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Sample records for catalytic hydrogen generation

  1. Formic Acid Free Flowsheet Development To Eliminate Catalytic Hydrogen Generation In The Defense Waste Processing

    Energy Technology Data Exchange (ETDEWEB)

    Lambert, Dan P.; Stone, Michael E.; Newell, J. David; Fellinger, Terri L.; Bricker, Jonathan M.

    2012-09-14

    The Defense Waste Processing Facility (DWPF) processes legacy nuclear waste generated at the Savannah River Site (SRS) during production of plutonium and tritium demanded by the Cold War. The nuclear waste is first treated via a complex sequence of controlled chemical reactions and then vitrified into a borosilicate glass form and poured into stainless steel canisters. Converting the nuclear waste into borosilicate glass canisters is a safe, effective way to reduce the volume of the waste and stabilize the radionuclides. Testing was initiated to determine whether the elimination of formic acid from the DWPF's chemical processing flowsheet would eliminate catalytic hydrogen generation. Historically, hydrogen is generated in chemical processing of alkaline High Level Waste sludge in DWPF. In current processing, sludge is combined with nitric and formic acid to neutralize the waste, reduce mercury and manganese, destroy nitrite, and modify (thin) the slurry rheology. The noble metal catalyzed formic acid decomposition produces hydrogen and carbon dioxide. Elimination of formic acid by replacement with glycolic acid has the potential to eliminate the production of catalytic hydrogen. Flowsheet testing was performed to develop the nitric-glycolic acid flowsheet as an alternative to the nitric-formic flowsheet currently being processed at the DWPF. This new flowsheet has shown that mercury can be reduced and removed by steam stripping in DWPF with no catalytic hydrogen generation. All processing objectives were also met, including greatly reducing the Slurry Mix Evaporator (SME) product yield stress as compared to the baseline nitric/formic flowsheet. Ten DWPF tests were performed with nonradioactive simulants designed to cover a broad compositional range. No hydrogen was generated in testing without formic acid.

  2. Elimination Of Catalytic Hydrogen Generation In Defense Waste Processing Facility Slurries

    Energy Technology Data Exchange (ETDEWEB)

    Koopman, D. C.

    2013-01-22

    Based on lab-scale simulations of Defense Waste Processing Facility (DWPF) slurry chemistry, the addition of sodium nitrite and sodium hydroxide to waste slurries at concentrations sufficient to take the aqueous phase into the alkaline region (pH > 7) with approximately 500 mg nitrite ion/kg slurry (assuming <25 wt% total solids, or equivalently 2,000 mg nitrite/kg total solids) is sufficient to effectively deactivate the noble metal catalysts at temperatures between room temperature and boiling. This is a potential strategy for eliminating catalytic hydrogen generation from the list of concerns for sludge carried over into the DWPF Slurry Mix Evaporator Condensate Tank (SMECT) or Recycle Collection Tank (RCT). These conclusions are drawn in large part from the various phases of the DWPF catalytic hydrogen generation program conducted between 2005 and 2009. The findings could apply to various situations, including a solids carry-over from either the Sludge Receipt and Adjustment Tank (SRAT) or Slurry Mix Evaporator (SME) into the SMECT with subsequent transfer to the RCT, as well as a spill of formic acid into the sump system and transfer into an RCT that already contains sludge solids. There are other potential mitigating factors for the SMECT and RCT, since these vessels are typically operated at temperatures close to the minimum temperatures that catalytic hydrogen has been observed to occur in either the SRAT or SME (pure slurry case), and these vessels are also likely to be considerably more dilute in both noble metals and formate ion (the two essential components to catalytic hydrogen generation) than the two primary process vessels. Rhodium certainly, and ruthenium likely, are present as metal-ligand complexes that are favored under certain concentrations of the surrounding species. Therefore, in the SMECT or RCT, where a small volume of SRAT or SME material would be significantly diluted, conditions would be less optimal for forming or sustaining the

  3. Marrying gas power and hydrogen energy: A catalytic system for combining methane conversion and hydrogen generation

    NARCIS (Netherlands)

    J. Beckers; C. Gaudillère; D. Farrusseng; G. Rothenberg

    2009-01-01

    Ceria-based catalysts are good candidates for integrating methane combustion and hydrogen generation. These new, tuneable catalysts are easily prepared. They are robust inorganic crystalline materials, and perform well at the 400 °C-550 °C range, in some cases even without precious metals. This make

  4. CATALYTIC INTERACTIONS OF RHODIUM, RUTHENIUM, AND MERCURY DURING SIMULATED DWPF CPC PROCESSING WITH HYDROGEN GENERATION

    Energy Technology Data Exchange (ETDEWEB)

    Koopman, D

    2008-10-09

    Simulations of the Defense Waste Processing Facility (DWPF) Chemical Processing Cell (CPC) vessels were performed as part of the ongoing investigation into catalytic hydrogen generation. Rhodium, ruthenium, and mercury have been identified as the principal elemental factors affecting the peak hydrogen generation rate in the DWPF Sludge Receipt and Adjustment Tank (SRAT) for a given acid addition. The primary goal of this study is to identify any significant interactions between the three factors. Noble metal concentrations were similar to recent sludge batches. Rh ranged from 0.0026-0.013% and Ru ranged from 0.010-0.050% in the dried sludge solids, while initial Hg ranged from 0.5-2.5 wt%. An experimental matrix was developed to ensure that the existence of statistically significant two-way interactions could be determined without confounding of the main effects with the two-way interaction effects. The nominal matrix design consisted of twelve SRAT cycles. Testing included: a three factor (Rh, Ru, and Hg) study at two levels per factor (eight runs), two duplicate midpoint runs, and two additional replicate runs to assess reproducibility away from the midpoint. Midpoint testing can identify potential quadratic effects from the three factors. A single sludge simulant was used for all tests. Acid addition was kept effectively constant except to compensate for variations in the starting mercury concentration. Six Slurry Mix Evaporator (SME) cycles were performed to supplement the SME hydrogen generation database. Some of the preliminary findings from this study include: (1) Rh was linked to the maximum SRAT hydrogen generation rate in the first two hours after acid addition in preliminary statistical modeling. (2) Ru was linked conclusively to the maximum SRAT hydrogen generation rate in the last four hours of reflux in preliminary statistical modeling. (3) Increasing the ratio of Hg/Rh shifted the noble metal controlling the maximum SRAT hydrogen generation rate from

  5. Catalytic combustor for hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Mercea, J.; Grecu, E.; Fodor, T.; Kreibik, S.

    1982-01-01

    The performance of catalytic combustors for hydrogen using platinum-supported catalysts is described. Catalytic plates of different sizes were constructed using fibrous and ceramic supports. The temperature distribution as well as the reaction efficiency as a function of the fuel input rate was determined, and a comparison between the performances of different plates is discussed.

  6. Evidence of catalytic production of hot hydrogen in rf generated hydrogen/argon plasmas

    CERN Document Server

    Phillips, J; Akhtar, K; Dhandapani, B; Mills, R; Phillips, Jonathan; Chen, Chun-Ku; Akhtar, Kamran; Dhandapani, Bala; Mills, Randell

    2005-01-01

    In this paper the selective broadening of the atomic hydrogen lines in pure H2 and Ar/H2 mixtures in a large 'GEC' cell (36 cm length_ 14 cm ID) was mapped as a function of position, H2/Ar ratio, time, power, and pressure. Several observations regarding the selective line broadening were particularly notable as they are unanticipated on the basis of earlier models. First, the anomalous broadening of the Balmer lines was found to exist throughout the plasma, and not just in the region between the electrodes. Second, the broadening was consistently a complex function of the operating parameters particularly gas composition (highest in pure H2), position, power, time and pressure. Clearly not anticipated by earlier models were the findings that under some conditions the highest concentration of 'hot' (>10 eV) hydrogen was found at the entry end, and not in the high field region between the electrodes and that in other conditions, the hottest H was at the (exit) pump (also grounded electrode) end. Third, excitati...

  7. Catalytic hydrolysis of ammonia borane for hydrogen generation using cobalt nanocluster catalyst supported on polydopamine functionalized multiwalled carbon nanotube

    International Nuclear Information System (INIS)

    Hydrogen was generated from ammonia borane complex by hydrolysis using cobalt nanocluster catalyst supported on polydopamine functionalized MWCNTs (multi-walled carbon nanotubes). The impregnation-chemical reduction method was used for the preparation of the supported catalyst. The nanocluster catalyst support was formed by in-situ oxidative polymerization of dopamine on the MWCNTs in alkaline solution at room temperature. The structural and physical–chemical properties of the nanocluster catalyst were characterized by FT-IR (Fourier transform infrared spectroscopy), EDX (energy-dispersive X-ray spectroscopy), SEM (scanning electron microscope), XRD (X-ray diffraction) and TEM (transmission electron microscopy). The nanocluster catalyst showed good catalytic activity for the hydrogen generation from aqueous ammonia borane complex. A reusability test to determine the practical usage of the catalyst was also investigated. The result revealed that the catalyst maintained an appreciable catalytic performance and stability in terms of its reusability after three cycle of reuse for the hydrolysis reaction. Also, the activation energy for the hydrolysis of ammonia borane complex was estimated to be 50.41 kJmol−1, which is lower than the values of some of the reported catalyst. The catalyst can be considered as a promising candidate in developing highly efficient portable hydrogen generation systems such as PEMFC (proton exchange membrane fuel cells). - Highlights: • Co/Pdop-o-MWCNT (Pdop functionalized MWCNT supported cobalt nanocluster) catalyst was synthesized for hydrogen generation. • It is an active catalyst for hydrogen generation via hydrolysis of ammonia borane. • It showed good stability in terms of reusability for the hydrogen generation

  8. A novel liquid system of catalytic hydrogenation

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    On the basis that endothermic aqueous-phase reforming of oxygenated hydrocarbons for H2 production and exothermic liquid phase hydrogenation of organic compounds are carried out under extremely close conditions of temperature and pressure over the same type of catalyst, a novel liquid system of catalytic hydrogenation has been proposed, in which hydrogen produced from aqueous-phase reforming of oxygenated hydrocarbons is in situ used for liquid phase hydrogenation of organic compounds. The usage of active hydrogen generated from aqueous-phase reforming of oxygenated hydrocarbons for liquid catalytic hydrogenation of organic compounds could lead to increasing the selectivity to H2 in the aqueous-phase reforming due to the prompt removal of hydrogen on the active centers of the catalyst. Meanwhile, this novel liquid system of catalytic hydrogenation might be a potential method to improve the selectivity to the desired product in liquid phase catalytic hydrogenation of organic compounds. On the other hand, for this novel liquid system of catalytic hydrogenation, some special facilities for H2 generation, storage and transportation in traditional liquid phase hydrogenation industry process are yet not needed. Thus, it would simplify the working process of liquid phase hydrogenation and increase the energy usage and hydrogen productivity.

  9. Complexes of earth-abundant metals for catalytic electrochemical hydrogen generation under aqueous conditions.

    Science.gov (United States)

    Thoi, V Sara; Sun, Yujie; Long, Jeffrey R; Chang, Christopher J

    2013-03-21

    Growing global energy demands and climate change motivate the development of new renewable energy technologies. In this context, water splitting using sustainable energy sources has emerged as an attractive process for carbon-neutral fuel cycles. A key scientific challenge to achieving this overall goal is the invention of new catalysts for the reductive and oxidative conversions of water to hydrogen and oxygen, respectively. This review article will highlight progress in molecular electrochemical approaches for catalytic reduction of protons to hydrogen, focusing on complexes of earth-abundant metals that can function in pure aqueous or mixed aqueous-organic media. The use of water as a reaction medium has dual benefits of maintaining high substrate concentration as well as minimizing the environmental impact from organic additives and by-products. PMID:23034627

  10. Complexes of earth-abundant metals for catalytic electrochemical hydrogen generation under aqueous conditions.

    Science.gov (United States)

    Thoi, V Sara; Sun, Yujie; Long, Jeffrey R; Chang, Christopher J

    2013-03-21

    Growing global energy demands and climate change motivate the development of new renewable energy technologies. In this context, water splitting using sustainable energy sources has emerged as an attractive process for carbon-neutral fuel cycles. A key scientific challenge to achieving this overall goal is the invention of new catalysts for the reductive and oxidative conversions of water to hydrogen and oxygen, respectively. This review article will highlight progress in molecular electrochemical approaches for catalytic reduction of protons to hydrogen, focusing on complexes of earth-abundant metals that can function in pure aqueous or mixed aqueous-organic media. The use of water as a reaction medium has dual benefits of maintaining high substrate concentration as well as minimizing the environmental impact from organic additives and by-products.

  11. Identification of intrinsic catalytic activity for electrochemical reduction of water molecules to generate hydrogen

    KAUST Repository

    Shinagawa, Tatsuya

    2015-01-01

    Insufficient hydronium ion activities at near-neutral pH and under unbuffered conditions induce diffusion-limited currents for hydrogen evolution, followed by a reaction with water molecules to generate hydrogen at elevated potentials. The observed constant current behaviors at near neutral pH reflect the intrinsic electrocatalytic reactivity of the metal electrodes for water reduction. This journal is © the Owner Societies.

  12. Hydrogen Generation from Catalytic Steam Reforming of Acetic Acid by Ni/Attapulgite Catalysts

    Directory of Open Access Journals (Sweden)

    Yishuang Wang

    2016-11-01

    Full Text Available In this research, catalytic steam reforming of acetic acid derived from the aqueous portion of bio-oil for hydrogen production was investigated using different Ni/ATC (Attapulgite Clay catalysts prepared by precipitation, impregnation and mechanical blending methods. The fresh and reduced catalysts were characterized by XRD, N2 adsorption–desorption, TEM and temperature program reduction (H2-TPR. The comprehensive results demonstrated that the interaction between active metallic Ni and ATC carrier was significantly improved in Ni/ATC catalyst prepared by precipitation method, from which the mean of Ni particle size was the smallest (~13 nm, resulting in the highest metal dispersion (7.5%. The catalytic performance of the catalysts was evaluated by the process of steam reforming of acetic acid in a fixed-bed reactor under atmospheric pressure at two different temperatures: 550 °C and 650 °C. The test results showed the Ni/ATC prepared by way of precipitation method (PM-Ni/ATC achieved the highest H2 yield of ~82% and a little lower acetic acid conversion efficiency of ~85% than that of Ni/ATC prepared by way of impregnation method (IM-Ni/ATC (~95%. In addition, the deactivation catalysts after reaction for 4 h were analyzed by XRD, TGA-DTG and TEM, which demonstrated the catalyst deactivation was not caused by the amount of carbon deposition, but owed to the significant agglomeration and sintering of Ni particles in the carrier.

  13. HYDROGEN TRANSFER IN CATALYTIC CRACKING

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Hydrogen transfer is an important secondary reaction of catalytic cracking reactions, which affects product yield distribution and product quality. It is an exothermic reaction with low activation energy around 43.3 kJ/mol. Catalyst properties and operation parameters in catalytic cracking greatly influence the hydrogen transfer reaction. Satisfactory results are expected through careful selection of proper catalysts and operation conditions.

  14. Hydrogen generation from catalytic hydrolysis of sodium borohydride solution using Cobalt-Copper-Boride (Co-Cu-B) catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Xin-Long; Yuan, Xianxia; Jia, Chao; Ma, Zi-Feng [Department of Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240 (China)

    2010-10-15

    Co-Cu-B, as a catalyst toward hydrolysis of sodium borohydride solution, has been prepared through chemical reduction of metal salts, CoCl{sub 2}.6H{sub 2}O and CuCl{sub 2}, by an alkaline solution composed of 7.5wt% NaBH{sub 4} and 7.5wt% NaOH. The effects of Co/Cu molar ratio, calcination temperature, NaOH and NaBH{sub 4} concentration and reaction temperature on catalytic activity of Co-Cu-B for hydrogen generation from alkaline NaBH{sub 4} solution have been studied. X-ray diffraction (XRD), scanning electron microscope (SEM) and Nitrogen adsorption-desorption isotherm have been employed to understand the results. The Co-Cu-B catalyst with a Co/Cu molar ratio of 3:1 and calcinated at 400 C showed the best catalytic activity at ambient temperature. The activation energy of this catalytic reaction is calculated to be 49.6 kJ mol{sup -1}. (author)

  15. Facile synthesis of polypyrrole functionalized nickel foam with catalytic activity comparable to Pt for the poly-generation of hydrogen and electricity

    Science.gov (United States)

    Tang, Tiantian; Li, Kan; Shen, Zhemin; Sun, Tonghua; Wang, Yalin; Jia, Jinping

    2016-01-01

    Polypyrrole functionalized nickel foam is facilely prepared through the potentiostatic electrodeposition. The PPy-functionalized Ni foam functions as a hydrogen-evolution cathode in a rotating disk photocatalytic fuel cell, in which hydrogen energy and electric power are generated by consuming organic wastes. The PPy-functionalized Ni foam cathode exhibits stable catalytic activities after thirteen continuous runs. Compared with net or plate structure, the Ni foam with a unique three-dimensional reticulate structure is conducive to the electrodeposition of PPy. Compared with Pt-group electrode, PPy-coated Ni foam shows a satisfactory catalytic performance for the H2 evolution. The combination of PPy and Ni forms a synergistic effect for the rapid trapping and removal of proton from solution and the catalytic reduction of proton to hydrogen. The PPy-functionalized Ni foam could be applied in photocatalytic and photoelectrochemical generation of H2. In all, we report a low cost, high efficient and earth abundant PPy-functionalized Ni foam with a satisfactory catalytic activities comparable to Pt for the practical application of poly-generation of hydrogen and electricity.

