH 2 CH 2 COOH) with BC 2 N nanotube is crucial for apperception behavior occurring at the nanobiointerface. Herein, we studied the adsorption of glycine in their radical and zwitterionic forms upon the surface of BC 2 N nanotube using M06 functional and 6-311G** standard basis set. We also considered the different orientations of the glycine amino acid on the surface of adsorbent. Further, we found out that the stability of glycine from its carbonyl group is higher than hydroxyl and amine groups. Our results also indicated that the electronic structure of BC 2 N nanotube on the adsorption of glycine from its amine group is more altered than the other groups. Our study exhibits that opto-electronic property of adsorbent is changed after the glycine adsorption.

  17. Ice-surface adsorption enhanced colligative effect of antifreeze proteins in ice growth inhibition

    Science.gov (United States)

    Mao, Yougang; Ba, Yong

    2006-09-01

    This Communication describes a mechanism to explain antifreeze protein's function to inhibit the growth of ice crystals. We propose that the adsorption of antifreeze protein (AFP) molecules on an ice surface induces a dense AFP-water layer, which can significantly decrease the mole fraction of the interfacial water and, thus, lower the temperature for a seed ice crystal to grow in a super-cooled AFP solution. This mechanism can also explain the nearly unchanged melting point for the ice crystal due to the AFP's ice-surface adsorption. A mathematical model combining the Langmuir theory of adsorption and the colligative effect of thermodynamics has been proposed to find the equilibrium constants of the ice-surface adsorptions, and the interfacial concentrations of AFPs through fitting the theoretical curves to the experimental thermal hysteresis data. This model has been demonstrated by using the experimental data of serial size-mutated beetle Tenebrio molitor (Tm) AFPs. It was found that the AFP's ice-surface adsorptions could increase the interfacial AFP's concentrations by 3 to 4 orders compared with those in the bulk AFP solutions.

  18. Periodic Mesoporous Organosilica Nanocubes with Ultrahigh Surface Areas for Efficient CO2 Adsorption

    Science.gov (United States)

    Wei, Yong; Li, Xiaomin; Zhang, Renyuan; Liu, Yong; Wang, Wenxing; Ling, Yun; El-Toni, Ahmed Mohamed; Zhao, Dongyuan

    2016-02-01

    Ultrahigh surface area single-crystals of periodic mesoporous organosilica (PMOs) with uniform cubic or truncated-cubic morphology and organic/inorganic components homogeneously distributed over the whole frameworks have successfully been prepared by a sol-gel surfactant-templating method. By tuning the porous feature and polymerization degree, the surface areas of the obtained PMO nanocubes can reach as high as 2370 m2/g, which is the highest for silica-based mesoporous materials. The ultrahigh surface area of the obtained PMO single crystals is mainly resulted from abundant micropores in the mesoporous frameworks. Furthermore, the diameter of the nanocubes can also be well controlled from 150 to 600 nm. The materials show ultrahigh CO2 adsorption capacity (up to 1.42 mmol/g at 273 K) which is much higher than other porous silica materials and comparable to some carbonaceous materials. The adsorption of CO2 into the PMO nanocubes is mainly in physical interaction, therefore the adsorption-desorption process is highly reversible and the adsorption capacity is much dependent on the surface area of the materials. Moreover, the selectivity is also very high (~11 times to N2) towards CO2 adsorption.

  19. Effects of topology on the adsorption of singly tethered ring polymers to attractive surfaces.

    Science.gov (United States)

    Li, Bing; Sun, Zhao-Yan; An, Li-Jia

    2015-07-14

    We investigate the effect of topology on the equilibrium behavior of singly tethered ring polymers adsorbed on an attractive surface. We focus on the change of square radius of gyration Rg(2), the perpendicular component Rg⊥(2) and the parallel component Rg‖(2) to the adsorbing surface, the mean contacting number of monomers with the surface , and the monomer distribution along z-direction during transition from desorption to adsorption. We find that both of the critical point of adsorption εc and the crossover exponent ϕ depend on the knot type when the chain length of ring ranges from 48 to 400. The behaviors of Rg(2), Rg⊥(2), and Rg‖(2) are found to be dependent on the topology and the monomer-surface attractive strength. At weak adsorption, the polymer chains with more complex topology are more adsorbable than those with simple topology. However, at strong adsorption, the polymer chains with complex topology are less adsorbable. By analyzing the distribution of monomer along z-direction, we give a possible mechanism for the effect of topology on the adsorption behavior.

  20. Link between chemotactic response to Ni2+ and its adsorption onto the Escherichia coli cell surface.

    Science.gov (United States)

    Borrok, David; Borrok, M Jack; Fein, Jeremy B; Kiessling, Laura L

    2005-07-15

    Bacterial chemotaxis is of medical, biological, and geological significance. Despite its importance, current chemotaxis measurements fail to account for the speciation of the chemical effector and the protonation state of the bacterial surface. We hypothesize that adsorption of Ni2+ onto the surface of Escherichia coli can influence its effective concentration and therefore influence its ability to induce a repellent response. By measuring repellent response at different pH values, the influence of Ni2+ adsorption on chemotaxis was assessed. In addition, we tested the effect of different Ni2+ chelating agents. Our data indicate that adsorption reactions influence the chemotactic response to Ni2+. We use potentiometric titration and Ni2+ adsorption experiments to develop and constrain a thermodynamic model capable of quantifying the concentration of Ni2+ at the bacteria/solution interface. Results from this model predict that the concentration of adsorbed Ni2+ is linearly proportional to the magnitude of the chemotactic response in E. coli. If adsorption is linked to chemotaxis in other cases, then chemotactic responses in realistic settings depend on a number of environmental factors such as pH, competing binding agents (e.g., aqueous organic acids, natural organic matter, mineral surfaces, etc.), and ionic strength. Our modeling approach quantifies adsorbed species on bacterial surfaces and may be used to predict the responses of different species to a variety of chemoeffectors. Our data suggest that specified changes in environmental conditions can be used to tune chemotactic responses in natural biological and geological settings.

  1. Study of Hexane Adsorption on Activated Carbons with Differences in Their Surface Chemistry.

    Science.gov (United States)

    Hernández-Monje, Diana; Giraldo, Liliana; Moreno-Piraján, Juan Carlos

    2018-02-22

    The study of aliphatic compounds adsorption on activated carbon can be carried out from the energetic change involved in the interaction; the energy values can be determined from isotherms or by the immersion enthalpy. Vapor phase adsorption isotherms of hexane at 263 K on five activated carbons with different content of oxygenated groups and the immersion enthalpy of the activated carbons in hexane and water were determined in order to characterize the interactions in the solid-liquid system, and for calculating the hydrophobic factor of the activated carbons. The micropore volume and characteristic energy from adsorption isotherms of hexane, the BET (Brunauer-Emmett-Teller) surface area from the adsorption isotherms of N₂, and the area accessible to the hexane from the immersion enthalpy were calculated. The activated carbon with the lowest content of oxygenated groups (0.30 µmolg - ¹) and the highest surface area (996 m²g - ¹) had the highest hexane adsorption value: 0.27 mmol g - ¹; the values for E o were between 5650 and 6920 Jmol - ¹ and for ΔH im were between -66.1 and -16.4 Jg - ¹. These determinations allow us to correlate energetic parameters with the surface area and the chemical modifications that were made to the solids, where the surface hydrophobic character of the activated carbon favors the interaction.

  2. Adsorption of the water molecule on monolayer graphene surface has effect on its optical properties

    International Nuclear Information System (INIS)

    Peng, Y F; Wang, J; Lu, Z S; Han, X Y

    2015-01-01

    The adsorption of water molecules on the surface of a monolayer graphene can be studied with the Materials Studio software and be applied density function theory from first principles. By studying the interaction of graphene with water molecule, it uses DFT (density function theory) with the PBE-GGA (the generalized gradient approximation of Perdew- Burke-Ernzerhof) and Periodic plane model, on the one hand working out the adsorption energy, and on the other hand getting related optical properties. It is shown that a single water molecule on graphene has very small adsorption energy, mainly owning to the van der Waals interactions. Graphene has high hydrophobic; adsorbed water molecule has little effect on the electronic structure of the graphene. The optical properties of the graphene have changed after the adsorption. (paper)

  3. Adsorption of small NaCl clusters on surfaces of silicon nanostructures

    International Nuclear Information System (INIS)

    Amsler, Maximilian; Alireza Ghasemi, S; Goedecker, Stefan; Neelov, Alexey; Genovese, Luigi

    2009-01-01

    We have studied possible adsorption geometries of neutral NaCl clusters on the disordered surface of a large silicon model tip used in non-contact atomic force microscopy. The minima hopping method was used to determine low energy model tip configurations as well as ground state geometries of isolated NaCl clusters. The combined system was treated with density functional theory. Alkali halides have proven to be strong structure seekers and tend to form highly stable ground state configurations whenever possible. The favored adsorption geometry for four Na and four Cl atoms was found to be an adsorption of four NaCl dimers due to the formation of Cl-Si bonds. However, for larger NaCl clusters, the increasing energy required to dissociate the cluster into NaCl dimers suggests that adsorption of whole clusters in their isolated ground state configuration is preferred.

  4. 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.

  5. Generation of Electricity at Graphene Interface Governed by Underlying Surface Dipole Induced Ion Adsorption

    Science.gov (United States)

    Yang, Shanshan; Su, Yudan; Wu, Qiong; Zhang, Yuanbo; Tian, Chuanshan

    Aqueous droplet moving along graphene surface can produce electricity This interesting phenomenon provided environment-friendly means to harvest energy from graphene interface in contact with sea wave or rain droplets. However, microscopically, the nature of charge adsorption at the graphene interface is still unclear. Here, utilizing sum-frequency spectroscopy in combined with measurement of electrical power generation, the origin of charge adsorption on graphene was investigated. It was found that the direct ion-graphene interaction is negligibly small, contrary to the early speculation, but the ordered surface dipole from the supporting substrate, such as PET, is responsible for ion adsorption at the interface. Graphene serves as a conductive layer with mild screening of Coulomb interaction when aqueous droplet slips over the surface. These results pave the way for optimization of energy harvesting efficiency of graphene-based device.

  6. AFM study of adsorption of protein A on a poly(dimethylsiloxane) surface

    International Nuclear Information System (INIS)

    Yu Ling; Lu Zhisong; Gan Ye; Liu Yingshuai; Li, C M

    2009-01-01

    In this paper, the morphology and kinetics of adsorption of protein A on a PDMS surface is studied by AFM. The results of effects of pH, protein concentration and contact time of the adsorption reveal that the morphology of adsorbed protein A is significantly affected by pH and adsorbed surface concentration, in which the pH away from the isoelectric point (IEP) of protein A could produce electrical repulsion to change the protein conformation, while the high adsorbed surface protein volume results in molecular networks. Protein A can form an adsorbed protein film on PDMS with a maximum volume of 2.45 x 10 -3 μm 3 . This work enhances our fundamental understanding of protein A adsorption on PDMS, a frequently used substrate component in miniaturized immunoassay devices.

  7. Adsorption behavior of DNA-wrapped carbon nanotubes on self-assembled monolayer surfaces.

    Science.gov (United States)

    Zangmeister, Rebecca A; Maslar, James E; Opdahl, Aric; Tarlov, Michael J

    2007-05-22

    We have examined the adsorption of DNA-wrapped single-walled carbon nanotubes (DNA-SWNTs) on hydrophobic, hydrophilic, and charged surfaces of alkylthiol self-assembled monolayers (SAMs) on gold. Our goal is to understand how DNA-SWNTs interact with surfaces of varying chemical functionality. These samples were characterized using reflection absorption FTIR (RAIRS), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. We have found that DNA-SWNTs preferentially adsorb to positively charged amine-terminated SAMs and to bare gold surfaces versus hydrophobic methyl-terminated or negatively charged carboxylic acid-terminated SAMs. Examination of the adsorption on gold of single-strand DNA (ssDNA) of the same sequence used to wrap the SWNTs suggests that the DNA wrapping plays a role in the adsorption behavior of DNA-SWNTs.

  8. Insights into the superhydrophobicity of metallic surfaces prepared by electrodeposition involving spontaneous adsorption of airborne hydrocarbons

    International Nuclear Information System (INIS)

    Liu, Peng; Cao, Ling; Zhao, Wei; Xia, Yue; Huang, Wei; Li, Zelin

    2015-01-01

    Graphical abstract: - Highlights: • Several superhydrophobic metallic surfaces were fabricated by fast electrodeposition. • Both micro/nanostructures and adsorption of airborne hydrocarbons make contributions. • XPS analyses confirm presence of airborne hydrocarbons on these metallic surfaces. • The adsorption of airborne hydrocarbons on the clean metal Au surface was very quick. • UV-O 3 treatment oxidized the hydrocarbons to hydrophilic oxygen-containing organics. - Abstract: Electrochemical fabrication of micro/nanostructured metallic surfaces with superhydrophobicity has recently aroused great attention. However, the origin still remains unclear why smooth hydrophilic metal surfaces become superhydrophobic by making micro/nanostructures without additional surface modifications. In this work, several superhydrophobic micro/nanostructured metal surfaces were prepared by a facile one-step electrodeposition process, including non-noble and noble metals such as copper, nickel, cadmium, zinc, gold, and palladium with (e.g. Cu) or without (e.g. Au) surface oxide films. We demonstrated by SEM and XPS that both hierarchical micro/nanostructures and spontaneous adsorption of airborne hydrocarbons endowed these surfaces with excellent superhydrophobicity. We revealed by XPS that the adsorption of airborne hydrocarbons at the Ar + -etched clean Au surface was rather quick, such that organic contamination can hardly be prevented in practical operation of surface wetting investigation. We also confirmed by XPS that ultraviolet-O 3 treatment of the superhydrophobic metal surfaces did not remove the adsorbed hydrocarbons completely, but mainly oxidized them into hydrophilic oxygen-containing organic substances. We hope our findings here shed new light on deeper understanding of superhydrophobicity for micro/nanostructured metal surfaces with and without surface oxide films

  9. Surface and adsorptive properties of Moringa oleifera bark for removal of V(V) from aqueous solutions.

    Science.gov (United States)

    Mnisi, Robert Londi; Ndibewu, Peter Papoh

    2017-11-04

    The bark of Moringa oleifera, a cheap and readily available natural biopolymeric resource material, found to significantly reduce coliform load and turbidity in contaminated water is investigated in this paper. Its surface and adsorptive properties are investigated to explore its adsorptive potential in removing V(V) from aqueous solutions. Surface properties were investigated using FTIR, HRSEM/EDS, IC, and BET-N 2 adsorption techniques. Adsorptive properties were investigated by optimizing adsorption parameters such as pH, temperature, initial metal concentration, and adsorbent dosage, using V(V) as an adsorbate. The adsorption-desorption isotherms are typical of type II with a H3 hysteresis loop and is characteristic of a largely macroporous material. Bottle ink pores are observed, which can provide good accessibility of the active sites, even though the internal BET surface area is typically low (1.79 g/m 2 ). Solution pH significantly influences the adsorptive potential of the material. The low surface area negatively impacts on the adsorption capacity, but is compensated for by the exchangeable anions (Cl - , F - , PO 4 3- , NO 3 - , and SO 4 2- ) and cations (Ca 2+ , K + , Mg 2+ , and Al 3+ ) at the surface and the accessibility of the active sites. Adsorption isotherm modeling show that the surface is largely heterogeneous with complex multiple sites and adsorption is not limited to monolayer.

  10. Oxygen adsorption on the Al0.25Ga0.75N (0001) surface: A first-principles study

    Science.gov (United States)

    Fu, Jiaqi; Song, Tielei; Liang, Xixia; Zhao, Guojun

    2018-04-01

    To understand the interaction mechanism for the oxygen adsorption on AlGaN surface, herein, we built the possible models of oxygen adsorption on Al0.25Ga0.75N (0001) surface. For different oxygen coverage, three kinds of adsorption site are considered. Then the favorable adsorption sites are characterized by first principles calculation for (2 × 2) supercell of Al0.25Ga0.75N (0001) surface. On basis of the optimal adsorption structures, our calculated results show that all the adsorption processes are exothermic, indicating that the (0001) surface orientation is active towards the adsorption of oxygen. The doping of Al is advantage to the adsorption of O atom. Additionally, the adsorption energy decreases with reducing the oxygen coverage, and the relationship between them is approximately linear. Owing to the oxygen adsorption, the surface states in the fundamental band gap are significant reduced with respect to the free Al0.25Ga0.75N (0001) surface. Moreover, the optical properties on different oxygen coverage are also discussed.

  11. Surface complexation modeling calculation of Pb(II) adsorption onto the calcined diatomite

    Science.gov (United States)

    Ma, Shu-Cui; Zhang, Ji-Lin; Sun, De-Hui; Liu, Gui-Xia

    2015-12-01

    Removal of noxious heavy metal ions (e.g. Pb(II)) by surface adsorption of minerals (e.g. diatomite) is an important means in the environmental aqueous pollution control. Thus, it is very essential to understand the surface adsorptive behavior and mechanism. In this work, the Pb(II) apparent surface complexation reaction equilibrium constants on the calcined diatomite and distributions of Pb(II) surface species were investigated through modeling calculations of Pb(II) based on diffuse double layer model (DLM) with three amphoteric sites. Batch experiments were used to study the adsorption of Pb(II) onto the calcined diatomite as a function of pH (3.0-7.0) and different ionic strengths (0.05 and 0.1 mol L-1 NaCl) under ambient atmosphere. Adsorption of Pb(II) can be well described by Freundlich isotherm models. The apparent surface complexation equilibrium constants (log K) were obtained by fitting the batch experimental data using the PEST 13.0 together with PHREEQC 3.1.2 codes and there is good agreement between measured and predicted data. Distribution of Pb(II) surface species on the diatomite calculated by PHREEQC 3.1.2 program indicates that the impurity cations (e.g. Al3+, Fe3+, etc.) in the diatomite play a leading role in the Pb(II) adsorption and dominant formation of complexes and additional electrostatic interaction are the main adsorption mechanism of Pb(II) on the diatomite under weak acidic conditions.

  12. Adsorption of DNA onto gold nanoparticles and graphene oxide: surface science and applications.

    Science.gov (United States)

    Liu, Juewen

    2012-08-14

    The interaction between DNA and inorganic surfaces has attracted intense research interest, as a detailed understanding of adsorption and desorption is required for DNA microarray optimization, biosensor development, and nanoparticle functionalization. One of the most commonly studied surfaces is gold due to its unique optical and electric properties. Through various surface science tools, it was found that thiolated DNA can interact with gold not only via the thiol group but also through the DNA bases. Most of the previous work has been performed with planar gold surfaces. However, knowledge gained from planar gold may not be directly applicable to gold nanoparticles (AuNPs) for several reasons. First, DNA adsorption affinity is a function of AuNP size. Second, DNA may interact with AuNPs differently due to the high curvature. Finally, the colloidal stability of AuNPs confines salt concentration, whereas there is no such limit for planar gold. In addition to gold, graphene oxide (GO) has emerged as a new material for interfacing with DNA. GO and AuNPs share many similar properties for DNA adsorption; both have negatively charged surfaces but can still strongly adsorb DNA, and both are excellent fluorescence quenchers. Similar analytical and biomedical applications have been demonstrated with these two surfaces. The nature of the attractive force however, is different for each of these. DNA adsorption on AuNPs occurs via specific chemical interactions but adsorption on GO occurs via aromatic stacking and hydrophobic interactions. Herein, we summarize the recent developments in studying non-thiolated DNA adsorption and desorption as a function of salt, pH, temperature and DNA secondary structures. Potential future directions and applications are also discussed.

  13. SeO2 adsorption on CaO surface: DFT and experimental study on the adsorption of multiple SeO2 molecules

    Science.gov (United States)

    Fan, Yaming; Zhuo, Yuqun; Li, Liangliang

    2017-10-01

    SeO2 adsorption mechanisms on CaO surface were firstly investigated by both density functional theory (DFT) calculations and adsorption experiments. Adsorption of multiple SeO2 on the CaO (001) surface was investigated using slab model. Based on the results of adsorption energy and surface property, a double-layer adsorption mechanisms were proposed. In experiments, the SeO2 adsorption products were prepared in a U-shaped quartz reactor at 200 °C. The surface morphology was investigated by field emission scanning electron microscopy (FE-SEM). The superficial and total SeO2 mass fractions were measured by X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma atomic emission spectroscopy (ICP-AES), respectively. The surface valence state and bulk structure are determined by XPS and X-Ray Diffraction (XRD). The experimental results are in good agreement with the DFT results. In conclusion, the fundamental SeO2 chemisorption mechanisms on CaO surface were suggested.

  14. Plasma graft of poly(ethylene glycol) methyl ether methacrylate (PEGMA) on RGP lens surface for reducing protein adsorption

    Science.gov (United States)

    Yin, Shiheng; Ren, Li; Wang, Yingjun

    2017-01-01

    Poly(ethylene glycol) methyl ether methacrylate (PEGMA) was grafted on fluorosilicone acrylate rigid gas permissible contact lens surface by means of argon plasma induced polymerization to improve surface hydrophilicity and reduce protein adsorption. The surface properties were characterized by contact angle measurement, x-ray photoelectron spectroscopy (XPS) and atomic force microscopy respectively. The surface protein adsorption was evaluated by lysozyme solution immersion and XPS analysis. The results indicated that a thin layer of PEGMA was successfully grafted. The surface hydrophilicity was bettered and surface free energy increased. The lysozyme adsorption on the lens surface was reduced greatly. The study was supported by National Natural Science Foundation of China (No. 51273072).

  15. Scaling Relationships for Adsorption Energies of C2 Hydrocarbons on Transition Metal Surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Jones, G

    2011-08-18

    Using density functional theory calculations we show that the adsorption energies for C{sub 2}H{sub x}-type adsorbates on transition metal surfaces scale with each other according to a simple bond order conservation model. This observation generalizes some recently recognized adsorption energy scaling laws for AH{sub x}-type adsorbates to unsaturated hydrocarbons and establishes a coherent simplified description of saturated as well as unsaturated hydrocarbons adsorbed on transition metal surfaces. A number of potential applications are discussed. We apply the model to the dehydrogenation of ethane over pure transition metal catalysts. Comparison with the corresponding full density functional theory calculations shows excellent agreement.

  16. Adsorption of fluids on solid surfaces: A route toward very dense layers

    Energy Technology Data Exchange (ETDEWEB)

    Sartarelli, S.A. [Instituto de Desarrollo Humano, Universidad Nacional de General Sarmiento, San Miguel (Argentina); Szybisz, L., E-mail: szybisz@tandar.cnea.gov.ar [Laboratorio TANDAR, Departamento de Fisica, Comision Nacional de Energia Atomica, RA-1429 Buenos Aires (Argentina); Departamento de Fiica, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires (Argentina); Consejo Nacional de Investigaciones Cientificas y Tecnicas, RA-1033 Buenos Aires (Argentina)

    2012-08-15

    Adsorption of Xe on single planar walls is investigated in the frame of a density functional theory. The strength of the adsorbate-substrate attraction is changed by considering surfaces of Cs, Na, Li, and Mg. The behavior is analyzed by varying the temperature T (between the triple point T{sub t} and the critical T{sub c}) and the coverage {Gamma}{sub Script-Small-L }. The obtained adsorption isotherms exhibit a variety of wetting situations. Density profiles are reported. It is shown that for strongly attractive surfaces the adsorbed liquid becomes very dense reaching densities characteristic of solids.

  17. Adsorption of carbon monoxide on the Si(111)-7 × 7 surface

    Science.gov (United States)

    Shong, Bonggeun

    2017-05-01

    The adsorption of CO and surface chemistry of Si are well-understood topics in surface science. However, research into the adsorption of CO on the Si(111)-7 × 7 surface is deficient. In this study, the adsorption of CO on Si(111)-7 × 7 is investigated via high-level density functional theory calculations using cluster model. Two adsorption configurations are found to be kinetically and thermodynamically viable: on-top on rest-atoms and back-bond insertion on adatoms, both binding to the surface via C atom. Structural, electronic, and spectroscopic properties of the adsorbates indicate a σ-donating/π-accepting nature of the COsbnd Si bonds in both configurations. The domination of σ-donation in the on-top configuration results in a net positive charge on the on-top adsorbate, and the opposite situation yields a net negative charge on the back-bond insertion adsorbates. Our study provides a detailed understanding of the previous experimental observations of fundamental surface chemical phenomena, suggesting possible applications of Si surface functionalization using CO.

  18. Risedronate adsorption on bioactive glass surface for applications as bone biomaterial

    Energy Technology Data Exchange (ETDEWEB)

    Mosbahi, Siwar [University of Rennes 1, UMR CNRS 6226, Campus de Beaulieu, 35042 Rennes (France); Orthopaedic and Traumatology Laboratory, Sfax Faculty of Medicine, Sfax (Tunisia); Oudadesse, Hassane, E-mail: hassane.oudadesse@univ-rennes1.fr [University of Rennes 1, UMR CNRS 6226, Campus de Beaulieu, 35042 Rennes (France); Lefeuvre, Bertand [University of Rennes 1, UMR CNRS 6226, Campus de Beaulieu, 35042 Rennes (France); Barroug, Allal [University Cadi Ayyad, Faculty of Science Semlalia, Marrakech (Morocco); CNRST, Rabat (Morocco); Elfeki, Hafed [Science Materials and Environement Laboratory, Sfax Faculty of Science, Sfax (Tunisia); Elfeki, Abdelfattah [Animal Ecophysiology Laboratory, Sfax Faculty of Science, Department of Life Sciences, Sfax (Tunisia); Roiland, Claire [University of Rennes 1, UMR CNRS 6226, Campus de Beaulieu, 35042 Rennes (France); Keskes, Hassib [Orthopaedic and Traumatology Laboratory, Sfax Faculty of Medicine, Sfax (Tunisia)

    2016-03-30

    Highlights: • The fixation of risèdronates on the bioactive glass surface has been highlighted. • Scanning electron microscopy shows the new morphology of this composite. • Chemical analyses reveal the stability of adsorption process after 40 min of incubation. - Abstract: The aim of the current work is to study the physicochemical interactions between bisphosphonates molecules, risedronate (RIS) and bioactive glass (46S6) after their association by adsorption phenomenon. To more understand the interaction processes of RIS with the 46S6 surface we have used complementary physicochemical techniques such as infrared (FTIR), Raman and nuclear magnetic resonance (NMR) spectroscopy. The obtained results suggest that risedronate adsorption corresponds to an ion substitution reaction with silicon ions occurring at the bioactive glass surface. Thus, a pure bioactive glass was synthesized and fully characterized comparing the solids after adsorption (46S6-XRIS obtained after the interaction of 46S6 and X% risedronate). Therefore, based on the spectroscopic results FTIR, Raman and MAS-NMR, it can be concluded that strong interactions have been established between RIS ions and 46S6 surface. In fact, FTIR and Raman spectroscopy illustrate the fixation of risedronate on the bioactive glass surface by the appearance of several bands characterizing risedronate. The {sup 31}P MAS-NMR of the composite 46S6-XRIS show the presence of two species at a chemical shift of 15 and 19 ppm demonstrating thus the fixation of the RIS on 46S6 surface.

  19. Theoretical study of CCl(4) adsorption and hydrogenation on a Pt (111) surface.

    Science.gov (United States)

    Lu, Guiwu; Lan, Jianhui; Li, Chunxi; Wang, Wenchuan; Wang, Chunlei

    2006-12-07

    The adsorption and hydrogenation of carbon tetrachloride (CCl(4)) on a Pt (111) surface have been investigated using density functional theory (DFT). We have performed calculations on the adsorption energies and structures of CCl(4) on four different adsorption sites of a Pt (111) surface using the full adsorbate geometry optimization method. The results show that the adsorption energy of all of the potential sites is less than -17 kcal/mol, which indicates that CCl(4) is physiosorbed on a Pt (111) surface through van der Waals interactions. The dissociation and hydrogenation pathways were investigated by a transition state search. For the Pt(15), Pt(19), and Pt(25) cluster surfaces, the activation energies of dissociation obtained in this work are 15.69, 16.94, and 16.77 kcal/mol, respectively. The hydrogenation of CCl(3). was studied at the on-top site of the Pt(15) cluster, and the calculated activation energy is 5.06 kcal/mol. The small activation energies indicate that the Pt (111) surface has high catalytic activity for the CCl(4) hydrogenation reaction. In addition, the Hirshfeld population analysis reveals that the charge transfer from the Pt (111) surface to the adsorbates occurs in both the dissociation and hydrogenation pathways.

  20. The effect of oxygen molecule adsorption on lead iodide perovskite surface by first-principles calculation

    Science.gov (United States)

    Ma, Xia-Xia; Li, Ze-Sheng

    2018-01-01

    Oxygen molecule has a negative effect on perovskite solar cells, which has been investigated experimentally. However, detailed theoretical research is still rare. This study presents a microscopic view to reveal the interaction mechanism between O2 and perovskite based on the first-principles calculation. The results show that O2 is adsorbed on the (100) surface of MAPbI3 perovskite mainly by Van der Waals force. O2 adsorption makes the MAPbI3 surface generate a small number of positive charges, which leads to the increase of the work function of the MAPbI3 surface. This is in agreement with the experimental measurement. And increased work function of MAPbI3 surface is not beneficial to electron transfer from perovskite to electronic extraction layer (such as TiO2). Comparison of the density of states (DOS) of the clean (100) surface and the adsorbed system shows that an in-gap state belonging to O2 appears, which can explain the phenomenon observed from experiments that electron transfers from the surface of perovskite to O2 to form superoxide. The theoretical power conversion efficiency of the system with and without O2 adsorption is evaluated, and it turns out that the power conversion efficiency of the system with O2 adsorption is slightly lower than that of the system without O2 adsorption. This result indicates that avoiding the introduction of O2 molecules between perovskite and electronic extraction layer is beneficial to the perovskite solar cell.

  1. Selective adsorption of nano-bio materials and nanostructure fabrication on molecular resists modified by proton beam irradiation

    International Nuclear Information System (INIS)

    Lee, H. W.; Kim, S. K.; Cheon, J.; Kwon, K. J.; Kim, H. S.

    2006-05-01

    The purpose of this research is to use the substrate modified with the proton or ion beam irradiation to form nanostructures and to selectively adsorb bio-nano materials on the patterned substrate. Recently, the miniaturization of the integrated devices with fine functional structures was intensively investigated, based on combination of nanotechnology (NT), biotechnology (BT) and information technology (IT). The molecular thin films such as a self-assembled monolayer or a polymer resist layer have been used as an alternative to modifying the surface property. Although proton or ion beam irradiation has been used as an efficient tool to modify the physical, chemical and electrical properties of a surface, the nano-patterning on the substrate or the molecular film modified with the beam irradiation has hardly been studied at both home and abroad. The selective adsorption of nano-bio materials such as carbon nanotubes and proteins on the patterns would contribute to developing the integrated devices

  2. Adsorption of branched and dendritic polymers onto flat surfaces: A Monte Carlo study

    Science.gov (United States)

    Sommer, J.-U.; Kłos, J. S.; Mironova, O. N.

    2013-12-01

    Using Monte Carlo simulations based on the bond fluctuation model we study the adsorption of starburst dendrimers with flexible spacers onto a flat surface. The calculations are performed for various generation number G and spacer length S in a wide range of the reduced temperature τ as the measure of the interaction strength between the monomers and the surface. Our simulations indicate a two-step adsorption scenario. Below the critical point of adsorption, τc, a weakly adsorbed state of the dendrimer is found. Here, the dendrimer retains its shape but sticks to the surface by adsorbed spacers. By lowering the temperature below a spacer-length dependent value, τ*(S) model of a dendrimer in two dimensions. We also performed simulations of star-polymers which display a simple crossover-behavior in full analogy to linear chains. By analyzing the order parameter of the adsorption transition, we determine the critical point of adsorption of the dendrimers which is located close to the critical point of adsorption for star-polymers. While the order parameter for the adsorbed spacers displays a critical crossover scaling, the overall order parameter, which combines both critical and discontinuous transition effects, does not display simple scaling. The step-like transition from the weak into the strong adsorbed regime is confirmed by analyzing the shape-anisotropy of the dendrimers. We present a mean-field model based on the concept of spacer adsorption which predicts a discontinuous transition of dendrimers due to an excluded volume barrier. The latter results from an increased density of the dendrimer in the flatly adsorbed state which has to be overcome before this state is thermodynamically stable.

  3. Adsorption of ibuprofen from aqueous solution on chemically surface-modified activated carbon cloths

    Directory of Open Access Journals (Sweden)

    Hanen Guedidi

    2017-05-01

    Full Text Available This study aims to investigate the performance of an activated carbon cloth for adsorption of ibuprofen. The cloth was oxidized by a NaOCl solution (0.13 mol L−1 or thermally treated under N2 (700 °C for 1 hour. The raw and modified cloths were characterized by N2 adsorption–desorption measurement at 77 K, CO2 adsorption at 273 K, Boehm titrations, pHPZC measurements, X-ray Photoelectron Spectroscopy analysis, and by infrared spectroscopy. The NaOCl treatment increases the acidic sites, mostly creating phenolic and carboxylic groups and decreases both the specific surface area and slightly the micropore volume. However, the thermal treatment at 700 °C under N2 induced a slight increase in the BET specific surface area and yielded to the only increase in the carbonyl group content. Ibuprofen adsorption studies of kinetics and isotherms were carried out at pH = 3 and 7. The adsorption properties were correlated to the cloth porous textures, surface chemistry and pH conditions. The isotherms of adsorption were better reproduced by Langmuir–Freundlich models at 298, 313 and 328 K. The adsorption of ibuprofen on the studied activated carbon cloths at pH 3 was an endothermic process. The pore size distributions of all studied ibuprofen-loaded fabrics were determined by DFT method to investigate the accessible porosity of the adsorbate. Both treatments do not influence the kind of micropores where the adsorption of ibuprofen occurred.

  4. An Analytical Model for Adsorption and Diffusion of Atoms/Ions on Graphene Surface

    Directory of Open Access Journals (Sweden)

    Yan-Zi Yu

    2015-01-01

    Full Text Available Theoretical investigations are made on adsorption and diffusion of atoms/ions on graphene surface based on an analytical continuous model. An atom/ion interacts with every carbon atom of graphene through a pairwise potential which can be approximated by the Lennard-Jones (L-J potential. Using the Fourier expansion of the interaction potential, the total interaction energy between the adsorption atom/ion and a monolayer graphene is derived. The energy-distance relationships in the normal and lateral directions for varied atoms/ions, including gold atom (Au, platinum atom (Pt, manganese ion (Mn2+, sodium ion (Na1+, and lithium-ion (Li1+, on monolayer graphene surface are analyzed. The equilibrium position and binding energy of the atoms/ions at three particular adsorption sites (hollow, bridge, and top are calculated, and the adsorption stability is discussed. The results show that H-site is the most stable adsorption site, which is in agreement with the results of other literatures. What is more, the periodic interaction energy and interaction forces of lithium-ion diffusing along specific paths on graphene surface are also obtained and analyzed. The minimum energy barrier for diffusion is calculated. The possible applications of present study include drug delivery system (DDS, atomic scale friction, rechargeable lithium-ion graphene battery, and energy storage in carbon materials.

  5. Insights of adsorption mechanisms of Trp-peptides on plasmonic surfaces by SERS

    Science.gov (United States)

    daFonseca, Bruno Guilherme; Costa, Luiz Antônio Sodré; Sant'Ana, Antonio Carlos

    2018-02-01

    The adsorptions of tryptophan (Trp) on silver or gold surfaces were investigated by surface-enhanced Raman scattering (SERS) measurements. In addition, peptides with Trp in different chain positions were studied and the adsorption sites were determined based on marker bands. The indole ring was the main group responsible for the interactions with gold nanoparticles (AuNPs). In the presence of HCl, the SERS spectra suggested that the anchoring of such peptides on AuNPs was reinforced by ionic pair interactions between protonated amine and chloride ions. The adsorptions of Trp and its derivatives on silver nanoparticles (AgNPs) show some variability in the spectral patterns, even though the enhanced carboxilate and amino features were ever ascribed as preferable adsorption site. Based on DFT calculations the vibrational assignment allows the reinterpretation of previous published works. The investigations showed that both the high affinity of indole moiety for the AuNP surfaces make these substrates adequate for studying the adsorption of peptides containing Trp and the proposed SERS assignments could be helpful for further studies of more complex structures.

  6. Additive surface complexation modeling of uranium(VI) adsorption onto quartz-sand dominated sediments.

    Science.gov (United States)

    Dong, Wenming; Wan, Jiamin

    2014-06-17

    Many aquifers contaminated by U(VI)-containing acidic plumes are composed predominantly of quartz-sand sediments. The F-Area of the Savannah River Site (SRS) in South Carolina (USA) is an example. To predict U(VI) mobility and natural attenuation, we conducted U(VI) adsorption experiments using the F-Area plume sediments and reference quartz, goethite, and kaolinite. The sediments are composed of ∼96% quartz-sand and 3-4% fine fractions of kaolinite and goethite. We developed a new humic acid adsorption method for determining the relative surface area abundances of goethite and kaolinite in the fine fractions. This method is expected to be applicable to many other binary mineral pairs, and allows successful application of the component additivity (CA) approach based surface complexation modeling (SCM) at the SRS F-Area and other similar aquifers. Our experimental results indicate that quartz has stronger U(VI) adsorption ability per unit surface area than goethite and kaolinite at pH ≤ 4.0. Our modeling results indicate that the binary (goethite/kaolinite) CA-SCM under-predicts U(VI) adsorption to the quartz-sand dominated sediments at pH ≤ 4.0. The new ternary (quartz/goethite/kaolinite) CA-SCM provides excellent predictions. The contributions of quartz-sand, kaolinite, and goethite to U(VI) adsorption and the potential influences of dissolved Al, Si, and Fe are also discussed.

  7. Effects of surface water on the adsorption of inert gases

    International Nuclear Information System (INIS)

    Gammage, R.B.; Holmes, H.F.

    1976-01-01

    Molecular water on mildly outgassed open oxide surfaces can, under special circumstances, significantly reduce the monolayer capacity for inert gas molecules. Non-porous thoria and cubic europia are two examples. The special proviso is that the surface be sufficiently uniform to permit the formation of a well structured, ice-like surface with non-polar character. This type of behavior reaches an extreme for a non-porous ground calcite; surface water converts a Type II isotherm for krypton into a Type III. These structured layers of adsorbed water adsorb nitrogen in a manner very similar to that found for various types of ice. For open oxide surface in a more thoroughly outgassed condition, the BET specific surface area does not generally vary with outgassing temperature at and above 150 0 C. The area occupied by an inert gas molecule does not change, therefore, with varying hydroxyl ion content of the surface

  8. Surface resistivity measurement of plasma treated polymers

    International Nuclear Information System (INIS)

    Simon, D.; Pigram, P.J.; Liesegang, J.

    2000-01-01

    Full text: Resistivity of insulators is an important property of materials used within the integrated circuit and packaging industries. The measurement of electrical resistivity of insulator materials in the surface region in this work is interpreted through observations of surface charge decay. A self-field driven and diffusion charge transport theory is used to model the process and resistivity values obtained computationally. Data for the charge decay of surface charged samples are collected by suspending them inside a coaxial cylinder connected to an electrometer. Samples used have been low density polyethylene LDPE sheet, both pristine and surface treated. Some samples have been treated by air plasma at low vacuum pressures for different periods of time; others have been washed in ethyl acetate and then plasma treated before the resistivity measurement. The sets of resistivity measurements form the various treatments are compared below. X-ray photoelectron spectroscopy (XPS) has also been used to investigate and account for the observed variations in surface resistivity

  9. Adsorption of nitrogen on potassium promoted Fe(111) and (100) surfaces

    Science.gov (United States)

    Ertl, G.; Lee, S. B.; Weiss, M.

    1982-02-01

    Dissociative nitrogen adsorption through N2 ⇌ N2, ad → 2 Ns is the rate limiting step in ammonia synthesis over iron catalysts. This model study deals with the "promoter" action of potassium by studying the influence of preadsorbed K on the energetics and kinetics of molecular and atomic nitrogen adsorption on Fe(111) and Fe(100). The heat of adsorption of molecular nitrogen is locally increased to about 11 kcal/mole in the vicinity of an adsorbed K atom, which phenomenon simultaneously lowers the activation barrier for dissociation. As a consequence the effective sticking coefficient for dissociative nitrogen adsorption is markedly increased. This effect is less pronounced for Fe(111) than for Fe(100) so that the difference in activity observed with the K-free surfaces is eliminated. The increase of the N 2 adsorption energy is attributed to the enhanced electron density of the substrate (due to charge transfer from K) which enables a more pronounced "backbonding" contribution to the adsorption bond.

  10. Photoexcitation effect on the adsorption of hazardous gases on silica surface.

    Science.gov (United States)

    Yang, Yonggang; Li, Donglin; Li, Chaozheng; Liu, Yufang; Jiang, Kai

    2018-01-05

    There is very little scientific understanding of photoexcitation effect on the adsorption properties of adsorbent. The adsorption of four hazardous gases (SARIN (propan-2-ylmethylphospho-nofluoridate), methyl dichlorophosphate (MDCP), trimethyl phosphate (TMP) and hydrogen sulfide (H 2 S)) on silica surface is taken as target sample in this work. The adsorption energy order (MDCPhazardous gas, and the desorption order of the three gases in previous reports. However, with the adsorption energy increase of MDCP and the decrease of SARIN and TMP, this order changes remarkably to SARINadsorption properties of adsorbent for its striking effect on adsorption behaviors. Copyright © 2017. Published by Elsevier B.V.

  11. Surface modification influencing adsorption of red wine constituents: The role of functional groups

    Science.gov (United States)

    Mierczynska-Vasilev, Agnieszka; Smith, Paul A.

    2016-11-01

    The adsorption of wine constituents at solid surfaces is important in applications such as filtration and membrane fouling, binding to tanks and fittings and interactions with processing aids such as bentonite. The interaction of wine constituents with surfaces is mediated through adsorbed wine components, where the type of constituents, amount, orientation, and conformation are of consequence for the surface response. This study examines the effect of surface chemical functionalities on the adsorption of red wine constituents. Plasma-polymerized films rich in amine, carboxyl, hydroxyl, formyl and methyl functional groups were generated on solid substrates whereas, glycidyltrimethylammonium chloride was covalently attached to allylamine plasma-polymer modified surface and poly(sodium styrenesulfonate) was electrostatically adsorbed to an amine plasma-polymerized surface. The surface chemical functionalities were characterized by X-ray photoelectron spectroscopy. The ability of different substrates to adsorb red wine constituents was evaluated by quartz crystal microbalance and atomic force microscopy. The results showed that substrates modified with -SO3H and -COOH groups can adsorb more of the wine nitrogen-containing compounds whereas -NH2 and -NR3 groups encourage carbon-containing compounds adsorption. Red wine constituents after filtration were adsorbed in higher extend on -NR3 and -CHO surfaces. The -OH modified surfaces had the lowest ability to absorb wine components.