  16. Catalytic hydro desulphurization study of heavy petroleum residue through in situ generated hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Shakirullah, Mohammad; Ahmad, Imtiaz; Ishaq, Mohammad; Ahmad, Waqas [Institute of Chemical Sciences, N.W.F.P., University of Peshawar, 25120 Peshawar (Pakistan)

    2010-05-15

    Hydrodesulphurization of heavy residue was carried out using various catalysts in the presence of co-reactants as the internal sources of hydrogen. Reactions were carried out in a micro autoclave at 320 C and 10 kg f/cm{sup 2} pressure inert atmosphere of N{sub 2} for 3 h reaction time. Tetralin, propane, methanol, ethylene glycol and formic acid were separately used as co-reactants as hydrogen donors. Among the solvents studied, methanol gave the highest hydrodesulphurization yield (52%). The reaction was then carried out in the presence of various catalysts to view the influence of each individual catalyst on the desulphurization yield under the same conditions of pressure and temperature. The catalysts used were Mo-Montmorillonite, Co-Montmorillonite, nickel oxide (NiO), cadmium oxide (CdO), Zn-ZSM5, kaolin and montmorillonite clays. The results show that all the catalysts exhibited desulphurization activity. In case of Mo-Montmorillonite and Co-Montmorillonite charges, the desulfurization yields of 63% and 46% were obtained, respectively. NiO, CdO, Zn-ZSM5, kaolin and montmorillonite clays gave desulphurization yields of 54%, 50%, 56%, 20% and 36%, respectively. The desulphurization activities of Mo-Montmorillonite and Co-Montmorillonite were compared with other catalysts used. The results show that Mo-Montmorillonite gave the highest hydrodesulphurization yield. FTIR studies also confirmed the hydrodesulphurization efficiency of the Mo-Montmorillonite. (author)

  17. Catalytic Hydrolysis of Ammonia Borane by Cobalt Nickel Nanoparticles Supported on Reduced Graphene Oxide for Hydrogen Generation

    Directory of Open Access Journals (Sweden)

    Yuwen Yang

    2014-01-01

    Full Text Available Well dispersed magnetically recyclable bimetallic CoNi nanoparticles (NPs supported on the reduced graphene oxide (RGO were synthesized by one-step in situ coreduction of aqueous solution of cobalt(II chloride, nickel (II chloride, and graphite oxide (GO with ammonia borane (AB as the reducing agent under ambient condition. The CoNi/RGO NPs exhibits excellent catalytic activity with a total turnover frequency (TOF value of 19.54 mol H2 mol catalyst−1 min−1 and a low activation energy value of 39.89 kJ mol−1 at room temperature. Additionally, the RGO supported CoNi NPs exhibit much higher catalytic activity than the monometallic and RGO-free CoNi counterparts. Moreover, the as-prepared catalysts exert satisfying durable stability and magnetically recyclability for the hydrolytic dehydrogenation of AB, which make the practical reusing application of the catalysts more convenient. The usage of the low-cost, easy-getting catalyst to realize the production of hydrogen under mild condition gives more confidence for the application of ammonia borane as a hydrogen storage material. Hence, this general method indicates that AB can be used as both a potential hydrogen storage material and an efficient reducing agent, and can be easily extended to facile preparation of other RGO-based metallic systems.

  18. Catalytic hydrogenation of carbon monoxide

    Energy Technology Data Exchange (ETDEWEB)

    Wayland, B.B.

    1992-12-01

    This project is focused on developing strategies to accomplish the reduction and hydrogenation of carbon monoxide to produce organic oxygenates at mild conditions. Our approaches to this issue are based on the recognition that rhodium macrocycles have unusually favorable thermodynamic values for producing a series of intermediate implicated in the catalytic hydrogenation of CO. Observations of metalloformyl complexes produced by reactions of H{sub 2} and CO, and reductive coupling of CO to form metallo {alpha}-diketone species have suggested a multiplicity of routes to organic oxygenates that utilize these species as intermediates. Thermodynamic and kinetic-mechanistic studies are used in constructing energy profiles for a variety of potential pathways, and these schemes are used in guiding the design of new metallospecies to improve the thermodynamic and kinetic factors for individual steps in the overall process. Variation of the electronic and steric effects associated with the ligand arrays along with the influences of the reaction medium provide the chemical tools for tuning these factors. Emerging knowledge of the factors that contribute to M-H, M-C and M-O bond enthalpies is directing the search for ligand arrays that will expand the range of metal species that have favorable thermodynamic parameters to produce the primary intermediates for CO hydrogenation. Studies of rhodium complexes are being extended to non-macrocyclic ligand complexes that emulate the favorable thermodynamic features associated with rhodium macrocycles, but that also manifest improved reaction kinetics. Multifunctional catalyst systems designed to couple the ability of rhodium complexes to produce formyl and diketone intermediates with a second catalyst that hydrogenates these imtermediates are promising approaches to accomplish CO hydrogenation at mild conditions.

  19. Magnetic Co@g-C3N4 Core-Shells on rGO Sheets for Momentum Transfer with Catalytic Activity toward Continuous-Flow Hydrogen Generation.

    Science.gov (United States)

    Duan, Shasha; Han, Guosheng; Su, Yongheng; Zhang, Xiaoyu; Liu, Yanyan; Wu, Xianli; Li, Baojun

    2016-06-28

    Magnetic core-shell structures provide abundant opportunities for the construction of multifunctional composites. In this article, magnetic core-shells were fabricated with Co nanoparticles (NPs) as cores and g-C3N4 as shells. In the fabrication process, the Co@g-C3N4 core-shells were anchored onto the rGO nanosheets to form a Co@g-C3N4-rGO composite (CNG-I). For hydrogen generation from the hydrolysis of NaBH4 or NH3BH3, the Co NP cores act as catalytic active sites. The g-C3N4 shells protect Co NPs cores from aggregating or growing. The connection between Co NPs and rGO was strengthened by the g-C3N4 shells to prevent them from leaching or flowing away. The g-C3N4 shells also work as a cocatalyst for hydrogen generation. The magnetism of Co NPs and the shape of rGO nanosheets achieve effective momentum transfer in the external magnetic field. In the batch reactor, a higher catalytic activity was obtained for CNG-I in self-stirring mode than in magneton stirring mode. In the continuous-flow process, stable hydrogen generation was carried out with CNG-I being fixed and propelled by the external magnetic field. The separation film is unnecessary because of magnetic momentum transfer. This idea of the composite design and magnetic momentum transfer will be useful for the development of both hydrogen generation and multifunctional composite materials. PMID:27276187

  20. Photo-stability of a-Si solar cells fabricated by “Liquid-Si printing method” and treated with catalytic generated atomic hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Murayama, Hiroko, E-mail: murayama.hiroko5@jp.panasonic.com [Device Solutions Center, Panasonic Corporation, 3-1-1 Yagumo-naka-machi, Moriguchi City, Osaka 570-8501 (Japan); Ohyama, Tatsushi; Yoshida, Isao; Terakawa, Akira [Device Solutions Center, Panasonic Corporation, 3-1-1 Yagumo-naka-machi, Moriguchi City, Osaka 570-8501 (Japan); Masuda, Takashi [Japan Advanced Institute of Science and Technology, 1-1 Asahidai, Nomi City, Ishikawa 923-1292 (Japan); JST-ERATO Shimoda Nano-Liquid Process Project, 1-1 Asahidai, Nomi City, Ishikawa 923-1292 (Japan); Ohdaira, Keisuke [Japan Advanced Institute of Science and Technology, 1-1 Asahidai, Nomi City, Ishikawa 923-1292 (Japan); Shimoda, Tatsuya [Japan Advanced Institute of Science and Technology, 1-1 Asahidai, Nomi City, Ishikawa 923-1292 (Japan); JST-ERATO Shimoda Nano-Liquid Process Project, 1-1 Asahidai, Nomi City, Ishikawa 923-1292 (Japan)

    2015-01-30

    The film properties and solar cell performances of hydrogenated amorphous silicon (a-Si:H) fabricated by a newly developed non-vacuum process “Liquid-Si printing method” were systematically investigated by comparing to the conventional plasma-chemical vapor deposition method. The as-printed a-Si:H films showed relatively high Urbach-tail characteristic energy (E{sub ch}), high [Si–H{sub 2}]/[Si–H], and low photoconductivity (~ 10{sup −7} S/cm). However, the [Si–H{sub 2}]/[Si–H] decreased, and the photoconductivity was improved to the device grade level (~ 10{sup −5} S/cm) after appropriate catalytic-generated atomic hydrogen treatment. It was also found that the light-induced degradation of the photoconductivity and solar cell efficiency of the printed samples were less than half of the conventional a-Si:H case.

  1. Photo-stability of a-Si solar cells fabricated by “Liquid-Si printing method” and treated with catalytic generated atomic hydrogen

    International Nuclear Information System (INIS)

    The film properties and solar cell performances of hydrogenated amorphous silicon (a-Si:H) fabricated by a newly developed non-vacuum process “Liquid-Si printing method” were systematically investigated by comparing to the conventional plasma-chemical vapor deposition method. The as-printed a-Si:H films showed relatively high Urbach-tail characteristic energy (Ech), high [Si–H2]/[Si–H], and low photoconductivity (~ 10−7 S/cm). However, the [Si–H2]/[Si–H] decreased, and the photoconductivity was improved to the device grade level (~ 10−5 S/cm) after appropriate catalytic-generated atomic hydrogen treatment. It was also found that the light-induced degradation of the photoconductivity and solar cell efficiency of the printed samples were less than half of the conventional a-Si:H case

  2. Numerical Study of Passive Catalytic Recombiner for Hydrogen Mitigation

    Directory of Open Access Journals (Sweden)

    Pavan K Sharma

    2010-10-01

    Full Text Available A significant amount of hydrogen is expected to be released within the containment of a water cooled power reactor after a severe accident. To reduce the risk of deflagration/detonation various means for hydrogen control have been adopted all over the world. Passive catalytic recombiner with vertical flat catalytic plate is one of such hydrogen mitigating device. Passive catalytic recombiners are designed for the removal of hydrogen generated in order to limit the impact of possible hydrogen combustion. Inside a passive catalytic recombiner, numerous thin steel sheets coated with catalyst material are vertically arranged at the bottom opening of a sheet metal housing forming parallel flow channels for the surrounding gas atmosphere. Already below conventional flammability limits, hydrogen and oxygen react exothermally on the catalytic surfaces forming harmless steam. Detailed numerical simulations and experiments are required for an in-depth knowledge of such plate type catalytic recombiners. Specific finite volume based in-house CFD code has been developed to model and analyse the working of these recombiner. The code has been used to simulate the recombiner device used in the Gx-test series of Battelle-Model Containment (B-MC experiments. The present paper briefly describes the working principle of such passive catalytic recombiner and salient feature of the CFD model developed at Bhabha Atomic Research Centre (BARC. Finally results of the calculations and comparison with existing data are discussed.

  3. Facile synthesis of near-monodisperse Ag-Ni core-shell nanoparticles and their application for catalytic generation of hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Guo Huizhang; Chen Yuanzhi; Chen Xiaozhen; Wen Ruitao; Yue Guanghui; Peng Dongliang, E-mail: yuanzhi@xmu.edu.cn, E-mail: dlpeng@xmu.edu.cn [Department of Materials Science and Engineering, College of Materials, Xiamen University, Xiamen 361005 (China)

    2011-05-13

    Magnetically recyclable Ag-Ni core-shell nanoparticles have been fabricated via a simple one-pot synthetic route using oleylamine both as solvent and reducing agent and triphenylphosphine as a surfactant. As characterized by transmission electron microscopy (TEM), the as-synthesized Ag-Ni core-shell nanoparticles exhibit a very narrow size distribution with a typical size of 14.9 {+-} 1.2 nm and a tunable shell thickness. UV-vis absorption spectroscopy study shows that the formation of a Ni shell on Ag core can damp the surface plasmon resonance (SPR) of the Ag core and lead to a red-shifted SPR absorption peak. Magnetic measurement indicates that all the as-synthesized Ag-Ni core-shell nanoparticles are superparamagnetic at room temperature, and their blocking temperatures can be controlled by modulating the shell thickness. The as-synthesized Ag-Ni core-shell nanoparticles exhibit excellent catalytic properties for the generation of H{sub 2} from dehydrogenation of sodium borohydride in aqueous solutions. The hydrogen generation rate of Ag-Ni core-shell nanoparticles is found to be much higher than that of Ag and Ni nanoparticles of a similar size, and the calculated activation energy for hydrogen generation is lower than that of many bimetallic catalysts. The strategy employed here can also be extended to other noble-magnetic metal systems.

  4. Catalytic glycerol steam reforming for hydrogen production

    Energy Technology Data Exchange (ETDEWEB)

    Dan, Monica, E-mail: monica.dan@itim-cj.ro; Mihet, Maria, E-mail: maria.mihet@itim-cj.ro; Lazar, Mihaela D., E-mail: diana.lazar@itim-cj.ro [National Institute for Research and Development of Isotopic and Molecular Technologies, 67-103 Donat Street, 400293 Cluj Napoca (Romania)

    2015-12-23

    Hydrogen production from glycerol by steam reforming combine two major advantages: (i) using glycerol as raw material add value to this by product of bio-diesel production which is obtained in large quantities around the world and have a very limited utilization now, and (ii) by implication of water molecules in the reaction the efficiency of hydrogen generation is increased as each mol of glycerol produces 7 mol of H{sub 2}. In this work we present the results obtained in the process of steam reforming of glycerol on Ni/Al{sub 2}O{sub 3}. The catalyst was prepared by wet impregnation method and characterized through different methods: N{sub 2} adsorption-desorption, XRD, TPR. The catalytic study was performed in a stainless steel tubular reactor at atmospheric pressure by varying the reaction conditions: steam/carbon ratio (1-9), gas flow (35 ml/min -133 ml/min), temperature (450-650°C). The gaseous fraction of the reaction products contain: H{sub 2}, CH{sub 4}, CO, CO{sub 2}. The optimum reaction conditions as resulted from this study are: temperature 550°C, Gly:H{sub 2}O ratio 9:1 and Ar flow 133 ml/min. In these conditions the glycerol conversion to gaseous products was 43% and the hydrogen yield was 30%.

  5. Catalytic glycerol steam reforming for hydrogen production

    Science.gov (United States)

    Dan, Monica; Mihet, Maria; Lazar, Mihaela D.

    2015-12-01

    Hydrogen production from glycerol by steam reforming combine two major advantages: (i) using glycerol as raw material add value to this by product of bio-diesel production which is obtained in large quantities around the world and have a very limited utilization now, and (ii) by implication of water molecules in the reaction the efficiency of hydrogen generation is increased as each mol of glycerol produces 7 mol of H2. In this work we present the results obtained in the process of steam reforming of glycerol on Ni/Al2O3. The catalyst was prepared by wet impregnation method and characterized through different methods: N2 adsorption-desorption, XRD, TPR. The catalytic study was performed in a stainless steel tubular reactor at atmospheric pressure by varying the reaction conditions: steam/carbon ratio (1-9), gas flow (35 ml/min -133 ml/min), temperature (450-650°C). The gaseous fraction of the reaction products contain: H2, CH4, CO, CO2. The optimum reaction conditions as resulted from this study are: temperature 550°C, Gly:H2O ratio 9:1 and Ar flow 133 ml/min. In these conditions the glycerol conversion to gaseous products was 43% and the hydrogen yield was 30%.

  6. Performance characterization of a hydrogen catalytic heater.

    Energy Technology Data Exchange (ETDEWEB)

    Johnson, Terry Alan; Kanouff, Michael P.

    2010-04-01

    This report describes the performance of a high efficiency, compact heater that uses the catalytic oxidation of hydrogen to provide heat to the GM Hydrogen Storage Demonstration System. The heater was designed to transfer up to 30 kW of heat from the catalytic reaction to a circulating heat transfer fluid. The fluid then transfers the heat to one or more of the four hydrogen storage modules that make up the Demonstration System to drive off the chemically bound hydrogen. The heater consists of three main parts: (1) the reactor, (2) the gas heat recuperator, and (3) oil and gas flow distribution manifolds. The reactor and recuperator are integrated, compact, finned-plate heat exchangers to maximize heat transfer efficiency and minimize mass and volume. Detailed, three-dimensional, multi-physics computational models were used to design and optimize the system. At full power the heater was able to catalytically combust a 10% hydrogen/air mixture flowing at over 80 cubic feet per minute and transfer 30 kW of heat to a 30 gallon per minute flow of oil over a temperature range from 100 C to 220 C. The total efficiency of the catalytic heater, defined as the heat transferred to the oil divided by the inlet hydrogen chemical energy, was characterized and methods for improvement were investigated.

  7. HYDROGEN GENERATION FROM SOLID SODIUM BOROHYDRIDE WITH FERRIC CATALYTS%基于铁盐催化的固态硼氢化钠制氢研究

    Institute of Scientific and Technical Information of China (English)

    方朝君; 闫常峰; 郭常青

    2012-01-01

    Sodium borohydride' s properties such as environmental friendly, reliability, efficiency etc. , make it a good source of hydrogen. Its hydrolysis reaction with the assistance of catalysts to liberate hydrogen gas is easily controllable. Tests were conducted to evaluate effects of ferric sulfate concentration, initial reaction temperature and solution feeding flow rate on hydrogen generation using non-noble ferric sulfate as catalyst. Ferric sulfate' s catalytic activity is evidently higher than ferric nitrate and ferric chloride. Maximum H2 flow was obtained under the condition of ferric sulfate in 1. 5mol/L. The conversion increases slowly with the increasing of reaction temperature in the range of 20-48℃. And the conversion could finally reach over 90% .%以非贵金属铁盐为催化剂,考察不同浓度的Fe2(SO4)3溶液、初始反应温度和不同进液速率下的固态NaBH4水解产氢性能.实验表明:相同浓度下,Fe2(SO4)3的催化产氢性能高于Fe(NO3)2和FeCl3.在Fe2(SO4)3溶液浓度为1.5mol/L时产氢速率出现最大值,提高Fe2(SO4)3浓度,可提高平均产氢速率;在20 ~48℃范围内,随反应温度的升高,产氢转化率略有上升,最终均能达到90%以上.

  8. Advanced Catalytic Hydrogenation Retrofit Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Reinaldo M. Machado

    2002-08-15

    Industrial hydrogenation is often performed using a slurry catalyst in large stirred-tank reactors. These systems are inherently problematic in a number of areas, including industrial hygiene, process safety, environmental contamination, waste production, process operability and productivity. This program proposed the development of a practical replacement for the slurry catalysts using a novel fixed-bed monolith catalyst reactor, which could be retrofitted onto an existing stirred-tank reactor and would mitigate many of the minitations and problems associated with slurry catalysts. The full retrofit monolith system, consisting of a recirculation pump, gas/liquid ejector and monolith catalyst, is described as a monolith loop reactor or MLR. The MLR technology can reduce waste and increase raw material efficiency, which reduces the overall energy required to produce specialty and fine chemicals.

  9. Zeolite-confined ruthenium(0) nanoclusters catalyst: record catalytic activity, reusability, and lifetime in hydrogen generation from the hydrolysis of sodium borohydride.

    Science.gov (United States)

    Zahmakiran, Mehmet; Ozkar, Saim

    2009-03-01

    Sodium borohydride, NaBH4, has been considered the most attractive hydrogen-storage material for portable fuel cell applications, as it provides a safe and practical means of producing hydrogen. In a recent communication (Zahmakiran, M.; Ozkar, S. Langmuir 2008, 24, 7065), we have reported a record total turnover number (TTON) of 103 200 mol H2/mol Ru and turnover frequency (TOF) up to 33 000 mol H2/mol Ru x h obtained by using intrazeolite ruthenium(0) nanoclusters in the hydrolysis of sodium borohydride. Here we report full details of the kinetic studies on the intrazeolite ruthenium(0) nanoclusters catalyzed hydrolysis of sodium borohydride in both aqueous and basic solutions. Expectedly, the intrazeolite ruthenium(0) nanoclusters show unprecedented catalytic lifetime, TTON = 27 200 mol H2/mol Ru, and TOF up to 4000 mol H2/mol Ru x h in the hydrolysis of sodium borohydride in basic solution (5% wt NaOH) as well. More importantly, the intrazeolite ruthenium(0) nanoclusters are isolable, bottleable, redispersible, and yet catalytically active. They retain 76% or 61% of their initial catalytic activity at the fifth run with a complete release of hydrogen in aqueous and basic medium, respectively. The intrazeolite ruthenium(0) nanoclusters were isolated as black powder and characterized by using a combination of advanced analytical techniques including XRD, HRTEM, TEM-EDX, SEM, XPS, ICP-OES, and N2 adsorption. PMID:19437749

  10. Catalytic converter with thermoelectric generator

    Energy Technology Data Exchange (ETDEWEB)

    Parise, R.J.

    1998-07-01

    The unique design of an electrically heated catalyst (EHC) and the inclusion of an ECO valve in the exhaust of an internal combustion engine will meet the strict new emission requirements, especially at vehicle cold start, adopted by several states in this country as well as in Europe and Japan. The catalytic converter (CC) has been a most useful tool in pollution abatement for the automobile. But the emission requirements are becoming more stringent and, along with other improvements, the CC must be improved to meet these new standards. Coupled with the ECO valve, the EHC can meet these new emission limits. In an internal combustion engine vehicle (ICEV), approximately 80% of the energy consumed leaves the vehicle as waste heat: out the tail pipe, through the radiator, or convected/radiated off the engine. Included with the waste heat out the tail pipe are the products of combustion which must meet strict emission requirements. The design of a new CC is presented here. This is an automobile CC that has the capability of producing electrical power and reducing the quantity of emissions at vehicle cold start, the Thermoelectric Catalytic Power Generator. The CC utilizes the energy of the exothermic reactions that take place in the catalysis substrate to produce electrical energy with a thermoelectric generator. On vehicle cold start, the thermoelectric generator is used as a heat pump to heat the catalyst substrate to reduce the time to catalyst light-off. Thus an electrically heated catalyst (EHC) will be used to augment the abatement of tail pipe emissions. Included with the EHC in the exhaust stream of the automobile is the ECO valve. This valve restricts the flow of pollutants out the tail pipe of the vehicle for a specified amount of time until the EHC comes up to operating temperature. Then the ECO valve opens and allows the full exhaust, now treated by the EHC, to leave the vehicle.

  11. Polarographic catalytic wave of hydrogen--Parallel catalytic hydrogen wave of bovine serum albumin in thepresence of oxidants

    Institute of Scientific and Technical Information of China (English)

    GUO; Wei(过玮); LIU; Limin(刘利民); LIN; Hong(林洪); SONG; Junfeng(宋俊峰)

    2002-01-01

    A polarographic catalytic hydrogen wave of bovine serum albumin (BSA) at about -1.80 V (vs. SCE) in NH4Cl-NH3@H2O buffer is further catalyzed by such oxidants as iodate, persulfate and hydrogen peroxide, producing a kinetic wave. Studies show that the kinetic wave is a parallel catalytic wave of hydrogen, which resulted from that hydrogen ion is electrochemically reduced and chemically regenerated through oxidation of its reduction product, atomic hydrogen, by oxidants mentioned above. It is a new type of poralographic catalytic wave of protein, which is suggested to be named as a parallel catalytic hydrogen wave.

  12. Catalytic Combustion for Ultra-Low NOx Hydrogen Turbines

    Energy Technology Data Exchange (ETDEWEB)

    Etemad, Shahrokh; Baird, Benjamin; Alavandi, Sandeep

    2011-06-30

    Precision Combustion, Inc., (PCI) in close collaboration with Solar Turbines, Incorporated, has developed and demonstrated a combustion system for hydrogen fueled turbines that reduces NOx to low single digit level while maintaining or improving current levels of efficiency and eliminating emissions of carbon dioxide. Full scale Rich Catalytic Hydrogen (RCH1) injector was developed and successfully tested at Solar Turbines, Incorporated high pressure test facility demonstrating low single digit NOx emissions for hydrogen fuel in the range of 2200F-2750F. This development work was based on initial subscale development for faster turnaround and reduced cost. Subscale testing provided promising results for 42% and 52% H2 with NOx emissions of less than 2 ppm with improved flame stability. In addition, catalytic reactor element testing for substrate oxidation, thermal cyclic injector testing to simulate start-stop operation in a gas turbine environment, and steady state 15 atm. operation testing were performed successfully. The testing demonstrated stable and robust catalytic element component life for gas turbine conditions. The benefit of the catalytic hydrogen combustor technology includes capability of delivering near-zero NOx without costly post-combustion controls and without requirement for added sulfur control. In addition, reduced acoustics increase gas turbine component life. These advantages advances Department of Energy (DOE’s) objectives for achievement of low single digit NOx emissions, improvement in efficiency vs. postcombustion controls, fuel flexibility, a significant net reduction in Integrated Gasification Combined Cycle (IGCC) system net capital and operating costs, and a route to commercialization across the power generation field from micro turbines to industrial and utility turbines.

  13. Electrochemical Hydrogen Peroxide Generator

    Science.gov (United States)

    Tennakoon, Charles L. K.; Singh, Waheguru; Anderson, Kelvin C.

    2010-01-01

    Two-electron reduction of oxygen to produce hydrogen peroxide is a much researched topic. Most of the work has been done in the production of hydrogen peroxide in basic media, in order to address the needs of the pulp and paper industry. However, peroxides under alkaline conditions show poor stabilities and are not useful in disinfection applications. There is a need to design electrocatalysts that are stable and provide good current and energy efficiencies to produce hydrogen peroxide under acidic conditions. The innovation focuses on the in situ generation of hydrogen peroxide using an electrochemical cell having a gas diffusion electrode as the cathode (electrode connected to the negative pole of the power supply) and a platinized titanium anode. The cathode and anode compartments are separated by a readily available cation-exchange membrane (Nafion 117). The anode compartment is fed with deionized water. Generation of oxygen is the anode reaction. Protons from the anode compartment are transferred across the cation-exchange membrane to the cathode compartment by electrostatic attraction towards the negatively charged electrode. The cathode compartment is fed with oxygen. Here, hydrogen peroxide is generated by the reduction of oxygen. Water may also be generated in the cathode. A small amount of water is also transported across the membrane along with hydrated protons transported across the membrane. Generally, each proton is hydrated with 3-5 molecules. The process is unique because hydrogen peroxide is formed as a high-purity aqueous solution. Since there are no hazardous chemicals or liquids used in the process, the disinfection product can be applied directly to water, before entering a water filtration unit to disinfect the incoming water and to prevent the build up of heterotrophic bacteria, for example, in carbon based filters. The competitive advantages of this process are: 1. No consumable chemicals are needed in the process. The only raw materials

  14. Hydrogen storage and generation system

    Science.gov (United States)

    Dentinger, Paul M.; Crowell, Jeffrey A. W.

    2010-08-24

    A system for storing and generating hydrogen generally and, in particular, a system for storing and generating hydrogen for use in an H.sub.2/O.sub.2 fuel cell. The hydrogen storage system uses the beta particles from a beta particle emitting material to degrade an organic polymer material to release substantially pure hydrogen. In a preferred embodiment of the invention, beta particles from .sup.63Ni are used to release hydrogen from linear polyethylene.

  15. Microchannel Reactor System for Catalytic Hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Adeniyi Lawal; Woo Lee; Ron Besser; Donald Kientzler; Luke Achenie

    2010-12-22

    We successfully demonstrated a novel process intensification concept enabled by the development of microchannel reactors, for energy efficient catalytic hydrogenation reactions at moderate temperature, and pressure, and low solvent levels. We designed, fabricated, evaluated, and optimized a laboratory-scale microchannel reactor system for hydrogenation of onitroanisole and a proprietary BMS molecule. In the second phase of the program, as a prelude to full-scale commercialization, we designed and developed a fully-automated skid-mounted multichannel microreactor pilot plant system for multiphase reactions. The system is capable of processing 1 – 10 kg/h of liquid substrate, and an industrially relevant immiscible liquid-liquid was successfully demonstrated on the system. Our microreactor-based pilot plant is one-of-akind. We anticipate that this process intensification concept, if successfully demonstrated, will provide a paradigm-changing basis for replacing existing energy inefficient, cost ineffective, environmentally detrimental slurry semi-batch reactor-based manufacturing practiced in the pharmaceutical and fine chemicals industries.

  16. Catalytic microreactors for portable power generation

    Energy Technology Data Exchange (ETDEWEB)

    Karagiannidis, Symeon [Paul Scherer Institute, Villigen (Switzerland)

    2011-07-01

    ''Catalytic Microreactors for Portable Power Generation'' addresses a problem of high relevance and increased complexity in energy technology. This thesis outlines an investigation into catalytic and gas-phase combustion characteristics in channel-flow, platinum-coated microreactors. The emphasis of the study is on microreactor/microturbine concepts for portable power generation and the fuels of interest are methane and propane. The author carefully describes numerical and experimental techniques, providing a new insight into the complex interactions between chemical kinetics and molecular transport processes, as well as giving the first detailed report of hetero-/homogeneous chemical reaction mechanisms for catalytic propane combustion. The outcome of this work will be widely applied to the industrial design of micro- and mesoscale combustors. (orig.)

  17. Hydrogen Generation From Electrolysis

    Energy Technology Data Exchange (ETDEWEB)

    Steven Cohen; Stephen Porter; Oscar Chow; David Henderson

    2009-03-06

    Small-scale (100-500 kg H2/day) electrolysis is an important step in increasing the use of hydrogen as fuel. Until there is a large population of hydrogen fueled vehicles, the smaller production systems will be the most cost-effective. Performing conceptual designs and analyses in this size range enables identification of issues and/or opportunities for improvement in approach on the path to 1500 kg H2/day and larger systems. The objectives of this program are to establish the possible pathways to cost effective larger Proton Exchange Membrane (PEM) water electrolysis systems and to identify areas where future research and development efforts have the opportunity for the greatest impact in terms of capital cost reduction and efficiency improvements. System design and analysis was conducted to determine the overall electrolysis system component architecture and develop a life cycle cost estimate. A design trade study identified subsystem components and configurations based on the trade-offs between system efficiency, cost and lifetime. Laboratory testing of components was conducted to optimize performance and decrease cost, and this data was used as input to modeling of system performance and cost. PEM electrolysis has historically been burdened by high capital costs and lower efficiency than required for large-scale hydrogen production. This was known going into the program and solutions to these issues were the focus of the work. The program provided insights to significant cost reduction and efficiency improvement opportunities for PEM electrolysis. The work performed revealed many improvement ideas that when utilized together can make significant progress towards the technical and cost targets of the DOE program. The cell stack capital cost requires reduction to approximately 25% of today’s technology. The pathway to achieve this is through part count reduction, use of thinner membranes, and catalyst loading reduction. Large-scale power supplies are available

  18. Short hydrogen bonds in the catalytic mechanism of serine proteases

    Directory of Open Access Journals (Sweden)

    VLADIMIR LESKOVAC

    2008-04-01

    Full Text Available The survey of crystallographic data from the Protein Data Bank for 37 structures of trypsin and other serine proteases at a resolution of 0.78–1.28 Å revealed the presence of hydrogen bonds in the active site of the enzymes, which are formed between the catalytic histidine and aspartate residues and are on average 2.7 Å long. This is the typical bond length for normal hydrogen bonds. The geometric properties of the hydrogen bonds in the active site indicate that the H atom is not centered between the heteroatoms of the catalytic histidine and aspartate residues in the active site. Taken together, these findings exclude the possibility that short “low-barrier” hydrogen bonds are formed in the ground state structure of the active sites examined in this work. Some time ago, it was suggested by Cleland that the “low-barrier hydrogen bond” hypothesis is operative in the catalytic mechanism of serine proteases, and requires the presence of short hydrogen bonds around 2.4 Å long in the active site, with the H atom centered between the catalytic heteroatoms. The conclusions drawn from this work do not exclude the validity of the “low-barrier hydrogen bond” hypothesis at all, but they merely do not support it in this particular case, with this particular class of enzymes.