  12. Adsorption Study of a Water Molecule on Vacancy-Defected Nonpolar CdS Surfaces

    Science.gov (United States)

    2017-01-01

    A detailed understanding of the water–semiconductor interface is of major importance for elucidating the molecular interactions at the photocatalyst’s surface. Here, we studied the effect of vacancy defects on the adsorption of a water molecule on the (101̅0) and (112̅0) CdS surfaces, using spin-polarized density functional theory. We observed that the local spin polarization did not persist for most of the cationic vacancies on the surfaces, unlike in bulk, owing to surface reconstructions caused by displaced S atoms. This result suggests that cationic vacancies on these surfaces may not be the leading cause of the experimentally observed magnetism in CdS nanostructures. The surface vacancies are predominantly nonmagnetic except for one case, where a magnetic cationic vacancy is relatively stable due to constraints posed by the (101̅0) surface geometry. At this particular magnetic defect site, we found a very strong interaction with the H2O molecule leading to a case of chemisorption, where the local spin polarization vanishes concurrently. At the same defect site, adsorption of an O2 molecule was also simulated, and the results were found to be consistent with experimental electron paramagnetic resonance findings for powdered CdS. The anion vacancies on these surfaces were always found to be nonmagnetic and did not affect the water adsorption at these surfaces. PMID:28539988

  13. Incorporating classic adsorption isotherms into modern surface complexation models: implications for sorption of radionuclides

    International Nuclear Information System (INIS)

    Kulik, D.A.

    2005-01-01

    Full text of publication follows: Computer-aided surface complexation models (SCM) tend to replace the classic adsorption isotherm (AI) analysis in describing mineral-water interface reactions such as radionuclide sorption onto (hydr) oxides and clays. Any site-binding SCM based on the mole balance of surface sites, in fact, reproduces the (competitive) Langmuir isotherm, optionally amended with electrostatic Coulomb's non-ideal term. In most SCM implementations, it is difficult to incorporate real-surface phenomena (site heterogeneity, lateral interactions, surface condensation) described in classic AI approaches other than Langmuir's. Thermodynamic relations between SCMs and AIs that remained obscure in the past have been recently clarified using new definitions of standard and reference states of surface species [1,2]. On this basis, a method for separating the Langmuir AI into ideal (linear) and non-ideal parts [2] was applied to multi-dentate Langmuir, Frumkin, and BET isotherms. The aim of this work was to obtain the surface activity coefficient terms that make the SCM site mole balance constraints obsolete and, in this way, extend thermodynamic SCMs to cover sorption phenomena described by the respective AIs. The multi-dentate Langmuir term accounts for the site saturation with n-dentate surface species, as illustrated on modeling bi-dentate U VI complexes on goethite or SiO 2 surfaces. The Frumkin term corrects for the lateral interactions of the mono-dentate surface species; in particular, it has the same form as the Coulombic term of the constant-capacitance EDL combined with the Langmuir term. The BET term (three parameters) accounts for more than a monolayer adsorption up to the surface condensation; it can potentially describe the surface precipitation of nickel and other cations on hydroxides and clay minerals. All three non-ideal terms (in GEM SCMs implementation [1,2]) by now are used for non-competing surface species only. Upon 'surface dilution

  14. CO2 adsorption on the copper surfaces: van der Waals density functional and TPD studies

    Science.gov (United States)

    Muttaqien, Fahdzi; Hamamoto, Yuji; Hamada, Ikutaro; Inagaki, Kouji; Shiozawa, Yuichiro; Mukai, Kozo; Koitaya, Takanori; Yoshimoto, Shinya; Yoshinobu, Jun; Morikawa, Yoshitada

    2017-09-01

    We investigated the adsorption of CO2 on the flat, stepped, and kinked copper surfaces from density functional theory calculations as well as the temperature programmed desorption and X-ray photoelectron spectroscopy. Several exchange-correlation functionals have been considered to characterize CO2 adsorption on the copper surfaces. We used the van der Waals density functionals (vdW-DFs), i.e., the original vdW-DF (vdW-DF1), optB86b-vdW, and rev-vdW-DF2, as well as the Perdew-Burke-Ernzerhof (PBE) with dispersion correction (PBE-D2). We have found that vdW-DF1 and rev-vdW-DF2 functionals slightly underestimate the adsorption energy, while PBE-D2 and optB86b-vdW functionals give better agreement with the experimental estimation for CO2 on Cu(111). The calculated CO2 adsorption energies on the flat, stepped, and kinked Cu surfaces are 20-27 kJ/mol, which are compatible with the general notion of physisorbed species on solid surfaces. Our results provide a useful insight into appropriate vdW functionals for further investigation of related CO2 activation on Cu surfaces such as methanol synthesis and higher alcohol production.

  15. A study of double stranded DNA adsorption on aluminum surface by means of electrochemical impedance spectroscopy.

    Science.gov (United States)

    Heli, H

    2014-04-01

    Immobilization of DNA on the solid surfaces is one of the goals in bio- and nano-technologies. Adsorption of double stranded DNA on the surface of aluminum was electrochemically studied by means of impedance spectroscopy. Nyquist diagram of aluminum in a tris (hydroxymethyl) ammoniummethane-HCl (Tris-HCl) buffer solution, pH 7.4 consisted of two overlapped capacitive semicircles. The high-frequency semicircle was related to the passivity of Cl(-)-containing aluminum species in the oxide layer, and low-frequency semicircle was attributed to metal dissolution. When DNA was added to the Tris-HCl buffer solution, Nyquist diagrams represented an inductive loop at low frequencies due to the adsorption of DNA on the pre-covered aluminum surface by hydroxy-contained species. The DNA adsorption on the aluminum surface was also confirmed by X-ray photoelectron spectroscopy. Open circuit potential variation with time also indicated the chemical adsorption of DNA on the aluminum surface. Copyright © 2014 Elsevier B.V. All rights reserved.

  16. DNA Adsorption to and Elution from Silica Surfaces: Influence of Amino Acid Buffers

    Science.gov (United States)

    Vandeventer, Peter E.; Mejia, Jorge; Nadim, Ali; Johal, Malkiat S.; Niemz, Angelika

    2014-01-01

    Solid phase extraction and purification of DNA from complex samples typically requires chaotropic salts that can inhibit downstream polymerase amplification if carried into the elution buffer. Amino acid buffers may serve as a more compatible alternative for modulating the interaction between DNA and silica surfaces. We characterized DNA binding to silica surfaces, facilitated by representative amino acid buffers, and the subsequent elution of DNA from the silica surfaces. Through bulk depletion experiments, we found that more DNA adsorbs to silica particles out of positively compared to negatively charged amino acid buffers. Additionally, the type of the silica surface greatly influences the amount of DNA adsorbed, and the final elution yield. Quartz crystal microbalance experiments with dissipation monitoring (QCM-D) revealed multiphasic DNA adsorption out of stronger adsorbing conditions such as arginine, glycine, and glutamine, with DNA more rigidly bound during the early stages of the adsorption process. The DNA film adsorbed out of glutamate was more flexible and uniform throughout the adsorption process. QCM-D characterization of DNA elution from the silica surface indicates an uptake in water mass during the initial stage of DNA elution for the stronger adsorbing conditions, which suggests that for these conditions the DNA film is partly dehydrated during the prior adsorption process. Overall, several positively charged and polar neutral amino acid buffers show promise as an alternative to methods based on chaotropic salts for solid phase DNA extraction. PMID:23931415

  17. Thermogravimetric determination of the enthalpy of astatine and radon adsorption on palladium surfaces

    International Nuclear Information System (INIS)

    Eichler, B.; Son Chun, K.

    1985-01-01

    In order to investigate the adsorption of astatine and radon on a palladium surface some on- and off-line thermochromatographic experiments were carried out with 210 At and 220 Rn tracers. The partial molar adsorption enthalpy for zero covering was found to be ΔH/sub a//sup 0, loc./(At) = -(15S +- 10) kJ mole -1 and ΔH/sub a//sup 0, mob./(Rn) = -(37 +- 4) kJ mole -1 . The results are compared with theoretical and experimental values for other elements of the sixth period. The adsorption behaviour of At is in conformity with that of the p-metals on a palladium surface. (author)

  18. "Kinetics of the adsorption of atomic oxygen (N2O) on the Si(001)2x1 surface as revealed by the change in the surface conductance"

    NARCIS (Netherlands)

    Wormeester, Herbert; Keim, Enrico G.; van Silfhout, Arend

    1992-01-01

    The adsorption behaviour of N2O on the Si(001)2 × 1 surface at 300 K substrate temperature has been investigated by measuring in situ the surface conductance during the reaction process. For comparison we monitored in the same way the adsorption of O2 on the same surface which ultimately leads to

  19. Adsorption of Polyanion onto Large Alpha Alumina Beads with Variably Charged Surface

    Directory of Open Access Journals (Sweden)

    Tien Duc Pham

    2014-01-01

    Full Text Available Adsorption of strong polyelectrolyte, poly(styrenesulfonate, PSS, of different molecular weights onto large α-Al2O3 beads was systematically investigated as functions of pH and NaCl concentrations. The ultraviolet (UV absorption spectra of PSS at different pH and salt concentrations confirmed that the structure of PSS is independent of pH. With the change of molecular weight from 70 kg/mol (PSS 70 to 1000 kg/mol (PSS 1000, adsorption amount of PSS increases and proton coadsorption on the surface of α-Al2O3 decreases at given pH and salt concentration. It suggests that higher molecular weight of PSS was less flat conformation than lower one. The adsorption density of PSS 70 and PSS 1000 decreases with decreasing salt concentrations, indicating that both electrostatic and nonelectrostatic interactions are involved. Experimental results of both PSS 70 and PSS 1000 adsorption isotherms onto α-Al2O3 at different pH and salt concentrations can be represented well by two-step adsorption model. The effects of molecular weight and salt concentration are explained by structure of adsorbed PSS onto α-Al2O3. The influence of added SDS on the isotherms is evaluated from the sequential adsorption. The SDS uptake onto α-Al2O3 in the presence of hemimicelles can prevent the adsorption of PSS at low concentration so that adsorption of PSS reduces with preadsorbed SDS.

  20. Surface modification of poly (styrene-b-(ethylene-co-butylene)-b-styrene) elastomer and its plasma protein adsorption by QCM-D

    Science.gov (United States)

    Li, Rui; Jin, Jing; Sun, Yingchun

    2014-05-01

    Protein adsorption is a dynamic process and plays a major role in determining the hemocompatibility of biomaterials. We have obtained different poly (ethylene glycol) (PEG) graft concentrations of SEBS-g-PEG and the surface chemical compositions are confirmed by X-ray photoelectron spectroscopy (XPS). Graft concentration is defined by peak-area ratio of [C--O]/[C] on modified SEBS surface. With increasing graft concentration, water contact angles of the modified SEBS have significantly decreased. The platelet adhesion and static protein adsorption demonstrate that the hemocompatibility of copolymers films are improved effectively and SEBS-g-PEG-2 with larger graft concentration has more superior anticoagulation than that of SEBS-g-PEG-1. Moreover, we have quantitatively investigated the adsorption process of bovine serum albumin (BSA) and fibrinogen (Fib) on the surfaces of pristine SEBS and modified SEBS using quartz crystal microbalance with dissipation (QCM-D) in real time. The results indicate that the inactivated BSA on the pristine SEBS can continuously induce the subsequent Fib adsorption. The hemocompatibility of SEBS-g-PEG-2 with the graft concentration of 0.207 has excellent anti-protein property and the bio-inert BSA layer on the film can resist the subsequent Fib adsorption.

  1. Methane adsorption on the surface of a model of shale: A density functional theory study

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, Yuan-qiang, E-mail: zhuline518@163.com [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500 (China); Su, Hong; Jing, Ya [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Guo, Jianchun [State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500 (China); Tang, Junlei [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China)

    2016-11-30

    Highlights: • The adsorption of methane on kerogen was investigated by DFT method with D3 dispersion correction. • Methane prefers to be adsorbed on the sites directly above the carbon atoms of the kerogen. • The interaction energy with BSSE corrections is around 14 kJ mol{sup −1}. • RDG gradient isosurface depicted the van der Waals interactions between methane and kerogen. • The adsorption of methane on kerogen slightly depends upon the adsorption sites on kerogen as well as the orientations of methane. - Abstract: As a model of shale, one part of polycyclic aromatic ring was used to represent the kerogen surface with the structural heterogeneity. The adsorption mechanisms of methane on the surface of the kerogen were investigated by M06-2× functional with D3 dispersion correction. Nine stable adsorption sites and the orientations of methane (CH{sub 4}) on the surface of the kerogen were systematically considered. Information from different methods lead to the same conclusion that methane prefers to be adsorbed on the sites directly above the carbon atoms of the kerogen rather than above the center of the six-membered rings. The interactions between methane and the surface of the kerogen are the van der Waals interactions. The interaction energies with the basis set superposition error (BSSE) corrections are around 14 kJ mol{sup −1} at the M06-2×-D3/Jun-cc-pVDZ level. The RDG scatter graphs and the RDG gradient isosurface further illustrate that the interactions between methane and the surface of the kerogen belong to the van der Waals interactions. The weak interactions indicate that the adsorption of methane on the surface of the kerogen is physical adsorption and it slightly depends upon the adsorption sites on kerogen as well as the orientations of methane. These results are helpful for the understanding of the microcosmic mechanism of methane–shale interactions and for the exploitation of shale gas.

  2. Adsorption mechanism of ribosomal protein L2 onto a silica surface: a molecular dynamics simulation study.

    Science.gov (United States)

    Tosaka, Ryo; Yamamoto, Hideaki; Ohdomari, Iwao; Watanabe, Takanobu

    2010-06-15

    A large-scale molecular dynamics simulation was carried out in order to investigate the adsorption mechanism of ribosomal protein L2 (RPL2) onto a silica surface at various pH values. RPL2 is a constituent protein of the 50S large ribosomal subunit, and a recent experimental report showed that it adsorbs strongly to silica surfaces and that it can be used to immobilize proteins on silica surfaces. The simulation results show that RPL2, especially domains 1 (residues 1-60) and 3 (residues 203-273), adsorbed more tightly to the silica surface above pH 7. We found that a major driving force for the adsorption of RPL2 onto the silica surface is the electrostatic interaction and that the structural flexibility of domains 1 and 3 may further contribute to the high affinity.

  3. The impact of the competitive adsorption of ions at surface sites on surface free energies and surface forces

    Science.gov (United States)

    Parsons, Drew F.; Salis, Andrea

    2015-04-01

    The relationship between surface charge and surface potential at the solid-liquid interface is often determined by a charge regulation process, the chemisorption of a potential determining ion such as H+. A subtle ion-specific effect can be observed when other ions compete with the primary potential determining ion to bind to a surface site. Site competition may involve alternative ions competing for a first binding site, e.g., metals ions competing with H+ to bind to a negatively charged oxide or carboxyl site. Second-binding sites with site competition may also be found, including amphoteric OH2+ sites, or anion binding to amine groups. In this work, a general theoretical model is developed to describe the competitive adsorption of ions at surface sites. Applied to the calculation of forces, the theory predicts a 20% increase in repulsion between titania surfaces in 1 mM NaCl, and a 25% reduction in repulsion between silica surfaces in 0.1M NaCl compared to calculations neglecting ion site competition.

  4. Surface study of gallium- and aluminum- doped graphenes upon adsorption of cytosine: DFT calculations

    Energy Technology Data Exchange (ETDEWEB)

    Shokuhi Rad, Ali, E-mail: a.shokuhi@gmail.com [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Zareyee, Daryoush [Department of Chemistry, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Peyravi, Majid; Jahanshahi, Mohsen [Faculty of Chemical Engineering, Babol University of Technology, Babol (Iran, Islamic Republic of)

    2016-12-30

    Highlights: • P1 and P4 are the most stable adsorption configurations for cytosine. • NBO analysis show n-type semiconductor property for both Al- and Ga-doped graphenes. • Important changes in the HOMO and LUMO of doped graphene upon adsorption of cytosine. • Increase in the conductivity of system when cytosine is adsorbed on doped graphenes. - Abstract: The adsorption of cytosine molecule on Al- and Ga- doped graphenes is studied using first-principles density functional theory (DFT) calculations. The energetically most stable geometries of cytosine on both Al- and Ga- doped graphenes are determined and the adsorption energies are calculated. The net charge of transfer as well as local charge of doped atoms upon adsorption of cytosine are studied by natural bond orbitals (NBO) analysis. Orbital hybridizing of complexes was searched by frontier molecular orbital theory (FMO), and density of states (DOS). Depending on the side of cytosine, there are four possible sites for its adsorption on doped graphene; denoted as P1, P2, P3, and P4, respectively. The order of binding energy in the case of Al-doped graphene is found as P1 > P4 > P3 > P2. Interestingly, the order in the case of Ga-doped graphene changes to: P4 ∼ P1 > P3 > P2. Both surfaces show superior adsorbent property, resulting chemisorption of cytosine, especially at P1 and P4 position configurations. The NBO charge analysis reveals that the charge transfers from Al- and Ga- doped graphene sheets to cytosine. The electronic properties of both surfaces undertake important changes after cytosine adsorption, which indicates notable change in its electrical conductivity.

  5. Surface study of gallium- and aluminum- doped graphenes upon adsorption of cytosine: DFT calculations

    International Nuclear Information System (INIS)

    Shokuhi Rad, Ali; Zareyee, Daryoush; Peyravi, Majid; Jahanshahi, Mohsen

    2016-01-01

    Highlights: • P1 and P4 are the most stable adsorption configurations for cytosine. • NBO analysis show n-type semiconductor property for both Al- and Ga-doped graphenes. • Important changes in the HOMO and LUMO of doped graphene upon adsorption of cytosine. • Increase in the conductivity of system when cytosine is adsorbed on doped graphenes. - Abstract: The adsorption of cytosine molecule on Al- and Ga- doped graphenes is studied using first-principles density functional theory (DFT) calculations. The energetically most stable geometries of cytosine on both Al- and Ga- doped graphenes are determined and the adsorption energies are calculated. The net charge of transfer as well as local charge of doped atoms upon adsorption of cytosine are studied by natural bond orbitals (NBO) analysis. Orbital hybridizing of complexes was searched by frontier molecular orbital theory (FMO), and density of states (DOS). Depending on the side of cytosine, there are four possible sites for its adsorption on doped graphene; denoted as P1, P2, P3, and P4, respectively. The order of binding energy in the case of Al-doped graphene is found as P1 > P4 > P3 > P2. Interestingly, the order in the case of Ga-doped graphene changes to: P4 ∼ P1 > P3 > P2. Both surfaces show superior adsorbent property, resulting chemisorption of cytosine, especially at P1 and P4 position configurations. The NBO charge analysis reveals that the charge transfers from Al- and Ga- doped graphene sheets to cytosine. The electronic properties of both surfaces undertake important changes after cytosine adsorption, which indicates notable change in its electrical conductivity.

  6. Bacterial resistance control on mineral surfaces of hydroxyapatite and human teeth via surface charge-driven antifouling coatings.

    Science.gov (United States)

    Venault, Antoine; Yang, Hui-Shan; Chiang, Yen-Che; Lee, Bor-Shuinn; Ruaan, Ruoh-Chyu; Chang, Yung

    2014-03-12

    This works reports a set of new functionalized polyethyleneimine (PEI) polymers, including a neutral PEGylated polymer PEI-g-PEGMA, a negatively charged polymer PEI-g-SA, and a zwitterionic polymer PEI-g-SBMA, and their use as antibiofouling coating agent for human teeth protection. Polymers were synthesized by Michael addition, XPS analysis revealed that each polymer could be efficiently coated onto hydroxyapatite, ceramic material used as a model tooth. Polymers carrying a negative net charge were more efficiently adsorbed, because of the establishment of electrostatic interactions with calcium ions. Protein adsorption tests revealed that two factors were important in the reduction of protein adsorption. Both the surface charge and the surface ability to bind and entrap water molecules had to be considered. PEI-g-SBMA, which zeta potential in PBS solution was negative, was efficient to inhibit the adsorption of BSA, a negative protein. On the other hand, it also resisted the adsorption of lysozyme, a positive protein, because zwitterionic molecules can easily entrap water and provide a very hydrophilic environment. Streptococcus mutans attachment tests performed unveiled that all modified polymers were efficient to resist this type of bacteria responsible for dental carries. Best results were also obtained with PEI-g-SBMA coating. This polymer was also shown to efficiently resist the adsorption of positively charged bacteria (Stenotrophomonas maltophilia). Tests performed on real human tooth showed that PEI-g-SBMA could inhibit up to 70% of bacteria adhesion, which constitutes a major result considering that surface of teeth is very rough, therefore physically promoting the attachment of proteins and bacteria.

  7. Adsorptive removal of residual catalyst from palm biodiesel: Application of response surface methodology

    Directory of Open Access Journals (Sweden)

    Mjalli Sabri Farouq

    2012-01-01

    Full Text Available In this work, the residual potassium hydroxide catalyst was removed from palm oil-based methyl esters using an adsorption technique. The produced biodiesel was initially purified through a water washing process. To produce a biodiesel with a better quality and also to meet standard specifications (EN 14214 and ASTM D6751, batch adsorption on palm shell activated carbon was used for further catalyst removal. The Central Composite Design (CCD of the Response Surface Methodology (RSM was used to study the influence of adsorbent amount, time and temperature on the adsorption of potassium species. The maximum catalyst removal was achieved at 40°C using 0.9 g activated carbon for 20 h adsorption time. The results from the Response Surface Methodology are in a good agreement with the measured values. The absolute error in prediction at the optimum condition was 3.7%, which is reasonably accurate. This study proves that adsorption post-treatment techniques can be successfully employed to improve the quality of biodiesel fuel for its effective use on diesel engines and to minimize the usage of water.

  8. Adsorption of ethanol on V2O5 (010) surface for gas-sensing applications: Ab initio investigation

    International Nuclear Information System (INIS)

    Qin, Yuxiang; Cui, Mengyang; Ye, Zhenhua

    2016-01-01

    Highlights: • Ethanol adsorbed on V 2 O 5 (010) surface was investigated by ab initio calculations. • Ethanol prefers to adsorb on “Hill”-like surface, rather than“Valley”-like region. • Surface O 1(H) site plays a key role to dominate the ethanol adsorption process. • Sensing mechanism is related with electronic structure and electron redistribution. • Gas sensitivity is reflected by quantitative electron population analysis. - Abstract: The adsorption of ethanol on V 2 O 5 (010) surface was investigated by means of density functional theory (DFT) with a combined generalized gradient approximation (GGA) plus Hubbard U approach to exploit the potential sensing applications. The adsorption configurations were first constructed by considering different orientations of ethanol molecule to V and O sites on the “Hill”- and “Valley”-like regions of corrugated (010) surface. It is found that ethanol molecule can adsorb on whole surface in multiple stable configurations. Nevertheless the molecular adsorption on the “Hill”-like surface is calculated to occur preferentially, and the single coordinated oxygen on “Hill”-like surface (O 1(H) ) acting as the most energetically favorable adsorption site shows the strongest adsorption ability to ethanol molecule. Surface adsorption of ethanol tunes the electronic structure of V 2 O 5 and cause an n-doping effect. As a consequence, the Fermi levels shift toward the conductive bond increasing the charge carrier concentration of electrons in adsorbed V 2 O 5 . The sensitive electronic structure and the multiple stable configurations to ethanol adsorption highlight the high adsorption activity and then the potential of V 2 O 5 (010) surface applied to high sensitive sensor for ethanol vapor detection. Further Mulliken population and Natural bond orbital (NBO) calculations quantify the electron transfer from the adsorbed ethanol to the surface, and correlates the adsorption ability of surface sites

  9. Adsorption of Different Fractions of Organic Matter on the Surface of Metal Oxide

    KAUST Repository

    Zaouri, Noor A

    2013-05-18

    The adsorption of different fractions of organic matter on the surface of Al2O3 and ZrO2 were investigated. The aim was to study the affinity of these fractions on the surface of metal oxide and the effect of several factors. Batch adsorption experiments were conducted with Low molecular weight oxygenated compounds. These chemical compound have been chosen to investigate:1) the aliphatic and aromatic structurer;2)contribution of hydroxyl group and; 3) the number of carboxyl group. HPLC and IC analysis used for determent the concentration of these chemical in the working solution. ATR-FTIR used to distinguish the type of coordination structure with the surface of metal oxide. The results fitted with Langmuir equation. The results showed that the chemical structure and the type and number of attached functional have an impact on the adsorption. Which it was proved via ATR-FTIR where the result showed that each chemical have different coordination structure on the surface of ZrO2 and Al2O3. Different fractions and sources of NOM were used (hydrophobic fraction of Suwannee and Colorado River, biopolymers extracted for the exuded of 2 species of algae, and low molecular acids that do not adsorb in XAD-8 resin). Results showed that these different fractions have different affinity with the surface of Al2O3 and ZrO2. These adsorption behaviors were varying according to the difference in the component of each NOM. Biopolymers showed significant adsorption at acidic pH. These biopolymers are mainly comprised of polysaccharides and this result proved that polysaccharide adsorb on the surface of ZrO2 more than Al2O3.

  10. Adsorption of nonionic surfactants on cellulose surfaces : adsorbed amounts and kinetics

    NARCIS (Netherlands)

    Torn, L.H.; Koopal, L.K.; Keizer, de A.; Lyklema, J.

    2005-01-01

    Kinetic and equilibrium aspects of three different poly(ethylene oxide) alkylethers (C12E5, C12E7, C14E7) near a flat cellulose surface are studied. The equilibrium adsorption isotherms look very similar for these surfactants, each showing three different regions with increasing surfactant

  11. Adsorption of Cationic Peptides to Solid Surfaces of Glass and Plastic

    DEFF Research Database (Denmark)

    Kristensen, Kasper; Henriksen, Jonas Rosager; Andresen, Thomas Lars

    2015-01-01

    , that the peptides adsorb to solid surfaces of glass and plastic. Specifically, we use analytical HPLC to systematically quantify the adsorption of the three cationic membraneactive peptides mastoparan X, melittin, and magainin 2 to the walls of commonly used glass and plastic sample containers. Our results show...

  12. Surface properties and phosphate adsorption of binary systems containing goethite and kaolinite

    NARCIS (Netherlands)

    Wei, S.Y.; Tan, W.F.; Liu, F.; Zhao, W.; Weng, L.

    2014-01-01

    In soils goethite and kaolinite are often cemented together as a binary association, which has a significant influence on the physical and chemical properties of soils. In this study, the surface properties and phosphate adsorption of goethite, kaolinite, goethite-kaolinite association (GKA) and

  13. Competition between surface adsorption and folding of fibril-forming polypeptides

    NARCIS (Netherlands)

    Ni, R.; Kleijn, J.M.; Cohen Stuart, M.A.; Bolhuis, P.G.

    2015-01-01

    Self-assembly of polypeptides into fibrillar structures can be initiated by planar surfaces that interact favorably with certain residues. Using a coarse-grained model, we systematically studied the folding and adsorption behavior of a ß -roll forming polypeptide. We find that there are two

  14. Competition between surface adsorption and folding of fibril-forming polypeptides

    NARCIS (Netherlands)

    Ni, R.; de Kleijn, M.; Abeln, S.; Cohen Stuart, M.A.; Bolhuis, P.G.

    2015-01-01

    Self-assembly of polypeptides into fibrillar structures can be initiated by planar surfaces that interact favorably with certain residues. Using a coarse-grained model, we systematically studied the folding and adsorption behavior of a β-roll forming polypeptide. We find that there are two different

  15. Competition between surface adsorption and folding of fibril-forming polypeptides

    NARCIS (Netherlands)

    Ni, R.; Kleijn, J.M.; Abeln, S.; Cohen Stuart, M.A.; Bolhuis, P.G.

    2015-01-01

    Self-assembly of polypeptides into fibrillar structures can be initiated by planar surfaces that interact favorably with certain residues. Using a coarse-grained model, we systematically studied the folding and adsorption behavior of a beta-roll forming polypeptide. We find that there are two

  16. A new analytical potential energy surface for the adsorption systemk CO/Cu(100)

    NARCIS (Netherlands)

    Marquardt, R.; Cuvelier, F.; Olsen, R.A.; Baerends, E.J.; Tremblay, J.C.; Saalfrank, P.

    2010-01-01

    Electronic structure data and analytical representations of the potential energy surface for the adsorption of carbon monoxide on a crystalline copper Cu(100) substrate are reviewed. It is found that a previously published and widely used analytical hypersurface for this process [J. C. Tully, M.

  17. Phosphate and phytate adsorption and precipitation on ferrihydrite surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Xiaoming [Department of Ecosystem Science and Management; University of Wyoming; Laramie; USA; Hu, Yongfeng [Canadian Light Source; University of Saskatchewan; Saskatoon; Canada; Tang, Yadong [Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River); Ministry of Agriculture; College of Resources and Environment; Huazhong Agricultural University; Wuhan 430070; Yang, Peng [Department of Ecosystem Science and Management; University of Wyoming; Laramie; USA; Feng, Xionghan [Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtze River); Ministry of Agriculture; College of Resources and Environment; Huazhong Agricultural University; Wuhan 430070; Xu, Wenqian [X-ray Science Division; Advanced Photon Source; Argonne National Laboratory; Argonne; USA; Zhu, Mengqiang [Department of Ecosystem Science and Management; University of Wyoming; Laramie; USA

    2017-01-01

    Transition of phosphate bidentate-binuclear surface complexation to precipitation with increasing P sorption loading was explored using differential pair distribution function (d-PDF) analysis.

  18. Road surface texture and skid resistance

    Science.gov (United States)

    Do, Minh-Tan; Cerezo, Veronique

    2015-12-01

    This paper deals with the relationship between road surface texture and skid resistance. Mechanisms underlying the tire/wet road friction are first described. Definitions of road surface irregularities scales are given. The rest of the paper is then focused on the macrotexture and microtexture scales and their respective roles in what happens at the tire/road interface. Existing methods to measure and characterize the road surface texture are presented. On the one hand, problems encountered when using sensors developed for machined surfaces for the measurement of road surface profiles or cartographies are discussed. On the other hand, potential improvements when applying characterization methods developed for machined surfaces to road surfaces are highlighted. The paper presents finally modeling approaches to calculate friction forces from road surface texture. The generalized form of the models is presented from which terms related respectively to the macrotexture and the microtexture are identified. Approaches used to calculate these terms, integrating eventually other variables, are presented.

  19. Ab initio study of the adsorption of antimony and arsenic on the Si(110) surface

    International Nuclear Information System (INIS)

    Huitzil-Tepanecatl, Arely; Cocoletzi, Gregorio H.; Takeuchi, Noboru

    2010-01-01

    We have performed first principles total energy calculations to investigate the adsorption of Sb and As adatoms on the Si(110) surface using a (2 x 3) supercell. The energetics and atomic structures have been investigated in four atomic configurations. One structure is obtained by placing 1/3 of a monolayer (ML) of Sb (As) atoms on the Si(110) surface. The other three geometries are obtained by depositing 1 ML of Sb (As) atoms on the surface. In the first case the structure is formed by four trimers, in the second case the geometry is formed by zigzag atomic chains and in the third case the structure contains 'microfacets'. The energetics results of the Sb adsorption show that for low coverage the tetrahedrons formed by the adsorption of 1/3 ML is the most stable configuration, while in the monolayer region the zigzag atomic chain is the most stable structure. However, the total energies of the trimer and microfacet structures are slightly higher, indicating that under some conditions, they may be formed. In an experimental report it has been suggested that the adsorption of 1/3 and 1 ML of Sb corresponds to the low and high coverage in the experiments of Zotov et al. [A. V. Zotov, V. G. Lifshifts, and A. N. Demidchik, Surf. Sci. 274, L583 (1992)]. On the other hand, our results of the As adsorption show that for low coverage, the tetrahedrons in the adsorption of 1/3 ML also give the most stable configuration. However, at the 1 ML coverage, a structure formed by microfacets is the most stable structure, in agreement with previous results.

  20. Surface study of platinum decorated graphene towards adsorption of NH3 and CH4

    International Nuclear Information System (INIS)

    Rad, Ali Shokuhi; Pazoki, Hossein; Mohseni, Soheil; Zareyee, Daryoush; Peyravi, Majid

    2016-01-01

    To distinguish the potential of graphene sensors, there is a need to recognize the interaction between graphene sheet and adsorbing molecules. We used density functional theory (DFT) calculations to study the properties of pristine as well as Pt-decorated graphene sheet upon adsorption of NH 3 and CH 4 on its surface to exploit its potential to be as gas sensors for them. We found much higher adsorption, higher charge transfer, lower intermolecular distance, and higher orbital hybridizing upon adsorption of NH 3 and CH 4 gas molecules on Pt-decorated graphene compared to pristine graphene. Also our calculations reveal that the adsorption energies on Pt-decorated graphene sheet are in order of NH 3 >CH 4 which could be corresponded to the order of their sensitivity on this modified surface. We used orbital analysis including density of states as well as frontier molecular orbital study for all analyte-surface systems to more understanding the kind of interaction (physisorption or chemisorption). Consequently, the Pt-decorated graphene can transform the existence of NH 3 and CH 4 molecules into electrical signal and it may be potentially used as an ideal sensor for detection of NH 3 and CH 4 in ambient situation. - Highlights: • Pt-decorated graphene was investigated as an adsorbent for NH 3 and CH 4 . • Much higher adsorption of NH 3 and CH 4 on Pt-decorated graphene than pristine graphene. • Higher adsorption of NH 3 compared to CH 4 on Pt-decorated graphene. • Pt influences the electronic structure of graphene.

  1. Ab initio study of the adsorption of antimony and arsenic on the Si(110) surface

    Energy Technology Data Exchange (ETDEWEB)

    Huitzil-Tepanecatl, Arely [Postgrado en Fisica Aplicada, Facultad de Ciencias Fisico-Matematicas, BUAP, Apartado Postal 52, Puebla 72000 (Mexico); Cocoletzi, Gregorio H., E-mail: cocoletz@sirio.ifuap.buap.m [Centro de Investigacion Cientifica y de Educacion Superior de Ensenada, Km. 107 Carretera Tijuana-Ensenada, Codigo Postal 22860, Apartado Postal 2732 Ensenada, Baja California (Mexico); Centro de Nanociencia y Nanotecnologia, Universidad Nacional Autonoma de Mexico, Apartado Postal 2681, Ensenada, Baja California, 22800 (Mexico); Instituto de Fisica, Universidad Autonoma de Puebla, Apartado Postal J-48, Puebla 72570 (Mexico); Takeuchi, Noboru [Centro de Nanociencia y Nanotecnologia, Universidad Nacional Autonoma de Mexico, Apartado Postal 2681, Ensenada, Baja California, 22800 (Mexico)

    2010-10-29

    We have performed first principles total energy calculations to investigate the adsorption of Sb and As adatoms on the Si(110) surface using a (2 x 3) supercell. The energetics and atomic structures have been investigated in four atomic configurations. One structure is obtained by placing 1/3 of a monolayer (ML) of Sb (As) atoms on the Si(110) surface. The other three geometries are obtained by depositing 1 ML of Sb (As) atoms on the surface. In the first case the structure is formed by four trimers, in the second case the geometry is formed by zigzag atomic chains and in the third case the structure contains 'microfacets'. The energetics results of the Sb adsorption show that for low coverage the tetrahedrons formed by the adsorption of 1/3 ML is the most stable configuration, while in the monolayer region the zigzag atomic chain is the most stable structure. However, the total energies of the trimer and microfacet structures are slightly higher, indicating that under some conditions, they may be formed. In an experimental report it has been suggested that the adsorption of 1/3 and 1 ML of Sb corresponds to the low and high coverage in the experiments of Zotov et al. [A. V. Zotov, V. G. Lifshifts, and A. N. Demidchik, Surf. Sci. 274, L583 (1992)]. On the other hand, our results of the As adsorption show that for low coverage, the tetrahedrons in the adsorption of 1/3 ML also give the most stable configuration. However, at the 1 ML coverage, a structure formed by microfacets is the most stable structure, in agreement with previous results.

  2. Surface-Energetic Heterogeneity of Nanoporous Solids for CO2 and CO Adsorption: The Key to an Adsorption Capacity and Selectivity at Low Pressures.

    Science.gov (United States)

    Kim, Moon Hyeon; Cho, Il Hum; Choi, Sang Ok; Lee, In Soo

    2016-05-01

    This study has been focused on surface energetic heterogeneity of zeolite (H-mordenite, "HM"), activated carbon ("RB2") and metal-organic framework family ("Z1200") materials and their isotherm features in adsorption of CO2 and CO at 25 degrees C and low pressures ≤ 850 Torr. The nanoporous solids showed not only distinctive shape of adsorption isotherms for CO2 with relatively high polarizability and quadrupole moment but also different capacities in the CO2 adsorption. These differences between the adsorbents could be well correlated with their surface nonuniformity. The most heterogeneous surfaces were found with the HM that gave the highest CO2 uptake at all pressures allowed, while the Z1200 consisted of completely homogeneous surfaces and even CO2 adsorption linearly increased with pressure. An intermediate character was indicated on the surface of RB2 and thus this sorbent possessed isotherm features between the HM and Z1200 in CO2 adsorption. Such different surface energetics was fairly consistent with changes in CO2/CO selectivity on the nanoporous adsorbents up to equilibrated pressures near 850 Torr.

  3. An initial research on solute migration model coupled with adsorption of surface complexation in groundwater

    International Nuclear Information System (INIS)

    Qian Tianwei; Chen Fanrong

    2003-01-01

    The influence of solution chemical action in groundwater on solute migration has attracted increasing public attention, especially adsorption action occurring on surface of solid phase and liquid phase, which has play a great role in solute migration. There are various interpretations on adsorption mechanism, in which surface complexion is one of successful hypothesis. This paper first establishes a geochemical model based on surface complexion and then coupled it with traditional advection-dispersion model to constitute a solute migration model, which can deal with surface complexion action. The simulated results fit very well with those obtained by the precursors, as compared with a published famous example, which indicates that the model set up by this paper is successful. (authors)

  4. Surface complexation modeling of Cu(II adsorption on mixtures of hydrous ferric oxide and kaolinite

    Directory of Open Access Journals (Sweden)

    Schaller Melinda S

    2008-09-01

    Full Text Available Abstract Background The application of surface complexation models (SCMs to natural sediments and soils is hindered by a lack of consistent models and data for large suites of metals and minerals of interest. Furthermore, the surface complexation approach has mostly been developed and tested for single solid systems. Few studies have extended the SCM approach to systems containing multiple solids. Results Cu adsorption was measured on pure hydrous ferric oxide (HFO, pure kaolinite (from two sources and in systems containing mixtures of HFO and kaolinite over a wide range of pH, ionic strength, sorbate/sorbent ratios and, for the mixed solid systems, using a range of kaolinite/HFO ratios. Cu adsorption data measured for the HFO and kaolinite systems was used to derive diffuse layer surface complexation models (DLMs describing Cu adsorption. Cu adsorption on HFO is reasonably well described using a 1-site or 2-site DLM. Adsorption of Cu on kaolinite could be described using a simple 1-site DLM with formation of a monodentate Cu complex on a variable charge surface site. However, for consistency with models derived for weaker sorbing cations, a 2-site DLM with a variable charge and a permanent charge site was also developed. Conclusion Component additivity predictions of speciation in mixed mineral systems based on DLM parameters derived for the pure mineral systems were in good agreement with measured data. Discrepancies between the model predictions and measured data were similar to those observed for the calibrated pure mineral systems. The results suggest that quantifying specific interactions between HFO and kaolinite in speciation models may not be necessary. However, before the component additivity approach can be applied to natural sediments and soils, the effects of aging must be further studied and methods must be developed to estimate reactive surface areas of solid constituents in natural samples.

  5. Investigation of the surface adsorption and biotribological properties of mucins

    DEFF Research Database (Denmark)

    Madsen, Jan Busk

    to a surface. However, in other instances the inverse properties are desirable. Mucins are found on epithelial surfaces throughout the body and are a key component of the mucus barrier. Here, they facilitate friction reduction, thus lowering the impact of physical abrasions, but they also act as a physical...... and their aqueous lubrication properties have led to them being proposed as possible biocompatible lubricants. In this thesis, we investigate the biotribological properties of two commercially available mucins on the soft, elastomeric and hydrophobic surface of PDMS under different conditions. Due to the presence...... of a significant amount of non-mucin biomolecules in the commercial mucins, a mild single column protein purification protocol was established. In the mucin biotribology community, many employ the mucins either “as received” or after dialysis. It was therefore investigated how the established purification process...

  6. Adsorption behavior of oxidized galactomannans onto amino terminated surfaces and their interaction with bovine serum albumin

    Energy Technology Data Exchange (ETDEWEB)

    Sierakowski, M.-R; Silva, Maria R.V. da [Universidade Federal do Parana, Curitiba, PR (Brazil). Dept. de Quimica. Lab. de Biopolimeros]. E-mail: mrbiopol@quimica.ufpr.br; Freitas, R.A.; Moreira, Jose S.R. [Universidade Federal do Parana, Curitiba, PR (Brazil). Dept. de Bioquimica; Fujimoto, J.; Petri, D.F.S.; Cordeiro, Paulo R.D. [Sao Paulo Univ., SP (Brazil). Inst. de Quimica]. E-mail: dfsp@quim.iq.usp.br; Andrade, Fabiana D

    2001-07-01

    A galactomannan (CF) extracted from Cassia fastuosa seeds was purified and oxidized with (2,2,6,6- tetramethylpiperidine-1-oxyl) to form a uronic acid-containing polysaccharide (CFOX) with a degree of oxidation (DO) of 0.22. The chemical structures of CF and CFOX were characterized. The adsorption behavior of CF and CFOX onto amino-terminated surfaces was studied by means of ellipsometric measurements. The influence of p H and ionic strength on the adsorption was also investigated. At p H 4, there was a maximum in the adsorbed amount caused by strong electrostatic attraction between the substrate and the oxidized galactomannans. There was no ionic strength effect on the adsorption behavior. The immobilization of bovine serum albumin onto CF and CFOX was studied as a function of p H. At the isoelectric point a maximum in the adsorbed amount was found. (author)

  7. Adsorption behavior of oxidized galactomannans onto amino terminated surfaces and their interaction with bovine serum albumin

    International Nuclear Information System (INIS)

    Sierakowski, M.-R; Silva, Maria R.V. da; Freitas, R.A.; Moreira, Jose S.R.; Fujimoto, J.; Petri, D.F.S.; Cordeiro, Paulo R.D.; Andrade, Fabiana D.