  19. Synthesis and Catalytic Hydrogen Transfer Reaction of Ruthenium(II) Complex

    Energy Technology Data Exchange (ETDEWEB)

    Son, Jung Ik; Kim, Aram; Noh, Hui Bog; Lee, Hyun Ju; Shim, Yoon Bo; Park, Kang Hyun [Pusan National University, Busan (Korea, Republic of)

    2012-01-15

    The ruthenium(II) complex [Ru(bpy){sub 2}-(PhenTPy)] was synthesized, and used for the transfer hydrogenation of ketones and the desired products were obtained in good yield. Based on the presented results, transition-metal complexes can be used as catalysts for a wide range of organic transformations. The relationship between the electro-reduction current density and temperature are being examined in this laboratory. Attempts to improve the catalytic activity and determine the transfer hydrogenation mechanism are currently in progress. The catalytic hydrogenation of a ketone is a basic and critical process for making many types of alcohols used as the final products and precursors in the pharmaceutical, agrochemical, flavor, fragrance, materials, and fine chemicals industries. The catalytic hydrogenation process developed by Noyori is a very attractive process. Formic acid and 2-propanol have been used extensively as hydrogenation sources. The advantage of using 2-propanol as a hydrogen source is that the only side product will be acetone, which can be removed easily during the workup process. Hydrogen transfer (HT) catalysis, which generates alcohols through the reduction of ketones, is an attractive protocol that is used widely. Ruthenium(II) complexes are the most useful catalysts for the hydrogen transfer (HT) of ketones. In this method, a highly active catalytic system employs a transition metal as a catalyst to synthesize alcohols, and is a replacement for the hydrogen-using hydrogenation process. The most active system is based on Ru, Rh and Ir, which includes a nitrogen ligand that facilitates the formation of a catalytically active hydride and phosphorus.

  20. Synthesis and Catalytic Hydrogen Transfer Reaction of Ruthenium(II) Complex

    International Nuclear Information System (INIS)

    The ruthenium(II) complex [Ru(bpy)2-(PhenTPy)] was synthesized, and used for the transfer hydrogenation of ketones and the desired products were obtained in good yield. Based on the presented results, transition-metal complexes can be used as catalysts for a wide range of organic transformations. The relationship between the electro-reduction current density and temperature are being examined in this laboratory. Attempts to improve the catalytic activity and determine the transfer hydrogenation mechanism are currently in progress. The catalytic hydrogenation of a ketone is a basic and critical process for making many types of alcohols used as the final products and precursors in the pharmaceutical, agrochemical, flavor, fragrance, materials, and fine chemicals industries. The catalytic hydrogenation process developed by Noyori is a very attractive process. Formic acid and 2-propanol have been used extensively as hydrogenation sources. The advantage of using 2-propanol as a hydrogen source is that the only side product will be acetone, which can be removed easily during the workup process. Hydrogen transfer (HT) catalysis, which generates alcohols through the reduction of ketones, is an attractive protocol that is used widely. Ruthenium(II) complexes are the most useful catalysts for the hydrogen transfer (HT) of ketones. In this method, a highly active catalytic system employs a transition metal as a catalyst to synthesize alcohols, and is a replacement for the hydrogen-using hydrogenation process. The most active system is based on Ru, Rh and Ir, which includes a nitrogen ligand that facilitates the formation of a catalytically active hydride and phosphorus

  1. Review of literature on catalytic recombination of hydrogen--oxygen

    International Nuclear Information System (INIS)

    The results are reported of a literature search for information concerning the heterogeneous, gas phase, catalytic hydrogen-oxygen recombination. Laboratory scale experiments to test the performance of specific metal oxide catalysts under conditions simulating the atmosphere within a nuclear reactor containment vessel following a loss-of-coolant blowdown accident are suggested

  2. Catalytic Hydrogenation Reaction of Naringin-Chalcone. Study of the Electrochemical Reaction

    OpenAIRE

    B. A. López de Mishima; H. T. Mishima; A. N. Giannuzzo; M. A. Nazareno

    2000-01-01

    The electrocatalytic hydrogenation reaction of naringin derivated chalcone is studied. The reaction is carried out with different catalysts in order to compare with the classic catalytic hydrogenation.

  3. Hydrogen-based power generation from bioethanol steam reforming

    International Nuclear Information System (INIS)

    This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO2 emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint

  4. Hydrogen-based power generation from bioethanol steam reforming

    Energy Technology Data Exchange (ETDEWEB)

    Tasnadi-Asztalos, Zs., E-mail: tazsolt@chem.ubbcluj.ro; Cormos, C. C., E-mail: cormos@chem.ubbcluj.ro; Agachi, P. S. [Babes-Bolyai University, Faculty of Chemistry and Chemical Engineering, 11 Arany Janos, Postal code: 400028, Cluj-Napoca (Romania)

    2015-12-23

    This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO{sub 2} emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.

  5. Hydrogen-based power generation from bioethanol steam reforming

    Science.gov (United States)

    Tasnadi-Asztalos, Zs.; Cormos, C. C.; Agachi, P. S.

    2015-12-01

    This paper is evaluating two power generation concepts based on hydrogen produced from bioethanol steam reforming at industrial scale without and with carbon capture. The power generation from bioethanol conversion is based on two important steps: hydrogen production from bioethanol catalytic steam reforming and electricity generation using a hydrogen-fuelled gas turbine. As carbon capture method to be assessed in hydrogen-based power generation from bioethanol steam reforming, the gas-liquid absorption using methyl-di-ethanol-amine (MDEA) was used. Bioethanol is a renewable energy carrier mainly produced from biomass fermentation. Steam reforming of bioethanol (SRE) provides a promising method for hydrogen and power production from renewable resources. SRE is performed at high temperatures (e.g. 800-900°C) to reduce the reforming by-products (e.g. ethane, ethene). The power generation from hydrogen was done with M701G2 gas turbine (334 MW net power output). Hydrogen was obtained through catalytic steam reforming of bioethanol without and with carbon capture. For the evaluated plant concepts the following key performance indicators were assessed: fuel consumption, gross and net power outputs, net electrical efficiency, ancillary consumptions, carbon capture rate, specific CO2 emission etc. As the results show, the power generation based on bioethanol conversion has high energy efficiency and low carbon footprint.

  6. Catalytic hydrogen evolution by polyaminoacids using mercury electrode

    Directory of Open Access Journals (Sweden)

    Marko Živanovič

    2010-12-01

    Full Text Available It was shown that using constant current chronopotentiometricstripping (CPS peptides and proteins at nanomolar concentrations produce protein structure–sensitive peak H at mercury electrodes. This peak is due to the catalytic hydrogen evolution reaction (HER. Polyamino acids can be considered as an intermediate model system between peptides and macromolecular proteins. Here we used polyamino acids (poly(aa such as polylysine (polyLys and polyarginine (polyArg and cyclic voltammetry or CPS in combination with hanging mercury drop electrode to explore how different amino acid residues in proteins contribute to the catalyticHER.

  7. Hydrogen generation from renewable resources

    Energy Technology Data Exchange (ETDEWEB)

    Loges, Bjoern

    2009-09-04

    In this thesis, the hydrogen generation by dehydrogenation of 2-propanol and formic acid as model substances for renewable resources have been studied, which is of importance for hydrogen storage. For the base-assisted dehydrogenation of 2-propanol, a ruthenium diamine catalyst system has been investigated. For the selective decomposition of formic acid to hydrogen and carbon dioxide, a system has been established containing ruthenium catalysts and formic acid amine adducts as substrates. The best catalyst activity and productivity have been achieved with in situ generated ruthenium phosphine catalysts, e.g. [RuCl{sub 2}(benzene)]{sub 2} / dppe (TOF = 900 h{sup -1}, TON = 260,000). The gas evolved has been directly used in fuel cells. Furthermore, the influence of irradiation with visible light has been described for the ruthenium phosphine catalysts. (orig.)

  8. Catalytic Hydrogenation of Acetone to Isopropanol: An Environmentally Benign Approach

    Directory of Open Access Journals (Sweden)

    Ateeq Rahman

    2011-01-01

    Full Text Available The catalytic hydrogenation of acetone is an important area of catalytic process to produce fine chemicals. Hydrogenation of acetone has important applications for heat pumps, fuel cells or in fulfilling the sizeable demand for the production of 2-propanol. Catalytic vapour phase hydrogenation of acetone has gained attention over the decades with variety of homogeneous catalysts notably Iridium, Rh, Ru complexes and heterogeneous catalysts comprising of Raney Nickel, Raney Sponge, Ni/Al2O3, Ni/SiO2, or Co-Al2O3, Pd, Rh, Ru, Re, or Fe/Al2O3 supported on SiO2 or MgO and even CoMgAl, NiMg Al layered double hydroxide, Cu metal, CuO, Cu2O. Nano catalysts are developed for actone reduction Ni maleate, cobalt oxide prepared in organic solvents. Author present a review on acetone hydrogenation under different conditions with various homogeneous and heterogeneous catalysts studied so far in literature and new strategies to develop economic and environmentally benign approach. ©2010 BCREC UNDIP. All rights reserved(Received: 16th June 2010, Revised: 18th October 2010; Accepted: 25th October 2010[How to Cite:Ateeq Rahman. (2010. Catalytic Hydrogenation of Acetone to Isopropanol: An Environmentally Benign Approach. Bulletin of Chemical Reaction Engineering and Catalysis, 5(2: 113-126. doi:10.9767/bcrec.5.2.798.113-126][DOI: http://dx.doi.org/10.9767/bcrec.5.2.798.113-126 || or local:  http://ejournal.undip.ac.id/index.php/bcrec/article/view/798

  9. Catalytic converter for next generation turbine engines

    Energy Technology Data Exchange (ETDEWEB)

    Saruhan, B.; Schulz, U.; Leyens, C. [German Aerospace Center (DLR), Inst. of Materials Research, Cologne (Germany)

    2004-07-01

    EB-PVD thermal barrier coatings (TBCs) are used on advanced turbine blades to increase the engine efficiency and improve the blade performance. partially yttria stabilized zirconia (PYSZ) is the standard material for current TBC applications. Lower thermal stability of the PYSZ-based TBCs, however, seriously affects the performance at demanding service temperatures. For the new generation turbines where higher operating gas temperatures (> 1200 C) are to expect, the performance of turbine blades can be improved by replacing the state-art-of-material PYSZ with superior thermal barrier coatings which belong to different crystal structures such as magnetoplumbite. Magnetoplumbite structure through its interlocking grain morphology and unique crystal structure provides essentially a sintering resistant, low thermal conductive layer, but also imparts a catalytic layer to reduce the environmentally harmful substances produced during propulsion and increase the catalytic performance. The complex structures of these compounds make it difficult to realize by conventional methods and requires careful adjustment of process parameters. The morphology and crystallographic aspects of these coatings as well as the mechanisms controlling the improvement are highlighted. (orig.)

  10. Selective catalytic reduction of nitrogen oxides from industrial gases by hydrogen or methane

    International Nuclear Information System (INIS)

    This work deals with the selective catalytic reduction of nitrogen oxides (NOx), contained in the effluents of industrial plants, by hydrogen or methane. The aim is to replace ammonia, used as reducing agent, in the conventional process. The use of others reducing agents such as hydrogen or methane is interesting for different reasons: practical, economical and ecological. The catalyst has to convert selectively NO into N2, in presence of an excess of oxygen, steam and sulfur dioxide. The developed catalyst is constituted by a support such as perovskites, particularly LaCoO3, on which are dispersed noble metals (palladium, platinum). The interaction between the noble metal and the support, generated during the activation of the catalyst, allows to minimize the water and sulfur dioxide inhibitor phenomena on the catalytic performances, particularly in the reduction of NO by hydrogen. (O.M.)

  11. Catalytic hydrogenation reactors for the fine chemicals industries. Their design and operation.

    OpenAIRE

    Westerterp, K.R.; Molga, E.J.; Gelder, van, M.

    1997-01-01

    The design and operation of reactors for catalytic, hydrogenation in the fine chemical industries are discussed. The requirements for a good multiproduct catalytic hydrogenation unit as well as the choice of the reactor type are considered. Packed bed bubble column reactors operated without hydrogen recycle are recommended as the best choice to obtain a flexible reactor with good selectivities. The results of an experimental study of the catalytic hydrogenation of 2,4-dinitrotoluene in a mini...

  12. Fuel cell using a hydrogen generation system

    Science.gov (United States)

    Dentinger, Paul M.; Crowell, Jeffrey A. W.

    2010-10-19

    A system is described for storing and generating hydrogen and, in particular, a system for storing and generating hydrogen for use in an H.sub.2/O.sub.2 fuel cell. The hydrogen storage system uses beta particles from a beta particle emitting material to degrade an organic polymer material to release substantially pure hydrogen. In a preferred embodiment of the invention, beta particles from .sup.63Ni are used to release hydrogen from linear polyethylene.

  13. Catalytic hydrogen peroxide decomposition on La1-xSrxCo03-d perovskite oxides

    NARCIS (Netherlands)

    Dam, Van-Ahn. T.; Olthuis, W.; Bergveld, P.; Berg, van den A.

    2005-01-01

    Lanthanide perovskite oxides are mentioned as material for hydrogen peroxide sensor because they can catalytically decompose hydrogen peroxide in an aqueous medium. The catalytic properties of these perovskite oxides to hydrogen peroxide are suggested due to their oxygen vacancies influenced by the

  14. Catalytic Response and Stability of Nickel/Alumina for the Hydrogenation of 5-Hydroxymethylfurfural in Water.

    Science.gov (United States)

    Perret, Noémie; Grigoropoulos, Alexios; Zanella, Marco; Manning, Troy D; Claridge, John B; Rosseinsky, Matthew J

    2016-03-01

    The catalytic response of Ni on Al2O3 obtained from Ni-Al layered double hydroxides was studied for the liquid-phase hydrogenation of hydroxymethyl furfural to tetrahydrofuran-2,5-diyldimethanol (THFDM) in water. The successive calcination and reduction of the precursors caused the removal of interlayer hydroxyl and carbonate groups and the reduction of Ni(2+) to Ni(0). Four reduced mixed oxide catalysts were obtained, consisting of different amount of Ni metal contents (47-68 wt%) on an Al-rich amorphous component. The catalytic activity was linked to Ni content whereas selectivity was mainly affected by reaction temperature. THFDM was formed in a stepwise manner at low temperature (353 K) whereas 3-hydroxymethyl cyclopentanone was generated at higher temperature. Coke formation caused deactivation; however, the catalytic activity can be regenerated using heat treatment. The results establish Ni on Al2O3 as a promising catalyst for the production of THFDM in water. PMID:26870940

  15. Research of Hydrogen Preparation with Catalytic Steam-Carbon Reaction Driven by Photo-Thermochemistry Process

    Directory of Open Access Journals (Sweden)

    Xiaoqing Zhang

    2013-01-01

    Full Text Available An experiment of hydrogen preparation from steam-carbon reaction catalyzed by K2CO3 was carried out at 700°C, which was driven by the solar reaction system simulated with Xenon lamp. It can be found that the rate of reaction with catalyst is 10 times more than that without catalyst. However, for the catalytic reaction, there is no obvious change for the rate of hydrogen generation with catalyst content range from 10% to 20%. Besides, the conversion efficiency of solar energy to chemical energy is more than 13.1% over that by photovoltaic-electrolysis route. An analysis to the mechanism of catalytic steam-carbon reaction with K2CO3 is given, and an explanation to the nonbalanced [H2]/[CO + 2CO2] is presented, which is a phenomenon usually observed in experiment.

  16. Catalytic hydrogenation of uranyl nitrate - engineering scale studies

    International Nuclear Information System (INIS)

    Uranous nitrate is employed as partitioning agent for the separation of plutonium from uranium in PUREX process, the conventional process for the reprocessing of spent nuclear fuel. It is currently produced from uranyl nitrate solution by the electrochemical route. Since the conversion is only 50%, an innovative method based on catalytic hydrogenation has been developed. Parametric studies have been carried out on 5 L scale using natural uranyl nitrate solution as fed. Based on these studies, number of runs were carried out on engineering scale using contaminated uranyl nitrate solution. More than 100 kg of uranous nitrate has been made. Performance of the reduction process is described in detail. (author)

  17. Hydrogen generation in tru waste transportation packages

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, B; Sheaffer, M K; Fischer, L E

    2000-03-27

    This document addresses hydrogen generation in TRU waste transportation packages. The potential sources of hydrogen generation are summarized with a special emphasis on radiolysis. After defining various TRU wastes according to groupings of material types, bounding radiolytic G-values are established for each waste type. Analytical methodologies are developed for prediction of hydrogen gas concentrations for various packaging configurations in which hydrogen generation is due to radiolysis. Representative examples are presented to illustrate how analytical procedures can be used to estimate the hydrogen concentration as a function of time. Methodologies and examples are also provided to show how the time to reach a flammable hydrogen concentration in the innermost confinement layer can be estimated. Finally, general guidelines for limiting the hydrogen generation in the payload and hydrogen accumulation in the innermost confinement layer are described.

  18. Catalytic nanoarchitectonics for environmentally compatible energy generation

    Directory of Open Access Journals (Sweden)

    Hideki Abe

    2016-01-01

    Full Text Available Environmentally compatible energy management is one of the biggest challenges of the 21st century. Low-temperature conversion of chemical to electrical energy is of particular importance to minimize the impact to the environment while sustaining the consumptive economy. In this review, we shed light on one of the most versatile energy-conversion technologies: heterogeneous catalysts. We establish the integrity of structural tailoring in heterogeneous catalysts at different scales in the context of an emerging paradigm in materials science: catalytic nanoarchitectonics. Fundamental backgrounds of energy-conversion catalysis are first provided together with a perspective through state-of-the-art energy-conversion catalysis including catalytic exhaust remediation, fuel-cell electrocatalysis and photosynthesis of solar fuels. Finally, the future evolution of catalytic nanoarchitectonics is overviewed: possible combinations of heterogeneous catalysts, organic molecules and even enzymes to realize reaction-selective, highly efficient and long-life energy conversion technologies which will meet the challenge we face.

  19. CATALYTIC HYDROGENATION OF ACRYLATE ASMMETRIC Dd(Ⅱ)—CHELATING RESINS CONTAINING AMINO ACID LIGANDS

    Institute of Scientific and Technical Information of China (English)

    Wangying; WangHongzuo; 等

    1995-01-01

    The catalytic hydrogenation of palladium chelating resins containing chiral amino acid ligands based on lower crosslinked poly(chloroethyl acrylate) and some effects on the rate of hydrogenation were studied.

  20. Catalytic Hydrogenation Reaction of Naringin-Chalcone. Study of the Electrochemical Reaction

    Directory of Open Access Journals (Sweden)

    B. A. López de Mishima

    2000-03-01

    Full Text Available The electrocatalytic hydrogenation reaction of naringin derivated chalcone is studied. The reaction is carried out with different catalysts in order to compare with the classic catalytic hydrogenation.

  1. Experimental and Numerical Evaluation of the By-Pass Flow in a Catalytic Plate Reactor for Hydrogen Production

    DEFF Research Database (Denmark)

    Sigurdsson, Haftor Örn; Kær, Søren Knudsen

    2011-01-01

    Numerical and experimental study is performed to evaluate the reactant by-pass flow in a catalytic plate reactor with a coated wire mesh catalyst for steam reforming of methane for hydrogen generation. By-pass of unconverted methane is evaluated under different wire mesh catalyst width to reactor...

  2. Production of hydrogen from biomass by catalytic steam reforming of fast pyrolysis oil

    Energy Technology Data Exchange (ETDEWEB)

    Czernik, S.; Wang, D.; Chornet, E. [National Renewable Energy Lab., Golden, CO (United States). Center for Renewable Chemical Technologies and Materials

    1998-08-01

    Hydrogen is the prototype of the environmentally cleanest fuel of interest for power generation using fuel cells and for transportation. The thermochemical conversion of biomass to hydrogen can be carried out through two distinct strategies: (a) gasification followed by water-gas shift conversion, and (b) catalytic steam reforming of specific fractions derived from fast pyrolysis and aqueous/steam processes of biomass. This paper presents the latter route that begins with fast pyrolysis of biomass to produce bio-oil. This oil (as a whole or its selected fractions) can be converted to hydrogen via catalytic steam reforming followed by a water-gas shift conversion step. Such a process has been demonstrated at the bench scale using model compounds, poplar oil aqueous fraction, and the whole pyrolysis oil with commercial Ni-based steam reforming catalysts. Hydrogen yields as high as 85% have been obtained. Catalyst initial activity can be recovered through regeneration cycles by steam or CO{sub 2} gasification of carbonaceous deposits.

  3. High Selective Determination of Anionic Surfactant Using Its Parallel Catalytic Hydrogen Wave

    Institute of Scientific and Technical Information of China (English)

    过玮; 何盈盈; 宋俊峰

    2003-01-01

    A faradaic response of anionic surfactants (AS), such as linear aikylbenzene sulfonate (LAS), dodecyl benzene sulfonate and dodecyl sulfate, was observed in weak acidic medium. The faradaic response of AS includes (1) a catalytic hydrogen wave of AS in HAc/NaAc buffer that was attributed to the reduction of proton associated with the sulfo-group of AS, and (2) a parallel catalytic hydrogen wave of AS in the presence of hydrogen peroxide, which was due to the catalysis of the catalytic hydrogen wave of AS by hydroxyl radical OH electrogenerated in the reduction of hydrogen peroxide. The parallel catalytic hydrogen wave is about 50 times as sensitive as the catalytic hydrogen wave. Based on the parallel catalytic hydrogen wave, a high selective method for the determination of AS was developed. In 0.1mol/L HAc/NaAc (pH=6.2±0.1)/1.0×10-3mol/L H2O2 supporting electrolyte, the second-order derivative peak current of the parallel catalytic hydrogen wave located at-1.33 V (vs. SCE) was rectilinear to AS concentration in the range of 3.0×10-6-2.5×10-4mol/L, without the interference of other surfactants. The proposed method was evaluated by quantitative analysis of AS in environmental wastewater.

  4. Modelling of the aerosol deposition in a hydrogen catalytic recombiner

    Energy Technology Data Exchange (ETDEWEB)

    Vendel, J.; Studer, E.; Zavaleta, P. [Inst. de Protection et de Surete Nucleaire, Dept. de Prevention et d' Etudes des Accidents, Gif-sur-Yvette Cedex (France); Hadida, Ph. [Quasar Informatique, Paris (France)

    1997-03-01

    Catalytic recombiners are used to remove the hydrogen released in case of a severe accident in a nuclear power plant, so as to reduce the risk of deflagration or detonation. H{sub 2}PAR experiments are carried out to precise the behaviour of recombiners in term of poisoning by aerosols. Firstly, some calculations have been done with the Trio-EF code to assess the structure of convection loops in the experimental tent. We note that when the recombiner is active, it may have a strong influence on the flow inside the tent and may even interact with an other heat source such as a furnace. In the second part, we study the deposition of aerosols on catalytic plates for a given recombiner, when it is active or passive. We list the different mechanisms and quantify them by introducing the deposition velocity. In fact, thermophoresis appears to be the main mechanism, compared to brownian diffusion or difrusiophoresis, which governs aerosols deposition. It favours deposition on <> plates and acts against it for <> plates. (author)

  5. Solar Fuels. Photocatalytic Hydrogen Generation

    OpenAIRE

    Kamat, Prashant V.; Bisquert, Juan

    2013-01-01

    The necessity for developing clean energy technology has led to the surge in renewable energy research. A major effort is in discovering new approaches for producing transportable fuels. Hydrogen, which possesses the highest energy density (120 MJ/kg) known for any fuel and no carbon footprint, is regarded as the leading contender for meeting future fuel needs. The term Hydrogen Economy is often referred collectively to the topics of production, storage, and transport of hydrogen.

  6. Experimental studies on catalytic hydrogen recombiners for light water reactors

    International Nuclear Information System (INIS)

    In the course of core melt accidents in nuclear power plants a large amount of hydrogen can be produced and form an explosive or even detonative gas mixture with aerial oxygen in the reactor building. In the containment atmosphere of pressurized water reactors hydrogen combines a phlogistically with the oxygen present to form water vapor even at room temperature. In the past, experimental work conducted at various facilities has contributed little or nothing to an understanding of the operating principles of catalytic recombiners. Hence, the purpose of the present study was to conduct detailed investigations on a section of a recombiner essentially in order to deepen the understanding of reaction kinetics and heat transport processes. The results of the experiments presented in this dissertation form a large data base of measurements which provides an insight into the processes taking place in recombiners. The reaction-kinetic interpretation of the measured data confirms and deepens the diffusion theory - proposed in an earlier study. Thus it is now possible to validate detailed numeric models representing the processes in recombiners. Consequently the present study serves to broaden and corroborate competence in this significant area of reactor technology. In addition, the empirical knowledge thus gained may be used for a critical reassessment of previous numeric model calculations. (orig.)

  7. Recent advances in catalytic asymmetric hydrogenation:Renaissance of the monodentate phosphorus ligands

    Institute of Scientific and Technical Information of China (English)

    GUO Hongchao; DING Kuiling; DAI Lixin

    2004-01-01

    The history for the development of chiral phosphorus ligands in catalytic asymmetric hydrogenation is briefly highlighted. This review focuses on the recent advances in the synthesis of the monodentate phosphorus ligands and their applications in catalytic asymmetric hydrogenation. The examples highlighted in this article clearly demonstrated the importance and advantages of monodentate phosphorus ligands, which had been ignored for 30 a and experienced a renaissance at the very beginning of this millennium, particularly in the area of asymmetric hydrogenation.

  8. Hydrogen production by catalytic gasification of cellulose in supercritical water

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    Cellulose,one of the important components of biomass,was gasified in supercritical water to produce hydrogen-rich gas in an autoclave which was operated batch-wise under high-pressure.K2CO3 and Ca(OH)2 were selected as the catalysts (or promoters).The temperature was kept between 450℃ and 500℃ while pressure was maintained at 24-26 MPa.The reaction time was 20 min.Experimental results showed that the two catalysts had good catalytic effect and optimum amounts were observed for each catalyst.When 0.2 g K2CO3 was added,the hydrogen yield could reach 9.456 mol.kg-1 which was two times of the H2 amount produced without catalyst.When 1.6 g Ca(OH)2 was added,the H2 yield was K2CO3 as catalyst but is still 1.7 times that achieved without catalyst.Comparing with the results obtained using KaCO3 or Ca(OH)2 alone,the use of a combination of K2CO3 and Ca(OH)2 could increase the H2 yield by up to 2.5 times that without catalyst and 25% and 45% more than that obtained using K2CO3 and Ca(OH)2 alone,respectively.It was found that methane was the dominant product at relatively low temperature.When the temperature was increased,the methane reacts with water and is converted to hydrogen and carbon dioxide.

  9. Alloying effects on hydrogen permeability of V without catalytic Pd overlayer

    Energy Technology Data Exchange (ETDEWEB)

    Nakamura, Y.; Yukawa, H.; Suzuki, A. [Department of Materials Science and Engineering, Graduate School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8603 (Japan); Nambu, T. [Department of Materials Science and Engineering, Suzuka National College of Technology, Shiroko-cho, Suzuka, Mie 510-0294 (Japan); Matsumoto, Y. [Department of Mechanical Engineering, Oita National College of Technology, Maki, Oita 870-0152 (Japan); Murata, Y. [Department of Materials Science and Engineering, Graduate School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8603 (Japan)

    2015-10-05

    Highlights: • Air–treated V–based alloy membranes without catalytic Pd overlayer are found to possess excellent hydrogen permeability. • They also exhibit good durability at high temperature. • Alloying effects are discussed in view of the new description of hydrogen permeation based on hydrogen chemical potential. - Abstract: Hydrogen permeability of air–treated V–based alloy membranes without Pd coating have been investigated. The diffusion–limiting hydrogen permeation reaction takes place even without catalytic Pd overlayer on the surface. It is shown that pure V and its alloy membranes without Pd overlayer possess excellent hydrogen permeability and good durability at high temperature. The new description of hydrogen permeation based on hydrogen chemical potential has been applied and the hydrogen flux is analyzed in terms of the mobility of hydrogen atom and the PCT factor, f{sub PCT}.

  10. Double heterojunction nanowire photocatalysts for hydrogen generation

    Science.gov (United States)

    Tongying, P.; Vietmeyer, F.; Aleksiuk, D.; Ferraudi, G. J.; Krylova, G.; Kuno, M.

    2014-03-01

    Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core/shell nanowires and their Pt nanoparticle-decorated counterparts. Femtosecond transient differential absorption measurements reveal how semiconductor/semiconductor and metal/semiconductor heterojunctions affect the charge separation and hydrogen generation efficiencies of these hybrid photocatalysts. In turn, we unravel the role of surface passivation, charge separation at semiconductor interfaces and charge transfer to metal co-catalysts in determining photocatalytic H2 generation efficiencies. This allows us to rationalize why Pt nanoparticle decorated CdSe/CdS NWs, a double heterojunction system, performs best with H2 generation rates of ~434.29 +/- 27.40 μmol h-1 g-1 under UV/Visible irradiation. In particular, we conclude that the CdS shell of this double heterojunction system serves two purposes. The first is to passivate CdSe NW surface defects, leading to long-lived charges at the CdSe/CdS interface capable of carrying out reduction chemistries. Upon photoexcitation, we also find that CdS selectively injects charges into Pt NPs, enabling simultaneous reduction chemistries at the Pt NP/solvent interface. Pt nanoparticle decorated CdSe/CdS NWs thus enable reduction chemistries at not one, but rather two interfaces, taking advantage of each junction's optimal catalytic activities.Charge separation and charge transfer across interfaces are key aspects in the design of efficient photocatalysts for solar energy conversion. In this study, we investigate the hydrogen generating capabilities and underlying photophysics of nanostructured photocatalysts based on CdSe nanowires (NWs). Systems studied include CdSe, CdSe/CdS core

  11. Skeletal Isomerization and Inter-molecular Hydrogen Transfer Reactions in Catalytic Cracking

    Institute of Scientific and Technical Information of China (English)

    Gao Yongcan; Zhang Jiushun; Xie Chaogang; Long Jun

    2002-01-01

    Bimolecular hydrogen transfer and skeletal isomerization are the important secondary reac tions among catalytic cracking reactions, which affect product yield distribution and product quality.Catalyst properties and operating parameters have great impact on bimolecular hydrogen transfer and skeletal isomerization reactions. Bimolecular hydrogen transfer activity and skeletal isomerization activity of USY-containing catalysts are higher than that of ZSM-5-containing catalyst. Coke deposition on the active sites of catalyst may suppress bimolecular hydrogen transfer activity and skeletal isomerization activity of catalyst in different degrees. Short reaction time causes a decrease of hydrogen trans fer reaction, but an increase of skeletal isomerization reaction compared to cracking reaction in catalytic cracking process.

  12. Catalytic Hydrogenation of Organic Compounds without H2 Supply: An Electrochemical System

    Science.gov (United States)

    Navarro, Daniela Maria do Amaral Ferraz; Navarro, Marcelo

    2004-01-01

    An experiment developed for an undergraduate organic chemistry laboratory course that can be used to introduce the catalytic hydrogenation reaction, catalysis electrochemical principles and gas chromatography is presented. The organic compounds hydrogenated by the electrocatalytic hydrogenation (ECH) process were styrene, benzaldehyde and…

  13. Detection of hydrogen peroxide in Photosystem II (PSII using catalytic amperometric biosensor

    Directory of Open Access Journals (Sweden)

    Ankush ePrasad

    2015-10-01

    Full Text Available Hydrogen peroxide (H2O2 is known to be generated in Photosystem II (PSII via enzymatic and non-enzymatic pathways. Hydrogen peroxide (H2O2 is known to be generated in Photosystem II (PSII via enzymatic and non-enzymatic pathways. Detection of H2O2 by different spectroscopic techniques has been explored, however its sensitive detection has always been a challenge in photosynthetic research. During the recent past, fluorescence probes such as Amplex Red has been used but is known to either lack specificity or limitation with respect to the minimum detection limit of H2O2. We have employed an electrochemical biosensor for real time monitoring of H2O2 generation at the level of sub-cellular organelles. The electrochemical biosensor comprises of counter electrode and working electrodes. The counter electrode is a platinum plate, while the working electrode is a mediator based catalytic amperometric biosensor device developed by the coating of a carbon electrode with osmium-horseradish peroxidase which acts as H2O2 detection sensor. In the current study, generation and kinetic behaviour of H2O2 in PSII membranes have been studied under light illumination. Electrochemical detection of H2O2 using the catalytic amperometric biosensor device is claimed to serve as a promising technique for detection of H2O2 in photosynthetic cells and subcellular structures including PSII or thylakoid membranes. It can also provide a precise information on qualitative determination of H2O2 and thus can be widely used in photosynthetic research.

  14. Data acquisition and quantitative analysis of stable hydrogen isotope in liquid and gas in the liquid phase catalytic exchange process

    International Nuclear Information System (INIS)

    A pilot plant for the Liquid Phase Catalytic Exchange process was built and has been operating to test the hydrophobic catalyst developed to remove the tritium generated at the CANDU nuclear power plants. The methods of quantitative analysis of hydrogen stable isotope were compared. Infrared spectroscopy was used for the liquid samples, and gas chromatography with hydrogen carrier gas showed the best result for gas samples. Also, a data acquisition system was developed to record the operation parameters. This record was very useful to investigate the causes of the system trip

  15. Nitric-glycolic flowsheet testing for maximum hydrogen generation rate

    Energy Technology Data Exchange (ETDEWEB)

    Martino, C. J. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Newell, J. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Williams, M. S. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-03-01

    The Defense Waste Processing Facility (DWPF) at the Savannah River Site is developing for implementation a flowsheet with a new reductant to replace formic acid. Glycolic acid has been tested over the past several years and found to effectively replace the function of formic acid in the DWPF chemical process. The nitric-glycolic flowsheet reduces mercury, significantly lowers the chemical generation of hydrogen and ammonia, allows purge reduction in the Sludge Receipt and Adjustment Tank (SRAT), stabilizes the pH and chemistry in the SRAT and the Slurry Mix Evaporator (SME), allows for effective adjustment of the SRAT/SME rheology, and is favorable with respect to melter flammability. The objective of this work was to perform DWPF Chemical Process Cell (CPC) testing at conditions that would bound the catalytic hydrogen production for the nitric-glycolic flowsheet.