    2001-01-01

    A galactomannan (CF) extracted from Cassia fastuosa seeds was purified and oxidized with (2,2,6,6- tetramethylpiperidine-1-oxyl) to form a uronic acid-containing polysaccharide (CFOX) with a degree of oxidation (DO) of 0.22. The chemical structures of CF and CFOX were characterized. The adsorption behavior of CF and CFOX onto amino-terminated surfaces was studied by means of ellipsometric measurements. The influence of p H and ionic strength on the adsorption was also investigated. At p H 4, there was a maximum in the adsorbed amount caused by strong electrostatic attraction between the substrate and the oxidized galactomannans. There was no ionic strength effect on the adsorption behavior. The immobilization of bovine serum albumin onto CF and CFOX was studied as a function of p H. At the isoelectric point a maximum in the adsorbed amount was found. (author)

  8. Graphene on metal surfaces and its hydrogen adsorption

    DEFF Research Database (Denmark)

    Andersen, Mie; Hornekær, L.; Hammer, B.

    2012-01-01

    The interaction of graphene with various metal surfaces is investigated using density functional theory and the meta-generalized gradient approximation (MGGA) M06-L functional. We demonstrate that this method is of comparable accuracy to the random-phase approximation (RPA). With M06-L we study l...

  9. Early stages of Cs adsorption mechanism for GaAs nanowire surface

    Science.gov (United States)

    Diao, Yu; Liu, Lei; Xia, Sihao; Feng, Shu

    2018-03-01

    In this study, the adsorption mechanism of Cs adatoms on the (100) surface of GaAs nanowire with [0001] growth direction is investigated utilizing first principles method based on density function theory. The adsorption energy, work function, atomic structure and electronic property of clean surface and Cs-covered surfaces with different coverage are discussed. Results show that when only one Cs is adsorbed on the surface, the most favorable adsorption site is BGa-As. With increasing Cs coverage, work function gradually decreases and gets its minimum at 0.75 ML, then rises slightly when Cs coverage comes to 1 ML, indicating the existence of 'Cs-kill' phenomenon. According to further analysis, Cs activation process can effectively reduce the work function due to the formation of a downward band bending region and surface dipole moment directing from Cs adatom to the surface. As Cs coverage increases, the conduction band minimum and valence band maximum both shift towards lower energy side, contributed by the orbital hybridization between Cs-5s, Cs-5p states and Ga-4p, As-4s, As-4p states near Fermi level. The theoretical calculations and analysis in this study can improve the Cs activation technology for negative electron affinity optoelectronic devices based on GaAs nanowires, and also provide a reference for the further Cs/O or Cs/NF3 activation process.

  10. Erosion resistance comparison of alternative surface treatments

    Science.gov (United States)

    Česánek, Z.; Schubert, J.; Houdková, Š.

    2017-05-01

    Erosion is a process characterized by the particle separation and the damage of component functional surfaces. Thermal spraying technology HP/HVOF (High Pressure / High Velocity Oxygen Fuel) is commonly used for protection of component surfaces against erosive wear. Alloy as well as cermet based coatings meet the requirements for high erosion resistance. Wear resistance is in many cases the determining property of required component functioning. The application suitability of coating materials is particularly influenced by different hardness. This paper therefore presents an erosion resistance comparison of alloy and cermet based coatings. The coatings were applied on steel substrates and were subjected to the erosive test using the device for evaluation of material erosion resistance working on the principle of centrifugal erodent flow. Abrasive sand Al2O3 with grain size 212-250 μm was selected as an erosive material. For this purpose, the specimens were prepared by thermal spraying technology HP/HVOF using commercially available powders Stellite 6, NiCrBSi, Cr3C2-25%NiCr, Cr3C2-25%CoNiCrAlY, Hastelloy C-276 and experimental coating TiMoCN-29% Ni. Erosion resistance of evaluated coatings was compared with erosive resistance of 1.4923 high alloyed steel without nitridation and in nitrided state and further with surface treatment using technology PVD. According to the evaluation, the resulting erosive resistance depends not only on the selected erodent and surface protection, but also on the erodent impact angle.

  11. Certain patterns of IgG adsorption by polystyrene bead surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Mamedov, M.K.

    1985-01-01

    The article reports on tests of domestic Soviet polystyrene beads that permit a simplified modification of the enzyme-adsorption method to identify the alpha hepatitis virus and its antibody in nonspecialized, general laboratories. Only patterns of Ig immunoglobulin adsorption were studied. Human IgG was conjugated with the radioactive isotope /sup 125/I by a chloramine method, with mean radioactivity and protein concentration measured frequently. Bovine serum albumin (BSA) and an anionic detergent Tween-20, and a phosphate-salt buffer with pH 5.8-8.2, were used to produce m-Ig and Ig. Adsorption involved incubation of the beads in various solutions, followed by measurement of their radioactivity. Results of several series of tests were subjected to Student-Fisher evaluation. This suggested that the presence of albumin in physiological concentrations in the solution had no important impact on m-Ig adsorption on the bead surface, which effectively adsorbed Ig from solutions without additional proteins, but also from Ig solutions containing serum albumin in physiological concentrations. Thus, it was possible to coat the beads with alpha Ig hepatitis virus. The Tween-20 weak detergent was effective for eliminating unwanted protein adsorption. 9 references, 3 figures.

  12. Polypropylene nonwoven surface modified through introducing porous microspheres: Preparation, characterization and adsorption

    Science.gov (United States)

    Du, Xiao; Wei, Junfu; Liu, Wei; Zhou, Xiangyu; Dai, Danyang

    2016-01-01

    A new porous fabric adsorbent (PM/PP nonwoven) was prepared by hydrogen bonding self-assembly method, in which poly(divinylbenzene-co-4-vinylpyridine) microspheres were introduced onto the surface of PP-g-AA (polypropylene grafted acrylic acid) nonwoven. The effects of the main conditions for self-assembly reaction such as mass ratio of microsphere to nonwoven, pH and the grafting degree of acrylic acid were studied. In addition, the adsorption mechanisms and interactions for three VOCs (styrene, cyclohexane, acetone) were systematically elucidated. The resulting 28.2% PM/PP nonwoven obtained a higher adsorption amount (52.8 mg/g) of styrene vapor, which was 88 times greater than that of original PP nonwoven. Meanwhile, the kinetic studies suggested that the Yoon and Nelson model is suitable to describe the adsorption mechanism of styrene over the modified nonwovens. Adsorption and pressure drop data showed that PM/PP nonwoven had good adsorption ability and air permeability due to its abundant functional groups and porous structures. Taken together, it is expected that PM/PP nonwoven would be a promising adsorbent for removal of VOCs from the gas streams.

  13. Chromate adsorption on selected soil minerals: Surface complexation modeling coupled with spectroscopic investigation

    Energy Technology Data Exchange (ETDEWEB)

    Veselská, Veronika, E-mail: veselskav@fzp.czu.cz [Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Kamýcka 129, CZ-16521, Prague (Czech Republic); Fajgar, Radek [Department of Analytical and Material Chemistry, Institute of Chemical Process Fundamentals of the CAS, v.v.i., Rozvojová 135/1, CZ-16502, Prague (Czech Republic); Číhalová, Sylva [Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Kamýcka 129, CZ-16521, Prague (Czech Republic); Bolanz, Ralph M. [Institute of Geosciences, Friedrich-Schiller-University Jena, Carl-Zeiss-Promenade 10, DE-07745, Jena (Germany); Göttlicher, Jörg; Steininger, Ralph [ANKA Synchrotron Radiation Facility, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, DE-76344, Eggenstein-Leopoldshafen (Germany); Siddique, Jamal A.; Komárek, Michael [Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Kamýcka 129, CZ-16521, Prague (Czech Republic)

    2016-11-15

    Highlights: • Study of Cr(VI) adsorption on soil minerals over a large range of conditions. • Combined surface complexation modeling and spectroscopic techniques. • Diffuse-layer and triple-layer models used to obtain fits to experimental data. • Speciation of Cr(VI) and Cr(III) was assessed. - Abstract: This study investigates the mechanisms of Cr(VI) adsorption on natural clay (illite and kaolinite) and synthetic (birnessite and ferrihydrite) minerals, including its speciation changes, and combining quantitative thermodynamically based mechanistic surface complexation models (SCMs) with spectroscopic measurements. Series of adsorption experiments have been performed at different pH values (3–10), ionic strengths (0.001–0.1 M KNO{sub 3}), sorbate concentrations (10{sup −4}, 10{sup −5}, and 10{sup −6} M Cr(VI)), and sorbate/sorbent ratios (50–500). Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy were used to determine the surface complexes, including surface reactions. Adsorption of Cr(VI) is strongly ionic strength dependent. For ferrihydrite at pH <7, a simple diffuse-layer model provides a reasonable prediction of adsorption. For birnessite, bidentate inner-sphere complexes of chromate and dichromate resulted in a better diffuse-layer model fit. For kaolinite, outer-sphere complexation prevails mainly at lower Cr(VI) loadings. Dissolution of solid phases needs to be considered for better SCMs fits. The coupled SCM and spectroscopic approach is thus useful for investigating individual minerals responsible for Cr(VI) retention in soils, and improving the handling and remediation processes.

  14. Modeling of peptide adsorption interactions with a poly(lactic acid) surface.

    Science.gov (United States)

    O'Brien, C P; Stuart, S J; Bruce, D A; Latour, R A

    2008-12-16

    The biocompatibility of implanted materials and devices is governed by the conformation, orientation, and composition of the layer of proteins that adsorb to the surface of the material immediately upon implantation, so an understanding of this adsorbed protein layer is essential to the rigorous and methodical design of implant materials. In this study, novel molecular dynamics techniques were employed in order to determine the change in free energy for the adsorption of a solvated nine-residue peptide (GGGG-K-GGGG) to a crystalline polylactide surface in an effort to elucidate the fundamental mechanisms that govern protein adsorption. This system, like many others, involves two distinct types of sampling problems: a spatial sampling problem, which arises due to entropic effects creating barriers in the free energy profile, and a conformational sampling problem, which occurs due to barriers in the potential energy landscape. In a two-step process that addresses each sampling problem in turn, the technique of biased replica exchange molecular dynamics was refined and applied in order to overcome these sampling problems and, using the information available at the atomic level of detail afforded by molecular simulation, both quantify and characterize the interactions between the peptide and a relevant biomaterial surface. The results from these simulations predict a fairly strong adsorption response with an adsorption free energy of -2.5 +/- 0.6 kcal/mol (mean +/- 95% confidence interval), with adsorption primarily due to hydrophobic interactions between the nonpolar groups of the peptide and the PLA surface. As part of a larger and ongoing effort involving both simulation and experimental investigations, this work contributes to the goal of transforming the engineering of biomaterials from one dominated by trial-and-error to one which is guided by an atomic-level understanding of the interactions that occur at the tissue-biomaterial interface.

  15. Oxygen adsorption on the Al9Co2(001) surface: first-principles and STM study

    International Nuclear Information System (INIS)

    Villaseca, S Alarcón; Loli, L N Serkovic; Ledieu, J; Fournée, V; Dubois, J-M; Gaudry, É; Gille, P

    2013-01-01

    Atomic oxygen adsorption on a pure aluminum terminated Al 9 Co 2 (001) surface is studied by first-principle calculations coupled with STM measurements. Relative adsorption energies of oxygen atoms have been calculated on different surface sites along with the associated STM images. The local electronic structure of the most favourable adsorption site is described. The preferential adsorption site is identified as a ‘bridge’ type site between the cluster entities exposed at the (001) surface termination. The Al–O bonding between the adsorbate and the substrate presents a covalent character, with s–p hybridization occurring between the states of the adsorbed oxygen atom and the aluminum atoms of the surface. The simulated STM image of the preferential adsorption site is in agreement with experimental observations. This work shows that oxygen adsorption generates important atomic relaxations of the topmost surface layer and that sub-surface cobalt atoms strongly influence the values of the adsorption energies. The calculated Al–O distances are in agreement with those reported in Al 2 O and Al 2 O 3 oxides and for oxygen adsorption on Al(111). (paper)

  16. Studying the role of common membrane surface functionalities on adsorption and cleaning of organic foulants using QCM-D.

    Science.gov (United States)

    Contreras, Alison E; Steiner, Zvi; Miao, Jing; Kasher, Roni; Li, Qilin

    2011-08-01

    Adsorption of organic foulants on nanofiltration (NF) and reverse osmosis (RO) membrane surfaces strongly affects subsequent fouling behavior by modifying the membrane surface. In this study, impact on organic foulant adsorption of specific chemistries including those in commercial thin-film composite membranes was investigated using self-assembled monolayers with seven different ending chemical functionalities (-CH(3), -O-phenyl, -NH(2), ethylene-glycol, -COOH, -CONH(2), and -OH). Adsorption and cleaning of protein (bovine serum albumin) and polysaccharide (sodium alginate) model foulants in two solution conditions were measured using quartz crystal microbalance with dissipation monitoring, and were found to strongly depend on surface functionality. Alginate adsorption correlated with surface hydrophobicity as measured by water contact angle in air; however, adsorption of BSA on hydrophilic -COOH, -NH(2), and -CONH(2) surfaces was high and dominated by hydrogen bond formation and electrostatic attraction. Adsorption of both BSA and alginate was the fastest on -COOH, and adsorption on -NH(2) and -CONH(2) was difficult to remove by surfactant cleaning. BSA adsorption kinetics was shown to be markedly faster than that of alginate, suggesting its importance in the formation of the conditioning layer. Surface modification to render -OH or ethylene-glycol functionalities are expected to reduce membrane fouling.

  17. Adsorption behavior of formaldehyde on ZnO (10 1 bar 0) surface: A first principles study

    Science.gov (United States)

    Jin, Wentao; Chen, Guangde; Duan, Xiangyang; Yin, Yuan; Ye, Honggang; Wang, Dan; Yu, Jinying; Mei, Xuesong; Wu, Yelong

    2017-11-01

    In a first principles study of the formaldehyde adsorption on ZnO surface, we found a novel chain adsorption structure on ZnO (10 1 bar 0) plane. This adsorption structure results from the electrostatic interactions between those adsorbed formaldehyde molecules and the unique arrangement of Zn-O surface dimers on (10 1 bar 0) plane. This adsorption mechanism has the potential to extend to other wurtzite materials' (10 1 bar 0) plane and other similar cases. As the physical adsorption configurations are unstable, the chemical adsorption has to happen. The electronic properties show that the Cdbnd O double bond in CH2O turns into Csbnd O single bond and the highest occupied molecule orbital (HOMO) of formaldehyde is lifted into ZnO band gap becoming the hole trapping center. These results may be meaningful for formaldehyde degradation and detection.

  18. Surface grafting of styrene on polypropylene fibers by argon plasma and its adsorption-regeneration of BTX

    Science.gov (United States)

    Xu, J. J.; Guo, M. L.; Chen, Q. G.; Lian, Z. Y.; Wei, W. J.; Luo, Z. W.; Xie, G.; Chen, H. N.; Dong, K.

    2017-08-01

    Active macromolecular free radicals were generated on polypropylene (PP) fibers surfaces by argon (Ar) plasma irradiation, then, PP surface modified fibers (PP-g-St fibers) were prepared by in-situ grafting reaction of styrene monomers (St). Effects of reaction parameters on grafting percentage were studied and adsorption capacities of PP-g-St fibers for benzene, toluene and xylene (BTX) were evaluated. Afterwards, regeneration adsorption efficiencies after maximum adsorption were explored. The results indicated that the optimum input power, irradiation time and grafting reaction time are 90 W, 3 min and 3 h respectively and the grafting percentage of St reached 5.7 %. The adsorption capacities of PP-g-St fibers towards toluene and xylene emulsions and solutions in water increased by 336.89 % and 344.57 % respectively, compared to pristine PP fibers. In addition, regeneration adsorption efficiencies of modified fibers remained > 90 % after six cycles of regeneration-adsorption experiments, which showed excellent regeneration ability.

  19. Chemistry of aqueous silica nanoparticle surfaces and the mechanism of selective peptide adsorption.

    Science.gov (United States)

    Patwardhan, Siddharth V; Emami, Fateme S; Berry, Rajiv J; Jones, Sharon E; Naik, Rajesh R; Deschaume, Olivier; Heinz, Hendrik; Perry, Carole C

    2012-04-11

    Control over selective recognition of biomolecules on inorganic nanoparticles is a major challenge for the synthesis of new catalysts, functional carriers for therapeutics, and assembly of renewable biobased materials. We found low sequence similarity among sequences of peptides strongly attracted to amorphous silica nanoparticles of various size (15-450 nm) using combinatorial phage display methods. Characterization of the surface by acid base titrations and zeta potential measurements revealed that the acidity of the silica particles increased with larger particle size, corresponding to between 5% and 20% ionization of silanol groups at pH 7. The wide range of surface ionization results in the attraction of increasingly basic peptides to increasingly acidic nanoparticles, along with major changes in the aqueous interfacial layer as seen in molecular dynamics simulation. We identified the mechanism of peptide adsorption using binding assays, zeta potential measurements, IR spectra, and molecular simulations of the purified peptides (without phage) in contact with uniformly sized silica particles. Positively charged peptides are strongly attracted to anionic silica surfaces by ion pairing of protonated N-termini, Lys side chains, and Arg side chains with negatively charged siloxide groups. Further, attraction of the peptides to the surface involves hydrogen bonds between polar groups in the peptide with silanol and siloxide groups on the silica surface, as well as ion-dipole, dipole-dipole, and van-der-Waals interactions. Electrostatic attraction between peptides and particle surfaces is supported by neutralization of zeta potentials, an inverse correlation between the required peptide concentration for measurable adsorption and the peptide pI, and proximity of cationic groups to the surface in the computation. The importance of hydrogen bonds and polar interactions is supported by adsorption of noncationic peptides containing Ser, His, and Asp residues, including

  20. Activation and adsorption of CO{sub 2} on copper surfaces and clusters

    Energy Technology Data Exchange (ETDEWEB)

    Gautam, Seema; Dharmvir, Keya, E-mail: keya@pu.ac.in [Department of Physics, Center of Advanced Studies, Panjab University, Chandigarh- 160014 (India); Goel, Neetu [Department of Chemistry, Center of Advanced Studies, Panjab University, Chandigarh-160014 (India)

    2014-04-24

    The activation and adsorption of CO{sub 2} over Cu{sub n} clusters have been investigated by first principle calculations. Results of these calculations are compared with the previous studies of adsorption of CO{sub 2} on Cu (hkl) surfaces [Wang et al. Surface Science 570 (2004) 205–217]. We find that CO{sub 2} is preferentially adsorbed over the clusters in comparison with Cu (hkl) surfaces. The Cu13 cluster in particular dissociates the CO{sub 2} molecule adsorbed on the one of the caps of the icosahedron into CO and atomic oxygen. This activated configuration can act as a precursor to reactions leading to hydrocarbon fuels from CO{sub 2}.

  1. Adsorption of DNA binding proteins to functionalized carbon nanotube surfaces with and without DNA wrapping.

    Science.gov (United States)

    Ishibashi, Yu; Oura, Shusuke; Umemura, Kazuo

    2017-09-01

    We examined the adsorption of DNA binding proteins on functionalized, single-walled carbon nanotubes (SWNTs). When SWNTs were functionalized with polyethylene glycol (PEG-SWNT), moderate adsorption of protein molecules was observed. In contrast, nanotubes functionalized with CONH 2 groups (CONH 2 -SWNT) exhibited very strong interactions between the CONH 2 -SWNT and DNA binding proteins. Instead, when these SWNT surfaces were wrapped with DNA molecules (thymine 30-mers), protein binding was a little decreased. Our results revealed that DNA wrapped PEG-SWNT was one of the most promising candidates to realize DNA nanodevices involving protein reactions on DNA-SWNT surfaces. In addition, the DNA binding protein RecA was more adhesive than single-stranded DNA binding proteins to the functionalized SWNT surfaces.

  2. A First Principles Study of H2 Adsorption on LaNiO3(001 Surfaces

    Directory of Open Access Journals (Sweden)

    Changchang Pan

    2017-01-01

    Full Text Available The adsorption of H2 on LaNiO3 was investigated using density functional theory (DFT calculations. The adsorption sites, adsorption energy, and electronic structure of LaNiO3(001/H2 systems were calculated and indicated through the calculated surface energy that the (001 surface was the most stable surface. By looking at optimized structure, adsorption energy and dissociation energy, we found that there were three types of adsorption on the surface. First, H2 molecules completely dissociate and then tend to bind with the O atoms, forming two –OH bonds. Second, H2 molecules partially dissociate with the H atoms bonding to the same O atom to form one H2O molecule. These two types are chemical adsorption modes; however, the physical adsorption of H2 molecules can also occur. When analyzing the electron structure of the H2O molecule formed by the partial dissociation of the H2 molecule and the surface O atom, we found that the interaction between H2O and the (001 surface was weaker, thus, H2O was easier to separate from the surface to create an O vacancy. On the (001 surface, a supercell was constructed to accurately study the most stable adsorption site. The results from analyses of the charge population; electron localization function; and density of the states indicated that the dissociated H and O atoms form a typical covalent bond and that the interaction between the H2 molecule and surface is mainly due to the overlap-hybridization among the H 1s, O 2s, and O 2p states. Therefore, the conductivity of LaNiO3(001/H2 is stronger after adsorption and furthermore, the conductivity of the LaNiO3 surface is better than that of the LaFeO3 surface.

  3. Biological protein-resistance layer construction of recombinant hirudin on polymethyl methacrylate IOL surface.

    Science.gov (United States)

    Zheng, Zhiwen; Jiao, Yan; Ren, Li; Wang, Yingjun

    2015-03-01

    In this article, the surface of intraocular len material PMMA was first aminated for activation on which some polar groups generated such as C-N, COO(-), -OH, NH3(+), etc. Then the anticoagulant drugs recombinant hirudin (rH) was grafted with amido bonds to look forward to resist the adsorption of nonspecific protein or cells in tear, even the cataract. The detailed analysis and discussion about the grafting quantity, molography, wettability, electric charges, chemical structure, and the dynamic adsorption of protein Fn on the material surface were carried on by the technology of ultraviolet photometric, contact angle, solid Zeta potential, X-ray photoelectron spectroscopy, and quartz crystal microbalance. The surface with a certain amount of rH modification existed more hydrophilic due to the amphiphilic structure than before, on which the protein adsorption was the most unstable. The results indicated that the rH modification improved the resistance of PMMA to nonspecific adsorption of protein Fn to achieve the expectative effect. © 2014 Wiley Periodicals, Inc.

  4. Adsorption, polymerization and decomposition of acetaldehyde on clean and carbon-covered Rh(111) surfaces

    Science.gov (United States)

    Kovács, Imre; Farkas, Arnold Péter; Szitás, Ádám; Kónya, Zoltán; Kiss, János

    2017-10-01

    The adsorption and dissociation of acetaldehyde were investigated on clean and carbon-covered Rh(111) single crystal surfaces by electron energy loss spectroscopy (EELS), temperature programmed desorption (TPD), high-resolution electron energy loss spectroscopy (HREELS) and work function (Δφ) measurements. Acetaldehyde is a starting material for the catalytic production of many important chemicals and investigation of its reactions motivated by environmental purposes too. The adsorption of acetaldehyde on clean Rh(111) surface produced various types of adsorption forms. η1-(O)-CH3CHOa and η2-(O,C)-CH3CHOa are developing and characterized by HREELS. η1-CH3CHOa partly desorbed at Tp = 150 K, another part of these species are incorporated in trimer and linear 2D polimer species. The desorption of trimers (at amu 132) were observed in TPD with a peak maximum at Tp = 225 K. Above this temperature acetaldehyde either desorbed or bonded as a stable surface intermediate (η2-CH3CHOa) on the rhodium surface. The molecules decomposed to adsorbed products, and only hydrogen and carbon monoxide were analyzed in TPD. Surface carbon decreased the uptake of adsorbed acetaldehyde, inhibited the formation of polymers, nevertheless, it induced the Csbnd O bond scission and CO formation with 40-50 K lower temperature after higher acetaldehyde exposure.

  5. Surface morphology and corrosion resistance of electrodeposited ...

    Indian Academy of Sciences (India)

    Administrator

    Surface morphology and corrosion resistance of electrodeposited composite coatings containing polyethylene or polythiophene in. Ni–Mo base. J NIEDBAŁA. Institute of Materials Science, University of Silesia, 40-007 Katowice, ul. Bankowa 12, Poland. MS received 11 December 2009; revised 30 April 2010. Abstract.

  6. SeO2 adsorption on CaO surface: DFT study on the adsorption of a single SeO2 molecule

    Science.gov (United States)

    Fan, Yaming; Zhuo, Yuqun; Lou, Yu; Zhu, Zhenwu; Li, Liangliang

    2017-08-01

    Selenium is a hazardous element in coal. During coal combustion, most of the selenium will convert to SeO2 in the flue gas. Ca-based adsorbents, especially CaO, have been considered as a potential sorbent to adsorb SeO2 due to its low cost. In this paper, the adsorption mechanisms of single SeO2 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 SeO2 on CaO surface is primarily chemisorption, while physisorption takes effects at the initial stage of the process. Under O2 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 SeO2 and CaO surface during adsorption. The results provide fundamental information of the adsorption process, which could be meaningful for the development of new absorbents.

  7. Hydrogen collisions with transition metal surfaces: Universal electronically nonadiabatic adsorption

    Science.gov (United States)

    Dorenkamp, Yvonne; Jiang, Hongyan; Köckert, Hansjochen; Hertl, Nils; Kammler, Marvin; Janke, Svenja M.; Kandratsenka, Alexander; Wodtke, Alec M.; Bünermann, Oliver

    2018-01-01

    Inelastic scattering of H and D atoms from the (111) surfaces of six fcc transition metals (Au, Pt, Ag, Pd, Cu, and Ni) was investigated, and in each case, excitation of electron-hole pairs dominates the inelasticity. The results are very similar for all six metals. Differences in the average kinetic energy losses between metals can mainly be attributed to different efficiencies in the coupling to phonons due to the different masses of the metal atoms. The experimental observations can be reproduced by molecular dynamics simulations based on full-dimensional potential energy surfaces and including electronic excitations by using electronic friction in the local density friction approximation. The determining factors for the energy loss are the electron density at the surface, which is similar for all six metals, and the mass ratio between the impinging atoms and the surface atoms. Details of the electronic structure of the metal do not play a significant role. The experimentally validated simulations are used to explore sticking over a wide range of incidence conditions. We find that the sticking probability increases for H and D collisions near normal incidence—consistent with a previously reported penetration-resurfacing mechanism. The sticking probability for H or D on any of these metals may be represented as a simple function of the incidence energy, Ein, metal atom mass, M, and incidence angle, 𝜗i n. S =(S0+a ṡEi n+b ṡM ) *(1 -h (𝜗i n-c ) (1 -cos(𝜗 i n-c ) d ṡh (Ei n-e ) (Ei n-e ) ) ) , where h is the Heaviside step function and for H, S0 = 1.081, a = -0.125 eV-1, b =-8.40 ṡ1 0-4 u-1, c = 28.88°, d = 1.166 eV-1, and e = 0.442 eV; whereas for D, S0 = 1.120, a = -0.124 eV-1, b =-1.20 ṡ1 0-3 u-1, c = 28.62°, d = 1.196 eV-1, and e = 0.474 eV.

  8. Adsorption of Amorphous Silica Nanoparticles onto Hydroxyapatite Surfaces Differentially Alters Surfaces Properties and Adhesion of Human Osteoblast Cells.

    Directory of Open Access Journals (Sweden)

    Priya Kalia

    Full Text Available Silicon (Si is suggested to be an important/essential nutrient for bone and connective tissue health. Silicon-substituted hydroxyapatite (Si-HA has silicate ions incorporated into its lattice structure and was developed to improve attachment to bone and increase new bone formation. Here we investigated the direct adsorption of silicate species onto an HA coated surface as a cost effective method of incorporating silicon on to HA surfaces for improved implant osseointegration, and determined changes in surface characteristics and osteoblast cell adhesion. Plasma-sprayed HA-coated stainless steel discs were incubated in silica dispersions of different concentrations (0-42 mM Si, at neutral pH for 12 h. Adsorbed Si was confirmed by XPS analysis and quantified by ICP-OES analysis following release from the HA surface. Changes in surface characteristics were determined by AFM and measurement of surface wettability. Osteoblast cell adhesion was determined by vinculin plaque staining. Maximum Si adsorption to the HA coated disc occurred after incubation in the 6 mM silica dispersion and decreased progressively with higher silica concentrations, while no adsorption was observed with dispersions below 6 mM Si. Comparison of the Si dispersions that produced the highest and lowest Si adsorption to the HA surface, by TEM-based analysis, revealed an abundance of small amorphous nanosilica species (NSP of ~1.5 nm in diameter in the 6 mM Si dispersion, with much fewer and larger NSP in the 42 mM Si dispersions. 29Si-NMR confirmed that the NSPs in the 6 mM silica dispersion were polymeric and similar in composition to the larger NSPs in the 42 mM Si dispersion, suggesting that the latter were aggregates of the former. Amorphous NSP adsorbed from the 6 mM dispersion on to a HA-coated disc surface increased the surface's water contact angle by 53°, whereas that adsorbed from the 42 mM dispersion decreased the contact angle by 18°, indicating increased and

  9. Polysiloxane surface modified with bipyrazolic tripodal receptor for quantitative lead adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Radi, Smaail, E-mail: radi_smaail@yahoo.fr [Laboratoire de Chimie Organique, Macromoleculaire et Produits Naturels, Equipe de Chimie Bio-organique et Macromoleculaire, Unite Associee au CNRST URAC 25, Departement de Chimie, Faculte des Sciences, Universite Med I, BP 524, 60 000 Oujda (Morocco); Tighadouini, Said; Toubi, Yahya [Laboratoire de Chimie Organique, Macromoleculaire et Produits Naturels, Equipe de Chimie Bio-organique et Macromoleculaire, Unite Associee au CNRST URAC 25, Departement de Chimie, Faculte des Sciences, Universite Med I, BP 524, 60 000 Oujda (Morocco); Bacquet, Maryse [Universite des Sciences et Technologies de Lille, UMET: Unite Materiaux et Transformations UMR8207, Equipe Ingenierie des Systemes Polymeres, Batiment C6 salle 119-59655 Villeneuve d' Ascq (France)

    2011-01-15

    A new silica gel compound modified N,N-bis(3,5-dimethylpyrazol-1-ylmethyl) amine (SiN{sub 2}Pz) was synthesized and characterized by elemental analysis, FT-IR, {sup 13}C NMR of the solid state, nitrogen adsorption-desorption isotherm, BET surface area and BJH pore sizes. The new surface exhibits good chemical and thermal stability determined by thermogravimetry curves (TGA). The effect of pH and stirring time on the adsorption of Pb(II) were studied. The process of metal retention was followed by batch method and the optimum pH value for the quantitative adsorption of this toxic metal ion was 7. At this pH value, the new functionalized polysiloxane presents further improvements and shows higher affinity (123 mg of Pb{sup 2+}/g of silica) for the effective adsorption of Pb(II) compared to others described sorbents. The extracted amounts of Pb(II) were determined by atomic absorption measurements.

  10. Bacterial Cell Surface Adsorption of Rare Earth Elements

    Science.gov (United States)

    Jiao, Y.; Park, D.; Reed, D.; Fujita, Y.; Yung, M.; Anderko, A.; Eslamimanesh, A.

    2015-12-01

    Rare earth elements (REE) play a critical role in many emerging clean energy technologies, including high-power magnets, wind turbines, solar panels, hybrid/electric vehicle batteries and lamp phosphors. In order to sustain demand for such technologies given current domestic REE shortages, there is a need to develop new approaches for ore processing/refining and recycling of REE-containing materials. To this end, we have developed a microbially-mediated bioadsorption strategy with application towards enrichment of REE from complex mixtures. Specifically, the bacterium Caulobacter crescentus was genetically engineered to display lanthanide binding tags (LBTs), short peptides that possess high affinity and specificity for rare earth elements, on its cell surface S-layer protein. Under optimal conditions, LBT-displayed cells adsorbed greater than 5-fold more REE than control cells lacking LBTs. Competition binding experiments with a selection of REEs demonstrated that our engineered cells could facilitate separation of light- from heavy- REE. Importantly, binding of REE onto our engineered strains was much more favorable compared to non-REE metals. Finally, REE bound to the cell surface could be stripped off using citrate, providing an effective and non-toxic REE recovery method. Together, this data highlights the potential of our approach for selective REE enrichment from REE containing mixtures.

  11. Influence of the pore structure and surface chemical properties of activated carbon on the adsorption of mercury from aqueous solutions

    International Nuclear Information System (INIS)

    Lu, Xincheng; Jiang, Jianchun; Sun, Kang; Wang, Jinbiao; Zhang, Yanping

    2014-01-01

    Highlights: • Activated carbons with different pore structure and surface chemical properties were prepared by modification process. • HgCl 2 as a pollution target to evaluate the adsorption performance. • Influence of pore structure and surface chemical properties of activated carbon on adsorption of mercury was investigated. -- Abstract: Reactivation and chemical modification were used to obtain modified activated carbons with different pore structure and surface chemical properties. The samples were characterized by nitrogen absorption–desorption, Fourier transform infrared spectroscopy and the Bothem method. Using mercury chloride as the target pollutant, the Hg 2+ adsorption ability of samples was investigated. The results show that the Hg 2+ adsorption capacity of samples increased significantly with increases in micropores and acidic functional groups and that the adsorption process was exothermic. Different models and thermodynamic parameters were evaluated to establish the mechanisms. It was concluded that the adsorption occurred through a monolayer mechanism by a two-speed process involving both rapid adsorption and slow adsorption. The adsorption rate was determined by chemical reaction

  12. Study of Cs adsorption on (100) surface of [001]-oriented GaN nanowires: A first principle research

    Energy Technology Data Exchange (ETDEWEB)

    Xia, Sihao [Department of Optoelectronic Technology, School of Electronic and Optical Engineering, Nanjing University of Science and Technology Nanjing, 210094 (China); Liu, Lei, E-mail: liu1133_cn@sina.com.cn [Department of Optoelectronic Technology, School of Electronic and Optical Engineering, Nanjing University of Science and Technology Nanjing, 210094 (China); Kong, Yike [Department of Optoelectronic Technology, School of Electronic and Optical Engineering, Nanjing University of Science and Technology Nanjing, 210094 (China); Wang, Honggang; Wang, Meishan [School of Information and Electrical Engineering, Ludong University, Yantai 264025 (China)

    2016-11-30

    Highlights: • B{sub N} is the most stable adsorption site. • Work function is reduced after Cs adsorption. • Surface atomic structures are reconstructed. • Surface states near fermi level is contributed to the hybridization of Cs 5s state with Ga 4p and N 2p state. • NEA surface is demonstrated after Cs adsorption on GaN nanowire surface. - Abstract: Based on first-principle study, the adsorption mechanism of Cs on (100) crystal plane of GaN nanowire surface with coverage of 1/12 monolayer is explored. It is discovered that the most stable adsorption site is B{sub N} because of its lowest adsorption energy. The work function of GaN nanowire surface is reduced by 1.69 eV and will be further reduced with increasing Cs adsorption, which promotes the development of negative electron affinity (NEA) state of the materials. Furthermore, Cs adatom will make a great influence on the surface atomic structure, oppositely, little influence on the center atomic structure. There appears a dipole moment valued −6.93 Debye on the nanowire surface contributed to the formation the heterojunction on the surface, which is beneficial to the photoelectrons liberation. After Cs adsorption, the valence band and conduction band both move to lower energy side. The surface states mainly result from the hybridization of Cs 5s state with Ga 4p state and N 2p state. This study can help us to further experiment on the Cs adsorption processing on GaN nanowire and improve the photoemission performance of GaN nanowire devices.

  13. Adsorption-Driven Surface Segregation of the Less Reactive Alloy Component

    DEFF Research Database (Denmark)

    Andersson, Klas Jerker; Calle Vallejo, Federico; Rossmeisl, Jan

    2009-01-01

    Counterintuitive to expectations and all prior observations of adsorbate-induced surface segregation of the more reactive alloy component (the one forming the stronger bond with the adsorbate), we show that CO adsorption at elevated pressures and temperatures pulls the less reactive Cu to the sur......Counterintuitive to expectations and all prior observations of adsorbate-induced surface segregation of the more reactive alloy component (the one forming the stronger bond with the adsorbate), we show that CO adsorption at elevated pressures and temperatures pulls the less reactive Cu...... to the surface of a CuPt near-surface alloy. The Cu surface segregation is driven by the formation of a stable self-organized CO/CuPt surface alloy structure and is rationalized in terms of the radically stronger Pt−CO bond when Cu is present in the first surface layer of Pt. The results, which are expected...... to apply to a range of coinage (Cu, Ag)/Pt-group bimetallic surface alloys, open up new possibilities in selective and dynamical engineering of alloy surfaces for catalysis....

  14. Dynamic surface tension and adsorption mechanism of surfactin biosurfactant at the air-water interface.

    Science.gov (United States)

    Onaizi, Sagheer A

    2018-03-01

    The dynamic adsorption of the anionic biosurfactant, surfactin, at the air-water interface has been investigated in this work and compared to those of two synthetic surfactants: the anionic sodium dodecylbenzenesulfonate (SDBS) and the nonionic octaethylene glycol monotetradecyl ether (C 14 E 8 ). The results revealed that surfactin adsorption at the air-water interface is purely controlled by diffusion mechanism at the initial stage of the adsorption process (i.e., [Formula: see text]), but shifts towards a mixed diffusion-barrier mechanism when surface tension approaches equilibrium (i.e., [Formula: see text]) due to the development of an energy barrier for adsorption. Such energy barrier has been found to be a function of the surfactin bulk concentration (increases with increasing surfactin concentration) and it is estimated to be in the range of 1.8-9.5 kJ/mol. Interestingly, such a trend (pure diffusion-controlled mechanism at [Formula: see text] and mixed diffusion-barrier mechanism at [Formula: see text]) has been also observed for the nonionic C 14 E 8 surfactant. Unlike the pure diffusion-controlled mechanism of the initial surfactin adsorption, which was the case in the presence and the absence of the sodium ion (Na + ), SDBS showed a mixed diffusion-barrier controlled at both short and long time, with an energy barrier of 3.0-9.0 and 3.8-18.0 kJ/mol, respectively. Such finding highlights the nonionic-like adsorption mechanism of surfactin despite its negative charge.

  15. The adsorption and dissociation of water molecule on goethite (010) surface: A DFT approach

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Long, E-mail: shuweixia@ouc.edu.cn [Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, Ocean University of China, College of Chemistry and Chemical Engineering (China); Xiu, Fangyuan [Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, Ocean University of China, College of Chemistry and Chemical Engineering (China); Qiu, Meng [Qingdao Institute of Bioenergy and Bioprocess Technology (China); Xia, Shuwei; Yu, Liangmin [Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, Ocean University of China, College of Chemistry and Chemical Engineering (China)

    2017-01-15

    Graphical abstract: The optimized structure of hydrated goethite (010) surface with medium water coverage (water density about 6.7 H{sub 2}O/nm{sup 2}). - Highlights: • Stable adsorption and dissociation structure of H{sub 2}O on goethite (010) surface was investigated by DFT. • Reasonable path for water dissociation was proposed by transitional state analysis. • The mechanism of water adsorption on goethite and binding nature were revealed by PDOS. - Abstract: Using density functional theory (DFT) calculation, we investigate the configuration, stability and electronic properties of fresh cleaved (010) goethite surface (Pnma) and this surface exposed to water monolayer at low, medium and high coverage. Water is predicted to be chemisorbed to the surface, together with the surface reconstruction. The interaction energy of the most stable configuration of both low and medium coverage per water molecule is almost the same (−1.17 eV), while that of high coverage is much lower (less than 1.03 eV). It indicates that highly hydrated surface is less stable. PDOS analysis reveals the adsorption of H{sub 2}O is due to the formation of Fe−O bond, caused by overlapping of Fe's 3d and O's 2p orbitals. Dissociation processes at low and medium water coverage are non-spontaneous; while at high coverage, it can undertake spontaneously both thermodynamically and dynamically. The dissociation paths of all three water coverage are the similar. The proton from one adsorbed water is likely to dissociate to bind to the vicinal surface μ{sub 3}−O as an intermediate product; the proton belonged to μ{sub 3}−O transferred to the neighbor surface μ{sub 2}−O as the dissociative configuration.

  16. Adsorption mechanism of an antimicrobial peptide on carbonaceous surfaces: A molecular dynamics study

    Science.gov (United States)

    Roccatano, Danilo; Sarukhanyan, Edita; Zangi, Ronen

    2017-02-01

    Peptides are versatile molecules with applications spanning from biotechnology to nanomedicine. They exhibit a good capability to unbundle carbon nanotubes (CNT) by improving their solubility in water. Furthermore, they are a powerful drug delivery system since they can easily be uptaken by living cells, and their high surface-to-volume ratio facilitates the adsorption of molecules of different natures. Therefore, understanding the interaction mechanism between peptides and CNT is important for designing novel therapeutical agents. In this paper, the mechanisms of the adsorption of antimicrobial peptide Cecropin A-Magainin 2 (CA-MA) on a graphene nanosheet (GNS) and on an ultra-short single-walled CNT are characterized using molecular dynamics simulations. The results show that the peptide coats both GNS and CNT surfaces through preferential contacts with aromatic side chains. The peptide packs compactly on the carbon surfaces where the polar and functionalizable Lys side chains protrude into the bulk solvent. It is shown that the adsorption is strongly correlated to the loss of the peptide helical structure. In the case of the CNT, the outer surface is significantly more accessible for adsorption. Nevertheless when the outer surface is already covered by other peptides, a spontaneous diffusion, via the amidated C-terminus into the interior of the CNT, was observed within 150 ns of simulation time. We found that this spontaneous insertion into the CNT interior can be controlled by the polarity of the entrance rim. For the positively charged CA-MA peptide studied, hydrogenated and fluorinated rims, respectively, hinder and promote the insertion.