  16. Hydrogen Generation from Plasmatron Reforming Ethanol

    Institute of Scientific and Technical Information of China (English)

    YOU Fu-bing; HU You-ping; LI Ge-sheng; GAO Xiao-hong

    2006-01-01

    Hydrogen generation through plasmatron reforming of ethanol has been carried out in a dielectric barrier discharge (DBD) reactor. The reforming of pure ethanol and mixtures of ethanol-water have been studied. The gas chromatography (GC) analysis has shown that in all conditions the reforming yield was H2, CO, CH4 and CO2 as the main products, and with little C2* . The hydrogen-rich gas can be used as fuel for gasoline engine and other applications.

  17. Field-controlled electron transfer and reaction kinetics of the biological catalytic system of microperoxidase-11 and hydrogen peroxide

    Directory of Open Access Journals (Sweden)

    Yongki Choi

    2011-12-01

    Full Text Available Controlled reaction kinetics of the bio-catalytic system of microperoxidase-11 and hydrogen peroxide has been achieved using an electrostatic technique. The technique allowed independent control of 1 the thermodynamics of the system using electrochemical setup and 2 the quantum mechanical tunneling at the interface between microperoxidase-11 and the working electrode by applying a gating voltage to the electrode. The cathodic currents of electrodes immobilized with microperoxidase-11 showed a dependence on the gating voltage in the presence of hydrogen peroxide, indicating a controllable reduction reaction. The measured kinetic parameters of the bio-catalytic reduction showed nonlinear dependences on the gating voltage as the result of modified interfacial electron tunnel due to the field induced at the microperoxidase-11-electrode interface. Our results indicate that the kinetics of the reduction of hydrogen peroxide can be controlled by a gating voltage and illustrate the operation of a field-effect bio-catalytic transistor, whose current-generating mechanism is the conversion of hydrogen peroxide to water with the current being controlled by the gating voltage.

  18. A new type of hydrogen generator-HHEG (high-compressed hydrogen energy generator)

    International Nuclear Information System (INIS)

    'Full text:' We have developed a new type of hydrogen generator named HHEG (High-compressed Hydrogen Energy Generator). HHEG can produce 35 MPa high-compressed hydrogen for fuel cell vehicle without any mechanical compressor. HHEG is a kind of PEM(proton exchange membrane)electrolysis. It was well known that compressed hydrogen could be generated by water electrolysis. However, the conventional electrolysis could not generate 35 MPa or higher pressure that is required for fuel cell vehicle, because electrolysis cell stack is destroyed in such high pressure. In HHEG, the cell stack is put in high-pressure vessel and the pressure difference of oxygen and hydrogen that is generated by the cell stack is always kept at nearly zero by an automatic compensator invented by Mitsubishi Corporation. The cell stack of HHEG is not so special one, but it is not broken under such high pressure, because the automatic compensator always offsets the force acting on the cell stack. Hydrogen for fuel cell vehicle must be produce by no emission energy such as solar and atomic power. These energies are available as electricity. So, water electrolysis is the only way of producing hydrogen fuel. Hydrogen fuel is also 35 MPa high-compressed hydrogen and will become 70 MPa in near future. But conventional mechanical compressor is not useful for such high pressure hydrogen fuel, because of the short lifetime and high power consumption. Construction of hydrogen station network is indispensable in order to come into wide use of fuel cell vehicles. For such network contraction, an on-site type hydrogen generator is required. HHEG can satisfy above these requirements. So we can conclude that HHEG is the only way of realizing the hydrogen economy. (author)

  19. Catalytic enantioselective OFF ↔ ON activation processes initiated by hydrogen transfer: concepts and challenges.

    Science.gov (United States)

    Quintard, Adrien; Rodriguez, Jean

    2016-08-18

    Hydrogen transfer initiated processes are eco-compatible transformations allowing the reversible OFF ↔ ON activation of otherwise unreactive substrates. The minimization of stoichiometric waste as well as the unique activation modes provided by these transformations make them key players for a greener future for organic synthesis. Long limited to catalytic reactions that form racemic products, considerable progress on the development of strategies for controlling diastereo- and enantioselectivity has been made in the last decade. The aim of this review is to present the different strategies that enable enantioselective transformations of this type and to highlight how they can be used to construct key synthetic building blocks in fewer operations with less waste generation. PMID:27381644

  20. Production of hydrogen, liquid fuels, and chemicals from catalytic processing of bio-oils

    Science.gov (United States)

    Huber, George W; Vispute, Tushar P; Routray, Kamalakanta

    2014-06-03

    Disclosed herein is a method of generating hydrogen from a bio-oil, comprising hydrogenating a water-soluble fraction of the bio-oil with hydrogen in the presence of a hydrogenation catalyst, and reforming the water-soluble fraction by aqueous-phase reforming in the presence of a reforming catalyst, wherein hydrogen is generated by the reforming, and the amount of hydrogen generated is greater than that consumed by the hydrogenating. The method can further comprise hydrocracking or hydrotreating a lignin fraction of the bio-oil with hydrogen in the presence of a hydrocracking catalyst wherein the lignin fraction of bio-oil is obtained as a water-insoluble fraction from aqueous extraction of bio-oil. The hydrogen used in the hydrogenating and in the hydrocracking or hydrotreating can be generated by reforming the water-soluble fraction of bio-oil.

  1. Partial catalytic oxidation of CH{sub 4} to synthesis gas for power generation - Final report

    Energy Technology Data Exchange (ETDEWEB)

    Mantzaras, I.; Schneider, A.

    2006-03-15

    The partial oxidation of methane to synthesis gas over rhodium catalysts has been investigated experimentally and numerically in the pressure range of 4 to 10 bar. The methane/oxidizer feed has been diluted with large amounts of H{sub 2}O and CO{sub 2} (up to 70% vol.) in order to simulate new power generation cycles with large exhaust gas recycle. Experiments were carried out in an optically accessible channel-flow reactor that facilitated laser-based in situ measurements, and also in a subscale gas-turbine catalytic reactor. Full-elliptic steady and transient two-dimensional numerical codes were used, which included elementary hetero-/homogeneous chemical reaction schemes. The following are the key conclusions: a) Heterogeneous (catalytic) and homogeneous (gas-phase) schemes have been validated for the partial catalytic oxidation of methane with large exhaust gas recycle. b) The impact of added H{sub 2}O and CO{sub 2} has been elucidated. The added H{sub 2}O increased the methane conversion and hydrogen selectivity, while it decreased the CO selectivity. The chemical impact of CO{sub 2} (dry reforming) was minimal. c) The numerical model reproduced the measured catalytic ignition times. It was further shown that the chemical impact of H{sub 2}O and CO{sub 2} on the catalytic ignition delay times was minimal. d) The noble metal dispersion increased with different support materials, in the order Rh/{alpha}-Al{sub 2}O{sub 3}, Rh/ZrO{sub 2}, and Rh/Ce-ZrO{sub 2}. An evident relationship was established between the noble metal dispersion and the catalytic behavior. (authors)

  2. Catalytic on-board hydrogen production from methanol and ammonia for mobile application

    Energy Technology Data Exchange (ETDEWEB)

    Soerijanto, H.

    2008-08-15

    This PhD thesis deals with the catalytic hydrogen production for mobile application, for example for the use in fuel cells for electric cars. Electric powered buses with fuel cells as driving system are well known, but the secure hydrogen storage in adequate amounts for long distance drive is still a topic of discussion. Methanol is an excellent hydrogen carrier. First of all it has a high H:C ratio and therefore a high energy density. Secondly the operating temperature of steam reforming of methanol is comparatively low (250 C) and there is no risk of coking since methanol has no C-C bond. Thirdly methanol is a liquid, which means that the present gasoline infrastructure can be used. For the further development of catalysts and for the construction of a reformer it is very important to characterize the catalysts very well. For the dimensioning and the control of an on-board production of hydrogen it is essential to draw accurately on the thermodynamic, chemical and kinetic data of the reaction. At the first part of this work the mesoporous Cu/ZrO{sub 2}/CeO{sub 2}-catalysts with various copper contents were characterized and their long-term stability and selectivity were investigated, and the kinetic data were determined. Carbon monoxide is generated by reforming of carbon containing material. This process is undesired since CO poisons the Pt electrode of the fuel cell. The separation of hydrogen by metal membranes is technically feasible and a high purity of hydrogen can be obtained. However, due to their high density this procedure is not favourable because of its energy loss. In this study a concept is presented, which enables an autothermal mode by application of ceramic membrane and simultaneously could help to deal with the CO problem. The search for an absolutely selective catalyst is uncertain. The production of CO can be neither chemically nor thermodynamically excluded, if carbon is present in the hydrogen carrier. Since enrichment or separation are

  3. Demonstration of the Catalytic Decomposition of Hydrogen Peroxide.

    Science.gov (United States)

    Conklin, Alfred R. Jr.; Kessinger, Angela

    1996-01-01

    Describes a demonstration known as Elephant's Toothpaste in which the decomposition of hydrogen peroxide is catalyzed by iodide. Oxygen is released and soap bubbles are produced. The foam produced is measured, and results show a good relationship between the amount of foam and the concentration of the hydrogen peroxide. (DDR)

  4. Catalytic hydrogenation using complexes of base metals with tridentate ligands

    Energy Technology Data Exchange (ETDEWEB)

    Vasudevan, Kalyan V.; Zhang, Guoqi; Hanson, Susan K.

    2016-09-06

    Complexes of cobalt and nickel with tridentate ligand PNHP.sup.R are effective for hydrogenation of unsaturated compounds. Cobalt complex [(PNHP.sup.Cy)Co(CH.sub.2SiMe.sub.3)]BAr.sup.F.sub.4 (PNHP.sup.Cy=bis[2-(dicyclohexylphosphino)ethyl]amine, BAr.sup.F.sub.4=B(3,5-(CF.sub.3).sub.2C.sub.6H.sub.3).sub.4)) was prepared and used with hydrogen for hydrogenation of alkenes, aldehydes, ketones, and imines under mild conditions (25-60.degree. C., 1-4 atm H.sub.2). Nickel complex [(PNHP.sup.Cy)Ni(H)]BPh.sub.4 was used for hydrogenation of styrene and 1-octene under mild conditions. (PNP.sup.Cy)Ni(H) was used for hydrogenating alkenes.

  5. Tunable Molecular MoS2 Edge-Site Mimics for Catalytic Hydrogen Production.

    Science.gov (United States)

    Garrett, Benjamin R; Polen, Shane M; Click, Kevin A; He, Mingfu; Huang, Zhongjie; Hadad, Christopher M; Wu, Yiying

    2016-04-18

    Molybdenum sulfides represent state-of-the-art, non-platinum electrocatalysts for the hydrogen evolution reaction (HER). According to the Sabatier principle, the hydrogen binding strength to the edge active sites should be neither too strong nor too weak. Therefore, it is of interest to develop a molecular motif that mimics the catalytic sites structurally and possesses tunable electronic properties that influence the hydrogen binding strength. Furthermore, molecular mimics will be important for providing mechanistic insight toward the HER with molybdenum sulfide catalysts. In this work, a modular method to tune the catalytic properties of the S-S bond in MoO(S2)2L2 complexes is described. We studied the homogeneous electrocatalytic hydrogen production performance metrics of three catalysts with different bipyridine substitutions. By varying the electron-donating abilities, we present the first demonstration of using the ligand to tune the catalytic properties of the S-S bond in molecular MoS2 edge-site mimics. This work can shed light on the relationship between the structure and electrocatalytic activity of molecular MoS2 catalysts and thus is of broad importance from catalytic hydrogen production to biological enzyme functions. PMID:27022836

  6. Hydrogen generation via photoelectrochemical water splitting using chemically exfoliated MoS2 layers

    International Nuclear Information System (INIS)

    Study on hydrogen generation has been of huge interest due to increasing demand for new energy sources. Photoelectrochemical reaction by catalysts was proposed as a promising technique for hydrogen generation. Herein, we report the hydrogen generation via photoelectrochecmial reaction using films of exfoliated 2-dimensional (2D) MoS2, which acts as an efficient photocatalyst. The film of chemically exfoliated MoS2 layers was employed for water splitting, leading to hydrogen generation. The amount of hydrogen was qualitatively monitored by observing overpressure of a water container. The high photo-current generated by MoS2 film resulted in hydrogen evolution. Our work shows that 2D MoS2 is one of the promising candidates as a photocatalyst for light-induced hydrogen generation. High photoelectrocatalytic efficiency of the 2D MoS2 shows a new way toward hydrogen generation, which is one of the renewable energy sources. The efficient photoelectrocatalytic property of the 2D MoS2 is possibly due to availability of catalytically active edge sites together with minimal stacking that favors the electron transfer

  7. Hydrogen generation via photoelectrochemical water splitting using chemically exfoliated MoS2 layers

    Directory of Open Access Journals (Sweden)

    R. K. Joshi

    2016-01-01

    Full Text Available Study on hydrogen generation has been of huge interest due to increasing demand for new energy sources. Photoelectrochemical reaction by catalysts was proposed as a promising technique for hydrogen generation. Herein, we report the hydrogen generation via photoelectrochecmial reaction using films of exfoliated 2-dimensional (2D MoS2, which acts as an efficient photocatalyst. The film of chemically exfoliated MoS2 layers was employed for water splitting, leading to hydrogen generation. The amount of hydrogen was qualitatively monitored by observing overpressure of a water container. The high photo-current generated by MoS2 film resulted in hydrogen evolution. Our work shows that 2D MoS2 is one of the promising candidates as a photocatalyst for light-induced hydrogen generation. High photoelectrocatalytic efficiency of the 2D MoS2 shows a new way toward hydrogen generation, which is one of the renewable energy sources. The efficient photoelectrocatalytic property of the 2D MoS2 is possibly due to availability of catalytically active edge sites together with minimal stacking that favors the electron transfer.

  8. Hydrogen generation via photoelectrochemical water splitting using chemically exfoliated MoS{sub 2} layers

    Energy Technology Data Exchange (ETDEWEB)

    Joshi, R. K., E-mail: r.joshi@unsw.edu.au, E-mail: alwarappan@cecri.res.in; Sahajwalla, V. [Centre for Sustainable Materials Research and Technology, School of Materials Science and Engineering, University of New South Wales, NSW 2052 (Australia); Shukla, S.; Saxena, S. [Department of Metallurgical Engineering and Materials Science, Indian Institute of Technology Bombay, Mumbai (India); Lee, G.-H. [Department of Material Science and Engineering, Yonsei University, Seoul 120-749 (Korea, Republic of); Alwarappan, S., E-mail: r.joshi@unsw.edu.au, E-mail: alwarappan@cecri.res.in [CSIR-Central Electrochemical Research Institute, Karaikudi 630006, Tamilnadu (India)

    2016-01-15

    Study on hydrogen generation has been of huge interest due to increasing demand for new energy sources. Photoelectrochemical reaction by catalysts was proposed as a promising technique for hydrogen generation. Herein, we report the hydrogen generation via photoelectrochecmial reaction using films of exfoliated 2-dimensional (2D) MoS{sub 2}, which acts as an efficient photocatalyst. The film of chemically exfoliated MoS{sub 2} layers was employed for water splitting, leading to hydrogen generation. The amount of hydrogen was qualitatively monitored by observing overpressure of a water container. The high photo-current generated by MoS{sub 2} film resulted in hydrogen evolution. Our work shows that 2D MoS{sub 2} is one of the promising candidates as a photocatalyst for light-induced hydrogen generation. High photoelectrocatalytic efficiency of the 2D MoS{sub 2} shows a new way toward hydrogen generation, which is one of the renewable energy sources. The efficient photoelectrocatalytic property of the 2D MoS{sub 2} is possibly due to availability of catalytically active edge sites together with minimal stacking that favors the electron transfer.

  9. Hydrogen generation via photoelectrochemical water splitting using chemically exfoliated MoS2 layers

    Science.gov (United States)

    Joshi, R. K.; Shukla, S.; Saxena, S.; Lee, G.-H.; Sahajwalla, V.; Alwarappan, S.