  17. Theoretical investigation of lead vapor adsorption on kaolinite surfaces with DFT calculations.

    Science.gov (United States)

    Wang, Xinye; Huang, Yaji; Pan, Zhigang; Wang, Yongxing; Liu, Changqi

    2015-09-15

    Kaolinite can be used as the in-furnace sorbent/additive to adsorb lead (Pb) vapor at high temperature. In this paper, the adsorptions of Pb atom, PbO molecule and PbCl2 molecule on kaolinie surfaces were investigated by density functional theory (DFT) calculation. Si surface is inert to Pb vapor adsorption while Al surfaces with dehydroxylation are active for the unsaturated Al atoms and the O atoms losing H atoms. The adsorption energy of PbO is much higher than that of Pb atom and PbCl2. Considering the energy barriers, it is easy for PbO and PbCl2 to adsorb on Al surfaces but difficult to escape. The high energy barriers of de-HCl process cause the difficulties of PbCl2 to form PbO·Al2O3·2SiO2 with kaolinite. Considering the inertia of Si atoms and the activity of Al atoms after dehydroxylation, calcination, acid/alkali treatment and some other treatment aiming at amorphous silica producing and Al activity enhancement can be used as the modification measures to improve the performance of kaolinite as the in-furnace metal capture sorbent. Copyright © 2015 Elsevier B.V. All rights reserved.

  18. A Universal Isotherm Model to Capture Adsorption Uptake and Energy Distribution of Porous Heterogeneous Surface

    KAUST Repository

    Ng, Kim Choon

    2017-08-31

    The adsorbate-adsorbent thermodynamics are complex as it is influenced by the pore size distributions, surface heterogeneity and site energy distribution, as well as the adsorbate properties. Together, these parameters defined the adsorbate uptake forming the state diagrams, known as the adsorption isotherms, when the sorption site energy on the pore surfaces are favorable. The available adsorption models for describing the vapor uptake or isotherms, hitherto, are individually defined to correlate to a certain type of isotherm patterns. There is yet a universal approach in developing these isotherm models. In this paper, we demonstrate that the characteristics of all sorption isotherm types can be succinctly unified by a revised Langmuir model when merged with the concepts of Homotattic Patch Approximation (HPA) and the availability of multiple sets of site energy accompanied by their respective fractional probability factors. The total uptake (q/q*) at assorted pressure ratios (P/P s ) are inextricably traced to the manner the site energies are spread, either naturally or engineered by scientists, over and across the heterogeneous surfaces. An insight to the porous heterogeneous surface characteristics, in terms of adsorption site availability has been presented, describing the unique behavior of each isotherm type.

  19. Dissolved organic matter adsorption to model surfaces: adlayer formation, properties, and dynamics at the nanoscale.

    Science.gov (United States)

    Armanious, Antonius; Aeppli, Meret; Sander, Michael

    2014-08-19

    Adlayers of dissolved organic matter (DOM) form on many surfaces in natural and engineered systems and affect a number of important processes in these systems. Yet, the nanoscalar properties and dynamics of DOM adlayers remain poorly investigated. This work provides a systematic analysis of the properties and dynamics of adlayers formed from a diverse set of eight humic and fulvic acids, used as DOM models, on surfaces of self-assembled monolayers (SAMs) of different alkylthiols covalently bound to gold supports. DOM adsorption to positively charged amine-terminated SAMs resulted in the formation of water-rich adlayers with nanometer thicknesses that were relatively rigid, irreversibly adsorbed, and collapsed upon air drying, as demonstrated by combined quartz crystal microbalance and ellipsometry measurements. DOM adlayer thicknesses varied only slightly with solution pH from 5 to 8 but increased markedly with increasing ionic strength. Contact angle measurements revealed that the DOM adlayers were relatively polar, likely due to the high water contents of the adlayers. Comparing DOM adsorption to SAM-coated sensors that systematically differed in surface charge and polarity characteristics showed that electrostatics dominated DOM-surface interactions. Laccase adsorption to DOM adlayers on amine-terminated SAMs served to demonstrate the applicability of the presented experimental approach to study the interactions of (bio)macromolecules and (nano)particles with DOM.

  20. CO adsorption, dissociation and coupling formation mechanisms on Fe2C(001) surface

    Science.gov (United States)

    Yu, Xiaohu; Zhang, Xuemei; Meng, Yan; Zhao, Yaoping; Li, Yuan; Xu, Wei; Liu, Zhong

    2018-03-01

    By means of density functional theory calculations and atomic thermodynamics, we systematically investigated the CO adsorption on the Fe2C(001) surface at different coverage. It has been found that CO prefers to adsorb on the surface iron atom at low coverage (1-8 CO); CO prefers to adsorb at the bridge site of Fe and C atoms at high coverage (9-12 CO). Eight CO molecules binding on the Fe2C(001) surface is favorable thermodynamically as indicated by the stepwise adsorption energy. The phase diagram shows that addition of more CO molecules up to a number of 8 is thermodynamically favorable, and that the incremental energy gained by adding one more CO molecule is almost constant up to 4 CO molecules, decreases up to 8 CO molecules, after which it becomes thermodynamically unfavorable to add more CO molecules. Probability distribution of different singe-CO adsorbed states on the Fe2C(001) surface as function of temperature shows that CO dissociation and coupling are least preferred, indicating that carbide mechanism is not dominant in the iron-based Fischer-Tropsch synthesis reaction. The projected density of states (PDOS) was used to analyze the CO adsorption mechanism.

  1. Plane micropolar elasticity with surface flexural resistance

    Science.gov (United States)

    Gharahi, Alireza; Schiavone, Peter

    2018-03-01

    We propose a linear surface/interface model for plane deformations of a micropolar elastic solid based on a higher-order surface elasticity theory capable of incorporating bending and twisting effects. The surface/interface is modeled as a bending-resistant Kirchhoff micropolar thin shell perfectly bonded to the boundary of the solid. It is anticipated that by combining micropolar bulk and surface effects in this way, the enhanced model will most accurately capture the essential characteristics (in particular, size dependency) required in the modeling of materials with significant microstructure as well as in the modeling of classes of nanomaterials. The corresponding boundary value problems are particularly interesting in that they involve boundary conditions of order higher than that of the governing field equations. We illustrate our theory by analyzing the simple problem of a circular hole in a micropolar sheet noting, in particular, the extent to which surface effects and micropolar properties each contribute to the deformation of the sheet.

  2. Water adsorption on amorphous silica surfaces: a Car-Parrinello simulation study

    International Nuclear Information System (INIS)

    Mischler, Claus; Horbach, Juergen; Kob, Walter; Binder, Kurt

    2005-01-01

    A combination of classical molecular dynamics (MD) and ab initio Car-Parrinello molecular dynamics (CPMD) simulations is used to investigate the adsorption of water on a free amorphous silica surface. From the classical MD, SiO 2 configurations with a free surface are generated which are then used as starting configurations for the CPMD. We study the reaction of a water molecule with a two-membered ring at the temperature T = 300 K. We show that the result of this reaction is the formation of two silanol groups on the surface. The activation energy of the reaction is estimated and it is shown that the reaction is exothermic

  3. Simulation insight into the cytochrome c adsorption on graphene and graphene oxide surfaces

    Science.gov (United States)

    Zhao, Daohui; Li, Libo; Zhou, Jian

    2018-01-01

    Graphene-based materials might serve as an ideal platform for the regulation and promotion of metalloprotein electron transfer (ET); however, the underpinning mechanism at the molecular level has not yet been fully revealed. The orientation of cytochrome c (Cyt c) on surfaces is vital for ET. In this work, the orientation of Cyt c on graphene and graphene oxide (GO) surfaces, as well as the dominant driving forces, the conformational change and the ET pathways were investigated by molecular dynamics simulations. The results show that Cyt c is adsorbed onto the GO surface mainly through lysine residues; whereas hydrophobic interaction contributes to the Cyt c adsorption on graphene surface. There is no significant conformational change of Cyt c upon adsorption. The heme plane of Cyt c tends to be horizontally oriented and far away from the graphene surface, which is not conducive to ET. On the GO surface, the heme plane is slightly deviated from the normal direction to the surface and the axial ligand Met80 is much closer to the surface, which facilitates the ET. These findings shed some light on the ET mechanism of Cyt c on graphene-based materials and provide guidance for the development of bionic electronic devices.

  4. Blood response to plasticized poly(vinyl chloride): dependence of fibrinogen adsorption on plasticizer selection and surface plasticizer level.

    Science.gov (United States)

    Zhao, X B; Courtney, J M

    2003-10-01

    The high level of plasticizer in plasticized poly(vinyl chloride) (PVC) ensures that plasticizer selection has an important influence on the suitability of PVC to function in blood-contacting applications. In this study, three types of plasticized PVC in sheet form, with di-(2-ethylhexyl)phthalate (DEHP), tri-(2-ethylhexyl)trimellitate (TEHTM) and n-butyryltri-n-hexyl citrate (BTHC) as plasticizer, were selected for assessment and single solute fibrinogen adsorption was utilized as an initial index of interactions with blood components. Fibrinogen adsorption behavior shows a strong dependence on the plasticizer selection, plasticizer level at the surface and the adsorption conditions, such as adsorption time and fibrinogen solution concentration. Results indicate that BTHC plasticized PVC possesses the lowest adsorption capacity in the three types of plasticized PVC, while TEHTM plasticized PVC seems to have the strongest reactivity in certain fibrinogen solution concentrations. The alteration of surface plasticizer level was achieved by a methanol-cleaning treatment with a variety of cleaning times and the fibrinogen adsorption on plasticized PVC decreases with the reduction of surface plasticizer level. The migration behavior of two phthalate esters (DEHP and TEHTM) was evaluated using UV-Spectrophotometer to determine the plasticizer level at the surfaces. In addition, the fibrinogen adsorption mechanism was examined with Freundlich adsorption modeling.

  5. Tuning the Surface of Nanoparticles: Impact of Poly(2-ethyl-2-oxazoline) on Protein Adsorption in Serum and Cellular Uptake

    NARCIS (Netherlands)

    Koshkina, O.; Westmeier, D.; Lang, T.; Bantz, C.; Hahlbrock, A.; Wurth, C.; Resch-Genger, U.; Braun, U.; Thiermann, R.; Weise, C.; Eravci, M.; Mohr, B.; Schlaad, H.; Stauber, R.H.; Docter, D.; Bertin, A.; Maskos, M.

    2016-01-01

    Due to the adsorption of biomolecules, the control of the biodistribution of nanoparticles is still one of the major challenges of nanomedicine. Poly(2-ethyl-2-oxazoline) (PEtOx) for surface modification of nanoparticles is applied and both protein adsorption and cellular uptake of PEtOxylated

  6. Adsorption and dissociation of dinitrogen on transition metal (Ta, W and Re) doped MgO surface

    KAUST Repository

    Yadav, Manoj Kumar

    2016-06-16

    The adsorption and dissociation of dinitrogen on transition metal (Ta, W and Re) doped MgO(100) surface has been studied employing density functional theory. It is found that all these transition metals (TM) on MgO(100) surface are capable of adsorbing dinitrogen (N2), however there is no dissociative adsorption of N2 on single transition metal dopant. When two TM atoms are doped on MgO(100) surface, dissociative adsorption of dinitrogen occurs in all the three cases. Whether the dissociation is spontaneous or is it associated with activation barrier depends on the orientation of N2 molecule approaching the dopant site.

  7. Adsorption of Atoms of 3 d Metals on the Surfaces of Aluminum and Magnesium Oxide Films

    Science.gov (United States)

    Ramonova, A. G.; Kibizov, D. D.; Kozyrev, E. N.; Zaalishvili, V. B.; Grigorkina, G. S.; Fukutani, K.; Magkoev, T. T.

    2018-01-01

    The adsorption and formation of submonolayer structures of Ti, Cr, Fe, Ni, Cu on the surfaces of aluminum and magnesium oxide films formed on Mo(110) under ultrahigh vacuum conditions are studied via X-ray, ultraviolet photo-, and Auger electron spectroscopy (XPS, UVES, AES); spectroscopy of energy losses of high-resolution electrons (SELHRE); spectroscopy of the backscattering of low-energy ions (SBSLEI); infrared absorption spectroscopy (IAS); and the diffraction of slow electrons (DSE). Individual atoms and small clusters of all the investigated metals deposited on oxides acquire a positive charge, due presumably to interaction with surface defects. As the concentration of adatoms increases when the adsorption centers caused by defects are filled, charge transfer from adatoms to substrates is reduced. This is accompanied by further depolarization caused by the lateral interaction of adatoms.

  8. Adsorption of neon and tetrafluoromethane on carbon nanohorn aggregates: differences in specific surface area values

    Science.gov (United States)

    Krungleviciute, Vaiva; Yudasaka, Masako; Iijima, Sumio; Migone, Aldo

    2008-03-01

    We have measured adsorption isotherms for two different adsorbates, neon and tetrafluoromethane, on dahlia-like carbon nanohorn aggregates. The experiments were performed at similar relative temperatures for both gases. The measurements were conducted to explore the effect of adsorbate diameter on the behavior of the resulting adsorbed systems. We measured the effective specific surface area value of the nanohorn sample using both gases, and we found that this quantity was about 22% smaller when we determined this quantity using tetrafluoromethane, the larger molecule. Isosteric heat and binding energy values were also determined from our measurements. We will compare our experimental results with those from a computer simulation study performed by Prof. M. Calbi. The simulations help us understand the source of the observed differences in the measured specific surface values, as well as the coverage dependence of the isosteric heat of adsorption for both gases.

  9. Surface Complexation Modeling in Variable Charge Soils: Prediction of Cadmium Adsorption

    Directory of Open Access Journals (Sweden)

    Giuliano Marchi

    2015-10-01

    Full Text Available ABSTRACT Intrinsic equilibrium constants for 22 representative Brazilian Oxisols were estimated from a cadmium adsorption experiment. Equilibrium constants were fitted to two surface complexation models: diffuse layer and constant capacitance. Intrinsic equilibrium constants were optimized by FITEQL and by hand calculation using Visual MINTEQ in sweep mode, and Excel spreadsheets. Data from both models were incorporated into Visual MINTEQ. Constants estimated by FITEQL and incorporated in Visual MINTEQ software failed to predict observed data accurately. However, FITEQL raw output data rendered good results when predicted values were directly compared with observed values, instead of incorporating the estimated constants into Visual MINTEQ. Intrinsic equilibrium constants optimized by hand calculation and incorporated in Visual MINTEQ reliably predicted Cd adsorption reactions on soil surfaces under changing environmental conditions.

  10. The optimization of As(V) removal over mesoporous alumina by using response surface methodology and adsorption mechanism.

    Science.gov (United States)

    Han, Caiyun; Pu, Hongping; Li, Hongying; Deng, Lian; Huang, Si; He, Sufang; Luo, Yongming

    2013-06-15

    The Box-Behnken Design of the response surface methodology was employed to optimize four most important adsorption parameters (initial arsenic concentration, pH, adsorption temperature and time) and to investigate the interactive effects of these variables on arsenic(V) adsorption capacity of mesoporous alumina (MA). According to analysis of variance (ANOVA) and response surface analyses, the experiment data were excellent fitted to the quadratic model, and the interactive influence of initial concentration and pH on As(V) adsorption capacity was highly significant. The predicted maximum adsorption capacity was about 39.06 mg/g, and the corresponding optimal parameters of adsorption process were listed as below: time 720 min, temperature 52.8 °C, initial pH 3.9 and initial concentration 130 mg/L. Based on the results of arsenate species definition, FT-IR and pH change, As(V) adsorption mechanisms were proposed as follows: (1) at pH 2.0, H₃AsO₄ and H₂AsO₄(-) were adsorbed via hydrogen bond and electrostatic interaction, respectively; (2) at pH 6.6, arsenic species (H₂AsO₄(-) and HAsO₄(2-)) were removed via adsorption and ion exchange, (3) at pH 10.0, HAsO₄(2-) was adsorbed by MA via ion exchange together with adsorption, while AsO₄(3-) was removed by ion exchange. Copyright © 2013 Elsevier B.V. All rights reserved.

  11. Accurate Description of Argon and Water Adsorption on Surfaces of Graphene-Based Carbon Allotropes

    Czech Academy of Sciences Publication Activity Database

    Kysilka, Jiří; Rubeš, Miroslav; Grajciar, L.; Nachtigall, P.; Bludský, Ota

    2011-01-01

    Roč. 115, č. 41 (2011), s. 11387-11393 ISSN 1089-5639 R&D Projects: GA ČR GAP208/10/0725; GA MŠk LC512 Institutional research plan: CEZ:AV0Z40550506 Keywords : density-functional-theory * coronene * potential-energy surfaces * basis-set convergence * physical adsorption * complexes Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.946, year: 2011

  12. Shear rheology of mixed protein adsorption layers vs their structure studied by surface force measurements.

    Science.gov (United States)

    Danov, Krassimir D; Kralchevsky, Peter A; Radulova, Gergana M; Basheva, Elka S; Stoyanov, Simeon D; Pelan, Eddie G

    2015-08-01

    The hydrophobins are proteins that form the most rigid adsorption layers at liquid interfaces in comparison with all other investigated proteins. The mixing of hydrophobin HFBII with other conventional proteins is expected to reduce the surface shear elasticity and viscosity, E(sh) and η(sh), proportional to the fraction of the conventional protein. However, the experiments show that the effect of mixing can be rather different depending on the nature of the additive. If the additive is a globular protein, like β-lactoglobulin and ovalbumin, the surface rigidity is preserved, and even enhanced. The experiments with separate foam films indicate that this is due to the formation of a bilayer structure at the air/water interface. The more hydrophobic HFBII forms the upper layer adjacent to the air phase, whereas the conventional globular protein forms the lower layer that faces the water phase. Thus, the elastic network formed by the adsorbed hydrophobin remains intact, and even reinforced by the adjacent layer of globular protein. In contrast, the addition of the disordered protein β-casein leads to softening of the HFBII adsorption layer. Similar (an even stronger) effect is produced by the nonionic surfactant Tween 20. This can be explained with the penetration of the hydrophobic tails of β-casein and Tween 20 between the HFBII molecules at the interface, which breaks the integrity of the hydrophobin interfacial elastic network. The analyzed experimental data for the surface shear rheology of various protein adsorption layers comply with a viscoelastic thixotropic model, which allows one to determine E(sh) and η(sh) from the measured storage and loss moduli, G' and G″. The results could contribute for quantitative characterization and deeper understanding of the factors that control the surface rigidity of protein adsorption layers with potential application for the creation of stable foams and emulsions with fine bubbles or droplets. Copyright © 2014

  13. Modeling of Bisphenol A (BPA) Removal from Aqueous Solutions by Adsorption Using Response Surface Methodology (RSM)

    OpenAIRE

    Mohammad Ali Zazouli; Farzaneh Veisi; Amir Veisi

    2016-01-01

    Bisphenol A (BPA) is an organic synthetic compound that has many applications in various industries and is known as persistent pollutant. The aim of this research was to evaluate the efficiency of bone ash and banana peel as adsorbents for BPA adsorption from aqueous solution by using Response Surface Methodology. The effects of some variables such as sorbent dose, detention time, solution pH, and BPA concentration on the sorption efficiency was examined. All analyses were carried out accordi...

  14. Modeling of Peptide Adsorption Interactions with a Poly(lactic acid) Surface

    OpenAIRE

    O'Brien, C. P.; Stuart, S. J.; Bruce, D. A.; Latour, R. A.

    2008-01-01

    The biocompatibility of implanted materials and devices is governed by the conformation, orientation, and composition of the layer of proteins that adsorb to the surface of the material immediately upon implantation, so an understanding of this adsorbed protein layer is essential to the rigorous and methodical design of implant materials. In this study, novel molecular dynamics techniques were employed in order to determine the change in free energy for the adsorption of a solvated nine-resid...

  15. Influence of surface oxides on the adsorption of naphthalene onto multiwalled carbon nanotubes.

    Science.gov (United States)

    Cho, Hyun-Hee; Smith, Billy A; Wnuk, Joshua D; Fairbrother, D Howard; Ball, William P

    2008-04-15

    As greater quantities of carbon nanotubes (CNTs) enter the environment, they will have an increasingly important effect on the availability and transport of aqueous contaminants. As a consequence of purification, deliberate surface functionalization, and/or exposure to oxidizing agents after release to the environment, CNTs often contain surface oxides (i.e., oxygen containing functional groups). To probe the influence that surface oxides exert on CNT sorption properties, multiwalled CNTs (MWCNTs) with varying oxygen concentrations were studied with respect to their sorption properties toward naphthalene. For pristine (as-received) MWCNTs, the sorption capacity was intermediate between that of a natural char and a granular activated carbon. Sorption data also reveal that a linear relationship exists between the oxygen content of MWCNTs and their maximum adsorption capacity for naphthalene, with 10% surface oxygen concentration resulting in a roughly 70% decrease in maximum adsorption capacity. The relative distribution of sorption energies, as characterized by Freundlich isotherm exponents was, however, unaffected by oxidation. Thus, the data are consistent with the idea that incorporated surface oxides create polar regions that reduce the surface area available for naphthalene sorption. These results highlight the important role of surface chemistry in controlling the environmental properties of CNTs.

  16. Optimizing adsorption of crystal violet dye from water by magnetic nanocomposite using response surface modeling approach.

    Science.gov (United States)

    Singh, Kunwar P; Gupta, Shikha; Singh, Arun K; Sinha, Sarita

    2011-02-28

    A magnetic nanocomposite was developed and characterized. Adsorption of crystal violet (CV) dye from water was studied using the nanocomposite. A four-factor central composite design (CCD) combined with response surface modeling (RSM) was employed for maximizing CV removal from aqueous solution by the nanocomposite based on 30 different experimental data obtained in a batch study. Four independent variables, viz. temperature (10-50°C), pH of solution (2-10), dye concentration (240-400 mg/l), and adsorbent dose (1-5 g/l) were transformed to coded values and a second-order quadratic model was built to predict the responses. The significance of independent variables and their interactions were tested by the analysis of variance (ANOVA) and t-test statistics. Adequacy of the model was tested by the correlation between experimental and predicted values of the response and enumeration of prediction errors. Optimization of the process variables for maximum adsorption of CV by nanocomposite was performed using the quadratic model. The Langmuir adsorption capacity of the adsorbent was determined as 81.70 mg/g. The model predicted maximum adsorption of 113.31 mg/g under the optimum conditions of variables (concentration 240 mg/l; temperature 50°C; pH 8.50; dose 1g/l), which was very close to the experimental value (111.80 mg/g) determined in batch experiment. Copyright © 2010 Elsevier B.V. All rights reserved.

  17. Significance of Graphitic Surfaces in Aurodicyanide Adsorption by Activated Carbon: Experimental and Computational Approach

    Science.gov (United States)

    Bhattacharyya, Dhiman; Depci, Tolga; Prisbrey, Keith; Miller, Jan D.

    Despite tremendous developments in industrial use of activated carbon (AC) for gold adsorption, specific aurodicyanide [Au(CN)2-] adsorption sites on the carbon have intrigued researchers. The graphitic structure of AC has been well established. Previously radiochemical and now, XPS and Raman characterizations have demonstrated higher site-specific gold adsorption on graphitic edges. Morphological characterizations have revealed the presence of slit-pores (5-10 Å). Molecular-dynamics-simulation (MDS) performed on graphitic slit-pores illustrated gold-cyanide ion-pair preferentially adsorbs on edges. Ab-initio simulations predicted lower barrier for electron sharing in pores with aurodic yanide, indicating tighter bonding than graphitic surface and was well supported by Gibbs energy calculations too. Interaction energy as function of the separation distance indicated tighter bonding of gold cyanide to the graphite edges than water molecules. Selective adsorption of aurodicyanide ion-pair seems to be related to low polarity of gold complex and its accommodation at graphitic edges.

  18. Adsorption of Ten Microcystin Congeners to Common Laboratory-Ware Is Solvent and Surface Dependent

    Directory of Open Access Journals (Sweden)

    Stefan Altaner

    2017-04-01

    Full Text Available Cyanobacteria can produce heptapetides called microcystins (MC which are harmful to humans due to their ability to inhibit cellular protein phosphatases. Quantitation of these toxins can be hampered by their adsorption to common laboratory-ware during sample processing and analysis. Because of their structural diversity (>100 congeners and different physico-chemical properties, they vary in their adsorption to surfaces. In this study, the adsorption of ten different MC congeners (encompassing non-arginated to doubly-arginated congeners to common laboratory-ware was assessed using different solvent combinations. Sample handling steps were mimicked with glass and polypropylene pipettes and vials with increasing methanol concentrations at two pH levels, before analysis by liquid chromatography-tandem mass spectrometry. We demonstrated that MC adsorb to polypropylene surfaces irrespective of pH. After eight successive pipet actions using polypropylene tips ca. 20% of the MC were lost to the surface material, which increased to 25%–40% when solutions were acidified. The observed loss was alleviated by changing the methanol (MeOH concentration in the final solvent. The required MeOH concentration varied depending on which congener was present. Microcystins only adsorbed to glass pipettes (loss up to 30% after eight pipet actions when in acidified aqueous solutions. The latter appeared largely dependent on the presence of ionizable groups, such as arginine residues.

  19. Time distribution of adsorption entropy of gases on heterogeneous surfaces by reversed-flow gas chromatography.

    Science.gov (United States)

    Katsanos, Nicholas A; Kapolos, John; Gavril, Dimitrios; Bakaoukas, Nicholas; Loukopoulos, Vassilios; Koliadima, Athanasia; Karaiskakis, George

    2006-09-15

    The reversed-flow gas chromatography (RF-GC) technique has been applied to measure the adsorption entropy over time, when gaseous pentane is adsorbed on the surface of two solids (gamma-alumina and a silica supported rhodium catalyst) at 393.15 and 413.15K, respectively. Utilizing experimental chromatographic data, this novel methodology also permits the simultaneous measurement of the local adsorption energy, epsilon, local equilibrium adsorbed concentration, c(s)(*), and local adsorption isotherm, theta(p, T, epsilon) in a time resolved way. In contrast with other inverse gas chromatographic methods, which determine the standard entropy at zero surface coverage, the present method operates over a wide range of surface coverage taking into account not only the adsorbate-adsorbent interaction, but also the adsorbate-adsorbate interaction. One of the most interesting observations of the present work is the fact that the interaction of n-pentane is spontaneous on the Rh/SiO(2) catalyst for a very short time interval compared to that on gamma-Al(2)O(3). This can explain the different kinetic behavior of each particular gas-solid system, and it can be attributed to the fact that large amounts of n-C(5)H(12) are present on the active sites of the Rh/SiO(2) catalyst compared to those on gamma-Al(2)O(3), as the local equilibrium adsorbed concentration values, c(s)(*), indicate.

  20. Fluoride removal by calcite: evidence for fluorite precipitation and surface adsorption.

    Science.gov (United States)

    Turner, Brett D; Binning, Philip; Stipp, S L S

    2005-12-15

    Fluoride contamination of groundwater, both anthropogenic and natural, is a major problem worldwide. In this study, fluoride removal by crushed limestone (99% pure calcite) was investigated by batch studies and surface-sensitive techniques from solutions with fluoride concentrations from 150 micromol/L (3 mg/L) to 110 mM (approximately 2100 mg/L). Surface-sensitive techniques, including atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS) as well as zeta potential measurements, confirm that, in addition to precipitation reactions, adsorption of fluoride also occurs. Results indicate that fluoride adsorption occurs immediately over the entire calcite surface with fluorite precipitating at step edges and kinks, where dissolved Ca2+ concentration is highest. The PHREEQ geochemical model was applied to the observed data and indicates that existing models, especially at low fluoride concentrations and high pH (>7.5) are not equipped to describe this complex system, largely because the PHREEQ model includes only precipitation reactions, whereas a combination of adsorption and precipitation parameters are required.

  1. Adsorption, desorption, and removal of polymeric nanomedicine on and from cellulose surfaces: effect of size.

    Science.gov (United States)

    Zhang, Ming; Akbulut, Mustafa

    2011-10-18

    The increased production and commercial use of nanoparticulate drug delivery systems combined with a lack of regulation to govern their disposal may result in their introduction to soils and ultimately into groundwater systems. To better understand how such particles interact with environmentally significant interfaces, we study the adsorption, desorption, and removal behavior of poly(ethylene glycol)-based nanoparticulate drug delivery systems on and from cellulose, which is the most common organic compound on Earth. It is shown that such an adsorption process is only partially reversible, and most of the adsorbate particles do not desorb from the cellulose surface even upon rinsing with a large amount of water. The rate constant of adsorption decreases with increasing particle size. Furthermore, hydrodynamic forces acting parallel to the surfaces are found to be of great importance in the context of particle dynamics near the cellulose surface, and ultimately responsible for the removal of some fraction of particles via rolling or sliding. As the particle size increases, the removal rates of the particles increase for a given hydrodynamical condition. © 2011 American Chemical Society

  2. Adsorption and dissociation of oxygen molecules on Si(111)-(7×7) surface

    International Nuclear Information System (INIS)

    Niu, Chun-Yao; Wang, Jian-Tao

    2013-01-01

    The adsorption and dissociation of O 2 molecules on Si(111)-(7×7) surface have been studied by first-principles calculations. Our results show that all the O 2 molecular species adsorbed on Si(111)-(7×7) surface are unstable and dissociate into atomic species with a small energy barrier about 0.1 eV. The single O 2 molecule adsorption tends to form an ins×2 or a new metastable ins×2* structure on the Si adatom sites and the further coming O 2 molecules adsorb on those structures to produce an ad-ins×3 structure. The ad-ins×3 structure is indeed highly stable and kinetically limited for diving into the subsurface layer to form the ins×3-tri structure by a large barrier of 1.3 eV. Unlike the previous views, we find that all the ad-ins, ins×2, and ad-ins×3 structures show bright images, while the ins×2*, ins×3, and ins×3-tri structures show dark images. The proposed oxidation pathways and simulated scanning tunneling microscope images account well for the experimental results and resolve the long-standing confusion and issue about the adsorption and reaction of O 2 molecules on Si(111) surface

  3. Adsorption and oxidation of oxalic acid on anatase TiO2 (001) surface: A density functional theory study.

    Science.gov (United States)

    Sun, Tao; Wang, Yun; Zhang, Haimin; Liu, Porun; Zhao, Huijun

    2015-09-15

    Anatase TiO2 (001) surfaces have attracted great interest for photo-degradation of organic species recently due to their high reactivity. In this work, adsorption properties and oxidation mechanisms of oxalic acid on the anatase TiO2 (001) surface have been theoretically investigated using the first-principles density functional theory. Various possible adsorption configurations are considered by diversifying the connectivity of carboxylic groups with the surface. It is found that the adsorption of oxalic acid on the anatase (001) surface prefer the dissociative states. A novel double-bidentate configuration has been found due to the structural match between oxalic acid and the (001) surface. More charge is transferred from the adsorbed oxalic acid to the surface with the double-bidentate configuration when comparing with other adsorption structures. Thus, there is a positive correlation relationship between the transferred charge amount and the interfacial bond numbers when oxalic acid adsorbs on the anatase TiO2 (001) surface. The adsorption energies with dispersion corrections have demonstrated that the van der Waals interactions play an important role in the adsorption, especially when adsorbates are close to the surface. Copyright © 2015 Elsevier Inc. All rights reserved.

  4. 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).

  5. Adsorption and correlations of selected aromatic compounds on a KOH-activated carbon with large surface area.

    Science.gov (United States)

    Yang, Kun; Zhu, Lianghong; Yang, Jingjing; Lin, Daohui

    2018-03-15

    Knowledge of adsorption mechanism and behavior of organic compounds by KOH-activated carbons (KOH-ACs) from wastewater is crucial to its environmental application in wastewater treatment as adsorbent. A superior adsorbent, KOH-activated carbon (KOH-AC), with large surface area (3143m 2 /g), total pore volume of 2.03cm 3 /g, relatively low micropore fraction of 53.2%, and having adsorption capacities of organic compounds up to >1000mg/g, was prepared. It is an adsorbent significantly different with common ACs because the molecular sieving effect, widely observed for common ACs, is insignificant for KOH-AC. This difference could be attributed to the lower micropore fraction of KOH-AC than common ACs. A negative relationship of adsorption capacity of 25 aromatic compounds (including phenols, anilines, nitrobenzenes and polycyclic aromatic hydrocarbons) with chemical melting point was observed, suggesting that adsorption is dependent on the packing efficiency and stacking density of molecules on KOH-AC. A linear solvation energy relationships of adsorption affinity of 25 aromatic compounds with solute solvatochromic parameters was also observed, that can be used to quantify the contributions of π-π interaction, hydrogen-bonding interaction and hydrophobic effect to adsorption on KOH-AC. Combined with the reported results of adsorption of organic compounds on carbon nanotubes and biochars, it was also observed that external surface area of adsorbents is controlling the packing efficiency and stacking density of molecules on adsorbents and thus affecting adsorption capacity of organic compounds. Moreover, micropore surface area and the fraction of micropores are the adsorbent properties mainly affecting adsorption affinity of organic compounds. The observations and the developed correlations in this study would be helpful in the application of KOH-AC as superior adsorbent by enhancing the understanding of adsorption mechanisms of organic compounds on KOH-AC and by

  6. Enhancing phosphate adsorption capacity of SDS-based magnetite by surface modification of citric acid

    Science.gov (United States)

    Yu, Zhigang; Zhang, Chang; Zheng, Zuhong; Hu, Liang; Li, Xuemei; Yang, Zhongzhu; Ma, Chi; Zeng, Guangming

    2017-05-01

    In this study, citric acid (CA) was employed as a low-molecule organic acid to influence the adsorption performance of phosphorus by as-obtained magnetite. The factors including initial phosphate concentrations, dosage of citric acid, pH value, ion strength, contact time and temperature were examined in detail. Results indicated that the dissolution of anion sodium dodecyl sulfate (SDS) covering on surface of magnetite, a slight decrease of Fe level and a superior structure of magnetite after CA modification occurred. The pH-dependence of phosphate adsorption was impeded and the surface potential of magnetite positively increased at pH > 5.0 when CA was added. Non-linear regression Langmuir-Freundlich model was fitted well in thermodynamics, and the opposite adsorption process as a function of temperatures with or without CA addition was due to the decrease of active energy and active mobility of phosphate ion. Finally, the declining adsorption efficiency with increasing cycles was observed while phosphate removal was approximately finished and had small change with 0.05 and 0.1 M of CA addition. Those improvements of removal efficiency of phosphorus by modified iron oxide were because of the removal of anionic SDS that increased the surface positive charge, and especially the dissolution of element Fe into solution to form precipitate with phosphorus ions. The enhanced stability of magnetite by CA also promoted the high removal efficiency of phosphorus. These implications of CA on phosphate removal can be extended to the field where phosphate pollution is notorious but urgent.

  7. Non-equilibrium Thermodynamic Dissolution Theory for Multi-Component Solid/Liquid Surfaces Involving Surface Adsorption and Radiolysis Kinetics

    International Nuclear Information System (INIS)

    Stout, R B

    2001-01-01

    A theoretical expression is developed for the dissolution rate response for multi-component radioactive materials that have surface adsorption kinetics and radiolysis kinetics when wetted by a multi-component aqueous solution. An application for this type of dissolution response is the performance evaluation of multi-component spent nuclear fuels (SNFs) for long term interim storage and for geological disposition. Typically, SNF compositions depend on initial composition, uranium oxide and metal alloys being most common, and on reactor burnup which results in a wide range of fission product and actinide concentrations that decay by alpha, beta, and gamma radiation. These compositional/burnup ranges of SNFs, whether placed in interim storage or emplaced in a geologic repository, will potentially be wetted by multi-component aqueous solutions, and these solutions may be further altered by radiolytic aqueous species due to three radiation fields. The solid states of the SNFs are not thermodynamically stable when wetted and will dissolve, with or without radiolysis. The following development of a dissolution theory is based on a non-equilibrium thermodynamic analysis of energy reactions and energy transport across a solid-liquid phase change discontinuity that propagates at a quasi-steady, dissolution velocity. The integral form of the energy balance equation is used for this spatial surface discontinuity analysis. The integral formulation contains internal energy functional of classical thermodynamics for both the SNFs' solid state and surface adsorption species, and the adjacent liquid state, which includes radiolytic chemical species. The steady-state concentrations of radiolytic chemical species are expressed by an approximate analysis of the decay radiation transport equation. For purposes of illustration a modified Temkin adsorption isotherm was assumed for the surface adsorption kinetics on an arbitrary, finite area of the solid-liquid dissolution interface. For

  8. Density functional theory formulation for fluid adsorption on correlated random surfaces

    Science.gov (United States)

    Aslyamov, Timur; Khlyupin, Aleksey

    2017-10-01

    We provide novel random surface density functional theory (RSDFT) formulation in the case of geometric heterogeneous surfaces of solid media which is essential for the description of thermodynamic properties of confined fluids. The major difference of our theoretical approach from the existing ones is a stochastic model of solid surfaces which takes into account the correlation properties of geometry. The main building blocks are effective fluid-solid potentials developed in the work of Khlyupin and Aslyamov [J. Stat. Phys. 167, 1519 (2017)] and geometry-based modification of the Helmholtz free energy for Lennard-Jones fluids. The efficiency of RSDFT is demonstrated in the calculation of argon and nitrogen low temperature adsorption on real heterogeneous surfaces (BP280 carbon black). These results are in good agreement with experimental data published in the literature. Also several models of corrugated materials are developed in the framework of RSDFT. Numerical analysis demonstrates a strong influence of surface roughness characteristics on adsorption isotherms. Thus the developed formalism provides a connection between a rigorous description of the stochastic surface and confined fluid thermodynamics.

  9. Adsorption effectiveness of β-lactoglobulin onto gold surface determined by quartz crystal microbalance.

    Science.gov (United States)

    Jachimska, B; Świątek, S; Loch, J I; Lewiński, K; Luxbacher, T

    2018-06-01

    Bovine β-lactoglobulin (LGB) is a transport protein that can bind to its structure hydrophobic bioactive molecules. Due to the lack of toxicity, high stability and pH-dependent molecular binding mechanism, lactoglobulin can be used as a carrier of sparingly soluble drugs. Dynamic light scattering has confirmed LGB's tendency to create oligomeric forms. The hydrodynamic diameter of LGB molecules varies from 4 nm to 6 nm in the pH range of 2-10 and ionic strength I = 0.001-0.15 M, which corresponds to the presence of mono or dimeric LGB forms. The LGB zeta potential varies from 26.5 mV to -33.3 mV for I = 0.01 M and from 13.3 mV to -16 mV for I = 0.15 M in the pH range of 2-10. The isoelectric point is at pH 4.8. As a result of strong surface charge compensation, the maximum effective ionization degree of the LGB molecule is 35% for ionic strength I = 0.01 M and 22% for I = 0.15 M. The effectiveness of adsorption is linked with the properties of the protein, as well as those of the adsorption surface. The functionalization of gold surfaces with β-lactoglobulin (LGB) was studied using a quartz crystal microbalance with energy dissipation monitoring (QCM-D). The effectiveness of LGB adsorption correlates strongly with a charge of gold surface and the zeta potential of the molecule. The greatest value of the adsorbed mass was observed in the pH range in which LGB has a positive zeta potential values, below pH 4.8. This observation shows that electrostatic interactions play a dominant role in LGB adsorption on gold surfaces. Based on the adsorbed mass, protein orientation on gold surfaces was determined. The preferential side-on orientation of LGB molecules observed in the adsorption layer is consistent with the direction of the molecule dipole momentum determined by molecular dynamics simulations of the protein (MD). The use of the QCM-D method also allowed us to determine the effectiveness of adsorption of LGB on gold

  10. Adsorption of methane and CO2 onto olivine surfaces in Martian dust conditions

    Science.gov (United States)

    Escamilla-Roa, Elizabeth; Martin-Torres, Javier; Sainz-Díaz, C. Ignacio

    2018-04-01

    Methane has been detected on all planets of our Solar System, and most of the larger moons, as well as in dwarf-planets like Pluto and Eric. The presence of this molecule in rocky planets is very interesting because its presence in the Earth's atmosphere is mainly related to biotic processes. Space instrumentation in orbiters around Mars has detected olivine on the Martian soil and dust. On the other hand the measurements of methane from the Curiosity rover report detection of background levels of atmospheric methane with abundance that is lower than model estimates of ultraviolet degradation of accreted interplanetary dust particles or carbonaceous chondrite material. Additionally, elevated levels of methane about this background have been observed implying that Mars is episodically producing methane from an additional unknown source, making the reasons of these temporal fluctuations of methane a hot topic in planetary research. The goal of this study is to investigate at atomic level the interactions during the adsorption processes of methane and other Mars atmospheric species (CO2, H2O) on forsterite surfaces, through electronic structure calculations based on the Density Functional Theory (DFT). We propose two models to simulate the interaction of adsorbates with the surface of dust mineral, such as binary mixtures (5CH4+5H2O/5CH4+5CO2) and as a semi-clathrate adsorption. We have obtained interesting results of the adsorption process in the mixture 5CH4+5CO2. Associative and dissociative adsorptions were observed for water and CO2 molecules. The methane molecules were only trapped and held by water or CO2 molecules. In the dipolar surface, the adsorption of CO2 molecules produced new species: one CO from a CO2 dissociation, and, two CO2 molecules chemisorbed to mineral surface forming in one case a carbonate group. Our results suggest that CO2 has a strong interaction with the mineral surface when methane is present. These results could be confirmed after the

  11. Adsorption of an endoglucanase from the hyperthermophilic Pyrococcus furiosus on hydrophobic (polystyrene) and hydrophilic (silica) surfaces increases protein heat stability

    NARCIS (Netherlands)

    Koutsopoulos, S.; van der Oost, J.; Norde, Willem

    2004-01-01

    The interaction of an endoglucanase from the hyperthermophilic microorganism Pyrococcus furiosus with two types of surfaces, that is, hydrophobic polystyrene and hydrophilic silica, was investigated, and the adsorption isotherms were determined. The adsorbed hyperthermostable enzyme did not undergo

  12. Proteolytic Degradation of Bovine Submaxillary Mucin (BSM) and Its Impact on Adsorption and Lubrication at a Hydrophobic Surface

    DEFF Research Database (Denmark)

    Madsen, Jan Busk; Svensson, Birte; Abou Hachem, Maher

    2015-01-01

    The effects of proteolytic digestion on bovinesubmaxillary mucin (BSM) were investigated in terms ofchanges in size, secondary structure, surface adsorption, and lubricating properties. Two proteases with distinctly different cleavage specificities, namely trypsin and pepsin, were employed. SDS...

  13. Thermodynamic Modeling of Surface Tension of Aqueous Electrolyte Solution by Competitive Adsorption Model

    Directory of Open Access Journals (Sweden)

    Mohamad Javad Kamali

    2015-01-01

    Full Text Available Thermodynamic modeling of surface tension of different electrolyte systems in presence of gas phase is studied. Using the solid-liquid equilibrium, Langmuir gas-solid adsorption, and ENRTL activity coefficient model, the surface tension of electrolyte solutions is calculated. The new model has two adjustable parameters which could be determined by fitting the experimental surface tension of binary aqueous electrolyte solution in single temperature. Then the values of surface tension for other temperatures in binary and ternary system of aqueous electrolyte solution are predicted. The average absolute deviations for calculation of surface tension of binary and mixed electrolyte systems by new model are 1.98 and 1.70%, respectively.

  14. Theoretical study of heavy metal Cd, Cu, Hg, and Ni(II) adsorption on the kaolinite(0 0 1) surface

    International Nuclear Information System (INIS)

    Zhao, Jian; He, Man-Chao

    2014-01-01

    Highlights: • We investigated the adsorption of Cd, Cu, Hg, and Ni(II) on kaolinite(0 0 1) surface. • The adsorption capabilities of the kaolinite for HM atoms were Ni > Cu > Cd > Hg(II). • The adsorption energy increases with the coverage for Cd, Cu, and Hg(II) atoms. • The adsorption energy decreases with the coverage for Ni(II) atoms. - Abstract: Heavy metal pollution is currently of great concern because it has been recognized as a potential threat to air, water, and soil. Adsorption was one of the most popular methods for the removal of heavy metal. The adsorption of heavy metal Cd, Cu, Hg, and Ni(II) atoms on the hydroxylated (0 0 1) surface of kaolinite was investigated using density-functional theory within the generalized gradient approximation and a supercell approach. The coverage dependence of the adsorption structures and energetics were systematically studied for a wide range of coverage Θ [from 0.11 to 1.0 monolayers (ML)] and adsorption sites. The most stable among all possible adsorption sites for Cd(II) atom was the two-fold bridge site followed by the one-fold top site, and the top site was the most favorite adsorption site for Cu and Ni(II) atoms, while the three-fold hollow site was the most stable adsorption site for Hg(II) atom followed by the two-fold bridge site. The adsorption energy increases with the coverage for Cd, Cu, and Hg(II) atoms, thus indicating the higher stability of surface adsorption and a tendency to the formation of adsorbate islands (clusters) with increasing the coverage. However, the adsorption energy of Ni(II) atoms decreases when increasing the coverage. The adsorption capabilities of the kaolinite clay for the heavy metal atoms were in the order of Ni > Cu > Cd > Hg(II). The other properties of the Cd, Cu, Hg, and Ni(II)/kaolinite(0 0 1) system including the different charge distribution, the lattice relaxation, and the electronic density of states were also studied and discussed in detail

  15. Heat-resistant organic molecular layer as a joint interface for metal reduction on plastics surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Sang, Jing [Department of Frontier Materials and Function Engineering, Graduate School of Engineering, Iwate University, 4-3-5 Ueda, Morioka 020-8551 (Japan); Aisawa, Sumio, E-mail: aisawa@iwate-u.ac.jp [Department of Frontier Materials and Function Engineering, Graduate School of Engineering, Iwate University, 4-3-5 Ueda, Morioka 020-8551 (Japan); Hirahara, Hidetoshi [Department of Frontier Materials and Function Engineering, Graduate School of Engineering, Iwate University, 4-3-5 Ueda, Morioka 020-8551 (Japan); Kudo, Takahiro [Sulfur Chemical Institute, 210, Collabo MIU, 4-3-5, Ueda, Morioka 020-0066 (Japan); Mori, Kunio [Department of Frontier Materials and Function Engineering, Graduate School of Engineering, Iwate University, 4-3-5 Ueda, Morioka 020-8551 (Japan); Sulfur Chemical Institute, 210, Collabo MIU, 4-3-5, Ueda, Morioka 020-0066 (Japan)

    2016-04-15

    Graphical abstract: - Highlights: • In situ adsorption behaviors of TES on PA6 surface were clarified by QCM. • Highest adsorption of TES on PA6 was obtained in pH 3 and 0.1 M solution. • Molecular layers of TES with uniform structures were prepared on PA6 surface. • TES layer improved PA6 local heat resistance from 150 °C to 230 °C. • TES molecular layer successfully reduced Ag ion to Ag{sup 0}. - Abstract: Heat-resistant organic molecular layers have been fabricated by triazine-based silane coupling agent for metal reduction on plastic surfaces using adsorption method. These molecular layers were used as an interfacial layer between polyamide (PA6) and metal solution to reduce Ag{sup +} ion to Ag{sup 0}. The interfacial behaviors of triazine molecular layer at the interfaces between PA6 and Ag solution were investigated using quartz crystal microbalance (QCM). The kinetics of molecular adsorption on PA6 was investigated by using triazine-based silane coupling agent solutions at different pH and concentration. X-ray photoelectron spectroscopy (XPS), atomic force microscope (AFM), and local nano thermal analysis were employed to characterize the surfaces and interfaces. The nano thermal analysis results show that molecular layers of triazine-based silane coupling agent greatly improved heat resistance of PA6 resin from 170 °C up to 230 °C. This research developed an in-depth insight for molecular behaviors of triazine-based silane coupling agent at the PA6 and Ag solution interfaces and should be of significant value for interfacial research between plastics and metal solution in plating industry.

  16. Antibody adsorption on the surface of water studied by neutron reflection.

    Science.gov (United States)

    Smith, Charles; Li, Zongyi; Holman, Robert; Pan, Fang; Campbell, Richard A; Campana, Mario; Li, Peixun; Webster, John R P; Bishop, Steven; Narwal, Rojaramani; Uddin, Shahid; van der Walle, Christopher F; Lu, Jian R

    2017-04-01

    Surface and interfacial adsorption of antibody molecules could cause structural unfolding and desorbed molecules could trigger solution aggregation, resulting in the compromise of physical stability. Although antibody adsorption is important and its relevance to many mechanistic processes has been proposed, few techniques can offer direct structural information about antibody adsorption under different conditions. The main aim of this study was to demonstrate the power of neutron reflection to unravel the amount and structural conformation of the adsorbed antibody layers at the air/water interface with and without surfactant, using a monoclonal antibody 'COE-3' as the model. By selecting isotopic contrasts from different ratios of H 2 O and D 2 O, the adsorbed amount, thickness and extent of the immersion of the antibody layer could be determined unambiguously. Upon mixing with the commonly-used non-ionic surfactant Polysorbate 80 (Tween 80), the surfactant in the mixed layer could be distinguished from antibody by using both hydrogenated and deuterated surfactants. Neutron reflection measurements from the co-adsorbed layers in null reflecting water revealed that, although the surfactant started to remove antibody from the surface at 1/100 critical micelle concentration (CMC) of the surfactant, complete removal was not achieved until above 1/10 CMC. The neutron study also revealed that antibody molecules retained their globular structure when either adsorbed by themselves or co-adsorbed with the surfactant under the conditions studied.

  17. Apatite deposition on titanium surfaces--the role of albumin adsorption.

    Science.gov (United States)

    Serro, A P; Fernandes, A C; Saramago, B; Lima, J; Barbosa, M A

    1997-07-01

    Titanium implant surfaces are known to spontaneously nucleate apatite layers when in contact with simulated body fluids. However, adsorption of proteins may influence the process of apatite layer formation. In this study the role of bovine serum albumin (BSA) adsorption in the process of apatite deposition on titanium substrates is investigated. Deposition of calcium phosphate was induced by immersing titanium substrates in a Hank's balanced salt solution (HBSS) for times ranging from 1 to 23 days. The resulting substrates were studied by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), wettability measurements and electrochemical impedance determinations. All these methods indicate the presence of a calcium phosphate layer. The same procedure was repeated substituting HBSS with a solution of BSA in HBSS. Although SEM, EDS and electrochemical impedance spectra do not reveal the presence of an apatite layer, XPS analysis strongly indicates that the inhibition of apatite formation by BSA is only partial. The competition between BSA adsorption and apatite deposition seems to lead to a mixed film where the protein co-exists with calcium phosphate. Wettability studies suggest that this surface film is heterogeneous and porous, similar to the thicker films formed in albumin-free HBSS.

  18. Adsorption behavior of some metal ions on hydrated amorphous titanium dioxide surface

    Directory of Open Access Journals (Sweden)

    Panit Sherdshoopongse

    2005-09-01

    Full Text Available Titanium dioxide was prepared from titanium tetrachloride and diluted ammonia solution at low temperature. The product obtained was characterized by XRD, EDXRF, TGA, DSC, and FT-IR techniques. It was found that the product was in the form of hydrated amorphous titanium dioxide, TiO2·1.6H2O (ha- TiO2. Ha-TiO2 exhibits high BET surface area at 449 m2/g. Adsorptions of metal ions onto the ha-TiO2 surface were investigated in the batch equilibrium experiments, using Mn(II, Fe(III, Cu(II, and Pb(II solutions. The concentrations of metal ions were determined by atomic absorption spectrometer. The adsorption isotherms of all metal ions were studied at pH 7. The adsorption of Mn(II, Cu(II, and Pb(II ions on ha-TiO2 conformed to the Langmuir isotherm while that of Fe(III fit equally well to both Langmuir and Freundlich isotherms.

  19. Kinetics and thermodynamics studies on the BMP-2 adsorption onto hydroxyapatite surface with different multi-morphological features

    Energy Technology Data Exchange (ETDEWEB)

    Lu, Zhiwei; Huangfu, Changxin; Wang, Yanying; Ge, Hongwei; Yao, Yao; Zou, Ping; Wang, Guangtu [College of Science, Sichuan Agricultural University, Ya' an 625014 (China); He, Hua [Institute of Animal Genetics and Breeding, Sichuan Agricultural University, Wenjiang, Sichuan 611130 (China); Rao, Hanbing, E-mail: rhbscu@gmail.com [College of Science, Sichuan Agricultural University, Ya' an 625014 (China)

    2015-07-01

    The effect of the surface topography on protein adsorption process is of great significance for designing hydroxyapatite (HA) ceramic material surfaces. In this work, three different topographies of HA materials HA-sheet, HA-rod, and HA-whisker were synthesized and testified by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), Brunauer–Emmett–Teller (BET) and a field emission scanning electron microscopy (FE-SEM). We have systematically investigated the adsorption kinetics and thermodynamics of bone morphogenetic proteins (BMP-2) on the three different topography surfaces of HA, respectively. The results showed that the maximum adsorption capacities of HA-sheet, HA-rod and HA-whisker were (219.96 ± 10.18), (247.13 ± 12.35), and (354.67 ± 17.73) μg · g{sup −1}, respectively. Kinetic parameters, rate constants, equilibrium adsorption capacities and related correlation coefficients, for each kinetic model were calculated as well as discussed. It demonstrated that the adsorption of BMP-2 onto HA could be described by the pseudo second-order equation. Adsorption of BMP-2 onto HA followed the Langmuir isotherm. It confirmed that compared with other samples HA-whisker had more adsorption sites for its high specific surface area which could provide more opportunities for protein molecules. The adsorption processes were endothermic (ΔH > 0), spontaneous (ΔG < 0) and entropy increasing (ΔS > 0). A possible adsorption mechanism has been proposed. In addition, the BMP-2 could be adsorbed to the surface which existed slight conformational changes by FT-IR. - Highlights: • A novel protein adsorption studies based on sheet, rod and whisker of HA were designed. • Kinetic and thermodynamics parameters of BMP-2 and HA bonded materials were evaluated. • Surface topographies of the HA effect BMP-2 adsorption • The HA-whisker material had excellent adsorption performance for protein enrichment. • The electrostatic interaction is responsible for the

  20. Kinetics and thermodynamics studies on the BMP-2 adsorption onto hydroxyapatite surface with different multi-morphological features

    International Nuclear Information System (INIS)

    Lu, Zhiwei; Huangfu, Changxin; Wang, Yanying; Ge, Hongwei; Yao, Yao; Zou, Ping; Wang, Guangtu; He, Hua; Rao, Hanbing

    2015-01-01

    The effect of the surface topography on protein adsorption process is of great significance for designing hydroxyapatite (HA) ceramic material surfaces. In this work, three different topographies of HA materials HA-sheet, HA-rod, and HA-whisker were synthesized and testified by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), Brunauer–Emmett–Teller (BET) and a field emission scanning electron microscopy (FE-SEM). We have systematically investigated the adsorption kinetics and thermodynamics of bone morphogenetic proteins (BMP-2) on the three different topography surfaces of HA, respectively. The results showed that the maximum adsorption capacities of HA-sheet, HA-rod and HA-whisker were (219.96 ± 10.18), (247.13 ± 12.35), and (354.67 ± 17.73) μg · g −1 , respectively. Kinetic parameters, rate constants, equilibrium adsorption capacities and related correlation coefficients, for each kinetic model were calculated as well as discussed. It demonstrated that the adsorption of BMP-2 onto HA could be described by the pseudo second-order equation. Adsorption of BMP-2 onto HA followed the Langmuir isotherm. It confirmed that compared with other samples HA-whisker had more adsorption sites for its high specific surface area which could provide more opportunities for protein molecules. The adsorption processes were endothermic (ΔH > 0), spontaneous (ΔG < 0) and entropy increasing (ΔS > 0). A possible adsorption mechanism has been proposed. In addition, the BMP-2 could be adsorbed to the surface which existed slight conformational changes by FT-IR. - Highlights: • A novel protein adsorption studies based on sheet, rod and whisker of HA were designed. • Kinetic and thermodynamics parameters of BMP-2 and HA bonded materials were evaluated. • Surface topographies of the HA effect BMP-2 adsorption • The HA-whisker material had excellent adsorption performance for protein enrichment. • The electrostatic interaction is responsible for the BMP-2

  1. A Comparison Study of Mechanism: Cu2+ Adsorption on Different Adsorbents and Their Surface-Modified Adsorbents

    OpenAIRE

    Yaqin Yu; Xinrui Li; Jiemin Cheng

    2016-01-01

    The isothermal adsorption kinetics of Cu2+ onto Carbon Black (CB) and Oxidized Carbon Black (OCB) were studied under different solution conditions and compared with bentonite and organic bentonite with the hexadecyltrimethylammonium bromide (HDTMA). The adsorption capacities followed the order of OCB > CB > organic bentonite > bentonite, which was consistent with the orders of their surface roughness and specific surface area. The Fourier transmission infrared (FT-IR) spectroscopy, scanning e...

  2. Controlled surface chemistry of diamond/β-SiC composite films for preferential protein adsorption.

    Science.gov (United States)

    Wang, Tao; Handschuh-Wang, Stephan; Yang, Yang; Zhuang, Hao; Schlemper, Christoph; Wesner, Daniel; Schönherr, Holger; Zhang, Wenjun; Jiang, Xin

    2014-02-04

    Diamond and SiC both process extraordinary biocompatible, electronic, and chemical properties. A combination of diamond and SiC may lead to highly stable materials, e.g., for implants or biosensors with excellent sensing properties. Here we report on the controllable surface chemistry of diamond/β-SiC composite films and its effect on protein adsorption. For systematic and high-throughput investigations, novel diamond/β-SiC composite films with gradient composition have been synthesized using the hot filament chemical vapor deposition (HFCVD) technique. As revealed by scanning electron microscopy (SEM), the diamond/β-SiC ratio of the composite films shows a continuous change from pure diamond to β-SiC over a length of ∼ 10 mm on the surface. X-ray photoelectron spectroscopy (XPS) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) was employed to unveil the surface termination of chemically oxidized and hydrogen treated surfaces. The surface chemistry of the composite films was found to depend on diamond/β-SiC ratio and the surface treatment. As observed by confocal fluorescence microscopy, albumin and fibrinogen were preferentially adsorbed from buffer: after surface oxidation, the proteins preferred to adsorb on diamond rather than on β-SiC, resulting in an increasing amount of proteins adsorbed to the gradient surfaces with increasing diamond/β-SiC ratio. By contrast, for hydrogen-treated surfaces, the proteins preferentially adsorbed on β-SiC, leading to a decreasing amount of albumin adsorbed on the gradient surfaces with increasing diamond/β-SiC ratio. The mechanism of preferential protein adsorption is discussed by considering the hydrogen bonding of the water self-association network to OH-terminated surfaces and the change of the polar surface energy component, which was determined according to the van Oss method. These results suggest that the diamond/β-SiC gradient film can be a promising material for biomedical applications which

  3. Physical adsorption: rare gas atoms on solid surfaces. Progress report, June 1, 1980-May 31, 1981

    Energy Technology Data Exchange (ETDEWEB)

    Cole, M.W.

    1981-02-01

    This project has entailed investigation of three areas during the current term: physical adsorption, photostimulated field emission (PSE), and phonon reflection at interfaces. The principal effort has been directed toward understanding interactions associated with physical adsorption and the associated properties of a film. The specific topics pursued include the detailed form of the long range interaction, the configuration space wave function, and the interaction between adatoms. Experimental confirmation of the last two come from neutron scattering and thermodynamic measurements, respectively. The research in PSE has yielded results which improve upon previous calculations. There is, however, a remaining disagreement with experiment; suggestions for the origin are discussed. The phonon reflection work is directed toward understanding the role of surface roughness, an important factor in increasing the energy transmission across interfaces. A formalism has been developed which will be evaluated in the future.

  4. Influence of Surface Charge/Potential of a Gold Electrode on the Adsorptive/Desorptive Behaviour of Fibrinogen

    International Nuclear Information System (INIS)

    Dargahi, Mahdi; Konkov, Evgeny; Omanovic, Sasha

    2015-01-01

    Highlights: • Adsorptive/desorptive behavior of fibrinogen (FG) on an electrochemically-polarized gold substrate is reported. • The adsorption affinity of FG (afFG) is constant on a negatively-charged substrate surface. • The afFG increases linearly with an increase in positive substrate surface charge. • The FG adsorption kinetics is strongly dependant on substrate surface charge. • The adsorbed FG layer can be desorbed by electrochemical evolution of hydrogen and oxygen. - Abstract: The effect of gold substrate surface charge (potential) on adsorptive/desorptive behaviour of fibrinogen (FG) was studied by employing differential capacitance (DC) and polarization modulated infrared reflection absorption spectroscopy (PM-IRRAS), in terms of FG adsorption thermodynamics, kinetics, and desorption kinetics. The gold substrate surface charge was modulated in-situ within the electrochemical double-layer region by means of electrochemical potentiostatic polarization in a FG-containing electrolyte, thus avoiding the interference of other physico-chemical properties of the gold surface on FG’s interfacial behaviour. The FG adsorption equilibrium was modeled using the Langmuir isotherm. Highly negative values of apparent Gibbs free energy of adsorption (ranging from from −52.1 ± 0.4 to −55.8 ± 0.8 kJ mol −1 , depending on the FG adsorption potential) indicated a highly spontaneous and strong adsorption of FG onto the gold surface. The apparent Gibbs free energy of adsorption was found to be independent of surface charge when the surface was negatively charged. However, when the gold surface was positively charged, the apparent Gibbs free energy of adsorption exhibited a pronounced linear relationship with the surface charge, shifting to more negative values with an increase in positive electrode potential. The adsorption kinetics of FG was also found to be dependent on gold surface charge in a similar manner to the apparent Gibbs free energy of adsorption

  5. Field evaluation of skid resistant surfaces : final report : part I.

    Science.gov (United States)

    1970-06-01

    This project was undertaken to establish a thin bituminous surface course that would possess good skid resistant qualities as well as, being both economical and durable. : This is the final report on the evaluation of skid resistant surfaces which wa...

  6. Surface field of forces and protein adsorption behavior of poly(hydroxyethylmethacrylate) films deposited from plasma.

    Science.gov (United States)

    Morra, M; Cassinelli, C

    1995-01-01

    Polymeric films were deposited from hydroxyethylmethacrylate (HEMA) plasma on non-woven poly(butyleneterephtalate) (PBT) filter materials. To test the effect of deposition conditions on surface properties, film were deposited using a constant monomer flow rate and a discharge power ranging from 40-100 W. Surface composition and surface energetics were evaluated by Electron Spectroscopy for Chemical Analysis (ESCA) and contact angle measurement, respectively. Albumin (Alb) and fibrinogen (Fg) adsorption from single protein solutions to the plasma-coated filters was measured. Results illustrate the marked effects of the deposition condition on the surface composition, the surface field of forces, and the protein adsorption behavior. The latter is modeled by the application of the Good-van Oss-Chaudhury theory of Lewis acid-base contribution to interfacial energetics. Materials endowed with widely different properties are obtained from the same monomer and different deposition conditions, a result that must be taken into account both in the production step, to assure constant quality, and in the development of specifically tailored materials.

  7. DFT study on the adsorption of diethyl, ethyl methyl, and dimethyl ethers on the surface of gallium doped graphene

    Energy Technology Data Exchange (ETDEWEB)

    Shokuhi Rad, Ali, E-mail: a.shokuhi@gmail.com [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Sani, Emad; Binaeian, Ehsan [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Peyravi, Majid; Jahanshahi, Mohsen [Faculty of Chemical Engineering, Babol University of Technology, Babol (Iran, Islamic Republic of)

    2017-04-15

    Highlights: • Adsorption of three ether molecules on the surface of Ga-doped graphene has been investigated. • High degree of adsorption for all analytes is found. • Ga-doped graphene shows p-type semiconductor property upon adsorption of ether molecules. - Abstract: In this study, we used density functional theory (DFT) to search on the adsorption properties of three important compounds of ether family; diethyl ether (DEE), ethyl methyl ether (EME), and dimethyl ether (DME) on the surface of Gallium doped graphene (GaG). We used three functionals (B3LYP, wb97xd, and MPW1PW91) for optimization and calculation of adsorption energy. After fully optimization, we scrutinized on the charge allocations on the adsorbed ethers as well as GaG (at the area of interaction) based on natural bond orbitals (NBO). Besides, we have calculated the amount of charge transfer upon adsorption of each analyte. We revel that GaG is an ideal adsorbent for chemisorption of all above-mentioned ethers. There is a little difference between the values of adsorption; −123.5, −120, and −118.3 kJ/mol (based on wb97xd) for DEE, EME, and DME, respectively. We found significant changes in the electronic structure of both adsorbent and adsorbate upon adsorption. Moreover, results of charge analyses confirm GaG is a p-type semiconductor.

  8. DFT study on the adsorption of diethyl, ethyl methyl, and dimethyl ethers on the surface of gallium doped graphene

    International Nuclear Information System (INIS)

    Shokuhi Rad, Ali; Sani, Emad; Binaeian, Ehsan; Peyravi, Majid; Jahanshahi, Mohsen

    2017-01-01

    Highlights: • Adsorption of three ether molecules on the surface of Ga-doped graphene has been investigated. • High degree of adsorption for all analytes is found. • Ga-doped graphene shows p-type semiconductor property upon adsorption of ether molecules. - Abstract: In this study, we used density functional theory (DFT) to search on the adsorption properties of three important compounds of ether family; diethyl ether (DEE), ethyl methyl ether (EME), and dimethyl ether (DME) on the surface of Gallium doped graphene (GaG). We used three functionals (B3LYP, wb97xd, and MPW1PW91) for optimization and calculation of adsorption energy. After fully optimization, we scrutinized on the charge allocations on the adsorbed ethers as well as GaG (at the area of interaction) based on natural bond orbitals (NBO). Besides, we have calculated the amount of charge transfer upon adsorption of each analyte. We revel that GaG is an ideal adsorbent for chemisorption of all above-mentioned ethers. There is a little difference between the values of adsorption; −123.5, −120, and −118.3 kJ/mol (based on wb97xd) for DEE, EME, and DME, respectively. We found significant changes in the electronic structure of both adsorbent and adsorbate upon adsorption. Moreover, results of charge analyses confirm GaG is a p-type semiconductor.

  9. Impact of hydrophilic and hydrophobic functionalization of flat TiO2/Ti surfaces on proteins adsorption

    Science.gov (United States)

    Fabre, Héloïse; Mercier, Dimitri; Galtayries, Anouk; Portet, David; Delorme, Nicolas; Bardeau, Jean-François

    2018-02-01

    Controlling adsorption of proteins onto medical devices is a key issue for implant-related infections. As self-assembled monolayers (SAMs) on titanium oxide represent a good model to study the surface-protein interactions, TiO2 surface properties were modified by grafting bisphosphonate molecules terminated with hydrophilic poly(ethylene glycol) groups and hydrophobic perfluoropolyether ones, respectively. Characterisation of the surface chemistry and surface topography of the modified surfaces was performed using XPS and atomic force microscopy (AFM). Quartz-crystal microbalance with dissipation (QCM-D) was used to determine the mass of adsorbed proteins as well as its kinetics. Poly(ethylene glycol)-terminated SAMs were the most effective surfaces to limit the adsorption of both BSA and fibrinogen in comparison to perfluorinated-terminated SAMs and non-modified TiO2 surfaces, as expected. The adsorption was not reversible in the case of BSA, while a partial reversibility was observed with Fg, most probably due to multilayers of proteins. The grafted surfaces adsorbed about the same quantity of proteins in terms of molecules per surface area, most probably in monolayer or island-like groups of adsorbed proteins. The adsorption on pristine TiO2 reveals a more important, non-specific adsorption of proteins.

  10. Atomistic simulation of the coupled adsorption and unfolding of protein GB1 on the polystyrenes nanoparticle surface

    Science.gov (United States)

    Xiao, HuiFang; Huang, Bin; Yao, Ge; Kang, WenBin; Gong, Sheng; Pan, Hai; Cao, Yi; Wang, Jun; Zhang, Jian; Wang, Wei

    2018-03-01

    Understanding the processes of protein adsorption/desorption on nanoparticles' surfaces is important for the development of new nanotechnology involving biomaterials; however, an atomistic resolution picture for these processes and for the simultaneous protein conformational change is missing. Here, we report the adsorption of protein GB1 on a polystyrene nanoparticle surface using atomistic molecular dynamic simulations. Enabled by metadynamics, we explored the relevant phase space and identified three protein states, each involving both the adsorbed and desorbed modes. We also studied the change of the secondary and tertiary structures of GB1 during adsorption and the dominant interactions between the protein and surface in different adsorption stages. The results we obtained from simulation were found to be more adequate and complete than the previous one. We believe the model presented in this paper, in comparison with the previous ones, is a better theoretical model to understand and explain the experimental results.

  11. Pd adsorption on Si(1 1 3) surface: STM and XPS study

    International Nuclear Information System (INIS)

    Hara, Shinsuke; Yoshimura, Masamichi; Ueda, Kazuyuki

    2008-01-01

    Pd-induced surface structures on Si(1 1 3) have been studied by scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS). In the initial process of the Pd adsorption below 0.10 ML, Pd silicide (Pd 2 Si) clusters are observed to form randomly on the surface. By increasing the Pd coverage to 0.10 ML, the clusters cover the entire surface, and an amorphous layer is formed. After annealing the Si(1 1 3)-Pd surface at 600 deg. C, various types of islands and chain protrusions appears. The agglomeration, coalescence and crystallization of these islands are observed by using high temperature (HT-) STM. It is also found by XPS that the islands correspond to Pd 2 Si structure. On the basis of these results, evolution of Pd-induced structures at high temperatures is in detail discussed

  12. 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

  13. The Role of Anion Adsorption in the Effect of Electrode Potential on Surface Plasmon Resonance Response.

    Science.gov (United States)

    Laurinavichyute, Veronika K; Nizamov, Shavkat; Mirsky, Vladimir M

    2017-06-20

    Surface plasmon resonance, being widely used in bioanalytics and biotechnology, is influenced by the electrical potential of the resonant gold layer. To evaluate the mechanism of this effect, we have studied it in solutions of various inorganic electrolytes. The magnitude of the effect decreases according to the series: KBr>KCl>KF>NaClO 4 . The data were treated by using different models of the interface. A quantitative description was obtained for the model, which takes into account the local dielectric function of gold being affected by the free electron charge, diffuse ionic layer near the gold/water interface, and specific adsorption of halides to the gold surface with partial charge transfer. Taking into account that most biological experiments are performed in chloride-containing solutions, detailed analysis of the model at these conditions was performed. The results indicate that the chloride adsorption is the main mechanism for the influence of potential on the surface plasmon resonance. The dependencies of surface concentration and residual charge of chloride on the applied potential were determined. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Adsorption of bovine serum albumin on amorphous carbon surfaces studied with dip pen nanolithography

    Science.gov (United States)

    Yadav, Pradeep K.; McKavanagh, Fiona; Maguire, Paul D.; Lemoine, Patrick

    2011-10-01

    This article reports the use of dip pen nanolithography (DPN) for the study of adsorption of bovine serum albumin (BSA) proteins on amorphous carbon surfaces; tetrahedral amorphous carbon (t-aC) and silicon doped hydrogenated amorphous carbon (a-C:H:Si). Contact angle study shows that the BSA proteins reduce the contact angle on both carbon materials. We also noticed that the drop volume dependence is consistent with a negative line tension, i.e. due to an attractive protein/surface interaction. The DPN technique was used to write short-spaced (100 nm) BSA line patterns on both samples. We found a line merging effect, stronger in the case of the a-C:H:Si material. We discuss possible contributions from tip blunting, scratching, cross-talk between lever torsion and bending and nano-shaving of the patterns. We conclude that the observed effect is caused in large measure by the diffusion of BSA proteins on the amorphous carbon surfaces. This interpretation of the result is consistent with the contact angle data and AFM force curve analysis indicating larger tip/surface adhesion and spreading for the a-C:H:Si material. We conclude by discussing the advantages and limitations of DPN lithography to study biomolecular adsorption in nanoscale wetting environments.

  15. Modeling of adsorption of toxic chromium on natural and surface modified lightweight expanded clay aggregate (LECA)

    Energy Technology Data Exchange (ETDEWEB)

    Kalhori, Ebrahim Mohammadi, E-mail: zarrabi62@yahoo.com [Department of Environmental Health Engineering, Faculty of Health, Alborz University of Medical Sciences, P.O. Box No: 31485/561, Alborz, Karaj (Iran, Islamic Republic of); Yetilmezsoy, Kaan, E-mail: yetilmez@yildiz.edu.tr [Department of Environmental Engineering, Faculty of Civil Engineering, Yildiz Technical University, 34220 Davutpasa, Esenler, Istanbul (Turkey); Uygur, Nihan, E-mail: uygur.n@gmail.com [Department of Environmental Engineering, Faculty of Engineering, Adiyaman University, 02040 Altinsehir, Adiyaman (Turkey); Zarrabi, Mansur, E-mail: mansor62@gmail.com [Department of Environmental Health Engineering, Faculty of Health, Alborz University of Medical Sciences, P.O. Box No: 31485/561, Alborz, Karaj (Iran, Islamic Republic of); Shmeis, Reham M. Abu, E-mail: r.abushmeis@yahoo.com [Department of Basic Pharmaceutical Sciences, Faculty of Pharmacy, Isra University, PO Box 140753, code 11814, Amman (Jordan)

    2013-12-15

    Lightweight Expanded Clay Aggregate (LECA) modified with an aqueous solution of magnesium chloride MgCl{sub 2} and hydrogen peroxide H{sub 2}O{sub 2} was used to remove Cr(VI) from aqueous solutions. The adsorption properties of the used adsorbents were investigated through batch studies, Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), X-ray Fluorescence Spectroscopy (XRF), and Fourier Transform Infrared (FTIR) spectroscopy. The effect created by magnesium chloride on the modification of the LECA surface was greater than that of hydrogen peroxide solution and showed a substantial increase in the specific surface area which has a value of 76.12 m{sup 2}/g for magnesium chloride modified LECA while the values of 53.72 m{sup 2}/g, and 11.53 m{sup 2}/g were found for hydrogen peroxide modified LECA and natural LECA, respectively. The extent of surface modification with enhanced porosity in modified LECA was apparent from the recorded SEM patterns. XRD and FTIR studies of themodified LECA surface did not show any structural distortion. The adsorption kinetics was found to follow the modified Freundlich kinetic model and the equilibrium data fitted the Sips and Dubinin-Radushkevich equations better than other models. Maximum sorption capacities were found to be 198.39, 218.29 and 236.24 mg/g for natural LECA, surface modified LECA with H{sub 2}O{sub 2} and surface modified LECA with MgCl{sub 2}, respectively. Adsorbents were found to have only a weak effect on conductivity and turbidity of aqueous solutions. Spent natural and surface modified LECA with MgCl{sub 2} was best regenerated with HCl solution, while LECA surface modified with H{sub 2}O{sub 2} was best regenerated with HNO{sub 3} concentrated solution. Thermal method showed a lower regeneration percentage for all spent adsorbents.

  16. In situ analysis of aqueous structure and adsorption at fluorocarbon, hydrocarbon and mineral surfaces

    Science.gov (United States)

    Hopkins, Adam Justin

    Altering and controlling the properties of solid surfaces in aqueous or other liquid phase environments has been a sought after objective for decades. With the discovery of chemisorbed self-assembled monolayers, this dream has become a reality. Oxide and metal surfaces can now be readily coated with an array of commercially available products to produce a desired fnctionality. The presence of these coatings on solid surfaces affects properties of the interfacial region by altering interfacial electrostatic fields, changing the structure of interfacial water molecules and altering the interactions of adsorbed species. This dissertation reports on in situ studies of adsorption at several solid/aqueous interfaces using vibrational sum-frequency spectroscopy, a surface specific technique. These studies are augmented by the use of atomic force microscopy and contact angle goniometry to characterize the prepared surfaces and their interactions with adsorbates. The studies investigate how changes in the surface structure and chemistry, as well as the bulk aqueous phase, affect interfacial structure. The studies within are primarily focused on the interactions of water with bare and functionalized fused silica and the relationship between the aqueous phase composition and the structure of fluorocarbon and hydrocarbon self-assembled monolayers. The variations in aqueous structure are then examined in detail using ionic strength controlled experiments to understand the direct interactions of water hydrophobically coated silica. This analysis is followed by an investigation of the competitive adsorption of methanol and water at fluorocarbon and hydrocarbon monolayers which show spectroscopic signatures of the interaction strength between fluorocarbons and hydrocarbons. Further studies are performed using butylammonium chloride to verify these spectroscopic signatures and reveal different molecular structures of adsorbed species at chemically different hydrophobic surfaces

  17. Fabrication of surface plasmon resonance sensor surface with control of the nonspecific adsorption and affinity for the detection of 2,4,6-trinitrotoluene using an antifouling copolymer

    Directory of Open Access Journals (Sweden)

    Rui eYatabe

    2014-04-01

    Full Text Available We fabricated a surface plasmon resonance (SPR sensor using a hydrophilic polymer for the highly sensitive detection of 2,4,6-trinitrotoluene (TNT. The hydrophilic polymer was made from mono-2-(methacryloyloxyethylsuccinate (MES and 2-hydroxyethylmethacrylate (HEMA by surface-initiated atom transfer radical polymerization (SI-ATRP. The detection of TNT was carried out by displacement assay with the SPR measurement. In displacement assay, the affinity between anti-TNT antibody and the sensor surface, affects to the sensitivity. In the SPR measurement, nonspecific adsorption should be controlled because SPR sensor cannot discriminate between specific and nonspecific adsorption. Therefore, the affinity and nonspecific adsorption were controlled by changing the ratio of HEMA to MES. A detection limit of 0.4 ng/ml (ppb for TNT was achieved using a sensor surface with the lowest affinity without nonspecific adsorption.

  18. Using surrogate modeling in the prediction of fibrinogen adsorption onto polymer surfaces.

    Science.gov (United States)

    Smith, Jack R; Knight, Doyle; Kohn, Joachim; Rasheed, Khaled; Weber, Norbert; Kholodovych, Vladyslav; Welsh, William J

    2004-01-01

    We present a Surrogate (semiempirical) Model for prediction of protein adsorption onto the surfaces of biodegradable polymers that have been designed for tissue engineering applications. The protein used in these studies, fibrinogen, is known to play a key role in blood clotting. Therefore, fibrinogen adsorption dictates the performance of implants exposed to blood. The Surrogate Model combines molecular modeling, machine learning and an Artificial Neural Network. This novel approach includes an accounting for experimental error using a Monte Carlo analysis. Briefly, measurements of human fibrinogen adsorption were obtained for 45 polymers. A total of 106 molecular descriptors were generated for each polymer. Of these, 102 descriptors were computed using the Molecular Operating Environment (MOE) software based upon the polymer chemical structures, two represented different monomer types, and two were measured experimentally. The Surrogate Model was developed in two stages. In the first stage, the three descriptors with the highest correlation to adsorption were determined by calculating the information gain of each descriptor. Here a Monte Carlo approach enabled a direct assessment of the effect of the experimental uncertainty on the results. The three highest-ranking descriptors, defined as those with the highest information gain for the sample set, were then selected as the input variables for the second stage, an Artificial Neural Network (ANN) to predict fibrinogen adsorption. The ANN was trained using one-half of the experimental data set (the training set) selected at random. The effect of experimental error on predictive capability was again explored using a Monte Carlo analysis. The accuracy of the ANN was assessed by comparison of the predicted values for fibrinogen adsorption with the experimental data for the remaining polymers (the validation set). The mean value of the Pearson correlation coefficient for the validation data sets was 0.54 +/- 0.12. The

  19. Optimizing adsorption of fluoride from water by modified banana peel dust using response surface modelling approach

    Science.gov (United States)

    Bhaumik, Ria; Mondal, Naba Kumar

    2016-06-01

    The present work highlighted the effective application of banana peel dust (BPD) for removal of fluoride (F-) from aqueous solution. The effects of operating parameters such as pH, initial concentration, adsorbent dose, contact time, agitation speed and temperature were analysed using response surface methodology. The significance of independent variables and their interactions were tested by the analysis of variance and t test statistics. Experimental results revealed that BPD has higher F- adsorption capacity (17.43, 26.31 and 39.5 mg/g). Fluoride adsorption kinetics followed pseudo-second-order model with high correlation of coefficient value (0.998). On the other hand, thermodynamic data suggest that adsorption is favoured at lower temperature, exothermic in nature and enthalpy driven. The adsorbents were characterised through scanning electron microscope, Fourier transform infrared spectroscopy and point of zero charges (pHZPC) ranges from pH 6.2-8.2. Finally, error analysis clearly demonstrates that all three adsorbents are well fitted with Langmuir isotherm compared to the other isotherm models. The reusable properties of the material support further development for commercial application purpose.

  20. Removal of fluoride from aqueous solution by adsorption on hydroxyapatite (HAp using response surface methodology

    Directory of Open Access Journals (Sweden)

    M. Mourabet

    2015-11-01

    Full Text Available A study on the adsorption of fluoride onto hydroxyapatite was conducted and the process parameters were optimized using Response Surface Methodology (RSM. Hydroxyapatite has been characterized by using different physicochemical methods. In order to determine the effects of process parameters namely temperature (20–40 °C, initial solution pH (4–11, adsorbent dose (0.1–0.3 g and initial fluoride concentration (10–20 mg L−1 on fluoride uptake from aqueous solution, a three-level, four-factor, Box–Behnken design has been employed. The second order mathematical model was developed by regression analysis of the experimental data obtained from 29 batch runs. The optimum pH, temperature, adsorbent dose and initial concentration were found by desirability function to be 4.16, 39.02 °C, 0.28 g and 20 mg L−1, respectively. Fluoride removal was 86.34% at the optimum combination of process parameters. Dynamic adsorption data were applied to pseudo-first-order and pseudo-second-order rate equations. The time data fitted well to pseudo second order kinetic model. According to the correlation coefficients, the adsorption of fluoride on the hydroxyapatite was correlated well with the Langmuir and Freundlich models.

  1. Ultrasensitive probing of the protein resistance of PEG surfaces by secondary ion mass spectrometry

    DEFF Research Database (Denmark)

    Kingshott, P.; McArthur, S.; Thissen, H.

    2002-01-01

    The highly sensitive surface analytical techniques X-ray photoelectron spectroscopy (XPS) and time-of-flight static secondary ion mass spectrometry (ToF-SIMS) were used to test the resistance of poly(ethylene glycol) (PEG) coatings towards adsorption of lysozyme (LYS) and fibronectin (FN). PEG...... temperature to maximise the graft density of the PEG chains. XPS showed that the grafted density of PEG chains was slightly higher on the allylamine surface. XPS detected no adsorption of either protein on either PEG coating. ToF-SIMS analysis, on the other hand, found, in the positive ion spectra, minute...... but statistically significant signals assignable to amino acid fragment ions from both proteins adsorbed to the lower density PEG coating and from LYS but not FN on the higher density PEG coating. Negative ion spectra contained relatively more intense protein fragment ion signals for the lower density PEG coating...

  2. Adsorptive removal of arsenic by novel iron/olivine composite: Insights into preparation and adsorption process by response surface methodology and artificial neural network.

    Science.gov (United States)

    Ghosal, Partha S; Kattil, Krishna V; Yadav, Manoj K; Gupta, Ashok K

    2018-03-01

    Olivine, a low-cost natural material, impregnated with iron is introduced in the adsorptive removal of arsenic. A wet impregnation method and subsequent calcination were employed for the preparation of iron/olivine composite. The major preparation process parameter, viz., iron loading and calcination temperature were optimized through the response surface methodology coupled with a factorial design. A significant variation of adsorption capacity of arsenic (measured as total arsenic), i.e., 63.15 to 310.85 mg/kg for arsenite [As(III) T ] and 76.46 to 329.72 mg/kg for arsenate [As(V) T ] was observed, which exhibited the significant effect of the preparation process parameters on the adsorption potential. The iron loading delineated the optima at central points, whereas a monotonous decreasing trend of adsorption capacity for both the As(III) T and As(V) T was observed with the increasing calcination temperature. The variation of adsorption capacity with the increased iron loading is more at lower calcination temperature showing the interactive effect between the factors. The adsorbent prepared at the optimized condition of iron loading and calcination temperature, i.e., 10% and 200 °C, effectively removed the As(III) T and As(V) T by more than 96 and 99%, respectively. The material characterization of the adsorbent showed the formation of the iron compound in the olivine and increase in specific surface area to the tune of 10 multifold compared to the base material, which is conducive to the enhancement of the adsorption capacity. An artificial neural network was applied for the multivariate optimization of the adsorption process from the experimental data of the univariate optimization study and the optimized model showed low values of error functions and high R 2 values of more than 0.99 for As(III) T and As(V) T . The adsorption isotherm and kinetics followed Langmuir model and pseudo second order model, respectively demonstrating the chemisorption in this

  3. Experimental and theoretical studies of the streaming flow due to the adsorption of particles at a liquid surface

    Science.gov (United States)

    Singh, P.; Musunuri, N.; Benouaguef, I.; Fischer, I.

    2017-11-01

    The particle image velocimetry (PIV) technique is used to study the streaming flow that is induced when particles are adsorbed at a liquid surface. The flow develops within a fraction of second after the adsorption of the particle. The fluid directly below the particle rises upward, and near the surface, it moves away from the particle. The flow causes powders sprinkled on a liquid surface to disperse on the surface. The flow strength, and the volume over which it extends, decreases with decreasing particle size. The streaming flow induced by the adsorption of two or more particles is a combination of the flows which they induce individually. Work supported by NSF.