    2016-01-01

    Study on hydrogen generation has been of huge interest due to increasing demand for new energy sources. Photoelectrochemical reaction by catalysts was proposed as a promising technique for hydrogen generation. Herein, we report the hydrogen generation via photoelectrochecmial reaction using films of exfoliated 2-dimensional (2D) MoS2, which acts as an efficient photocatalyst. The film of chemically exfoliated MoS2 layers was employed for water splitting, leading to hydrogen generation. The amount of hydrogen was qualitatively monitored by observing overpressure of a water container. The high photo-current generated by MoS2 film resulted in hydrogen evolution. Our work shows that 2D MoS2 is one of the promising candidates as a photocatalyst for light-induced hydrogen generation. High photoelectrocatalytic efficiency of the 2D MoS2 shows a new way toward hydrogen generation, which is one of the renewable energy sources. The efficient photoelectrocatalytic property of the 2D MoS2 is possibly due to availability of catalytically active edge sites together with minimal stacking that favors the electron transfer.

  10. Preparation of Hydrogen through Catalytic Steam Reforming of Bio-oil

    Institute of Scientific and Technical Information of China (English)

    吴层; 颜涌捷; 李庭琛; 亓伟

    2007-01-01

    Hydrogen was prepared via catalytic steam reforming of bio-oil which was obtained from fast pyrolysis of biomass in a fluidized bed reactor. Influential factors including temperature, weight hourly space velocity (WHSV) of bio-oil, mass ratio of steam to bio-oil (S/B) as well as catalyst type on hydrogen selectivity and other desirable gas products were investigated. Based on hydrogen in stoichiometric potential and carbon balance in gaseous phase and feed, hydrogen yield and carbon selectivity were examined. The experimental results show that higher temperature favors the hydrogen selectivity by H2 mole fraction in gaseous products stream and it plays an important role in hydrogen yield and carbon selectivity. Higher hydrogen selectivity and yield, and carbon selectivity were obtained at lower bio-oil WHSV. In catalytic steam reforming system a maximum steam concentration value exists, at which hydrogen selectivity and yield, and carbon selectivity keep constant. Through experiments, preferential operation conditions were obtained as follows: temperature 800~850℃, bio-oil WHSV below 3.0 h-1, and mass ratio of steam to bio-oil 10~12. The performance tests indicate that Ni-based catalysts are optional, especially Ni/a-Al2O3 effective in the steam reforming process.

  11. Low temperature catalytic combustion of natural gas - hydrogen - air mixtures

    Energy Technology Data Exchange (ETDEWEB)

    Newson, E.; Roth, F. von; Hottinger, P.; Truong, T.B. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

    1999-08-01

    The low temperature catalytic combustion of natural gas - air mixtures would allow the development of no-NO{sub x} burners for heating and power applications. Using commercially available catalysts, the room temperature ignition of methane-propane-air mixtures has been shown in laboratory reactors with combustion efficiencies over 95% and maximum temperatures less than 700{sup o}C. After a 500 hour stability test, severe deactivation of both methane and propane oxidation functions was observed. In cooperation with industrial partners, scaleup to 3 kW is being investigated together with startup dynamics and catalyst stability. (author) 3 figs., 3 refs.

  12. Catalytic Metal Free Production of Large Cage Structure Carbon Particles: A Candidate for Hydrogen Storage

    Science.gov (United States)

    Kimura, Yuki; Nuth, Joseph A., III; Ferguson, Frank T.

    2005-01-01

    We will demonstrate that carbon particles consisting of large cages can be produced without catalytic metal. The carbon particles were produced in CO gas as well as by introduction of 5% methane gas into the CO gas. The gas-produced carbon particles were able to absorb approximately 16.2 wt% of hydrogen. This value is 2.5 times higher than the 6.5 wt% goal for the vehicular hydrogen storage proposed by the Department of Energy in the USA. Therefore, we believe that this carbon particle is an excellent candidate for hydrogen storage for fuel cells.

  13. Molecular catalytic hydrogenation of aromatic hydrocarbons and hydrotreating of coal liquids.

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Shiyong; Stock, L.M.

    1996-05-01

    This report presents the results of research on the development of new catalytic pathways for the hydrogenation of multiring aromatic hydrocarbons and the hydrotreating of coal liquids at The University of Chicago under DOE Contract No. DE-AC22-91PC91056. The work, which is described in three parts, is primarily concerned with the research on the development of new catalytic systems for the hydrogenation of aromatic hydrocarbons and for the improvement of the quality of coal liquids by the addition of dihydrogen. Part A discusses the activation of dihydrogen by very basic molecular reagents to form adducts that can facilitate the reduction of multiring aromatic hydrocarbons. Part B examines the hydrotreating of coal liquids catalyzed by the same base-activated dihydrogen complexes. Part C concerns studies of molecular organometallic catalysts for the hydrogenation of monocyclic aromatic hydrocarbons under mild conditions.

  14. Catalytic Hydrogenation of Bio-Oil for Chemicals and Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Elliott, Douglas C.

    2006-02-14

    The scope of work includes optimizing processing conditions and demonstrating catalyst lifetime for catalyst formulations that are readily scaleable to commercial operations. We use a bench-scale, continuous-flow, packed-bed, catalytic, tubular reactor, which can be operated in the range of 100-400 mL/hr., from 50-400 C and up to 20MPa (see Figure 1). With this unit we produce upgraded bio-oil from whole bio-oil or useful bio-oil fractions, specifically pyrolytic lignin. The product oils are fractionated, for example by distillation, for recovery of chemical product streams. Other products from our tests have been used in further testing in petroleum refining technology at UOP and fractionation for product recovery in our own lab. Further scale-up of the technology is envisioned and we will carry out or support process design efforts with industrial partners, such as UOP.

  15. Hydrogen Recombination Rates of Plate-type Passive Auto-catalytic Recombiner

    International Nuclear Information System (INIS)

    The hydrogen mitigation system may include igniters, passive autocatalytic recombiner (PAR), and venting or dilution system. Recently PAR is commonly used as a main component of HMS in a NPP containment because of its passive nature. PARs are categorized by the shape and material of catalytic surface. Catalytic surface coated by platinum is mostly used for the hydrogen recombiners. The shapes of the catalytic surface can be grouped into plate type, honeycomb type and porous media type. Among them, the plate-type PAR is well tested by many experiments. PAR performance analysis can be approached by a multi-scale method which is composed of micro, meso and macro scales. The criterion of the scaling is the ratio of thickness of boundary layer developed on a catalytic surface to representative length of a computational domain. Mass diffusion in the boundary layer must be resolved in the micro scale analysis. In a lumped parameter (LP) analysis using a system code such as MAAP or MELCOR, the chamber of the PAR is much smaller than a computational node. The hydrogen depletion by a PAR is modeled as a source of mass and energy conservation equations. Te catalytic surface reaction of hydrogen must be modeled by a volume-averaged correlation. In this study, a micro scale analysis method is developed using libraries in OpenFOAM to evaluate a hydrogen depletion rate depending on parameters such as size and number of plates and plate arrangement. The analysis code is validated by simulating REKO-3 experiment. And hydrogen depletion analysis is conducted by changing the plate arrangement as a trial of the performance enhancement of a PAR. In this study, a numerical code for an analysis of a PAR performance in a micro scale has been developed by using OpenFOAM libraries. The physical and numerical models were validated by simulating the REKO-3 experiment. As a try to enhance the performance of the plate-type PAR, it was proposed to apply a staggered two-layer arrangement of the

  16. Hydrogen Recombination Rates of Plate-type Passive Auto-catalytic Recombiner

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jongtae; Hong, Seong-Wan [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Kim, Gun Hong [Kyungwon E-C Co., Seongnam (Korea, Republic of)

    2014-10-15

    The hydrogen mitigation system may include igniters, passive autocatalytic recombiner (PAR), and venting or dilution system. Recently PAR is commonly used as a main component of HMS in a NPP containment because of its passive nature. PARs are categorized by the shape and material of catalytic surface. Catalytic surface coated by platinum is mostly used for the hydrogen recombiners. The shapes of the catalytic surface can be grouped into plate type, honeycomb type and porous media type. Among them, the plate-type PAR is well tested by many experiments. PAR performance analysis can be approached by a multi-scale method which is composed of micro, meso and macro scales. The criterion of the scaling is the ratio of thickness of boundary layer developed on a catalytic surface to representative length of a computational domain. Mass diffusion in the boundary layer must be resolved in the micro scale analysis. In a lumped parameter (LP) analysis using a system code such as MAAP or MELCOR, the chamber of the PAR is much smaller than a computational node. The hydrogen depletion by a PAR is modeled as a source of mass and energy conservation equations. Te catalytic surface reaction of hydrogen must be modeled by a volume-averaged correlation. In this study, a micro scale analysis method is developed using libraries in OpenFOAM to evaluate a hydrogen depletion rate depending on parameters such as size and number of plates and plate arrangement. The analysis code is validated by simulating REKO-3 experiment. And hydrogen depletion analysis is conducted by changing the plate arrangement as a trial of the performance enhancement of a PAR. In this study, a numerical code for an analysis of a PAR performance in a micro scale has been developed by using OpenFOAM libraries. The physical and numerical models were validated by simulating the REKO-3 experiment. As a try to enhance the performance of the plate-type PAR, it was proposed to apply a staggered two-layer arrangement of the

  17. CATALYTIC BEHAVIOR OF A SILICA-SUPPORTED POLYTITAZANE-PLATINUM COMPLEX FOR THE HYDROGENATION OF PHENOL

    Institute of Scientific and Technical Information of China (English)

    CHEN Chunwei; HUANG Meiyu; JIANG Yingyan

    1996-01-01

    A new kind of inorganic polymer, viz. silica-supported polytitazane (Ti-N), and its platinum complex (Ti-N-Pt) were prepared. Cyclohexanone can be obtained in a maximum yield of about 62.2% in the hydrogenation of phenol over Ti-N-Pt at room temperature under atmospheric pressure. The effects of mole ratio of N/Pt in the complex, concentration of the catalyst and reaction temperature on the catalytic activity and selectivity have been studied. The complex can be reused several times without loss in its catalytic activity.

  18. Biomass to hydrogen via fast pyrolysis and catalytic steam reforming

    Energy Technology Data Exchange (ETDEWEB)

    Chornet, E.; Wang, D.; Montane, D. [National Renewable Energy Lab., Golden, CO (United States)] [and others

    1995-09-01

    Fast pyrolysis of biomass results in a pyrolytic oil which is a mixture of (a) carbohydrate-derived acids, aldehydes and polyols, (b) lignin-derived substituted phenolics, and (c) extractives-derived terpenoids and fatty acids. The conversion of this pyrolysis oil into H{sub 2} and CO{sub 2} is thermodynamically favored under appropriate steam reforming conditions. Our efforts have focused in understanding the catalysis of steam reforming which will lead to a successful process at reasonable steam/carbon ratios arid process severities. The experimental work, carried out at the laboratory and bench scale levels, has centered on the performance of Ni-based catalysts using model compounds as prototypes of the oxygenates present in the pyrolysis oil. Steam reforming of acetic acid, hydroxyacetaldehyde, furfural and syringol has been proven to proceed rapidly within a reasonable range of severities. Time-on-stream studies are now underway using a fixed bed barometric pressure reactor to ascertain the durability of the catalysts and thus substantiate the scientific and technical feasibility of the catalytic reforming option. Economic analyses are being carried out in parallel to determine the opportunity zones for the combined fast pyrolysis/steam reforming approach. A discussion on the current state of the project is presented.

  19. Modeling of hydrogen/deuterium dynamics and heat generation on palladium nanoparticles for hydrogen storage and solid-state nuclear fusion.

    Science.gov (United States)

    Tanabe, Katsuaki

    2016-01-01

    We modeled the dynamics of hydrogen and deuterium adsorbed on palladium nanoparticles including the heat generation induced by the chemical adsorption and desorption, as well as palladium-catalyzed reactions. Our calculations based on the proposed model reproduce the experimental time-evolution of pressure and temperature with a single set of fitting parameters for hydrogen and deuterium injection. The model we generated with a highly generalized set of formulations can be applied for any combination of a gas species and a catalytic adsorbent/absorbent. Our model can be used as a basis for future research into hydrogen storage and solid-state nuclear fusion technologies. PMID:27441240

  20. Modeling of hydrogen/deuterium dynamics and heat generation on palladium nanoparticles for hydrogen storage and solid-state nuclear fusion.

    Science.gov (United States)

    Tanabe, Katsuaki

    2016-01-01

    We modeled the dynamics of hydrogen and deuterium adsorbed on palladium nanoparticles including the heat generation induced by the chemical adsorption and desorption, as well as palladium-catalyzed reactions. Our calculations based on the proposed model reproduce the experimental time-evolution of pressure and temperature with a single set of fitting parameters for hydrogen and deuterium injection. The model we generated with a highly generalized set of formulations can be applied for any combination of a gas species and a catalytic adsorbent/absorbent. Our model can be used as a basis for future research into hydrogen storage and solid-state nuclear fusion technologies.

  1. Nitrogen-Doped Graphene for Photocatalytic Hydrogen Generation.

    Science.gov (United States)

    Chang, Dong Wook; Baek, Jong-Beom

    2016-04-20

    Photocatalytic hydrogen (H2 ) generation in a water splitting process has recently attracted tremendous interest because it allows the direct conversion of clean and unlimited solar energy into the ideal energy resource of H2 . For efficient photocatalytic H2 generation, the role of the photocatalyst is critical. With increasing demand for more efficient, sustainable, and cost-effective photocatalysts, various types of semiconductor photocatalysts have been intensively developed. In particular, on the basis of its superior catalytic and tunable electronic properties, nitrogen-doped graphene is a potential candidate for a high-performance photocatalyst. Nitrogen-doped graphene also offers additional advantages originating from its unique two-dimensional sp(2) -hybridized carbon network including a large specific surface area and exceptional charge transport properties. It has been reported that nitrogen-doped graphene can play diverse but positive functions including photo-induced charge acceptor/meditator, light absorber from UV to visible light, n-type semiconductor, and giant molecular photocatalyst. Herein, we summarize the recent progress and general aspects of nitrogen-doped graphene as a photocatalyst for photocatalytic H2 generation. In addition, challenges and future perspectives in this field are also discussed. PMID:26762892

  2. A new process for preparing dialdehyde by catalytic oxidation of cyclic olefins with aqueous hydrogen peroxide

    Institute of Scientific and Technical Information of China (English)

    YU, Hong-Kun; PANG, Zhen; HUANG, Zu-En; CAI, Rui-Fang

    2000-01-01

    A novel peroxo-nioboplosphate was synthesized for the first time and used as a catalyst in the oxidation reaction of cyclic olefins with aqueous hydrogen peroxide to prepare dialdehydes. The catalyst was characterized by elemental analysis,thermographic analyses, IR, UV/vis, 31P NMR and XPS ~ as [ π-C5H5N(CH2)i3CH3 ]2 [Nb406 (O2)2 (PO4)2] ·6H20 (PTNP). It showed high selectivity to glutaraldehyde in the catalytic oxidation of cyclopentene with aqueous hydrogen peroxide in ethanol.

  3. Exploiting high pressure advantages in catalytic hydrogenation of carbon dioxide to methanol

    OpenAIRE

    Bansode, Atul Baban

    2014-01-01

    The aim of this thesis was to develop highly efficient CO2 hydrogenation process towards methanol by making use of high pressure approach. A high pressure lab scale plant was developed to conduct CO2 hydrogenation up to 400 bar. High pressure and low temperature were found to be the favourable conditions to excellent catalytic activity. Improved reaction performance towards methanol synthesis and reverse water-gas shift reaction was observed for the Ba and K promoted Cu/Al2O3 catalysts, respe...