  4. The Adsorption of Short Single-Stranded DNA Oligomers on Mineral Surfaces

    Science.gov (United States)

    Kopstein, M.; Sverjensky, D. A.; Hazen, R. M.; Cleaves, H. J.

    2009-12-01

    Previous studies have described feasible pathways for the synthesis of simple organic building blocks such as formaldehyde and hydrogen cyanide, and their reaction to form more complex biomolecules such as nucleotide bases, amino acids and sugars (Miller and Orgel 1974, Miller and Cleaves 2006). However, the polymerization of monomers into a useful genetic material remains problematic (Orgel 2004). Organic building blocks were unlikely to polymerize from very dilute aqueous solution in the primitive oceans. Mineral surface adsorption has been suggested as a possible mechanism for concentrating the necessary building blocks (Bernal 1951). This study focused on the adsorption behavior of single-stranded DNA homo-oligomers of adenine and thymine (including the monomers, dimers, tetramers, hexamers, octomers, and decamers) with five different mineral surfaces (pyrite, rutile, hematite, olivine and calcite). Adsorption was studied in 0.1 M pH 8.1 KHCO3 with0.05 M NaCl as background electrolyte. Solutions were mixed for 24 hours at room temperature, centrifuged and the supernatants analyzed by UV/visible spectrophotometry. Equilibrium solution concentrations were measured and used to determine the number of moles adsorbed per square meter. Langmuir isotherms were constructed using the experimental data. It was found that adenine-containing molecules tend to bind much more strongly than thymine-containing molecules. It was also found that the number of moles adsorbed at saturation tends to fall with increasing chain length, while adsorption affinity tends to rise. Oligomer length appears to affect adsorption more than the mineral type. These results may have implications for the primordial organization of the first nucleic acid molecules as the persistence of extra-cellular nucleic acids in the environment. References Bernal, J. D. (1951) The Physical Basis of Life (Routledge, London). Miller S.L. and Cleaves, H.J. (2006) Prebiotic chemistry on the primitive Earth. In

  5. Enhancing phosphate adsorption capacity of SDS-based magnetite by surface modification of citric acid

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Zhigang [College of Environmental Science and Engineering, Hunan University, Changsha 410082 (China); Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082 (China); Zhang, Chang, E-mail: zhangchang@hnu.edu.cn [College of Environmental Science and Engineering, Hunan University, Changsha 410082 (China); Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082 (China); Zheng, Zuhong [College of Life Science and Technology, Hubei Engineering University, Xiaogan 432000, Hubei Province (China); Hu, Liang; Li, Xuemei; Yang, Zhongzhu; Ma, Chi; Zeng, Guangming [College of Environmental Science and Engineering, Hunan University, Changsha 410082 (China); Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082 (China)

    2017-05-01

    Highlights: • Citric acid (CA) was used to modify the surface structures of SDS-based magnetite. • Dosage of CA, pH values, ion strength, isotherms and dynamics were analyzed. • High CA dissolved anionic SDS and Fe{sup n+} but increased the stability of magnetite. • 0.05 and 0.1 M CA-modified iron oxide removed about 100% phosphorus. • Precipitation of phosphate and Fe {sup n+} was the main removal mechanism. - Abstract: In this study, citric acid (CA) was employed as a low-molecule organic acid to influence the adsorption performance of phosphorus by as-obtained magnetite. The factors including initial phosphate concentrations, dosage of citric acid, pH value, ion strength, contact time and temperature were examined in detail. Results indicated that the dissolution of anion sodium dodecyl sulfate (SDS) covering on surface of magnetite, a slight decrease of Fe level and a superior structure of magnetite after CA modification occurred. The pH-dependence of phosphate adsorption was impeded and the surface potential of magnetite positively increased at pH > 5.0 when CA was added. Non-linear regression Langmuir-Freundlich model was fitted well in thermodynamics, and the opposite adsorption process as a function of temperatures with or without CA addition was due to the decrease of active energy and active mobility of phosphate ion. Finally, the declining adsorption efficiency with increasing cycles was observed while phosphate removal was approximately finished and had small change with 0.05 and 0.1 M of CA addition. Those improvements of removal efficiency of phosphorus by modified iron oxide were because of the removal of anionic SDS that increased the surface positive charge, and especially the dissolution of element Fe into solution to form precipitate with phosphorus ions. The enhanced stability of magnetite by CA also promoted the high removal efficiency of phosphorus. These implications of CA on phosphate removal can be extended to the field where

  6. Enhancing phosphate adsorption capacity of SDS-based magnetite by surface modification of citric acid

    International Nuclear Information System (INIS)

    Yu, Zhigang; Zhang, Chang; Zheng, Zuhong; Hu, Liang; Li, Xuemei; Yang, Zhongzhu; Ma, Chi; Zeng, Guangming

    2017-01-01

    Highlights: • Citric acid (CA) was used to modify the surface structures of SDS-based magnetite. • Dosage of CA, pH values, ion strength, isotherms and dynamics were analyzed. • High CA dissolved anionic SDS and Fe n+ but increased the stability of magnetite. • 0.05 and 0.1 M CA-modified iron oxide removed about 100% phosphorus. • Precipitation of phosphate and Fe n+ was the main removal mechanism. - Abstract: In this study, citric acid (CA) was employed as a low-molecule organic acid to influence the adsorption performance of phosphorus by as-obtained magnetite. The factors including initial phosphate concentrations, dosage of citric acid, pH value, ion strength, contact time and temperature were examined in detail. Results indicated that the dissolution of anion sodium dodecyl sulfate (SDS) covering on surface of magnetite, a slight decrease of Fe level and a superior structure of magnetite after CA modification occurred. The pH-dependence of phosphate adsorption was impeded and the surface potential of magnetite positively increased at pH > 5.0 when CA was added. Non-linear regression Langmuir-Freundlich model was fitted well in thermodynamics, and the opposite adsorption process as a function of temperatures with or without CA addition was due to the decrease of active energy and active mobility of phosphate ion. Finally, the declining adsorption efficiency with increasing cycles was observed while phosphate removal was approximately finished and had small change with 0.05 and 0.1 M of CA addition. Those improvements of removal efficiency of phosphorus by modified iron oxide were because of the removal of anionic SDS that increased the surface positive charge, and especially the dissolution of element Fe into solution to form precipitate with phosphorus ions. The enhanced stability of magnetite by CA also promoted the high removal efficiency of phosphorus. These implications of CA on phosphate removal can be extended to the field where phosphate

  7. Carbon key-properties for microcystin adsorption in drinking water treatment: structure or surface chemistry?

    OpenAIRE

    Júlio, Maria de Fátima de Jesus Leal

    2011-01-01

    Dissertação para Obtenção de Grau de Mestre em Engenharia Química e Bioquímica The carbon key-properties (structure and surface chemistry) for microcystin-LR (MC-LR) adsorption onto activated carbon were investigated. Waters with an inorganic background matrix approaching that of the soft natural water (2.5 mM ionic strength) were used. Also, model waters with controlled ionic make-up and NOM surrogate with similar size of MC-LR (tannic acid - TA) with MC-LR extracts were tested with activ...

  8. Memory Effects and Coverage Dependence of Surface Diffusion in a Model Adsorption System

    DEFF Research Database (Denmark)

    Vattulainen, Ilpo Tapio; Ying, S. C.; Ala-Nissila, T.

    1999-01-01

    We study the coverage dependence of surface diffusion coefficients for a strongly interacting adsorption system O/W(110) via Monte Carlo simulations of a lattice-gas model. In particular, we consider the nature and emergence of memory effects as contained in the corresponding correlation factors...... diffusion is found to decay following a power law after an initial transient period. This behavior persists until the hydrodynamic regime is reached, after which the memory effect decays exponentially. The time required to reach the hydrodynamical regime and the related exponential decay is strongly...

  9. Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments

    Science.gov (United States)

    Davis, J.A.; Meece, D.E.; Kohler, M.; Curtis, G.P.

    2004-01-01

    Uranium(VI) adsorption onto aquifer sediments was studied in batch experiments as a function of pH and U(VI) and dissolved carbonate concentrations in artificial groundwater solutions. The sediments were collected from an alluvial aquifer at a location upgradient of contamination from a former uranium mill operation at Naturita, Colorado (USA). The ranges of aqueous chemical conditions used in the U(VI) adsorption experiments (pH 6.9 to 7.9; U(VI) concentration 2.5 ?? 10-8 to 1 ?? 10-5 M; partial pressure of carbon dioxide gas 0.05 to 6.8%) were based on the spatial variation in chemical conditions observed in 1999-2000 in the Naturita alluvial aquifer. The major minerals in the sediments were quartz, feldspars, and calcite, with minor amounts of magnetite and clay minerals. Quartz grains commonly exhibited coatings that were greater than 10 nm in thickness and composed of an illite-smectite clay with occluded ferrihydrite and goethite nanoparticles. Chemical extractions of quartz grains removed from the sediments were used to estimate the masses of iron and aluminum present in the coatings. Various surface complexation modeling approaches were compared in terms of the ability to describe the U(VI) experimental data and the data requirements for model application to the sediments. Published models for U(VI) adsorption on reference minerals were applied to predict U(VI) adsorption based on assumptions about the sediment surface composition and physical properties (e.g., surface area and electrical double layer). Predictions from these models were highly variable, with results overpredicting or underpredicting the experimental data, depending on the assumptions used to apply the model. Although the models for reference minerals are supported by detailed experimental studies (and in ideal cases, surface spectroscopy), the results suggest that errors are caused in applying the models directly to the sediments by uncertain knowledge of: 1) the proportion and types of

  10. Kinetics, thermodynamics and surface heterogeneity assessment of uranium(VI) adsorption onto cation exchange resin derived from a lignocellulosic residue

    Energy Technology Data Exchange (ETDEWEB)

    Anirudhan, T.S., E-mail: tsani@rediffmail.com [Department of Chemistry, University of Kerala, Kariavattom, Trivandrum 695581 (India); Radhakrishnan, P.G. [Department of Chemistry, University of Kerala, Kariavattom, Trivandrum 695581 (India)

    2009-02-15

    A new cation exchange resin (PGTFS-COOH) having a carboxylate functional group at the chain end was prepared by grafting poly(hydroxyethylmethacrylate) onto tamarind fruit shell, TFS (a lignocellulosic residue) using potassium peroxydisulphate-sodium thiosulphate redox initiator, and in the presence of N,N'-methylenebisacrylamide (MBA) as a crosslinking agent, followed by functionalisation. The adsorbent was characterized with the help of FTIR, XRD, scanning electron micrographs (SEM), and potentiometric titrations. The kinetic and isotherm data, obtained at optimum pH value 6.0 at different temperatures could be fitted with pseudo-second-order equation and Sips isotherm model, respectively. An increase in temperature induces positive effect on the adsorption process. The calculated activation energy of adsorption (E{sub a}, 18.67 kJ/mol) indicates that U(VI) adsorption was largely due to diffusion-controlled process. The values of adsorption enthalpy, Gibbs free energy, and entropy were calculated using thermodynamic function relationships. The decrease in adsorption enthalpy with increasing U(VI) uploading on the adsorbent, reflects the surface energetic heterogeneity of the adsorbent. The isosteric heat of adsorption was quantitatively correlated with the fractional loading for the U(VI) ions adsorption onto PGTFS-COOH. The results showed that the PGTFS-COOH possessed heterogeneous surface with sorption sites having different activities.

  11. Kinetics, thermodynamics and surface heterogeneity assessment of uranium(VI) adsorption onto cation exchange resin derived from a lignocellulosic residue

    Science.gov (United States)

    Anirudhan, T. S.; Radhakrishnan, P. G.

    2009-02-01

    A new cation exchange resin (PGTFS-COOH) having a carboxylate functional group at the chain end was prepared by grafting poly(hydroxyethylmethacrylate) onto tamarind fruit shell, TFS (a lignocellulosic residue) using potassium peroxydisulphate-sodium thiosulphate redox initiator, and in the presence of N,N'-methylenebisacrylamide (MBA) as a crosslinking agent, followed by functionalisation. The adsorbent was characterized with the help of FTIR, XRD, scanning electron micrographs (SEM), and potentiometric titrations. The kinetic and isotherm data, obtained at optimum pH value 6.0 at different temperatures could be fitted with pseudo-second-order equation and Sips isotherm model, respectively. An increase in temperature induces positive effect on the adsorption process. The calculated activation energy of adsorption ( Ea, 18.67 kJ/mol) indicates that U(VI) adsorption was largely due to diffusion-controlled process. The values of adsorption enthalpy, Gibbs free energy, and entropy were calculated using thermodynamic function relationships. The decrease in adsorption enthalpy with increasing U(VI) uploading on the adsorbent, reflects the surface energetic heterogeneity of the adsorbent. The isosteric heat of adsorption was quantitatively correlated with the fractional loading for the U(VI) ions adsorption onto PGTFS-COOH. The results showed that the PGTFS-COOH possessed heterogeneous surface with sorption sites having different activities.

  12. Characterization of AZ91 magnesium alloy and organosilane adsorption on its surface

    International Nuclear Information System (INIS)

    Kim, J.; Wong, K.C.; Wong, P.C.; Kulinich, S.A.; Metson, J.B.; Mitchell, K.A.R.

    2007-01-01

    Oxide formation on a clean AZ91-Mg alloy surface has been characterized by X-ray photoelectron spectroscopy (XPS), while the chemical composition of a mirror-polished sample was assessed by scanning Auger microscopy (SAM) and scanning electron microscopy (SEM) at different microstructural regions, referred to as the grain boundary, matrix and particle regions. XPS and SAM confirmed that Mg and Al are always present in the surface regions probed, whereas bulk characterization with energy dispersive X-ray (EDX) analysis was necessary to detect the additional alloying elements, Mn and Zn. Coating by 1% solutions of BTSE, γ-GPS and γ-APS at their natural pH values gave etching of the surface Mg oxide. Adsorption occurs on the different regions, but the attachment is weak, especially because of the fragile nature of the underlying substrate. However, increasing the concentration of BTSE to 4% formed a thicker and denser coating with better prospects for substrate protection

  13. Copper(II) adsorption on the kaolinite(001) surface: Insights from first-principles calculations and molecular dynamics simulations

    Energy Technology Data Exchange (ETDEWEB)

    Kong, Xiang-Ping, E-mail: kxp2004@163.com; Wang, Juan, E-mail: juaner80@163.com

    2016-12-15

    Highlights: • Several issues about Cu(II) adsorption on the kaolinite (0 0 1) surface were solved. • Complexation of water molecules with Cu(II) was considered for adsorption complex. • Charge transfer and bonding mechanism of Cu–O{sub s} (surface oxygen) were explored. - Abstract: The adsorption behavior of Cu(II) on the basal hydroxylated kaolinite(001) surface in aqueous environment was investigated by first-principles calculations and molecular dynamics simulations. Structures of possible monodentate and bidentate inner-sphere adsorption complexes of Cu(II) were examined, and the charge transfer and bonding mechanism were analyzed. Combining the binding energy of complex, the radial distribution function of Cu(II) with oxygen and the extended X-ray absorption fine structure data, monodentate complex on site of surface oxygen with “upright” hydrogen and bidentate complex on site of two oxygens (one with “upright” hydrogen and one with “lying” hydrogen) of single Al center have been found to be the major adsorption species of Cu(II). Both adsorption species are four-coordinated with a square planar geometry. The distribution of surface hydroxyls with “lying” hydrogen around Cu(II) plays a key role in the structure and stability of adsorption complex. Upon the Mulliken population analysis and partial density of states, charge transfer occurs with Cu(II) accepting some electrons from both surface oxygens and aqua oxygens, and the bonding Cu 3d-O 2p state filling is primarily responsible for the strong covalent interaction of Cu(II) with surface oxygen.

  14. Modification of surface wettability through adsorption of partly fluorinated statistical and block polyelectrolytes from aqueous medium.

    Science.gov (United States)

    Nurmi, Leena; Kontturi, Katri; Houbenov, Nikolay; Laine, Janne; Ruokolainen, Janne; Seppälä, Jukka

    2010-10-05

    The wetting properties of electrostatically charged hydrophilic substrates were modified through adsorption of ultrathin layer of amphiphilic block or statistical polyelectrolyte from aqueous medium. The studied polymers were copolymers of 2-(dimethylamino)ethyl methacrylate (DMAEMA) and 2,2,2-trifluoroethyl methacrylate (TFEMA). They were adsorbed on mica from varying pH conditions, either as dissolved unimers or as kinetically trapped aqueous nanoparticles. The structures (by atomic force microscopy) and wetting properties (by dynamic contact angle measurements) of the obtained surface layers were determined. The majority of the surface layers consisted of polymeric nanoparticles with varying surface coverage. Annealing at 150 °C flattened and spread the particles on the surfaces. The surface wettability was found to be significantly influenced by the morphology and chemical composition of the obtained polymeric surface layer. The surfaces with the most homogeneous and smooth polymer layers exhibited the lowest contact angle hysteresis. The advancing/receding contact angles on the most hydrophilic copolymer layer on mica were 47°/cellulose fiber substrates and annealed at 120 °C, highly hydrophobic surfaces were obtained, with advancing contact angles around 160°.

  15. Adsorption of natural surfactants present in sea waters at surfaces of minerals: contact angle measurements

    Directory of Open Access Journals (Sweden)

    Katarzyna Boniewicz-Szmyt

    2009-09-01

    Full Text Available The wetting properties of solid mineral samples (by contact angles in original surfactant-containing sea water (Gulf of Gdańsk, Baltic were characterised under laboratory conditions on a large set (31 samples of well-classified stones of diverse hydrophobicity using the sessile drop (ADSA-P approach, captive bubble and inclined plate methods. An experimental relation between the static contact angle θeq and stone density ρ was obtained in the form θeq = Bρ + C, where B = 12.23 ± 0.92, C = - (19.17 ± 0.77, and r2 = 0.92. The histogram of θeq distribution for polished stone plates exhibited a multimodal feature indicating that the most abundant solid materials (hydrophilic in nature have contact angles θeq = 7.2, 10.7, 15.7 and 19.2º, which appear to be applicable to unspecified field stones as well. The contact angle, a pH-dependent quantity, appears to be a sensitive measure of stone grain size, e.g. granite. The captive bubble method gives reproducible results in studies of porous and highly hydrophilic surfaces such as stones and wood. The authors consider the adsorption of natural sea water surfactants on stone surfaces to be the process responsible for contact angle hysteresis. In the model, an equation was derived for determining the solid surface free energy from the liquid's surface tension γLV it also enabled the advancing θA and receding θR contact angles of this liquid to be calculated. Measurements of contact angle hysteresis Δθ (=θA - θR with surfactant-containing sea water and distilled water (reference on the same stone surfaces allowed the film pressure ΔΠ (1.22 to 8.80 mJ m-2, solid surface free energy ΔγS (-17.03 to -23.61 mJ m-2 and work done by spreading ΔWS (-1.23 to -11.52 mJ m-2 to be determined. The variability in these parameters is attributed to autophobing, an effect operative on a solid surface covered with an adsorptive layer of surfactants. The wetting behaviour of solid particles is of great

  16. Adsorption/desorption kinetics of Na atoms on reconstructed Si (111)-7 x 7 surface

    International Nuclear Information System (INIS)

    Chauhan, Amit Kumar Singh; Govind; Shivaprasad, S.M.

    2010-01-01

    Self-assembled nanostructures on a periodic template are fundamentally and technologically important as they put forward the possibility to fabricate and pattern micro/nano-electronics for sensors, ultra high-density memories and nanocatalysts. Alkali-metal (AM) nanostructure grown on a semiconductor surface has received considerable attention because of their simple hydrogen like electronic structure. However, little efforts have been made to understand the fundamental aspects of the growth mechanism of self-assembled nanostructures of AM on semiconductor surfaces. In this paper, we report organized investigation of kinetically controlled room-temperature (RT) adsorption/desorption of sodium (Na) metal atoms on clean reconstructed Si (111)-7 x 7 surface, by X-ray photoelectron spectroscopy (XPS). The RT uptake curve shows a layer-by-layer growth (Frank-vander Merve growth) mode of Na on Si (111)-7 x 7 surfaces and a shift is observed in the binding energy position of Na (1s) spectra. The thermal stability of the Na/Si (111) system was inspected by annealing the system to higher substrate temperatures. Within a temperature range from RT to 350 o C, the temperature induced mobility to the excess Na atoms sitting on top of the bilayer, allowing to arrange themselves. Na atoms desorbed over a wide temperature range of 370 o C, before depleting the Si (111) surface at temperature 720 o C. The acquired valence-band (VB) spectra during Na growth revealed the development of new electronic-states near the Fermi level and desorption leads the termination of these. For Na adsorption up to 2 monolayers, decrease in work function (-1.35 eV) was observed, whereas work function of the system monotonically increases with Na desorption from the Si surface as observed by other studies also. This kinetic and thermodynamic study of Na adsorbed Si (111)-7 x 7 system can be utilized in fabrication of sensors used in night vision devices.

  17. Experimental and theoretical investigations of mercury adsorption on hematite (1-102) surfaces

    Science.gov (United States)

    Jung, J.; Wilcox, J.; Jew, A. D.; Rupp, E. C.; Brown, G. E.

    2013-12-01

    Fly ash is a primary byproduct of the coal combustion process. The release of fly ash into the environment and its use in consumer products are public health concerns because of the presence of toxic trace metals and metalloids, such as mercury (Hg), selenium (Se), and arsenic (As), which may exist as components of fly ash, partition onto fly ash as it cools, or is lost to the environment through smoke stacks in a vapor phase. Therefore, it is important to understand the components of fly ash and their interaction with trace metals. In this study, calculations using density functional theory (DFT) were carried out in conjunction with experimental studies to investigate the interaction between Hg and hematite, an important mineral component of fly ash. Our experimental study, designed to simulate Hg sorption in a coal-fired power plant exhaust system, involved exposure of the fine fraction of bituminous coal fly ash (≤ 0.1 μm) to methane combustion flue gas, supplemented with SO2, NOx, HCl, and Hg in a packed-bed reactor. Sorption reaction products were characterized by synchrotron-based x-ray fluorescence mapping (s-XRF), x-ray diffraction (XRD), and extended x-ray absorption fine structure (EXAFS) spectroscopy. Preliminary s-XRF results showed that Hg in the sample is correlated with Fe, S, Cl, Br, and to a lesser extent with Se and As. From the XRD analysis, the dominant mineral phases detected were quartz, iron oxide (hematite), and various sulfate-bearing cements. Based on the experimental results, DFT studies were carried out to investigate the adsorption of Hg on hematite (α-Fe2O3) (1-102) surfaces. The two α-Fe2O3 (1-102) surfaces modeled consisted of two different surface terminations: (1) M2-clean, which corresponds to the oxygen terminated r-cut surface with the first layer of cations removed and no hydroxyl group and (2) M2-OH2-OH which has bihydroxylated top oxygen atoms and a second layer of hydroxylated oxygen atoms. These surface terminations

  18. Adsorption of polypropylene oxide-polyethylene oxide type surfactants at surfaces of pharmaceutical relevant materials: effect of surface energetics and surfactant structures.

    Science.gov (United States)

    Li, Jinjiang; Rudraraju, Sneha; Zheng, Songyan; Jaiswal, Archana

    2018-01-18

    Protein therapeutics are exposed to various surfaces during product development, where their adsorption possibly causes unfolding, denaturation, and aggregation. In this paper, we aim to characterize four types of typical surfaces used in the development of biologics: polycarbonate, polyethersulfone, borosilicate glass, and cellulose. Contact angles of these surfaces were measured using three probing liquids: water, formamide, and diidomethane, from which acid/base (AB) and Lifshitz-van der Waals (LW) interaction components were derived. To explore the interactions of surfactants of Pluronics/Poloxamers (PEO-PPO-PEO copolymers) with these surfaces, the adsorption of three Pluronics (F68, F127, and L44) at these surfaces was determined using a quartz crystal microbalance with dissipation technique (QCM-D). For hydrophobic surfaces without AB component (polycarbonate and polyethersulfone), these copolymers exhibited significant adsorption with a little dissipation at low concentrations. For hydrophilic surfaces with AB component (cellulose and borosilicate), the adsorption at low-surfactant concentration is low while dissipation is relatively high. Additionally, the chemical properties of Pluronics such as the ratio of PPO to PEO, along with the interaction of PPO with surfaces were observed to play a critical role in adsorption. Furthermore, the interfacial structure of the adsorbed layer was affected by both AB interaction and the presence of PEO block.

  19. 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

  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. In-situ NAP XPS studies of dissociative water adsorption on GaAs(100) surfaces

    Science.gov (United States)

    Ptasinska, Sylwia; Zhang, Xueqiang

    2014-03-01

    In current semiconductor-based technology it is important to design and fabricate new materials in order to achieve specific well-defined properties and functionalities. Before such systems can be applied they first need to be understood, refined and controlled. Therefore, a basic knowledge about molecule/semiconductor surface interfaces is essential. In the present work dissociative water adsorption on the GaAs(100) surface is monitored using X-ray Photoelectron Spectroscopy (XPS) performed in situ under near ambient conditions. Firstly, the crystal surface is exposed to water vapor pressures ranging from UHV to 0.5 kPa. At elevated pressures an increase of oxygenation and hydroxylation of Ga surface atoms has been observed in the Ga2p XPS spectra. Moreover, intense signals obtained from molecularly adsorbed water molecules or water molecules adsorbed via hydrogen bond to surface OH groups have been also observed in the O1s spectra. Finally, the crystal surface is annealed up to 700 K at water vapor pressure of 0.01 kPa, which leads to desorption of physisorbed water molecules and further increase of surface oxidation. The research described herein was supported by the Division of Chemical Sciences, Geosciences and Biosciences, Basic Energy Sciences, Office of Science, United States Department of Energy through grant number DE-FC02-04ER15533.

  2. DNA adsorption and desorption on mica surface studied by atomic force microscopy

    International Nuclear Information System (INIS)

    Sun Lanlan; Zhao Dongxu; Zhang Yue; Xu Fugang; Li Zhuang

    2011-01-01

    The adsorption of DNA molecules on mica surface and the following desorption of DNA molecules at ethanol-mica interface were studied using atomic force microscopy. By changing DNA concentration, different morphologies on mica surface have been observed. A very uniform and orderly monolayer of DNA molecules was constructed on the mica surface with a DNA concentration of 30 ng/μL. When the samples were immersed into ethanol for about 15 min, various desorption degree of DNA from mica (0-99%) was achieved. It was found that with the increase of DNA concentration, the desorption degree of DNA from the mica at ethanol-mica interface decreased. And when the uniform and orderly DNA monolayers were formed on the mica surface, almost no DNA molecule desorbed from the mica surface in this process. The results indicated that the uniform and orderly DNA monolayer is one of the most stable DNA structures formed on the mica surface. In addition, we have studied the structure change of DNA molecules after desorbed from the mica surface with atomic force microscopy, and found that the desorption might be ascribed to the ethanol-induced DNA condensation.

  3. Ions-induced nanostructuration: effect of specific ionic adsorption on hydrophobic polymer surfaces.

    Science.gov (United States)

    Siretanu, Igor; Chapel, Jean-Paul; Bastos-González, Delfi; Drummond, Carlos

    2013-06-06

    The effect of surface charges on the ionic distribution in close proximity to an interface has been extensively studied. On the contrary, the influence of ions (from dissolved salts) on deformable interfaces has been barely investigated. Ions can adsorb from aqueous solutions on hydrophobic surfaces, generating forces that can induce long-lasting deformation of glassy polymer films, a process called ion-induced polymer nanostructuration, IPN. We have found that this process is ion-specific; larger surface modifications are observed in the presence of water ions and hydrophobic and amphiphilic ions. Surface structuration is also observed in the presence of certain salts of lithium. We have used streaming potential and atomic force microscopy to study the effect of dissolved ions on the surface properties of polystyrene films, finding a good correlation between ionic adsorption and IPN. Our results also suggest that the presence of strongly hydrated lithium promotes the interaction of anions with polystyrene surfaces and more generally with hydrophobic polymer surfaces, triggering then the IPN process.

  4. Adsorption interaction of carrier-free thallium species with gold and quartz surfaces

    International Nuclear Information System (INIS)

    Serov, A.; Eichler, R.; Tuerler, A.; Wittwer, D.; Gaeggeler, H.W.; Bern Univ.; Dressler, R.; Piquet, D.; Voegele, A.

    2013-01-01

    The adsorption interactions of thallium and its compounds with gold and quartz surfaces were investigated. Carrier-free amounts of thallium were produced in nuclear fusion reactions of alpha particles with thick gold targets. The method chosen for the studies was gas thermochromatography and varying the redox potential of the carrier gases. It was observed that thallium is extremely sensitive to trace amounts of oxygen and water, and can even be oxidized by the hydroxyl groups located on the quartz surface. The experiments on a quartz surface with O 2 , He, H 2 gas in addition with water revealed the formation and deposition of only one thallium species - TlOH. The adsorption enthalpy was determined to be Δ H ads SiO 2 (TlOH) = -134 ± 5 kJ mol -1 . A series of experiments using gold as stationary surface and different carrier gases resulted in the detection of two thallium species - metallic Tl (H 2 as carrier gas) and TlOH (O 2 , O 2 + H 2 O and H 2 + H 2 O as pure carrier gas or carrier gas mixture) with Δ H Au ads (Tl) = -270 ± 10 kJ mol -1 and Δ H Au ads (TlOH) = -146 ± 3 kJ mol -1 . These data demonstrate a weak interaction of TlOH with both quartz and gold surfaces. The data represent important information for the design of future experiments with the heavier homologue of Tl in group 13 of the periodic table - element 113 (E113). (orig.)

  5. Uniform surface modification of diatomaceous earth with amorphous manganese oxide and its adsorption characteristics for lead ions

    Science.gov (United States)

    Li, Song; Li, Duanyang; Su, Fei; Ren, Yuping; Qin, Gaowu

    2014-10-01

    A novel method to produce composite sorbent material compromising porous diatomaceous earth (DE) and surface functionalized amorphous MnO2 is reported. Via a simple in situ redox reaction over the carbonized DE powders, a uniform layer of amorphous MnO2 was anchored onto the DE surface. The hybrid adsorbent was characterized by X-ray diffraction, scanning electron microscopy, and infrared spectroscopy. The batch method has been employed to investigate the effects of surface coating on adsorption performance of DE. According to the equilibrium studies, the adsorption capacity of DE for adsorbing lead ions after MnO2 modification increased more than six times. And the adsorption of Pb2+ on the MnO2 surface is based on ion-exchange mechanism. The developed strategy presents a novel opportunity to prepare composite adsorbent materials by integrating nanocrystals with porous matrix.

  6. First-principles study of the adsorption properties of atoms and molecules on UN2 (001) surface

    Science.gov (United States)

    Xu, Mengjuan; Liu, Guangdong; Ao, Bingyun; Chen, Piheng; Hu, Wangyu; Deng, Huiqiu

    2017-09-01

    Uranium nitrides are one kind of accident-tolerant fuels and have been paid more attention recently. With the first-principles Density-Functional Theory (DFT) calculations, the adsorptions properties of some typical atoms, molecules and radical (including O, H, H2, O2, H2O and OH) adsorbed on the UN2 (001) surface have been studied in the present work. The preferred sites and stable configurations for those adsorbates on the UN2 (001) surface have been obtained. It's found that O or H atom prefers to be adsorbed at the bridge site; O2 adsorption will dissociate into two O atoms and occupy the nearest neighbor bridge sites; the interaction between H2 molecule and the UN2 (001) surface is very weak; OH prefers to occupy the bridge site with its O-H bond vertical to the surface; the surface adsorption of H2O is non-dissociated and adsorption energies are dependent on the initial structures and adsorption modes.

  7. Effect of surface structure and wettability of DLC and N-DLC thin films on adsorption of glycine

    International Nuclear Information System (INIS)

    Ahmed, Mukhtar H.; Byrne, John A.

    2012-01-01

    Diamond-like carbon (DLC) is known to have excellent biocompatibility. Various samples of DLC and nitrogen-doped DLC thin films (N-DLC) were deposited onto silicon substrates using plasma-enhanced chemical vapour deposition (PECVD). Subsequently, the adsorption of amino acid glycine onto the surfaces of the thin films was investigated to elucidate the mechanisms involved in protein adhesion. The physicochemical characteristics of the surfaces, before and after adsorption of glycine, were investigated using Fourier transfer infrared (FTIR), Raman spectroscopy, spectroscopic ellipsometry (SE) and contact angle (θ). The Raman study highlighted decrease slightly in the ID/IG ratio at low levels of N (5.4 at.%), whilst increasing the nitrogen dopant level (>5.4 at.%) resulted in a increase of the ID/IG ratio, and the FTIR band at related to C=N. Following exposure to glycine solutions, the presence of Raman bands at 1727 cm -1 and 1200 cm -1 , and FTIR bands at 1735 cm -1 indicates that the adsorption of glycine onto the surfaces has taken place. These results which obtained from SE and surface free energy, show that low levels of nitrogen doping in DLC enhances the adsorption of the amino acid, while, increased doping led to a reduced adsorption, as compared to undoped DLC. Glycine is bound to the surface of the DLC films via both de-protonated carboxyl and protonated amino groups while, in the case of N-DLC gylcine was bound to the surface via anionic carboxyl groups and the amino group did not interact strongly with the surface. Doping of DLC may allow control of protein adsorption to the surface.

  8. Theoretical investigation on the adsorption and dissociation behaviors of TiCl4 on pyrolytic carbon surface

    Science.gov (United States)

    Jin, Na; Yang, Yanqing; Luo, Xian; Liu, Shuai; Li, Pengtao

    2018-01-01

    We present a theoretical investigation of the reaction mechanism of TiCl4 dissociation on pyrolytic carbon surface and discuss the influence of H atom on adsorption and dissociation behaviors of TiCl4 by using density functional theory. The adsorption behaviors of TiClx (x = 4-0) and the interactions between pre-adsorbed H atom and TiClx are studied by calculating adsorption energies Eads and interaction energies HTi, respectively. The pre-adsorbed H atom significantly facilitates the adsorption of TiClx on pyrolytic carbon surface. Specially, TiCl3 adsorption on pyrolytic carbon surface converts from an endothermic process into an exothermic process due to the present of pre-adsorbed H atom. The calculation results of HTi show that the interactions between pre-adsorbed H atom and TiClx are attractive. The dissociation of TiCl4 on pre-adsorbed H pyrolytic carbon surface is an exothermic process, and TiCl4 → TiCl3 is the limited step. The dissociation barriers of each step are less than 1.5 eV except for TiCl → Ti, which does not need to overcome any barriers, that is to say, once TiCl is adsorbed on pre-adsorbed H surface the reaction of TiCl → Ti spontaneously occurs. It thus can be concluded that the dissociation of TiCl4 on pyrolytic carbon surface is a favorable process as long as H2 molecular have decomposed into atomic H and adsorbed on pyrolytic carbon surface, and the intermediate species (TiCl3, TiCl2 and TiCl) play an important role on the titanium CVD deposition. We also study the adsorption behavior of H atom and the dissociation behavior of H2 molecular on pyrolytic carbon surface.

  9. An Approach to the Estimation of Adsorption Enthalpies of Polycyclic Aromatic Hydrocarbons on Particle Surfaces.

    Science.gov (United States)

    Cochran, Richard E; Kubátová, Alena; Kozliak, Evguenii I

    2016-08-04

    Current atmospheric models incorporate the values of vaporization enthalpies, ΔHvap, obtained for neat standards, thus disregarding the matrix effects on volatilization. To test the adequacy of this approximation, this study measured enthalpies of vaporization for five polycyclic aromatic hydrocarbons (PAHs) in the form of neat standards (ΔHvap) as well as adsorbed on the surface of silica, graphite, and graphene particles (ΔHvap(eff)), by using simultaneous thermogravimetry-differential scanning calorimetry (TGA-DSC). Measurement of the corresponding activation energy values, Ea(vap) and Ea vap(eff), by TGA using a derivative method was shown to be the most reliable and practical way to assess ΔHvap and ΔHvap(eff). Enthalpies of adsorption (ΔHads) were then calculated from the differences between Ea(vap) and Ea vap(eff), thus paving a way to modeling the solid-gas phase partitioning in atmospheric particulate matter (PM). The PAH adsorption on silica particle surfaces (representing n-π* interactions) resulted in negative values of ΔHads, indicating significant interactions. For graphite particles, positive ΔHads values were obtained; i.e., PAHs did not interact with the particle surface as strongly as observed for PM. PAHs on the surface of graphene particles evaporated in two stages, with the bulk of the mass loss occurring at temperatures lower than those with the neat standard, just as on graphite. Yet, unlike graphite, a small PAH fraction did not evaporate until higher temperatures compared to case of the neat standards and other particle surfaces (37.4-145.7 K), signifying negative, more PM-relevant values of ΔHads, apparently reflecting π-π* interactions and ranging between -7.6 and +32.6 kJ mol(-1), i.e., even larger than for silica, -3.3 to +8.3 kJ mol(-1). Thus, current atmospheric models may underestimate the partitioning of organic species in the particle phase unless matrix adsorption is taken into account.

  10. Adsorption of acetyl halide molecules on the surface of pristine and Al-doped graphene: Ab initio study

    Energy Technology Data Exchange (ETDEWEB)

    Rad, Ali Shokuhi, E-mail: a.shokuhi@gmail.com [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Kashani, Omid Razaghi [Department of Polymer Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of)

    2015-11-15

    Graphical abstract: - Highlights: • The adsorption of acetyl chloride and acetyl fluoride on Al-doped graphene were investigated. • The doped Al induces some changes in the electronic structure of graphene. • Notable orbital hybridizations are achieved upon adsorption. • Al-doped graphene can be used as a superior sensor for Acetyl halides. - Abstract: We have scrutinized the adsorption energy, electronic structure, natural bond analysis (NBO), density of state (DOS) and global indices for adsorption of acetyl chloride (AC) and acetyl fluoride (AF) on the surface of pristine graphene as well as Al-doped graphene. The adsorption energies have been calculated for the most stable configurations of the molecules on the surface of pristine and Al-doped graphene. According to the calculated parameters, there is very weak physical adsorption of AC and AF on pristine graphene while strong adsorption takes place in the case of Al-doped graphene. The charge transfer from adsorbed molecules to Al-doped graphene surface was confirmed by the natural bond orbital as well as the Mulliken population analysis while there is no charge transfer with pristine graphene. Additionally, the density of states results reveal that orbital hybridization takes place between above-mentioned molecules and Al-doped graphene sheet, whereas there is no hybridization between the molecules and the pristine graphene. Our calculated adsorption energies for the most stable position configurations of AC and AF on Al-doped graphene were −68.8 kJ mol{sup −1} (−52.6 kJ mol{sup −1} BSSE corrected energy) and −78.4 kJ mol{sup −1} (−64.3 kJ mol{sup −1} BSSE corrected energy) which are correspond to chemisorptions process respectively. These results point to the appropriateness of Al-doped graphene as a powerful adsorbent for practical applications.

  11. CO2 adsorption-assisted CH4 desorption on carbon models of coal surface: A DFT study

    Science.gov (United States)

    Xu, He; Chu, Wei; Huang, Xia; Sun, Wenjing; Jiang, Chengfa; Liu, Zhongqing

    2016-07-01

    Injection of CO2 into coal is known to improve the yields of coal-bed methane gas. However, the technology of CO2 injection-enhanced coal-bed methane (CO2-ECBM) recovery is still in its infancy with an unclear mechanism. Density functional theory (DFT) calculations were performed to elucidate the mechanism of CO2 adsorption-assisted CH4 desorption (AAD). To simulate coal surfaces, different six-ring aromatic clusters (2 × 2, 3 × 3, 4 × 4, 5 × 5, 6 × 6, and 7 × 7) were used as simplified graphene (Gr) carbon models. The adsorption and desorption of CH4 and/or CO2 on these carbon models were assessed. The results showed that a six-ring aromatic cluster model (4 × 4) can simulate the coal surface with limited approximation. The adsorption of CO2 onto these carbon models was more stable than that in the case of CH4. Further, the adsorption energies of single CH4 and CO2 in the more stable site were -15.58 and -18.16 kJ/mol, respectively. When two molecules (CO2 and CH4) interact with the surface, CO2 compels CH4 to adsorb onto the less stable site, with a resulting significant decrease in the adsorption energy of CH4 onto the surface of the carbon model with pre-adsorbed CO2. The Mulliken charges and electrostatic potentials of CH4 and CO2 adsorbed onto the surface of the carbon model were compared to determine their respective adsorption activities and changes. At the molecular level, our results showed that the adsorption of the injected CO2 promoted the desorption of CH4, the underlying mechanism of CO2-ECBM.

  12. Surface texture and specific adsorption sites of sol-gel synthesized anatase TiO{sub 2} nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Zaki, Mohamed I., E-mail: mizaki@link.net [Chemistry Department, Faculty of Science, Minia University, El-Minia, 61519 (Egypt); Mekhemer, Gamal A.H.; Fouad, Nasr E. [Chemistry Department, Faculty of Science, Minia University, El-Minia, 61519 (Egypt); Jagadale, Tushar C. [Physical and Materials Chemistry Division, National Chemical Laboratory, Dr. Homi Bhabha Road, Pashan, Pune 411008 (India); Ogale, Satishchandra B., E-mail: sb.ogale@ncl.res.in [Physical and Materials Chemistry Division, National Chemical Laboratory, Dr. Homi Bhabha Road, Pashan, Pune 411008 (India)

    2010-10-15

    The surface properties of sol-gel synthesized anatase titania (TiO{sub 2}) nanoparticles are probed by sorptiometry, infrared absorption spectroscopy, UV-vis diffuse reflectance spectroscopy and high resolution transmission electron microscopy. The results reveal strong correlations of the surface area, porosity, pyridine adsorption capacity and strength, and catalytic methylbutynol decomposition activity.

  13. HREELS study of the adsorption and evolution of diethylamine (DEA) on Si(1 0 0) surfaces

    International Nuclear Information System (INIS)

    Yeninas, S.; Brickman, A.; Craig, J.H.; Lozano, J.

    2008-01-01

    The adsorption of diethylamine (DEA) on Si(1 0 0) at 100 K was investigated using high-resolution electron energy loss spectroscopy (HREELS) and electron stimulated desorption (ESD). The thermal evolution of DEA on Si(1 0 0) was studied using temperature programmed desorption (TPD). Our results demonstrate DEA bonds datively to the Si(1 0 0) surface with no dissociation at 100 K. Thermal desorption of DEA takes place via a β-hydride elimination process leaving virtually no carbon behind. Electronic processing of DEA/Si(1 0 0) at 100 K results in desorption of ethyl groups; however, carbon and nitrogen are deposited on the surface as a result of electron irradiation. Thermal removal of carbon and nitrogen was not possible, indicating the formation of silicon carbide and silicon nitride

  14. Surface chemistry on bimetallic alloy surfaces: adsorption of anions and oxidation of CO on Pt3Sn(111).

    Science.gov (United States)

    Stamenković, Vojislav R; Arenz, Matthias; Lucas, Christopher A; Gallagher, Mark E; Ross, Philip N; Marković, Nenad M

    2003-03-05

    The microscopic structure of the Pt(3)Sn(111) surface in an electrochemical environment has been studied by a combination of ex situ low-energy electron diffraction (LEED), Auger electron spectroscopy (AES), and low-energy ion scattering (LEIS) and in situ surface X-ray scattering (SXS) and Fourier transform infrared (FTIR) spectroscopy. In ultrahigh vacuum (UHV) the clean-annealed surface produces a p(2 x 2) LEED pattern consistent with the surface composition, determined by LEIS, of 25 at. % Sn. SXS results show that the p(2 x 2) structure can be "transferred" from UHV into 0.5 M H(2)SO(4) and that the surface structure remains stable from 0.05 to 0.8 V. At 0.05 V the expansion of Pt surface atoms, ca. +2% from the bulk lattice spacing, is induced by adsorption of underpotential-deposited (UPD) hydrogen. At 0.5 V, where Pt atoms are covered by (bi)sulfate anions, the topmost layer is contracted relative to 0.05 V, although Sn atoms expand significantly, ca. 8.5%. The p(2 x 2) structure is stable even in solutions containing CO. In contrast to the Pt(111)-CO system, no ordered structures of CO are formed on the Pt(3)Sn(111) surface and the topmost layer expands relatively little (ca. 1.5%) from the bulk lattice spacing upon the adsorption of CO. The binding site geometry of CO on Pt(3)Sn(111) is determined by FTIR. In contrast to the near invariant band shape of a-top CO on Pt(111), changes in band morphology (splitting of the band) and vibrational properties (increase in the frequency mode) are clearly visible on the Pt(3)Sn(111) surface. To explain the line shape of the CO bands, we suggest that in addition to alloying effects other factors, such as intermolecular repulsion between coadsorbed CO and OH species, are controlling segregation of CO into cluster domains where the local CO coverage is different from the coverage expected for the CO-CO interaction on an unmodified Pt(111) surface.

  15. Competition between surface adsorption and folding of fibril-forming polypeptides.

    Science.gov (United States)

    Ni, Ran; Kleijn, J Mieke; Abeln, Sanne; Cohen Stuart, Martien A; Bolhuis, Peter G

    2015-02-01

    Self-assembly of polypeptides into fibrillar structures can be initiated by planar surfaces that interact favorably with certain residues. Using a coarse-grained model, we systematically studied the folding and adsorption behavior of a β-roll forming polypeptide. We find that there are two different folding pathways depending on the temperature: (i) at low temperature, the polypeptide folds in solution into a β-roll before adsorbing onto the attractive surface; (ii) at higher temperature, the polypeptide first adsorbs in a disordered state and folds while on the surface. The folding temperature increases with increasing attraction as the folded β-roll is stabilized by the surface. Surprisingly, further increasing the attraction lowers the folding temperature again, as strong attraction also stabilizes the adsorbed disordered state, which competes with folding of the polypeptide. Our results suggest that to enhance the folding, one should use a weakly attractive surface. They also explain the recent experimental observation of the nonmonotonic effect of charge on the fibril formation on an oppositely charged surface [C. Charbonneau et al., ACS Nano 8, 2328 (2014)].

  16. Competition between surface adsorption and folding of fibril-forming polypeptides

    Science.gov (United States)

    Ni, Ran; Kleijn, J. Mieke; Abeln, Sanne; Cohen Stuart, Martien A.; Bolhuis, Peter G.

    2015-02-01

    Self-assembly of polypeptides into fibrillar structures can be initiated by planar surfaces that interact favorably with certain residues. Using a coarse-grained model, we systematically studied the folding and adsorption behavior of a β -roll forming polypeptide. We find that there are two different folding pathways depending on the temperature: (i) at low temperature, the polypeptide folds in solution into a β -roll before adsorbing onto the attractive surface; (ii) at higher temperature, the polypeptide first adsorbs in a disordered state and folds while on the surface. The folding temperature increases with increasing attraction as the folded β -roll is stabilized by the surface. Surprisingly, further increasing the attraction lowers the folding temperature again, as strong attraction also stabilizes the adsorbed disordered state, which competes with folding of the polypeptide. Our results suggest that to enhance the folding, one should use a weakly attractive surface. They also explain the recent experimental observation of the nonmonotonic effect of charge on the fibril formation on an oppositely charged surface [C. Charbonneau et al., ACS Nano 8, 2328 (2014), 10.1021/nn405799t].

  17. Modeling of thorium (IV) ions adsorption onto a novel adsorbent material silicon dioxide nano-balls using response surface methodology.

    Science.gov (United States)

    Kaynar, Ümit H; Şabikoğlu, Israfil; Kaynar, Sermin Çam; Eral, Meral

    2016-09-01

    The silicon dioxide nano-balls (nano-SiO2) were prepared for the adsorption of thorium (IV) ions from aqueous solution. The synthesized silicon dioxide nano-balls were characterized by Scanning Electron Microscopy/Energy Dispersive X-ray, X-ray Diffraction, Fourier Transform Infrared and BET surface area measurement spectroscopy. The effects of pH, concentration, temperature and the solid-liquid ratio on the adsorption of thorium by nano-balls were optimized using central composite design of response surface methodology. The interaction between four variables was studied and modelled. Furthermore, the statistical analysis of the results was done. Analysis of variance revealed that all of the single effects found statistically significant on the sorption of Th(IV). Probability F-values (F=4.64-14) and correlation coefficients (R(2)=0.99 for Th(IV)) indicate that model fit the experimental data well. The ability of this material to remove Th(IV) from aqueous solution was characterized by Langmuir, Freunlinch and Temkin adsorption isotherms. The adsorption capacity of thorium (IV) achieved 188.2mgg(-1). Thermodynamic parameters were determined and discussed. The batch adsorption condition with respect to interfering ions was tested. The results indicated that silicon dioxide nano-balls were suitable as sorbent material for adsorption and recovery of Th(IV) ions from aqueous solutions. Copyright © 2016 Elsevier Ltd. All rights reserved.

  18. Platelet adhesion and plasma protein adsorption control of collagen surfaces by He+ ion implantation

    International Nuclear Information System (INIS)

    Kurotobi, K.; Suzuki, Y.; Nakajima, H.; Suzuki, H.; Iwaki, M.

    2003-01-01

    He + ion implanted collagen-coated tubes with a fluence of 1 x 10 14 ions/cm 2 were exhibited antithrombogenicity. To investigate the mechanisms of antithrombogenicity of these samples, plasma protein adsorption assay and platelet adhesion experiments were performed. The adsorption of fibrinogen (Fg) and von Willebrand factor (vWf) was minimum on the He + ion implanted collagen with a fluence of 1 x 10 14 ions/cm 2 . Platelet adhesion (using platelet rich plasma) was inhibited on the He + ion implanted collagen with a fluence of 1 x 10 14 ions/cm 2 and was accelerated on the untreated collagen and ion implanted collagen with fluences of 1 x 10 13 , 1 x 10 15 and 1 x 10 16 ions/cm 2 . Platelet activation with washed platelets was observed on untreated collagen and He + ion implanted collagen with a fluence of 1 x 10 14 ions/cm 2 and was inhibited with fluences of 1 x 10 13 , 1 x 10 15 and 1 x 10 16 ions/cm 2 . Generally, platelets can react with a specific ligand inside the collagen (GFOGER sequence). The results of platelets adhesion experiments using washed platelets indicated that there were no ligands such as GFOGER on the He + ion implanted collagen over a fluence of 1 x 10 13 ions/cm 2 . On the 1 x 10 14 ions/cm 2 implanted collagen, no platelet activation was observed due to the influence of plasma proteins. >From the above, it is concluded that the decrease of adsorbed Fg and vWf caused the antithrombogenicity of He + ion implanted collagen with a fluence of 1 x 10 14 ions/cm 2 and that plasma protein adsorption took an important role repairing the graft surface

  19. Surface functionalization of zirconium dioxide nano-adsorbents with 3-aminopropyl triethoxysilane and promoted adsorption activity for bovine serum albumin

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Gen; Wu, Chaochao [Department of Chemistry, College of Sciences, Northeastern University, Shenyang 110819 (China); Zhang, Xia, E-mail: xzhang@mail.neu.edu.cn [Department of Chemistry, College of Sciences, Northeastern University, Shenyang 110819 (China); Liu, Yufeng, E-mail: liuyufeng@bjmu.edu.cn [College of Pharmacy, Liaoning University, Shenyang 110036 (China); Meng, Hao; Xu, Junli; Han, Yide; Xu, Xinxin; Xu, Yan [Department of Chemistry, College of Sciences, Northeastern University, Shenyang 110819 (China)

    2016-06-15

    Surface functionalization of zirconium dioxide (ZrO{sub 2}) nano-adsorbents was carried out by using 3-aminopropyl triethoxysilane (APTES) as the modifier. The addition amount of APTES was varied to determine the optimum modification extent, and the bulk ZrO{sub 2} microparticles were also modified by APTES for comparison. Some means, such as TEM, XRD, FT-IR, XPS and TG-DSC were used to character these ZrO{sub 2} particles. The results showed that the APTES molecules were chemically immobilized on the surface of ZrO{sub 2} nanoparticles via Zr−O−Si bonds, and the nano-ZrO{sub 2} samples showed larger special surface area. In the adsorption of bovine serum albumin (BSA), nano-ZrO{sub 2} samples exhibited enhanced adsorption activity, and APTES modified nano-ZrO{sub 2} with proper APTES content presented the best adsorption property. Under the same adsorption conditions, the equilibrium adsorption capacity of BSA on APTES-ZrO{sub 2}-2 was almost 2.3 times as that on pristine nano-ZrO{sub 2} and 3.0 times as on bulk ZrO{sub 2} microparticles. The increased adsorption capacity of APTES-ZrO{sub 2} nano-adsorbents can be attributed to the chemical interaction between amino and carboxyl groups at APTES-ZrO{sub 2}/BSA interface. The pH-dependent experiments showed that the optimum pH value for the adsorption and desorption was 5.0 and 9.0, respectively, which suggested that the adsorption and release of BSA could be controlled simply by adjusting the solution pH condition. - Highlights: • APTES chemically immobilized on ZrO{sub 2} nanoparticles via Zr−O−Si bond. • Enhanced adsorption capacity of BSA was observed on APTES-ZrO{sub 2}. • Chemical adsorption character of BSA on APTES-ZrO{sub 2}. • Adsorption/release of BSA on APTES-ZrO{sub 2} accomplished by adjusting pH value.

  20. Adsorption of Ni, Pd, Pt, Cu, Ag and Au on the Fe3O4(111) surface

    Science.gov (United States)

    Yu, Xiaohu; Tian, Xinxin; Wang, Shengguang

    2014-10-01

    The interaction of Group 10 and 11 transition metals with the magnetite (111) surface has been investigated using the GGA + U density functional theory and periodic slab surface models. It was found that these transition metals adsorb stronger on an oxygen-terminated magnetite (111) surface than on an iron-terminated surface. On an oxygen-terminated surface, the adsorption strength is in the order of Ni > Pt Cu > Pd > Ag Au. In contrast, the order on an iron-terminated surface is Ni > Pt Cu > Au > Pd Ag. The adsorption strength was found to correlate well with the average lengths of metal-oxygen bonds. The magnetite (111) surfaces largely modify the electronic structures of the transition metals. Compared to their density of states in bulk structures, the atomically adsorbed transition metals have narrower d bands, and their d-band centers are closer to the Fermi levels. This implies the higher activities of the atomically adsorbed transition metals.

  1. First-Principles Calculations of the Adsorption of Nitromethane and 1,1-Diamino-2,2-dinitroethylene (FOX-7) Molecules on the Al(111) Surface

    National Research Council Canada - National Science Library

    Sorescu, Dan

    2003-01-01

    .... Based on these calculations, we have determined that both dissociative and nondissociative adsorption mechanisms are possible, depending on the molecular orientation and the particular surface sites involved...

  2. Competitive adsorption and ordered packing of counterions near highly charged surfaces: From mean-field theory to Monte Carlo simulations.

    Science.gov (United States)

    Wen, Jiayi; Zhou, Shenggao; Xu, Zhenli; Li, Bo

    2012-04-01

    Competitive adsorption of counterions of multiple species to charged surfaces is studied by a size-effect-included mean-field theory and Monte Carlo (MC) simulations. The mean-field electrostatic free-energy functional of ionic concentrations, constrained by Poisson's equation, is numerically minimized by an augmented Lagrangian multiplier method. Unrestricted primitive models and canonical ensemble MC simulations with the Metropolis criterion are used to predict the ionic distributions around a charged surface. It is found that, for a low surface charge density, the adsorption of ions with a higher valence is preferable, agreeing with existing studies. For a highly charged surface, both the mean-field theory and the MC simulations demonstrate that the counterions bind tightly around the charged surface, resulting in a stratification of counterions of different species. The competition between mixed entropy and electrostatic energetics leads to a compromise that the ionic species with a higher valence-to-volume ratio has a larger probability to form the first layer of stratification. In particular, the MC simulations confirm the crucial role of ionic valence-to-volume ratios in the competitive adsorption to charged surfaces that had been previously predicted by the mean-field theory. The charge inversion for ionic systems with salt is predicted by the MC simulations but not by the mean-field theory. This work provides a better understanding of competitive adsorption of counterions to charged surfaces and calls for further studies on the ionic size effect with application to large-scale biomolecular modeling.

  3. Polydopamine-mediated surface functionalization of electrospun nanofibrous membranes: Preparation, characterization and their adsorption properties towards heavy metal ions

    International Nuclear Information System (INIS)

    Wu, Chunlin; Wang, Heyun; Wei, Zhong; Li, Chuan; Luo, Zhidong

    2015-01-01

    Graphical abstract: - Highlights: • A simple and versatile approach to produce PEI-functionalized nanofibers. • Novel PEI-functionalized PVC nanofibrous membrane was prepared. • Adsorption of PVC@PDA and PVC@PDA-PEI nanofibrous membranes for Cu 2+ was tested. • Isotherms, kinetic model and thermodynamic parameters were investigated. • Adsorption mechanism of Cu 2+ on modified membranes was inferred. - Abstract: In this paper, a simple and versatile approach for the fabrication of a polyethyleneimine (PEI)-functionalized nanofibrous membrane utilizing polydopamine (PDA) as a mediator is proposed. The morphology and structure of the PDA-coated and PEI-grafted nanofibrous membranes were confirmed using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy. Due to a large specific surface area and long fibrous morphology, the synthesized membranes were used as novel adsorbents for copper ion (Cu 2+ ) removal from aqueous solutions. The adsorption of Cu 2+ was investigated on the synthesized membranes regarding the membrane dosages, initial solution pH values, initial solution concentrations, contact times and temperatures. In addition, the adsorption equilibrium data of PEI-grafted membranes were well fitted with the Langmuir adsorption isotherm, and a maximum adsorption capacity value of 33.59 mg g −1 was determined (while it was 21.94 mg g −1 for the PDA-coated membranes). The thermodynamic parameters indicated that Cu 2+ absorption was a spontaneous and exothermic adsorption process. In addition, XPS peak differentiation imitating analysis permitted the proposal of a copper-amine coordination adsorption mechanism that can be used to explain changes in the adsorption properties compared to PDA coating nanofibrous membranes

  4. The effect of Cu on O adsorption on a ZnO(0001) surface: a first-principles study

    International Nuclear Information System (INIS)

    Dai Xianqi; Yan Huijuan; Wang Jianli; Liu Yaming; Yang Zongxian; Xie, M H

    2008-01-01

    Density functional theory and a pseudopotential plane-wave approach are employed to study the effect of Cu on the adsorption of O on a ZnO(0001) surface. The results show that the Cu adlayer enhances the adsorption of O on ZnO(0001). The energetically favored configuration for Cu and O co-adsorption on ZnO(0001) is that the Cu adatoms are located at the face-centered cubic (fcc) hollow sites, while O adatoms are at the top site of the Zn-terminated ZnO(0001) surface. The possible interchange between Cu adatoms and substrate Zn atoms in the ZnO(0001)-(2 x 2) ideal surface is also examined. The result suggests that the diffusion of Cu into the ZnO substrate is not favorable under equilibrium conditions

  5. Quantifying the availability of clay surfaces in soils for adsorption of nitrocyanobenzene and diuron.

    Science.gov (United States)

    Charles, Simone M; Li, Hui; Teppen, Brian J; Boyd, Stephen A

    2006-12-15

    Coverage of clay surfaces by soil organic matter (SOM) may limitthe efficacy of the soil mineral fractions for adsorption of organic contaminants and pesticides. Two methods were scrutinized for quantitatively assessing the availability of clay surfaces in a smectitic Webster A-horizon soil for sorption of p-nitrocyanobenzene (p-NCB) and diuron. One method, described previously, involves the summation of independent contributions of SOM and swelling clays to sorption of organic solutes. For this method, several assumptions must be made and/or procedural difficulties overcome in the determination of certain terms in the equation proposed for calculating the fractional availability of mineral surfaces (fa). To alleviate the methodological limitations, we developed an alternative approach for determining fa. Good agreement between fa values was obtained from both methods for p-NCB but not diuron. For p-NCB sorption, fa values varied between 0.55 and 0.71. For diuron sorption, our alternative equation estimated fa values varied between 0.41 and 0.61; the other approach yielded negative values. The results demonstrate that SOM does reduce the availability of clay surfaces, hence, suppressing sorption by the Webster A-horizon soil. Our newly developed method provides more reasonable estimates of the availability of soil-clay surfaces for sorption than an earlier published approach.

  6. Investigation of fluorine adsorption on nitrogen doped MgAl2O4 surface by first-principles

    International Nuclear Information System (INIS)

    Lv, Xiaojun; Xu, Zhenming; Li, Jie; Chen, Jiangan; Liu, Qingsheng

    2016-01-01

    Graphical abstract: First-principles calculations indicate that MgAl 2 O 4 surface is fluorine-loving, but hydrophobic. N doped MgAl 2 O 4 (100) surface structure shows the highest fluorine adsorption performance and fluorine atom is more preferentially adsorbed on the Mg-Al bridge site. The fluorine adsorption intensity follow this order: N doped MgAl 2 O 4 (100) > Al 2 O 3 (0001) > MgAl 2 O 4 (100) > MgO (100). N doped MgAl 2 O 4 is a promising candidate for fluorine removal. - Highlights: • MgAl 2 O 4 surface is fluorine-loving, not hydrophilic. • Fluorine preferentially adsorbs on the Mg-Al bridge site. • Adsorption intensity follow this order: N doped MgAl 2 O 4 > Al 2 O 3 > MgAl 2 O 4 > MgO. • Excellent adsorption performance attributes to electron compensation of N atom. • Nitrogen doped MgAl 2 O 4 is a promising candidate for fluorine removal. - Abstract: The nature of fluorine adsorption on pure and N doped MgAl 2 O 4 surface has been investigated by first-principles calculations based on the density functional theory. Calculated results indicate that MgAl 2 O 4 surface is fluorine-loving, not hydrophilic. Nitrogen doped MgAl 2 O 4 (100) surface shows the highest fluorine adsorption performance and fluorine atom preferentially adsorbs on the Mg-Al bridge site. The fluorine adsorption intensity follow this order: Nitrogen doped MgAl 2 O 4 (100) > Al 2 O 3 (0001) > MgAl 2 O 4 (100) > MgO (100). In-depth PDOS analysis suggested that 2p orbitals of F atom strongly hybridized with 3s- and 3p-orbitals of Al atom contribute to its high adsorption intensity. According to the analysis of Hirshfeld charge, the excellent fluorine adsorption performance of nitrogen doped MgAl 2 O 4 attributes to the electron compensation effect of nitrogen atom and strong electrostatic interactions. All these evidences demonstrate a fact nitrogen doped MgAl 2 O 4 is a promising candidate for fluorine removal.

  7. The inhibition of methane hydrate formation by water alignment underneath surface adsorption of surfactants

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, Ngoc N.; Nguyen, Anh V.; Dang, Liem X.

    2017-06-01

    Sodium dodecyl sulfate (SDS) has been widely shown to strongly promote the formation of methane hydrate. Here we show that SDS displays an extraordinary inhibition effect on methane hydrate formation when the surfactant is used in sub-millimolar concentration (around 0.3 mM). We have also employed Sum Frequency Generation vibrational spectroscopy (SFG) and molecular dynamics simulation (MDS) to elucidate the molecular mechanism of this inhibition. The SFG and MDS results revealed a strong alignment of water molecules underneath surface adsorption of SDS in its sub-millimolar solution. Interestingly, both the alignment of water and the inhibition effect (in 0.3 mM SDS solution) went vanishing when an oppositely-charged surfactant (tetra-n-butylammonium bromide, TBAB) was suitably added to produce a mixed solution of 0.3 mM SDS and 3.6 mM TBAB. Combining structural and kinetic results, we pointed out that the alignment of water underneath surface adsorption of dodecyl sulfate (DS-) anions gave rise to the unexpected inhibition of methane hydration formation in sub-millimolar solution of SDS. The adoption of TBAB mitigated the SDS-induced electrostatic field at the solution’s surface and, therefore, weakened the alignment of interfacial water which, in turn, erased the inhibition effect. We discussed this finding using the concept of activation energy of the interfacial formation of gas hydrate. The main finding of this work is to reveal the interplay of interfacial water in governing gas hydrate formation which sheds light on a universal molecular-scale understanding of the influence of surfactants on gas hydrate formation. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. The calculations were carried out using computer resources provided by the Office of Basic Energy Sciences.

  8. An experimental study of furan adsorption and decomposition on vicinal palladium surfaces using scanning tunneling microscopy

    Science.gov (United States)

    Loui, A.; Chiang, S.

    2018-04-01

    The intact adsorption and decomposition of furan (C4H4O) on vicinal palladium surfaces with (111)-oriented terraces has been studied by scanning tunneling microscopy (STM) over a range of temperatures. STM images at 225 K show that furan molecules lie flat and prefer to adsorb at upper step edges. At 225 K, furan molecules adsorbed on "narrow" terraces of 20 to 45 Å in width appear to diffuse more readily than those adsorbed on "wide" terraces of 160 to 220 Å. A distinct population of smaller features appears in STM images on "narrow" terraces at 288 K and on "wide" terraces at 415 K and is identified with the C3H3 decomposition product, agreeing with prior studies which demonstrated that furan dissociates on Pd(111) to yield carbon monoxide (CO) and a C3H3 moiety in the 280 to 320 K range. Based on our direct visualization of this reaction using STM, we propose a spatial mechanism in which adsorption of furan at upper step edges allows catalysis of the dissociation, followed by diffusion of the product to lower step edges.

  9. Effects of an electric field on the adsorption of water molecules on the Cd(0001) surface

    Science.gov (United States)

    Tu, Yu-Bing; Tao, Min-Long; Sun, Kai; Wang, Jun-Zhong

    2018-02-01

    The adsorption of water molecules on the Cd(0001) surface has been systematically investigated in the absence or presence of the electric field using first principles calculations based on density functional theory. It has been determined that the adsorption is enhanced by the electric field. From the geometries and energetics, we find that the water-cadmium interaction become stronger (weaker) under a negative (positive) field in the adsorbed monomer. Otherwise, the formation of the hydrogen bonds makes it difficult for molecules in the water clusters to response the electric field. Most importantly, the stability of the water bilayers depends on the strength of the negative electric field. Instead of the H-up bilayer, the H-down bilayer is more stable when the negative field is sufficiently strong. In this case, the dipole-field interaction is the dominant interaction in the change of stability. These results are helpful in the understanding of the fundamental processes at the water-electrode interfaces.

  10. CO adsorption and dissociation on Pt(111) and Ni(111) surfaces

    DEFF Research Database (Denmark)

    Morikawa, Y.; Mortensen, Jens Jørgen; Hammer, Bjørk

    1997-01-01

    CO adsorption and dissociation processes have been studied using first-principles total energy and force calculations. The adsorption energies, atomic structures and vibrational modes of molecularly chemisorbed states are well reproduced in the present calculations. We have examined several...

  11. Influence of spacer length on heparin coupling efficiency and fibrinogen adsorption of modified titanium surfaces

    Directory of Open Access Journals (Sweden)

    Gbureck Uwe

    2007-07-01

    Full Text Available Abstract Background Chemical bonding of the drug onto surfaces by means of spacer molecules is accompanied with a reduction of the biological activity of the drug due to a constricted mobility since normally only short spacer molecule like aminopropyltrimethoxysilane (APMS are used for drug coupling. This work aimed to study covalent attachment of heparin to titanium(oxide surfaces by varying the length of the silane coupling agent, which should affect the biological potency of the drug due to a higher mobility with longer spacer chains. Methods Covalent attachment of heparin to titanium metal and TiO2 powder was carried out using the coupling agents 3-(Trimethoxysilyl-propylamine (APMS, N- [3-(Trimethoxysilylpropyl]ethylenediamine (Diamino-APMS and N1- [3-(Trimethoxy-silyl-propyl]diethylenetriamine (Triamino-APMS. The amount of bound coupling agent and heparin was quantified photometrically by the ninhydrin reaction and the tolidine-blue test. The biological potency of heparin was determined photometrically by the chromogenic substrate Chromozym TH and fibrinogen adsorption to the modified surfaces was researched using the QCM-D (Quartz Crystal Microbalance with Dissipation Monitoring technique. Results Zeta-potential measurements confirmed the successful coupling reaction; the potential of the unmodified anatase surface (approx. -26 mV shifted into the positive range (> + 40 mV after silanisation. Binding of heparin results in a strongly negatively charged surface with zeta-potentials of approx. -39 mV. The retaining biological activity of heparin was highest for the spacer molecule Triamino-APMS. QCM-D measurements showed a lower viscosity for adsorbed fibrinogen films on heparinised surfaces by means of Triamino-APMS. Conclusion The remaining activity of heparin was found to be highest for the covalent attachment with Triamino-APMS as coupling agent due to the long chain of this spacer molecule and therefore the highest mobility of the drug

  12. Surface properties of nanocrystalline TiO2 coatings in relation to the in vitro plasma protein adsorption

    International Nuclear Information System (INIS)

    Lorenzetti, M; Kobe, S; Novak, S; Bernardini, G; Santucci, A; Luxbacher, T

    2015-01-01

    This study reports on the selective adsorption of whole plasma proteins on hydrothermally (HT) grown TiO 2 -anatase coatings and its dependence on the three main surface properties: surface charge, wettability and roughness. The influence of the photo-activation of TiO 2 by UV irradiation was also evaluated. Even though the protein adhesion onto Ti-based substrates was only moderate, better adsorption of any protein (at pH = 7.4) occurred for the most negatively charged and hydrophobic substrate (Ti non-treated) and for the most nanorough and hydrophilic surface (HT Ti3), indicating that the mutual action of the surface characteristics is responsible for the attraction and adhesion of the proteins. The HT coatings showed a higher adsorption of certain proteins (albumin ‘passivation’ layer, apolipoproteins, vitamin D-binding protein, ceruloplasmin, α-2-HS-glycoprotein) and higher ratios of albumin to fibrinogen and albumin to immunoglobulin γ-chains. The UV pre-irradiation affected the surface properties and strongly reduced the adsorption of the proteins. These results provide in-depth knowledge about the characterization of nanocrystalline TiO 2 coatings for body implants and provide a basis for future studies on the hemocompatibility and biocompatibility of such surfaces. (paper)

  13. New bonding configuration on Si(111) and Ge(111) surfaces induced by the adsorption of alkali metals

    DEFF Research Database (Denmark)

    Lottermoser, L.; Landemark, E.; Smilgies, D.M.

    1998-01-01

    The structure of the (3×1) reconstructions of the Si(111) and Ge(111) surfaces induced by adsorption of alkali metals has been determined on the basis of surface x-ray diffraction and low-energy electron diffraction measurements and density functional theory. The (3×1) surface results primarily f...... from the substrate reconstruction and shows a new bonding configuration consisting of consecutive fivefold and sixfold Si (Ge) rings in 〈11̅ 0〉 projection separated by channels containing the alkali metal atoms. © 1998 The American Physical Society......The structure of the (3×1) reconstructions of the Si(111) and Ge(111) surfaces induced by adsorption of alkali metals has been determined on the basis of surface x-ray diffraction and low-energy electron diffraction measurements and density functional theory. The (3×1) surface results primarily...

  14. Adsorption and reaction of CO and H2O on WC(0001) surface: A first-principles investigation

    Science.gov (United States)

    Tong, Yu-Jhe; Wu, Shiuan-Yau; Chen, Hsin-Tsung

    2018-01-01

    We have performed a spin-polarized density functional theory (DFT) study for understanding the detailed reaction mechanism of CO and H2O on WC (0001) surface. The adsorption properties and vibrational frequencies of H2O, OH, O, H, CO and CO2 on the WC (0001) surface were illustrated. These results are well in consistent with the experimental observations studied by temperature-programmed desorption (TPD) and high-resolution electron energy loss spectroscopy (HREELS). Based on the adsorption results, potential energy profiles of H2O and OH dehydrogenation and HCO, COH, COOH, and CO2 formation on the WC (0001) surface were predicted. The calculation results demonstrated that the WC (0001) surface as Fe (110) surface exhibits significantly reaction activity toward the dehydrogenation of H2O and OH but less activity toward the formation of HCO, COH, COOH and CO2 compared to the Cu (111) and Pt (111) surfaces.

  15. Surface charge regulation upon polyelectrolyte adsorption, hematite, polystyrene sulfonate, surface charge regulation - Theoretical calculations and hematite-poly(styrene sulfonate) system

    NARCIS (Netherlands)

    Riemsdijk, van W.H.; Koopal, L.K.; Stuart, M.A.C.; Klein Wolterink, J.

    2006-01-01

    The charge regulation of a mineral surface upon adsorption of a strong polyelectrolyte is studied theoretically and experimentally. Self-consistent-field calculations were done to evaluate the charge characteristics of a model oxide surface in the absence and presence of a linear strong

  16. [Isolation, identification and lead adsorption study of lead-resistant Lactobacillus casei strains from feces of healthy newborns].

    Science.gov (United States)

    Shen, Wei; Yu, Qin-Fei; Wang, Yu-Hao; Zhang, Yi-Duo; Meng, Xiao-Jing; Fan, Hong-Ying

    2016-12-20

    To isolate and identify lead-resistant Lactobacillus casei strains with lead adsorption ability from the stool of healthy newborns as a new source of bacteria for developing lead-eliminating food products. MRS was used to isolate lead-resistant bacteria from the feces of 30 healthy and full-term neonates. A phylogenetic tree was constructed based on the morphological characteristics and 16S rRNA sequences of the isolated bacteria. Physiological and biochemical characterizations of the bacteria were performed according to the Berger's Systematic Bacteriology Handbook, followed by antimicrobial susceptibility test and acid-tolerant bile salt test. The adsorption capacity of Pb 2+ of the bacteria was determined by inductively coupled plasma-optical emission spectroscopy (ICP-OES). Three strains of Lactobacillus casei were isolated, which were resistant to penicillin and ceftriaxone and could tolerate the exposure to 500 mg/L Pb 2+ . Acid-tolerant bile salt test showed that the bacteria were resistant to culture in the presence of artificial gastric juice (pH 2.0) for 3 h, and their survival rate reached 62.5% following exposure to 0.3% bile salt for 8 h. The bacteria showed a Pb 2+ adsorption rate of 90.4% at a low Pb 2+ concentration (1 mg/L) and of 86.27% at a high Pb 2+ concentration (50 mg/L). Three Lactobacillus casei strains lead adsorption ability were isolated from the feces of newborns. These bacterial strains provide a new solution to alleviate lead poisoning by probiotic dietary.

  17. Surface resistance of superconductors - examples from Nb - O systems

    International Nuclear Information System (INIS)

    Palmer, F.

    1988-01-01

    The observed surface resistance of most superconductors can be written as the sum of two terms. R/sub obs/ = R/sub BCS/ + R/sub res/. This paper is divided into three sections. The first section describes the BCS theory of surface resistance in terms of a simplified two-fluid model. The second section describes several possible causes of residual resistance including normal conducting materials, tunneling across cracks in the surface, and direct generation of phonons by the RF electric field. The last section describes recent experiments having to do with the effects of oxide layers on surface resistance. Layers grown in pure oxygen at room temperature were found to have little or no effect, but if these layers are heated to temperatures near 300 0 C, they can alter both the BCS resistance and the residual resistance. Heated oxide layers also increased the dependence of the residual resistance on ambient magnetic field. 31 references, 13 figures, 3 tables

  18. Surface reactions of iron - enriched smectites: adsorption and transformation of hydroxy fatty acids and phenolic acids

    Science.gov (United States)

    Polubesova, Tamara; Olshansky, Yaniv; Eldad, Shay; Chefetz, Benny

    2014-05-01

    Iron-enriched smectites play an important role in adsorption and transformation of soil organic components. Soil organo-clay complexes, and in particular humin contain hydroxy fatty acids, which are derived from plant biopolymer cutin. Phenolic acids belong to another major group of organic acids detected in soil. They participate in various soil processes, and are of concern due to their allelopathic activity. We studied the reactivity of iron-enriched smectites (Fe(III)-montmorillonite and nontronite) toward both groups of acids. We used fatty acids- 9(10),16-dihydroxypalmitic acid (diHPA), isolated from curtin, and 9,10,16-trihydroxypalmitic acid (triHPA); the following phenolic acids were used: ferulic, p-coumaric, syringic, and vanillic. Adsorption of both groups of acids was measured. The FTIR spectra of fatty acid-mineral complexes indicated inner-sphere complexation of fatty acids with iron-enriched smectites (versus outer-sphere complexation with Ca(II)-montmorillonite). The LC-MS results demonstrated enhanced esterification of fatty acids on the iron-enriched smectite surfaces (as compared to Ca(II)-montmorillonite). This study suggests that fatty acids can be esterified on the iron-enriched smectite surfaces, which results in the formation of stable organo-mineral complexes. These complexes may serve as a model for the study of natural soil organo-clay complexes and humin. The reaction of phenolic acids with Fe(III)-montmorillonite demonstrated their oxidative transformation by the mineral surfaces, which was affected by molecular structure of acids. The following order of their transformation was obtained: ferulic >syringic >p-coumaric >vanillic. The LC-MS analysis demonstrated the presence of dimers, trimers, and tetramers of ferulic acid on the surface of Fe(III)-montmorillonite. Oxidation and transformation of ferulic acid were more intense on the surface of Fe(III)-montmorillonite as compared to Fe(III) in solution due to stronger complexation on

  19. Apparatus to measure adsorption of condensable solvents on technical surfaces by photothermal deflection

    Science.gov (United States)

    Plimmer, M. D.; du Colombier, D.; Iraqi Houssaini, N.; Silvestri, Z.; Pinot, P.; Hannachi, R.

    2012-11-01

    This article describes an instrument for the measurement of the mirage effect as a tool to determine the molar adsorption per unit surface area Y1 of condensable solvents in the presence of a non-condensable carrier gas. The present apparatus is a much improved version of previous prototypes developed in our laboratory and elsewhere with a higher surface bake-out temperature (150 °C rather than 40 °C), lower residual vacuum (3 Pa versus 100 Pa), greater sample surface (40 mm diameter instead of 10 mm), more powerful optical pump beam (150 W cf. 50 W), and larger saturated vapour preparation volume (4 L instead of 1 L). The new set-up also includes the in situ monitoring of the surface via a reflected HeNe laser beam for the real-time detection of the onset of condensation. Here, we give a detailed description of the various components, outline the experimental procedure, show typical results, and suggest some straightforward improvements.

  20. Water adsorption and dissociation on the PuO2(1 1 0) surface

    International Nuclear Information System (INIS)

    Jomard, Gérald; Bottin, François; Geneste, Grégory

    2014-01-01

    Adsorption of the H 2 O molecule on the PuO 2 (1 1 0) surface is studied by density-functional calculations. The strong electronic correlations in the PuO 2 compound are treated in the DFT+U (Hubbard) formalism. A dissociated state of water is identified, resulting in the formation of hydroxyl groups and corresponding to a very exothermic process. However, a non-dissociated (molecular) form does exist as a metastable state. The Infra-Red and XPS signature of both forms are identified and compared to experiments. Kinetic Monte Carlo simulations show that adsorbed molecular water might have a long life-time before dissociating at low temperature, due to a small energy barrier between the molecular and dissociated configurations, in agreement with experiments

  1. Water adsorption on non polar ZnO surfaces: from single molecules to multilayers

    Science.gov (United States)

    Kenmoe, Stephane; Biedermann, P. Ulrich

    2015-03-01

    The interface between water and ZnO plays an important role in many domains of technological relevance. Following the vital role of adsorbed water on substrate properties and the fascinating properties of interfacial water, there is a great interest in characterizing this interface. We use DFT to study the possible aggregation regimes that can form on the ZnO non-polar low-index (1010) and (1120) surfaces. We study the adsorption of water monomers, small water clusters like water dimers, water chains, ladder-like water structures, water thin films and water multilayers. Based on this, trends in binding energy as well as the binding mechanisms are analyzed to understand the driving forces and the nature of the fundamental interactions that stabilize the adsorbed layers.

  2. Preparation and Characterization of Chitosan/Feldspar Biohybrid as an Adsorbent: Optimization of Adsorption Process via Response Surface Modeling

    Directory of Open Access Journals (Sweden)

    Maryam Yazdani

    2014-01-01

    Full Text Available Chitosan/feldspar biobased beads were synthesized, characterized, and tested for the removal of Acid Black 1 dye from aquatic phases. A four-factor central composite design (CCD accompanied by response surface modeling (RSM and optimization was used to optimize the dye adsorption by the adsorbent (chitosan/feldspar composite in 31 different batch experiments. Independent variables of temperature, pH, initial dye concentration, and adsorbent dose were used to change to coded values. To anticipate the responses, a quadratic model was applied. Analysis of variance (ANOVA tested the significance of the process factors and their interactions. The adequacy of the model was investigated by the correlation between experimental and predicted data of the adsorption and the calculation of prediction errors. The results showed that the predicted maximum adsorption amount of 21.63 mg/g under the optimum conditions (pH 3, temperature 15°C, initial dye concentration 125 mg/L, and dose 0.2 g/50 mL was close to the experimental value of 19.85 mg/g. In addition, the results of adsorption behaviors of the dye illustrated that the adsorption process followed the Langmuir isotherm model and the pseudo-second-order kinetic model. Langmuir sorption capacity was found to be 17.86 mg/g. Besides, thermodynamic parameters were evaluated and revealed that the adsorption process was exothermic and favourable.

  3. Preparation and characterization of chitosan/feldspar biohybrid as an adsorbent: optimization of adsorption process via response surface modeling.

    Science.gov (United States)

    Yazdani, Maryam; Bahrami, Hajir; Arami, Mokhtar

    2014-01-01

    Chitosan/feldspar biobased beads were synthesized, characterized, and tested for the removal of Acid Black 1 dye from aquatic phases. A four-factor central composite design (CCD) accompanied by response surface modeling (RSM) and optimization was used to optimize the dye adsorption by the adsorbent (chitosan/feldspar composite) in 31 different batch experiments. Independent variables of temperature, pH, initial dye concentration, and adsorbent dose were used to change to coded values. To anticipate the responses, a quadratic model was applied. Analysis of variance (ANOVA) tested the significance of the process factors and their interactions. The adequacy of the model was investigated by the correlation between experimental and predicted data of the adsorption and the calculation of prediction errors. The results showed that the predicted maximum adsorption amount of 21.63 mg/g under the optimum conditions (pH 3, temperature 15°C, initial dye concentration 125 mg/L, and dose 0.2 g/50 mL) was close to the experimental value of 19.85 mg/g. In addition, the results of adsorption behaviors of the dye illustrated that the adsorption process followed the Langmuir isotherm model and the pseudo-second-order kinetic model. Langmuir sorption capacity was found to be 17.86 mg/g. Besides, thermodynamic parameters were evaluated and revealed that the adsorption process was exothermic and favourable.

  4. Magnetic Zn (II) ion-imprinted polymer prepared by the surface imprinting technique and its adsorption properties.

    Science.gov (United States)

    Zhang, Hui-xin; Dou, Qian; Jin, Xiu-hong; Zhang, Jie; Yang, Ting-ru; Han, Xu; Wang, Dong-dong

    2015-01-01

    A novel magnetic Zn (II) ion-imprinted polymer was prepared by the surface ion-imprinted technique by using magnetic Fe3O4@SiO2 microspheres as supporter, methacrylic acid and salicylaldoxime as monomers, ethylene glycol dimethacrylate as the crosslinker. The products were characterized by Fourier transform infrared, X-ray photoelectron spectrometer, vibrating sample magnetometer and scanning electron microscope. The adsorption experiments showed that the imprinted polymer was employed successfully in comparison with non-imprinted polymer. When the temperature was in a range of 291-297 K, the maximum adsorption was about 52.69 mg g(-1) with an optimal pH 6.0 for an equilibrium time of 40 min. The imprinted polymer possessed high selectivity and specific recognition towards Zn (II). The Langmuir adsorption model was more favourable than the Freundlich or the Temkin adsorption model. Thermodynamic experiment showed that the adsorption was a spontaneous and endothermic process for Zn (II). The mechanism for Zn (II) adsorption on the imprinted polymer was investigated.

  5. Adsorption of TX-100 and SDBS on the surface of alumina and maghemite nanoparticles from aqueous solutions

    Directory of Open Access Journals (Sweden)

    R. R. Mansurov

    2014-11-01

    Full Text Available Adsorption equilibriums in aqueous aluminum and iron oxides nanosuspensions stabilized by SDBS and TX-100 were investigated using UV spectrophotometry. It was established that the non-ionic surfactant TritonX-100 is not adsorbed from aqueous solution on a hydrophilic surface of both aluminum and iron oxide nanoparticles. At the same time adsorption of the anionic surfactant SDBS was observed in both oxides nanoparticles. In the investigated range of concentrations adsorption isotherms SDBS from aqueous solution on the surfaces of nanoparticles Al2O3 and γ-Fe2O3 not reach saturation. The share of the particles surface occupied by surfactant molecules were estimated based on the value of an area of molecules SDBS in the adsorption layer, which was derived from the isotherm of surface tension (0.10 nm2. The calculations showed that at the investigated concentrations SDBS Al2O3 employed approximately 30 % of surface of nanoparticles, and for γ-Fe2O3 – up to 10%.

  6. Effects of textural and surface characteristics of microporous activated carbons on the methane adsorption capacity at high pressures

    Energy Technology Data Exchange (ETDEWEB)

    Bastos-Neto, M. [Grupo de Pesquisas em Separacoes por Adsorcao (GPSA), Departamento de Engenharia Quimica, Universidade Federal do Ceara, Campus Universitario do Pici, Bl 709 60455-760 Fortaleza, CE (Brazil); Canabrava, D.V. [Grupo de Pesquisas em Separacoes por Adsorcao (GPSA), Departamento de Engenharia Quimica, Universidade Federal do Ceara, Campus Universitario do Pici, Bl 709 60455-760 Fortaleza, CE (Brazil); Torres, A.E.B. [Grupo de Pesquisas em Separacoes por Adsorcao (GPSA), Departamento de Engenharia Quimica, Universidade Federal do Ceara, Campus Universitario do Pici, Bl 709 60455-760 Fortaleza, CE (Brazil); Rodriguez-Castellon, E. [Departamento de Quimica Inorganica, Cristalografia y Mineralogia (Unidad Asociada al ICP-CSIC), Facultad de Ciencias, Universidad de Malaga, 29071 Malaga (Spain); Jimenez-Lopez, A. [Departamento de Quimica Inorganica, Cristalografia y Mineralogia (Unidad Asociada al ICP-CSIC), Facultad de Ciencias, Universidad de Malaga, 29071 Malaga (Spain); Azevedo, D.C.S. [Grupo de Pesquisas em Separacoes por Adsorcao (GPSA), Departamento de Engenharia Quimica, Universidade Federal do Ceara, Campus Universitario do Pici, Bl 709 60455-760 Fortaleza, CE (Brazil)]. E-mail: diana@gpsa.ufc.br; Cavalcante, C.L. [Grupo de Pesquisas em Separacoes por Adsorcao (GPSA), Departamento de Engenharia Quimica, Universidade Federal do Ceara, Campus Universitario do Pici, Bl 709 60455-760 Fortaleza, CE (Brazil)

    2007-04-30

    The objective of this study is to relate textural and surface characteristics of selected microporous activated carbons to their methane storage capacity. In this work, a magnetic suspension balance (Rubotherm, Germany) was used to measure methane adsorption isotherms of several activated carbon samples. Textural characteristics were assessed by nitrogen adsorption on a regular surface area analyzer (Autosorb-MP, by Quantachrome, USA). N{sub 2} adsorption was analysed by conventional models (BET, DR, HK) and by Monte Carlo molecular simulations. Elemental and surface analyses were performed by X-ray photoelectronic spectroscopy (XPS) for the selected samples. A comparative analysis was then carried out with the purpose of defining some correlation among the variables under study. For the system under study, pore size distribution and micropore volume seem to be a determining factor as long as the solid surface is perfectly hydrophobic. It was concluded that the textural parameters per se do not unequivocally determine natural gas storage capacities. Surface chemistry and methane adsorption equilibria must be taken into account in the decision-making process of choosing an adsorbent for gas storage.

  7. Uniform surface modification of diatomaceous earth with amorphous manganese oxide and its adsorption characteristics for lead ions

    International Nuclear Information System (INIS)

    Li, Song; Li, Duanyang; Su, Fei; Ren, Yuping; Qin, Gaowu

    2014-01-01

    Graphical abstract: - Highlights: • A uniform MnO 2 layer was anchored onto diatomite surface. • Kinetics and isotherms over MnO 2 modified diatomite were studied. • The Pb(II) adsorption is based on ion-exchange mechanism. - Abstract: A novel method to produce composite sorbent material compromising porous diatomaceous earth (DE) and surface functionalized amorphous MnO 2 is reported. Via a simple in situ redox reaction over the carbonized DE powders, a uniform layer of amorphous MnO 2 was anchored onto the DE surface. The hybrid adsorbent was characterized by X-ray diffraction, scanning electron microscopy, and infrared spectroscopy. The batch method has been employed to investigate the effects of surface coating on adsorption performance of DE. According to the equilibrium studies, the adsorption capacity of DE for adsorbing lead ions after MnO 2 modification increased more than six times. And the adsorption of Pb 2+ on the MnO 2 surface is based on ion-exchange mechanism. The developed strategy presents a novel opportunity to prepare composite adsorbent materials by integrating nanocrystals with porous matrix

  8. Uniform surface modification of diatomaceous earth with amorphous manganese oxide and its adsorption characteristics for lead ions

    Energy Technology Data Exchange (ETDEWEB)

    Li, Song; Li, Duanyang; Su, Fei; Ren, Yuping; Qin, Gaowu, E-mail: lis@atm.neu.edu.cn

    2014-10-30

    Graphical abstract: - Highlights: • A uniform MnO{sub 2} layer was anchored onto diatomite surface. • Kinetics and isotherms over MnO{sub 2} modified diatomite were studied. • The Pb(II) adsorption is based on ion-exchange mechanism. - Abstract: A novel method to produce composite sorbent material compromising porous diatomaceous earth (DE) and surface functionalized amorphous MnO{sub 2} is reported. Via a simple in situ redox reaction over the carbonized DE powders, a uniform layer of amorphous MnO{sub 2} was anchored onto the DE surface. The hybrid adsorbent was characterized by X-ray diffraction, scanning electron microscopy, and infrared spectroscopy. The batch method has been employed to investigate the effects of surface coating on adsorption performance of DE. According to the equilibrium studies, the adsorption capacity of DE for adsorbing lead ions after MnO{sub 2} modification increased more than six times. And the adsorption of Pb{sup 2+} on the MnO{sub 2} surface is based on ion-exchange mechanism. The developed strategy presents a novel opportunity to prepare composite adsorbent materials by integrating nanocrystals with porous matrix.

  9. Molecular dynamics simulation of the effect of pH on the adsorption of rhodamine laser dyes on TiO2 hydroxylated surfaces

    OpenAIRE

    2009-01-01

    Abstract We have carried out a study of the adsorption, on the (101) surface of anatase TiO2, of two industrially relevant rhodamines molecules (rhodamine 6G and rhodamine 800) employing Molecular Dynamics. These theoretical studies have shown that Rhodamine 6G must adsorb on surfaces under basic conditions. Moreover, the adsorption of this molecule shows a strong dependence upon the pH of the system, i.e. under neutral conditions the adsorption energy is quite smaller, and under ...

  10. Carbon disulfide (CS{sub 2}) adsorption and dissociation on the Cu(100) surface: A quantum chemical study

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Wenju, E-mail: wangwenju1982@163.com; Fan, Lili; Wang, Guoping, E-mail: wgp1976@163.com

    2017-08-31

    Highlights: • CS{sub 2}, CS, C and S are strongly chemadsorbed on the Cu(100) surface. • C/S/S, S/CS and CS{sub 2} accord to a decreased adsorption strength on the Cu(100). • The asymmetric model CS{sub 2}(II) is easier to dissociate on the Cu(100) surface. - Abstract: Density functional theory (DFT) is used to examine the adsorption and dissociation of CS{sub 2} on the Cu(100) surface. This study evaluates the adsorption energies and geometries of the species (CS{sub 2}, CS, C and S) adsorption on the Cu(100) surface, as well as that coadsorption of CS and a S atom, and that coadsorption of C atom and two S atoms. The results indicate that the species (CS{sub 2}, CS, C and S) are strongly chemadsorbed on the Cu(100) surface through the C−Cu and/or S−Cu bond with an increased adsorption energy (C/S/S > S/CS > CS{sub 2}). Two pathways for CS{sub 2} dissociation on the Cu(100) surface are constructed, and the energy barrier and reaction energy of each step are calculated. It shows that the dissociated energy barrier of the second C−S bond is 0.25 eV higher than that of the first C−S bond in the pathway 1, but in the pathway 2, the dissociated energy barrier of the second C−S bond is 0.11 eV lower than that of the first C−S bond. Comparing the highest dissociated energy barrier of pathway 1 (0.68 eV) and pathway 2 (0.5 eV), the structure of S/C/S(II) is regarded as a preferable product for the dissociation of CS{sub 2} on the Cu(100) surface.

  11. Adsorption of a small protein to a methyl-terminated hydrophobic surfaces

    DEFF Research Database (Denmark)

    Otzen, Daniel; Oliveberg, M.; Höök, F.

    2003-01-01

    We have studied the adsorption kinetics of a small monomeric protein S6 using the quartz crystal microbalance with dissipation monitoring (QCM-D) technique. Competitive adsorption from various proportions of native (Nat) and denatured (Den) protein in the bulk phase was carried out using a range...... of chemical denaturant concentrations. The ratio between Nat and Den in bulk has a profound affect on the adsorption behavior, most obvious from a significant (one order of magnitude) increase in the rate of a lag– and consolidation–adsorption phase when Nat is the major species present in bulk, signaling...... that these adsorption phases originates from the Den fraction of proteins in the bulk. To determine whether the kinetics of protein unfolding in the bulk phase are rate-limiting for adsorption of Nat, the adsorption kinetics of wildtype S6 with the mutant VA85 (whose unfolding kinetics are around 30 times more rapid...

  12. Accelerator Analysis of Tributyltin Adsorbed onto the Surface of a Tributyltin Resistant Marine Pseudoalteromonas sp. Cell

    Directory of Open Access Journals (Sweden)

    Akira Kitamura

    2008-10-01

    Full Text Available Tributyltin (TBT released into seawater from ship hulls is a stable marine pollutant and obviously remains in marine environments. We isolated a TBT resistant marine Pseudoalteromonas sp. TBT1 from sediment of a ship’s ballast water. The isolate (109.3 ± 0.2 colony-forming units mL-1 adsorbed TBT in proportion to the concentrations of TBTCl externally added up to 3 mM, where the number of TBT adsorbed by a single cell was estimated to be 108.2. The value was reduced to about one-fifth when the lysozyme-treated cells were used. The surface of ethanol treated cells became rough, but the capacity of TBT adsorption was the same as that for native cells. These results indicate that the function of the cell surface, rather than that structure, plays an important role to the adsorption of TBT. The adsorption state of TBT seems to be multi-layer when the number of more than 106.8 TBT molecules is adsorbed by a single cell.

  13. Surface modification of spinel λ-MnO2 and its lithium adsorption properties from spent lithium ion batteries

    International Nuclear Information System (INIS)

    Li, Li; Qu, Wenjie; Liu, Fang; Zhao, Taolin; Zhang, Xiaoxiao; Chen, Renjie; Wu, Feng

    2014-01-01

    Highlights: • A method is designed to synthesize a λ-MnO 2 ion-sieve for lithium ions adsorption. • Ultrasonic treatment with acid is highly efficient for lithium ions extraction. • Surface modification by CeO 2 is used to improve the adsorption capacity. • A 0.5 wt.% CeO 2 -coated ion-sieve shows the best adsorption properties. • λ-MnO 2 ion-sieves are promising for recovering scarce lithium resources. - Abstract: Spinel λ-MnO 2 ion-sieves are promising materials because of their high selectivity toward lithium ions, and this can be applied to the recovery of lithium from spent lithium ion batteries. However, manganese dissolution loss during the delithiation of LiMn 2 O 4 causes a decrease in adsorption capacity and poor cycling stability for these ion-sieves. To improve the lithium adsorption properties of λ-MnO 2 ion-sieves, surface modification with a CeO 2 coating was studied using hydrothermal-heterogeneous nucleation. The structure, morphology and composition of the synthesized materials were determined by XRD, SEM, TEM and EDS. The effect of hydrothermal synthesis conditions and the amount of CeO 2 coating on the adsorption performance of λ-MnO 2 were also investigated. A 0.5 wt.% CeO 2 -coated ion-sieve was synthesized by heating at 120 °C for 3 h and it had better adsorption properties than the bare samples. The effect of ultrasonic treatment on the lithium extraction ratio from LiMn 2 O 4 upon acid treatment at various temperatures was studied and the results were compared with conventional mechanical stirring. We found that ultrasonic treatment at lower temperature gave almost the same maximum lithium extraction ratio and was more efficient and economic

  14. Study of the Adsorption of Atoms and Molecules on Silicon Surfaces: Crystallographics and Electronic Structure

    International Nuclear Information System (INIS)

    Bengio, Silvina

    2003-01-01

    This thesis work has been concerned with adsorption properties of silicon surfaces.The atomic and electronic structure of molecules and atoms adsorbed on Si has been investigated by means of photoemission experiments combined with synchrotron radiation.The quantitative atomic structure determination was held applying the photoelectron diffraction technique.This technique is sensible to the local structure of a reference atomic specie and has elemental and chemical-state specificity.This approach has been applied to three quite different systems with different degrees of complexity, Sb/Si(111) √3x √3R30 0 , H 2 O/Si(100)2x1 and NH 3 /Si(111)7x7.Our results show that Sb which forms a ( √3√3)R30 0 phase produces a bulklike-terminated Si(111)1x1 substrate free of stacking faults.Regarding the atomic structure of its interface, this study strongly favours the T4-site milkstool model over the H3 one.An important aspect regarding the H 2 O/Si(100)(2x1) system was establishing the limits of precision with which one can determine not only the location of the adsorbed hydroxyl (OH) species, but also the extent to which this adsorption modifes the asymmetric dimers of the clean surface to which it is bonded.On the Si(111)(7x7) surface the problem is particularly complex because there are several different potentially active sites for NH3 adsorption and fragmentation.The application of the PhD method, however, has shown that the majority of the N atoms are on so-called 'rest atom' sites when deposited at RT.This is consistent with the N in the NH2 chemical state.This investigation represents the first quantitative structural study of any molecular adsorbate on the complex Si(111)(7x7) surface.This atomic structures determination shows the PhD is a powerful tool for the atomic structure determination.The molecular systems interacting with the active sites of the substrate fragments producing a short-range order surface.This long-range disorder is produced by the

  15. Influence of activated carbon surface acidity on adsorption of heavy metal ions and aromatics from aqueous solution

    International Nuclear Information System (INIS)

    Sato, Sanae; Yoshihara, Kazuya; Moriyama, Koji; Machida, Motoi; Tatsumoto, Hideki

    2007-01-01

    Adsorption of toxic heavy metal ions and aromatic compounds onto activated carbons of various amount of surface C-O complexes were examined to study the optimum surface conditions for adsorption in aqueous phase. Cadmium(II) and zinc(II) were used as heavy metal ions, and phenol and nitrobenzene as aromatic compounds, respectively. Activated carbon was de-ashed followed by oxidation with nitric acid, and then it was stepwise out-gassed in helium flow up to 1273 K to gradually remove C-O complexes introduced by the oxidation. The oxidized activated carbon exhibited superior adsorption for heavy metal ions but poor performance for aromatic compounds. Both heavy metal ions and aromatics can be removed to much extent by the out-gassed activated carbon at 1273 K. Removing C-O complexes, the adsorption mechanisms would be switched from ion exchange to Cπ-cation interaction for the heavy metals adsorption, and from some kind of oxygen-aromatics interaction to π-π dispersion for the aromatics

  16. A computational investigation of adsorption of organics on mineral surfaces: Implications for organics delivery in the early solar system

    Science.gov (United States)

    Asaduzzaman, A. M.; Zega, T. J.; Laref, Slimane; Runge, K.; Deymier, P. A.; Muralidharan, Krishna

    2014-12-01

    The adsorption of simple organic compounds onto minerals that are known to occur in the early solar nebula such as olivine, spinel and water-ice, is examined using first-principles density functional theory. The calculations show that electron-rich organics and organics containing cyanide, amine and carboxylic functional groups can strongly bind to low-index surfaces of olivine and spinel. Based on the surface coverage as obtained from these calculations, it can be inferred that an estimated amount of 1013 kg of organics could have been delivered to early Earth via direct adsorption mechanisms, thereby providing an endogenous source of planetary organics. In addition, adsorption of organic compounds on magnesite, a carbonate phase believed to have formed via aqueous processes on asteroidal bodies, is also studied. The adsorption behavior of the organics is observed to be similar in both cases, i.e., for minerals that formed during the earliest stages of nebular evolution through condensation (spinel and olivine) or other processes and for those that formed via hydration processes on asteroidal bodies (magnesite). These results suggest that direct incorporation via adsorption is an important delivery mechanism of organics to both asteroidal bodies and terrestrial planets.

  17. Adsorption and revaporisation studies on iodine oxide aerosols deposited on containment surface materials in LWR

    Energy Technology Data Exchange (ETDEWEB)

    Tietze, S.; Foreman, M.R.StJ.; Ekberg, C. [Chalmers Univ. of Technology, Goeteborg (Sweden); Kaerkelae, T.; Auvinen, A.; Tapper, U.; Lamminmaeki, S.; Jokiniemi, J. [VTT Technical Research Centre of Finland, Espoo (Finland)

    2012-12-15

    During a hypothetical severe nuclear accident, the radiation field will be very high in the nuclear reactor containment building. As a result gaseous radiolysis products will be formed. Elemental iodine can react in the gaseous phase with ozone to form solid iodine oxide aerosol particles (iodine oxide). Within the AIAS (Adsorption of Iodine oxide Aerosols on Surfaces) project the interactions of iodine oxide (IOx) aerosols with common containment surface materials were investigated. Common surface materials in Swedish and Finnish LWRs are Teknopox Aqua V A paint films and metal surfaces such as Cu, Zn, Al and SS, as well as Pt and Pd surfaces from hydrogen recombiners. Non-radioactive and {sup 131}I labelled iodine oxide aerosols were produced with the EXSI CONT facility from elemental iodine and ozone at VTT Technical Research Centre of Finland. The iodine oxide deposits were analysed with microscopic and spectroscopic measurement techniques to identify the kind of iodine oxide formed and if a chemical conversion on the different surface materials occurs. The revaporisation behaviour of the deposited iodine oxide aerosol particles from the different surface materials was studied under the influence of heat, humidity and gamma irradiation at Chalmers University of Technology, Sweden. Studies on the effects of humidity were performed using the FOMICAG facility, while heat and irradiation experiments were performed in a thermostated heating block and with a gammacell 22 having a dose rate of 14 kGy/h. The revaporisation losses were measured using a HPGe detector. The revaporisated {sup 131}I species from the surfaces were chemically tested for elemental iodine formation. The parameter dominating the degradation of the produced iodine oxide aerosols was humidity. Cu and Zn surfaces were found to react with iodine from the iodine oxide aerosols to form iodides, while no metal iodides were detected for Al and SS samples. Most of the iodine oxide aerosols are assumed to

  18. Adsorption and dissociation of O2on MoO2(1[combining macron]11) surfaces: a DFT study.

    Science.gov (United States)

    Zhang, Quan; Zhang, Minhua; Wiltowski, Tomasz

    2017-11-08

    The adsorption and dissociation of O 2 on MoO 2 (1[combining macron]11) surfaces were studied by density functional theory (DFT). The results show that O 2 molecules prefer to be adsorbed on the five-coordinated Mo top sites. Density of states analysis shows strong hybridization of Mo 4d orbitals and O 2p orbitals in the Mo-O bond. Clean MoO 2 slabs and slabs with O 2 adsorption are metallic conductors, whereas the surface with high O atom coverage is reconstructed and becomes a semiconductor. Surface Mo atoms without adsorbed O or O 2 are spin-polarized. The oxygen adsorption shows the ability to reduce the spin of surface Mo atoms. The adsorption energy of the O 2 and O atoms decreases as coverage increases. The transition states of O 2 dissociation were located. The energy barriers for O 2 dissociation on the five-coordinated and four-coordinated Mo top sites are 0.227 eV and 0.281 eV, respectively.

  19. Surface-modified nanoparticles as a new, versatile, and mechanically robust nonadhesive coating : Suppression of protein adsorption and bacterial adhesion

    NARCIS (Netherlands)

    Holmes, P. F.; Currie, E. P. K.; Thies, J. C.; van der Mei, H. C.; Busscher, H. J.; Norde, W.

    2009-01-01

    The synthesis of surface-modified silica nanoparticles, chemically grafted with acrylate and poly(ethylene glycol) (PEG) groups, and the ability of the resulting crosslinked coatings to inhibit protein adsorption and bacterial adhesion are explored. Water contact angles, nanoindentation, and atomic

  20. Adsorption of charged and neutral polymer chains on silica surfaces: The role of electrostatics, volume exclusion, and hydrogen bonding

    NARCIS (Netherlands)

    Spruijt, Evan; Biesheuvel, P.M.; de Vos, Wiebe Matthijs

    2015-01-01

    We develop an off-lattice (continuum) model to describe the adsorption of neutral polymer chains and polyelectrolytes to surfaces. Our continuum description allows taking excluded volume interactions between polymer chains and ions directly into account. To implement those interactions, we use a

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

    NARCIS (Netherlands)

    Boateng, Isaac W.; Tia, Richard; Adei, Evans; Dzade, N.Y.|info:eu-repo/dai/nl/41249311X; Catlow, C. Richard A.; de Leeuw, Nora H.|info:eu-repo/dai/nl/376421061

    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

  2. Atomic and molecular adsorption on transition-metal carbide (111) surfaces from density-functional theory: a trend study of surface electronic factors

    DEFF Research Database (Denmark)

    Vojvodic, Aleksandra; Ruberto, C.; Lundqvist, Bengt

    2010-01-01

    This study explores atomic and molecular adsorption on a number of early transition-metal carbides (TMCs) in NaCl structure by means of density-functional theory calculations. The investigated substrates are the TM-terminated TMC(111) surfaces, of interest because of the presence of different types......, surface relaxations, Bader charges, and surface-localized densities of states (DOSs). Detailed comparisons between surface and bulk DOSs reveal the existence of transition-metal localized SRs (TMSRs) in the pseudogap and of several C-localized SRs (CSRs) in the upper valence band on all considered TMC(111......) surfaces. The spatial extent and the dangling bond nature of these SRs are supported by real-space analyses of the calculated Kohn-Sham wavefunctions. Then, atomic and molecular adsorption energies, geometries, and charge transfers are presented. An analysis of the adsorbate-induced changes in surface DOSs...

  3. Surface science of DNA adsorption onto citrate-capped gold nanoparticles.

    Science.gov (United States)

    Zhang, Xu; Servos, Mark R; Liu, Juewen

    2012-02-28

    Single-stranded DNA can be adsorbed by citrate capped gold nanoparticles (AuNPs), resulting in increased AuNP stability, which forms the basis of a number of biochemical and analytical applications, but the fundamental interaction of this adsorption reaction remains unclear. In this study, we measured DNA adsorption kinetics, capacity, and isotherms, demonstrating that the adsorption process is governed by electrostatic forces. The charge repulsion among DNA strands and between DNA and AuNPs can be reduced by adding salt, reducing pH or by using noncharged peptide nucleic acid (PNA). Langmuir adsorption isotherms are obtained, indicating the presence of both adsorption and desorption of DNA from AuNPs. While increasing salt concentration facilitates DNA adsorption, the desorption rate is also enhanced in higher salt due to DNA compaction. DNA adsorption capacity is determined by DNA oligomer length, DNA concentration, and salt. Previous studies indicated faster adsorption of short DNA oligomers by AuNPs, we find that once adsorbed, longer DNAs are much more effective in protecting AuNPs from aggregation. DNA adsorption is also facilitated by using low pH buffers and high alcohol concentrations. A model based on electrostatic repulsion on AuNPs is proposed to rationalize the DNA adsorption/desorption behavior. © 2012 American Chemical Society

  4. First principles study of elemental mercury (Hg0) adsorption on low index CoMnO3 surfaces

    International Nuclear Information System (INIS)

    Ji, Wenchao; Su, Pingru; Tang, Qingli; Cheng, Zhiwen; Shen, Zhemin; Fan, Maohong

    2017-01-01

    Highlights: • Hg 0 adsorption on low index CoMnO 3 surface was predicted by DFT method. • Hg 0 is adsorbed on the CoMnO 3 surface with chemisorption interaction. • Hg 0 has highest adsorption energy on CoMnO 3 (1 0 0) surface with Hg-Mn mechanism. • The electron transfer of Hg 0 has positive relationship with adsorption energy. - Abstract: The density functional theory (DFT) is applied to predict elemental mercury (Hg 0 ) adsorption on CoMnO 3 surface for the first time. GGA/PBE functional were selected to determine the potential Hg 0 capture mechanisms. The results show that Hg 0 has good affinity with CoMnO 3 surfaces with chemical adsorption. The adsorption energy of Hg 0 -CoMnO 3 (1 0 0), Hg 0 -CoMnO 3 (1 0 1) and Hg 0 -CoMnO 3 (1 1 0) are −85.225, −72.305 and −70.729 kJ/mol, respectively. The Hg-Mn and Hg-Co mechanisms were revealed on low index surfaces. Hg 0 was oxidized to its valence state of 0.236 on Mn site in CoMnO 3 (1 0 0) surface. The Hg-Co interaction mechanism occurred on Hg 0 -CoMnO 3 (1 0 1) and Hg 0 -CoMnO 3 (1 1 0) with 0.209e − and 0.189e − transformation, respectively. The PDOS analysis shows that Hg-Mn interaction depends on the hybridization of Hg(s- and d-orbitals) and Mn (s-, p- and d- orbitals). However, Hg-Co interaction stems from s- and d- orbitals of Hg, which only overlapping with d- and p- orbital of Co. Both the adsorption energy and electronic structure analysis indicated that CoMnO 3 catalyst performed excellent in Hg 0 oxidation. Exposing CoMnO 3 (1 0 0) is most favorable in Hg 0 control, which provides theoretical instruction on certain crystal plane synthesis in experiment.

  5. Surface Adsorption of Oppositely Charged SDS:C(12)TAB Mixtures and the Relation to Foam Film Formation and Stability.

    Science.gov (United States)

    Fauser, Heiko; Uhlig, Martin; Miller, Reinhard; von Klitzing, Regine

    2015-10-08

    The complexation, surface adsorption, and foam film stabiliztation of the oppositely charged surfactants, sodium dodecyl sulfate (SDS) and dodecyl trimethylammonium bromide (C12TAB), is analyzed. The SDS:C12TAB mixing ratio is systematically varied to investigate whether the adsorption of equimolar or irregular catanionic surfactant complexes, and thus a variation in surface charge (i.e., surface excess of either SDS or C12TAB), governs foam film properties. Surface tension measurements indicate that SDS and C12TAB interact electrostatically in order to form stoichometric catanionic surfactant complexes and enhance surface adsorption. On the other hand it can be demonstrated that the SDS:C12TAB mixing ratio and, thus, a change in surface charge and composition plays a decisive role in foam film stabilization. The present study demonstrates that varying the mixing ratio between SDS and C12TAB offers a tool for tailoring surface composition and foam film properties, which are therefore not exclusively mediated by the presence of equimolar catanionic surfactant complexes. The SDS:C12TAB net amount and mixing ratio determine the type, stability, and thinning behavior of the corresponding foam film. These observations indicate the formation of a mixed surface layer, composed of the catanionic surfactant species surrounded by either free SDS or C12TAB molecules in excess. Furthermore, a systematic variation in CBF-NBF transition kinetics is rationalized on the basis of a microscopic phase transition within the foam films. Fundamental knowlegde gained from this research gives insight into the surface adsorption and foam film formation of catanionic surfactant mixtures. The study helps researchers to understand basic mechanisms of foam film stabilization and to use resources more efficiently.

  6. Adsorptive kinetic mechanism of heavy metal cations on the surface of graphite oxide and its SiO2 composite

    Science.gov (United States)

    Sheet, Imtithal; Kabbani, Ahmad; Holail, Hanafy

    2017-02-01

    Nanomaterials have gained great attention because of their novel size- and shape-dependent properties, large specific surface area and high reaction activity. Moreover, nanomaterials have a wide range of applications, as in the technological and environmental challenges in the areas of solar energy conversion, catalysis, medicine, and water treatments. In the present study, nanostructured graphite oxide, silica/graphite oxide composites and silica nanoparticles were used for the removal of the heavy metal ions from aqueous solutions by a batch adsorption method and the adsorptive kinetic mechanism of heavy metal cations on the surface of graphite oxide and its SiO2 composite was evaluated. The experimental results revealed a strong adsorption of the metal cations on the surface of graphite oxide, this is reflected in the shifts in wave numbers after adsorption with nanostructured graphite oxide and the big shift in wave numbers (Δv¯) for nickel ions reflects chemosorption type of adsorption. This is confirmed by the coherence between Δv¯, removal percentage and crystal field stabilization energy (CFSE). Silica/ GO (2:3) composite showed the greatest removal percentage at different concentrations compared to pure graphite oxide and silica nanoparticles. The higher removal percentage of nickel ions by silica /GO composite (2:3) was observed at 180 min contact time and basic pH. The kinetic studies showed that silica/ GO (2:3) composite had rapid adsorption rate and efficiency and it was found to follow first order rate expression or an exponential decay of the metal cations from water study.

  7. The toxicity of plastic nanoparticles to green algae as influenced by surface modification, medium hardness and cellular adsorption

    Energy Technology Data Exchange (ETDEWEB)

    Nolte, Tom M., E-mail: T.Nolte@science.ru.nl [Department of Environmental Engineering, Technical University of Denmark, Miljøvej, B113, 2800 Kgs. Lyngby (Denmark); Radboud University Nijmegen, Institute for Water and Wetland Research, Department of Environmental Science, P.O. Box 9010, NL-6500 GL, Nijmegen (Netherlands); Hartmann, Nanna B. [Department of Environmental Engineering, Technical University of Denmark, Miljøvej, B113, 2800 Kgs. Lyngby (Denmark); Kleijn, J. Mieke [Physical Chemistry Soft Matter, Wageningen University, Stippeneng 4, NL-6708WE Wageningen (Netherlands); Garnæs, Jørgen [Danish Fundamental Metrology, Matematiktorvet 307, 2800 Kgs. Lyngby (Denmark); Meent, Dik van de [Radboud University Nijmegen, Institute for Water and Wetland Research, Department of Environmental Science, P.O. Box 9010, NL-6500 GL, Nijmegen (Netherlands); National Institute of Public Health and the Environment RIVM, P.O. Box 1, 3720 BA, Bilthoven (Netherlands); Jan Hendriks, A. [Radboud University Nijmegen, Institute for Water and Wetland Research, Department of Environmental Science, P.O. Box 9010, NL-6500 GL, Nijmegen (Netherlands); Baun, Anders [Department of Environmental Engineering, Technical University of Denmark, Miljøvej, B113, 2800 Kgs. Lyngby (Denmark)

    2017-02-15

    Highlights: • P. subcapitata cultures were exposed to plastic nanoparticles in adsorption assays. • UV/Vis and AFM showed ionic strength and surface chemistry influence adsorption of anionic and neutral nanoplastics. • Growth inhibition of algae is antagonistically influenced by carboxylate-modified polystyrene and calcium. • Physico-chemical characterization and proper dose metrics can be used to predict ecotoxicity. - Abstract: To investigate processes possibly underlying accumulation and ecological effects of plastic nano-particles we have characterized their interaction with the cell wall of green algae. More specifically, we have investigated the influence of particle surface functionality and water hardness (Ca{sup 2+} concentration) on particle adsorption to algae cell walls. Polystyrene nanoparticles with different functional groups (non-functionalized, −COOH and −NH{sub 2}) as well as coated (starch and PEG) gold nanoparticles were applied in these studies. Depletion measurements and atomic force microscopy (AFM) showed that adsorption of neutral and positively charged plastic nanoparticles onto the cell wall of P. subcapitata was stronger than that of negatively charged plastic particles. Results indicated that binding affinity is a function of both inter-particle and particle-cell wall interactions which are in turn influenced by the medium hardness and particle concentration. Physicochemical modelling using DLVO theory was used to interpret the experimental data, using also values for interfacial surface free energies. Our study shows that material properties and medium conditions play a crucial role in the rate and state of nanoparticle bio-adsorption for green algae. The results show that the toxicity of nanoparticles can be better described and assessed by using appropriate dose metrics including material properties, complexation/agglomeration behavior and cellular attachment and adsorption. The applied methodology provides an efficient

  8. Use of response surface methodology for optimization of fluoride adsorption in an aqueous solution by Brushite

    Directory of Open Access Journals (Sweden)

    M. Mourabet

    2017-05-01

    Full Text Available In the present study, Response surface methodology (RSM was employed for the removal of fluoride on Brushite and the process parameters were optimized. Four important process parameters including initial fluoride concentration (40–50 mg/L, pH (4–11, temperature (10–40 °C and B dose (0.05–0.15 g were optimized to obtain the best response of fluoride removal using the statistical Box–Behnken design. The experimental data obtained were analyzed by analysis of variance (ANOVA and fitted to a second-order polynomial equation using multiple regression analysis. Numerical optimization applying desirability function was used to identify the optimum conditions for maximum removal of fluoride. The optimum conditions were found to be initial concentration = 49.06 mg/L, initial solution pH = 5.36, adsorbent dose = 0.15 g and temperature = 31.96 °C. A confirmatory experiment was performed to evaluate the accuracy of the optimization procedure and maximum fluoride removal of 88.78% was achieved under the optimized conditions. Several error analysis equations were used to measure the goodness-of-fit. Kinetic studies showed that the adsorption followed a pseudo-second order reaction. The equilibrium data were analyzed using Langmuir, Freundlich, and Sips isotherm models at different temperatures. The Langmuir model was found to be describing the data. The adsorption capacity from the Langmuir isotherm (QL was found to be 29.212, 35.952 and 36.260 mg/g at 298, 303, and 313 K respectively.

  9. Effect of surfaces similarity on contact resistance of fractal rough surfaces under cyclic loading

    Science.gov (United States)

    Gao, Yuanwen; Liu, Limei; Ta, Wurui; Song, Jihua

    2018-03-01

    Although numerous studies have shown that contact resistance depends significantly on roughness and fractal dimension, it remains elusive how they affect contact resistance between rough surfaces. The interface similarity index is first proposed to describe the similarity of the contact surfaces, which gives a good indication of the actual contact area between surfaces. We reveal that the surfaces' similarity be an origin of contact resistance variation. The cyclic loading can increase the contact stiffness, and the contact stiffness increases with the increase of the interface similarity index. These findings explain the mechanism of surface roughness and fractal dimension on contact resistance, and also provide reference for the reliability design of the electrical connection.

  10. 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.

  11. Surface morphology and corrosion resistance of electrodeposited ...

    Indian Academy of Sciences (India)

    Electrochemical corrosion resistance investigations were carried out in 5 M KOH, using potentiodynamic and electrochemical impedance spectroscopy (EIS) methods. On the basis of these investigations it was found, that the composite coatings containing thiophene are more corrosion resistant in alkaline solution than the ...

  12. In situ identification of the adsorption of 4,4'-thiobisbenzenethiol on silver nanoparticles surface: a combined investigation of surface-enhanced Raman scattering and density functional theory study.

    Science.gov (United States)

    You, Ting-ting; Yin, Peng-gang; Jiang, Li; Lang, Xiu-feng; Guo, Lin; Yang, Shi-he

    2012-05-21

    We investigated the configuration characteristic and adsorption behavior of 4,4'-thiobisbenzenethiol (TBBT) on the surface of silver nanoparticles (NPs). Under different conditions and preparation processes, several possible surface species were produced including single-end adsorption on a silicon wafer, double-end adsorption and bridge-like adsorption. Although consisting of the same molecule and nano material, different adsorption systems exhibited different spectral characteristics in the surface-enhanced Raman spectroscopy (SERS). A density functional theory (DFT) study further verified the corresponding adsorption states. The combined SERS-DFT study provided a framework towards investigating and designing adsorption systems at a molecular level, indicating the potential use in applications such as nano-sensors.

  13. Atom and Amine Adsorption on Flat and Stepped Gold Surfaces & Structure, Stability and Spin Ordering in Manganese Sulfide Clusters

    Science.gov (United States)

    Lewoczko, April D.

    In part I, we investigate gold catalysis in the chemistry of organonitrogen compounds. We examine the adsorption of oxygen, nitrogen and sulfur atoms on the gold (111), (100) and (211) surfaces using density functional theory (DFT). Sulfur atoms bind most strongly, followed by oxygen and nitrogen atoms with stronger adsorption for greater coordination to the surface. We see a trend of stronger adsorption to undercoordinated gold, but find it is non-universal with the adsorption strength trend: (111) > (211) > (100). We consider the diffusion of oxygen, nitrogen and sulfur adatoms and find facile long-range diffusion of oxygen atoms on the (100) surface. Lastly, we compare the adsorption of methylamine on gold to that of a selection of alkylamines, methanol and methanethiol. In each case, the ontop site is preferred with stronger adsorption at low coordinated gold. At oxygen atom coverages of 0.125 -- 0.25 ML on Au (111), we find cooperative adsorption of methylamine and oxygen atoms. Energetic costs for adsorbate tilt from the surface normal and rotation about the gold-nitrogen bond are calculated. While methylamine rotation is barrierless on the (111) and (211) surfaces, it has a low energetic barrier for the 0.125 ML and 0.25 ML O atom pre-covered Au (111) surfaces. In part II, we interpret the experimental mass spectrum of small gas phase manganese sulfide clusters using DFT and elucidate the role of ionicity and spin ordering in sizes with special stability, i.e. magic clusters. We first consider nine low lying minima (MnS)6 structures and reveal antiferromagnetic (AFM) spin ordering with a ˜0.1 eV/pair AFM energy benefit and a ˜0.1 A shrinkage of average Mn-Mn distances over clusters with ferromagnetic (FM) spin ordering. We calculate energetic barriers for interconversion between the two lowest lying (MnS)6 isomers and predict an elevated cluster melting temperature due to increased configurational entropy in a pre-melted state. Second, we demonstrate the

  14. Adsorption of active ingredients of surface disinfectants depends on the type of fabric used for surface treatment.

    Science.gov (United States)

    Bloss, R; Meyer, S; Kampf, G

    2010-05-01

    The disinfection of surfaces in the immediate surrounding of a hospitalised patient is considered to be an important element for prevention of nosocomial infection. The type of fabric in a mop, however, has to our knowledge never been regarded as relevant for an effective disinfection of surfaces. We have therefore studied the adsorption of benzalkonium chloride (BAC), glutardialdehyde and propan-1-ol from working solutions of three surface disinfectants to four different types of fabric (A: white pulp and polyester; B: viscose rayon; C: polyester; D: mixture of viscose, cellulose and polyester). The working solutions of each disinfectant were exposed to each fabric for up to 24h. Before and after exposure, tissues were removed and squeezed in a standardised way. The eluate was used for determination of the concentration of the active ingredient in quadruplicate. The analysis of glutardialdehyde and BAC was performed using high performance liquid chromatography; the analysis of propan-1-ol was done using gas chromatography. BAC was strongly adsorbed to the tissues based on white pulp (up to 61% after 30 min), followed by the viscose rayon tissues (up to 70% after 30 min) and the mixed tissues (up to 54% after 7h). The polyester fibre tissue adsorbed the smallest amounts of BAC with up to 17% after 15 min. Only with the polyester fibre tissue were BAC concentrations found in the range of the calculated BAC concentrations. Glutardialdehyde and propan-1-ol did not adsorb to any of the fibres. Effective surface disinfection also includes selection of an appropriate fabric. Copyright (c) 2009 The Hospital Infection Society. Published by Elsevier Ltd. All rights reserved.

  15. [Corrosion resistant properties of different anodized microtopographies on titanium surfaces].

    Science.gov (United States)

    Fangjun, Huo; Li, Xie; Xingye, Tong; Yueting, Wang; Weihua, Guo; Weidong, Tian

    2015-12-01

    To investigate the corrosion resistant properties of titanium samples prepared by anodic oxidation with different surface morphologies. Pure titanium substrates were treated by anodic oxidation to obtain porous titanium films in micron, submicron, and micron-submicron scales. The surface morphologies, coating cross-sectional morphologies, crystalline structures, and surface roughness of these samples were characterized. Electrochemical technique was used to measure the corrosion potential (Ecorr), current density of corrosion (Icorr), and polarization resistance (Rp) of these samples in a simulated body fluid. Pure titanium could be modified to exhibit different surface morphologies by the anodic oxidation technique. The Tafel curve results showed that the technique can improve the corrosion resistance of pure titanium. Furthermore, the corrosion resistance varied with different surface morphologies. The submicron porous surface sample demonstrated the best corrosion resistance, with maximal Ecorr and Rp and minimal Icorr. Anodic oxidation technology can improve the corrosion resistance of pure titanium in a simulated body fluid. The submicron porous surface sample exhibited the best corrosion resistance because of its small surface area and thick barrier layer.

  16. Pore Scale Heterogeneity in the Mineral Distribution, Surface Area and Adsorption in Porous Rocks

    Science.gov (United States)

    Lai, P. E. P.; Krevor, S. C.

    2014-12-01

    The impact of heterogeneity in chemical transport and reaction is not understood in continuum (Darcy/Fickian) models of reactive transport. This is manifested in well-known problems such as scale dependent dispersion and discrepancies in reaction rate observations made at laboratory and field scales [1]. Additionally, this is a source of uncertainty for carbon dioxide injection, which produces a reactive fluid-rock system particularly in carbonate rock reservoirs. A potential cause is the inability of the continuum approach to incorporate the impact of heterogeneity in pore-scale reaction rates. This results in part from pore-scale heterogeneities in surface area of reactive minerals [2, 3]. We use x-ray micro tomography to describe the non-normal 3-dimensional distribution of reactive surface area within a porous medium according to distinct mineral groups. Using in-house image processing techniques, thin sections, nitrogen BET surface area, backscattered electron imaging and energy dispersive spectroscopy, we compare the surface area of each mineral phase to those obtained from x-ray CT imagery. In all samples, there is little correlation between the reactive surface area fraction and the volumetric fraction of a mineral in a bulk rock. Berea sandstone was far less heterogeneous and has a characteristic pore size at which a surface area distribution may be used to quantify heterogeneity. In carbonates, heterogeneity is more complex and surface area must be characterized at multiple length scales for an accurate description of reactive transport. We combine the mineral specific surface area characterisation to dynamic tomography, imaging the flow of water and solutes, to observe flow dependent and mineral specific adsorption. The observations may contribute to the incorporation of experimentally based statistical descriptions of pore scale heterogeneity in reactive transport into upscaled models, moving it closer to predictive capabilities for field scale

  17. Adsorption of squaraine molecules to Au(111) and Ag(001) surfaces

    Science.gov (United States)

    Luft, Maike; Groß, Boris; Schulz, Matthias; Lützen, Arne; Schiek, Manuela; Nilius, Niklas

    2018-02-01

    The adsorption of anilino squar