  4. Catalytic Transfer Hydrogenation with a Methandiide-Based Carbene Complex: An Experimental and Computational Study.

    Science.gov (United States)

    Weismann, Julia; Gessner, Viktoria H

    2015-11-01

    The transfer hydrogenation (TH) reaction of ketones with catalytic systems based on a methandiide-derived ruthenium carbene complex was investigated and optimised. The complex itself makes use of the noninnocent behaviour of the carbene ligand (M=CR2 →MH-C(H)R2 ), but showed only moderate activity, thus requiring long reaction times to achieve sufficient conversion. DFT studies on the reaction mechanism revealed high reaction barriers for both the dehydrogenation of iPrOH and the hydrogen transfer. A considerable improvement of the catalytic activity could be achieved by employing triphenylphosphine as additive. Mechanistic studies on the role of PPh3 in the catalytic cycle revealed the formation of a cyclometalated complex upon phosphine coordination. This ruthenacycle was revealed to be the active species under the reaction conditions. The use of the isolated complex resulted in high catalytic activities in the TH of aromatic as well as aliphatic ketones. The complex was also found to be active under base-free conditions, suggesting that the cyclometalation is crucial for the enhanced activity. PMID:26403918

  5. State of the art on hydrogen passive auto-catalytic recombiner (european union Parsoar project)

    Energy Technology Data Exchange (ETDEWEB)

    Arnould, F.; Bachellerie, E. [Technicatome, 13 - Aix en Provence (France); Auglaire, M. [Tractebel Energy Engineering, Brussels (Belgium); Boeck, B. de [Association Vincotte Nuclear, Brussels (Belgium); Braillard, O. [CEA Cadarache, 13 - Saint Paul lez Durance (France); Eckardt, B. [Siemens AG, Offenbach am Main (Germany); Ferroni, F. [Electrowatt Engineering Limited, Zurich (Switzerland); Moffett, R. [Atomic Energy Canada Limited, Pinawa (Canada); Van Goethem, G. [European Commission, Brussels (Belgium)

    2001-07-01

    This paper presents an overview of the European Union PARSOAR project, which consists in carrying out a state of the art on hydrogen passive auto-catalytic recombiner (PAR) and a handbook guide for implementing these devices in nuclear power plants. This work is performed in the area ''Operational Safety of Existing Installations'' of the key action ''Nuclear Fission'' of the fifth Euratom Framework Programme (1998-2002). (author)

  6. Ruthenium on rutile catalyst, catalytic system, and method for aqueous phase hydrogenations

    Science.gov (United States)

    Elliot, Douglas C.; Werpy, Todd A.; Wang, Yong; Frye, Jr., John G.

    2001-01-01

    An essentially nickel- and rhenium-free catalyst is described comprising ruthenium on a titania support where the titania is greater than 75% rutile. A catalytic system containing a nickel-free catalyst comprising ruthenium on a titania support where the titania is greater than 75% rutile, and a method using this catalyst in the hydrogenation of an organic compound in the aqueous phase is also described.

  7. State of the art on hydrogen passive auto-catalytic recombiner (european union Parsoar project)

    International Nuclear Information System (INIS)

    This paper presents an overview of the European Union PARSOAR project, which consists in carrying out a state of the art on hydrogen passive auto-catalytic recombiner (PAR) and a handbook guide for implementing these devices in nuclear power plants. This work is performed in the area ''Operational Safety of Existing Installations'' of the key action ''Nuclear Fission'' of the fifth Euratom Framework Programme (1998-2002). (author)

  8. Liquid-Phase Catalytic Transfer Hydrogenation of Furfural over Homogeneous Lewis Acid-Ru/C Catalysts.

    Science.gov (United States)

    Panagiotopoulou, Paraskevi; Martin, Nickolas; Vlachos, Dionisios G

    2015-06-22

    The catalytic performance of homogeneous Lewis acid catalysts and their interaction with Ru/C catalyst are studied in the catalytic transfer hydrogenation of furfural by using 2-propanol as a solvent and hydrogen donor. We find that Lewis acid catalysts hydrogenate the furfural to furfuryl alcohol, which is then etherified with 2-propanol. The catalytic activity is correlated with an empirical scale of Lewis acid strength and exhibits a volcano behavior. Lanthanides are the most active, with DyCl3 giving complete furfural conversion and a 97 % yield of furfuryl alcohol at 180 °C after 3 h. The combination of Lewis acid and Ru/C catalysts results in synergy for the stronger Lewis acid catalysts, with a significant increase in the furfural conversion and methyl furan yield. Optimum results are obtained by using Ru/C combined with VCl3 , AlCl3 , SnCl4 , YbCl3 , and RuCl3 . Our results indicate that the combination of Lewis acid/metal catalysts is a general strategy for performing tandem reactions in the upgrade of furans.

  9. Nanostructured, complex hydride systems for hydrogen generation

    Directory of Open Access Journals (Sweden)

    Robert A. Varin

    2015-02-01

    Full Text Available Complex hydride systems for hydrogen (H2 generation for supplying fuel cells are being reviewed. In the first group, the hydride systems that are capable of generating H2 through a mechanical dehydrogenation phenomenon at the ambient temperature are discussed. There are few quite diverse systems in this group such as lithium alanate (LiAlH4 with the following additives: nanoiron (n-Fe, lithium amide (LiNH2 (a hydride/hydride system and manganese chloride MnCl2 (a hydride/halide system. Another hydride/hydride system consists of lithium amide (LiNH2 and magnesium hydride (MgH2, and finally, there is a LiBH4-FeCl2 (hydride/halide system. These hydride systems are capable of releasing from ~4 to 7 wt.% H2 at the ambient temperature during a reasonably short duration of ball milling. The second group encompasses systems that generate H2 at slightly elevated temperature (up to 100 °C. In this group lithium alanate (LiAlH4 ball milled with the nano-Fe and nano-TiN/TiC/ZrC additives is a prominent system that can relatively quickly generate up to 7 wt.% H2 at 100 °C. The other hydride is manganese borohydride (Mn(BH42 obtained by mechano-chemical activation synthesis (MCAS. In a ball milled (2LiBH4 + MnCl2 nanocomposite, Mn(BH42 co-existing with LiCl can desorb ~4.5 wt.% H2 at 100 °C within a reasonable duration of dehydrogenation. Practical application aspects of hydride systems for H2 generation/storage are also briefly discussed.

  10. TEC as electric generator in an automobile catalytic converter

    Energy Technology Data Exchange (ETDEWEB)

    Svensson, R. [Chalmers Univ. of Technology, Goeteborg (Sweden); Holmlid, L. [Univ. of Goeteborg (Sweden). Dept. of Physical Chemistry

    1996-12-31

    Modern cars use more and more electric power due to more on-board electric systems, e.g., ABS brakes, active suspension systems, electric windows, chair adjustment systems and electronic engine control systems. One possible energy source for electricity generation is to use the waste heat from the car`s engine, which generally is as much as 80% of the total energy from the combustion of the gasoline. Maybe the best location to tap the excess heat is the Catalytic Converter (Cat) in the exhaust system or perhaps at the exhaust pipes close to the engine. The Cat must be kept within a certain temperature interval. Large amounts of heat are dissipated through the wall of the Cat. A Thermionic Energy Converter (TEC) in coaxial form could conveniently be located around the ceramic cartridge of the Cat. Since the TEC is a rather good heat insulator before it reaches its working temperature the Cat will reach working temperature faster, and the final temperature of it can be controlled better when encapsulated in a concentric TEC arrangement. It is also possible to regulate the temperature of the Cat and the TEC by controlling the electrical load of the TEC. The possible working temperatures of present and future Cats appear very suitable for the new low work function collector TEC, which has been demonstrated to work down to 470 K.

  11. Dendrimer Templated Synthesis of One Nanometer Rh and Pt Particles Supported on Mesoporous Silica: Catalytic Activity for Ethylene and Pyrrole Hydrogenation.

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Wenyu; Kuhn, John N.; Tsung, Chia-Kuang; Zhang, Yawen; Habas, Susan E.; Yang, Peidong; Somorjai, Gabor A.

    2008-05-09

    Monodisperse rhodium (Rh) and platinum (Pt) nanoparticles as small as {approx}1 nm were synthesized within a fourth generation polyaminoamide (PAMAM) dendrimer, a hyperbranched polymer, in aqueous solution and immobilized by depositing onto a high-surface-area SBA-15 mesoporous support. X-ray photoelectron spectroscopy indicated that the as-synthesized Rh and Pt nanoparticles were mostly oxidized. Catalytic activity of the SBA-15 supported Rh and Pt nanoparticles was studied with ethylene hydrogenation at 273 and 293 K in 10 torr of ethylene and 100 torr of H{sub 2} after reduction (76 torr of H{sub 2} mixed with 690 torr of He) at different temperatures. Catalysts were active without removing the dendrimer capping but reached their highest activity after hydrogen reduction at a moderate temperature (423 K). When treated at a higher temperature (473, 573, and 673 K) in hydrogen, catalytic activity decreased. By using the same treatment that led to maximum ethylene hydrogenation activity, catalytic activity was also evaluated for pyrrole hydrogenation.

  12. A bimodal catalytic membrane having a hydrogen-permselective silica layer on a bimodal catalytic support: Preparation and application to the steam reforming of methane

    OpenAIRE

    Tsuru, Toshinori; Shintani, Hiroaki; Yoshioka, Tomohisa; Asaeda, Masashi

    2006-01-01

    The steam reforming of methane for hydrogen production was experimentally investigated using catalytic membrane reactors, consisting of a microporous silica top layer, for the selective permeation of hydrogen, and an α-alumina support layer, for catalytic reaction of the steam reforming of methane. An α-alumina support layer with a bimodal structure, which was proposed for the enhanced dispersion of Ni catalysts, was prepared by impregnating γ-Al2O3 inside α-Al2O3 microfiltration membranes (1...

  13. Catalytic heat exchangers for small-scale production of hydrogen - feasibility study

    Energy Technology Data Exchange (ETDEWEB)

    Silversand, F. [Catator AB, Lund (Sweden)

    2002-02-01

    A feasibility study concerning heat-exchanger reactors in small-scale production of hydrogen has been performed on the request of Svenskt Gastekniskt Center AB and SWEP International AB. The basic idea is to implement different catalysts into brazed plate-type heat exchangers. This can be achieved by installing catalytic cylinders in the inlet-and outlet ports of the heat exchangers or through treatment of the plates to render them catalytically active. It is also possible to sandwich catalytically active wire meshes between the plates. Experiments concerning steam reforming of methanol and methane have been performed in a micro-reactor to gather kinetic data for modelling purposes. Performance calculations concerning heat exchanger reactors have then been conducted with Catator's generic simulation code for catalytic reactors (CatalystExplorer). The simulations clearly demonstrate the technical performance of these reactors. Indeed, the production rate of hydrogen is expected to be about 10 nm{sup 3}/h per litre of heat exchanger. The corresponding value for a conventional steam-reforming unit is about 1 nm{sup 3}/h or less per litre of reactor volume. Also, the compactness and the high degree of integration together with the possibilities of mass production will give an attractive cost for such units. Depending on the demands concerning the purity of the hydrogen it is possible to add secondary catalytic steps like water-gas shifters, methanation and selective oxidation, into a one-train unit, i.e. to design an all-inclusive design. Such reactors can be used for the supply of hydrogen to fuel cells. The production cost for hydrogen can be cut by 60 - 70% through the utilisation of heat exchanger reactors instead of conventional electrolysis. This result is primarily a result of the high price for electricity compared to the feed stock prices in steam reforming. It is important to verify the performance calculations and the simulation results through

  14. Substrate-mediated enhanced activity of Ru nanoparticles in catalytic hydrogenation of benzene

    KAUST Repository

    Liu, Xin

    2012-01-01

    The impact of carbon substrate-Ru nanoparticle interactions on benzene and hydrogen adsorption that is directly related to the performance in catalytic hydrogenation of benzene has been investigated by first-principles based calculations. The stability of Ru 13 nanoparticles is enhanced by the defective graphene substrate due to the hybridization between the dsp states of the Ru 13 particle with the sp 2 dangling bonds at the defect sites. The local curvature formed at the interface will also raise the Ru atomic diffusion barrier, and prohibit the particle sintering. The strong interfacial interaction results in the shift of averaged d-band center of the deposited Ru nanoparticle, from -1.41 eV for a freestanding Ru 13 particle, to -1.17 eV for the Ru/Graphene composites, and to -1.54 eV on mesocellular foam carbon. Accordingly, the adsorption energies of benzene are increased from -2.53 eV for the Ru/mesocellular foam carbon composites, to -2.62 eV on freestanding Ru 13 particles, to -2.74 eV on Ru/graphene composites. A similar change in hydrogen adsorption is also observed, and all these can be correlated to the shift of the d-band center of the nanoparticle. Thus, Ru nanoparticles graphene composites are expected to exhibit both high stability and superior catalytic performance in hydrogenation of arenes. © 2012 The Royal Society of Chemistry.

  15. Catalytic process for control of NO.sub.x emissions using hydrogen

    Science.gov (United States)

    Sobolevskiy, Anatoly; Rossin, Joseph A.; Knapke, Michael J.

    2010-05-18

    A selective catalytic reduction process with a palladium catalyst for reducing NOx in a gas, using hydrogen as a reducing agent. A zirconium sulfate (ZrO.sub.2)SO.sub.4 catalyst support material with about 0.01-2.0 wt. % Pd is applied to a catalytic bed positioned in a flow of exhaust gas at about 70-200.degree. C. The support material may be (ZrO.sub.2--SiO.sub.2)SO.sub.4. H.sub.2O and hydrogen may be injected into the exhaust gas upstream of the catalyst to a concentration of about 15-23 vol. % H.sub.2O and a molar ratio for H.sub.2/NO.sub.x in the range of 10-100. A hydrogen-containing fuel may be synthesized in an Integrated Gasification Combined Cycle power plant for combustion in a gas turbine to produce the exhaust gas flow. A portion of the fuel may be diverted for the hydrogen injection.

  16. Liquid-Phase Catalytic Hydrogenation of Furfural in Variable Solvent Media

    Institute of Scientific and Technical Information of China (English)

    夏淑倩; 李阳; 商巧燕; 张成武; 马沛生

    2016-01-01

    Water is the most abundant compound inherently existing in bio-oils. Thus understanding the role of water within bio-oils upgrading process is essential for future engineering scale-up design. In this study, furfural was chosen as bio-oils model compound, and the catalytic hydrogenation of furfural over commercial 5%, Ru/C catalyst was firstly investigated in a series of gradient variable water/ethanol mixture solvents. Water had a signifi-cant effect on the distribution of product yields. The dominant reaction pathways varied with the water contents in the water/ethanol mixture solvents. Typically, when ethanol was used as the solvent, the main products were ob-tained by the hydrogenation of carbonyl group or furan ring. When pure water was used as the solvent, the rear-rangement reaction of furfural to cyclopentanone should be selectively promoted theoretically. However, serious polymerization and resinification were observed herein in catalytic hydrogenation system of pure water. The cata-lyst surface was modified by the water-insoluble polymers, and consequently, a relative low yield of cyclopenta-none was obtained. A plausible multiple competitive reaction mechanism between polymerization reaction and the hydrogenation of furfural was suggested in this study. Characterizations(TG,FT-IR,SEM)were employed to analyze and explain our experiments.

  17. Passive auto-catalytic recombiners operation in the presence of hydrogen and carbon monoxide: Experimental study and model development

    Energy Technology Data Exchange (ETDEWEB)

    Klauck, Michael, E-mail: klauck@lrst.rwth-aachen.de [RWTH Aachen University, Institute for Reactor Safety and Reactor Technology, 52072 Aachen (Germany); Reinecke, Ernst-Arndt, E-mail: e.reinecke@fz-juelich.de [Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety (IEK-6), 52425 Jülich (Germany); Kelm, Stephan, E-mail: s.kelm@fz-juelich.de [Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety (IEK-6), 52425 Jülich (Germany); Meynet, Nicolas, E-mail: nicolas.meynet@irsn.fr [Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES/SAG/BPhAG, BP 17 92262 Fontenay aux Roses (France); Bentaïb, Ahmed, E-mail: ahmed.bentaib@irsn.fr [Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES/SAG/BPhAG, BP 17 92262 Fontenay aux Roses (France); Allelein, Hans-Josef, E-mail: allelein@lrst.rwth-aachen.de [RWTH Aachen University, Institute for Reactor Safety and Reactor Technology, 52072 Aachen (Germany); Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research – Nuclear Waste Management and Reactor Safety (IEK-6), 52425 Jülich (Germany)

    2014-01-15

    Highlights: • We studied the hydrogen conversion in the presence of carbon monoxide (CO). • CO recombines at a lower efficiency than hydrogen. • Under the given conditions, hydrogen conversion is not affected by CO. • We used three different numerical codes to simulate the experimental findings. • All codes are reproducing the experimental data well. -- Abstract: In a LWR severe accident, carbon monoxide (CO) may be generated inside the containment due to molten corium concrete interaction (MCCI). As a component of the accident atmosphere, CO will interact with passive auto-catalytic recombiners (PARs) which are installed inside LWR containments for hydrogen (H{sub 2}) removal. Depending on the boundary conditions, CO may either react with oxygen to carbon dioxide (CO{sub 2}) or act as catalyst poison, reducing the catalyst activity and hence the hydrogen conversion efficiency. A new experimental test programme performed in co-operation between JÜLICH and RWTH investigates these aspects aiming at providing data for model development for advanced severe accident analyses. In the first test series presented here, the parallel catalytic reaction of H{sub 2} and CO on the catalyst surface has been studied, i.e. the hydrogen recombination reaction was started before CO was injected. In total, 33 steady state measurements have been performed. The test series was jointly evaluated by JÜLICH, RWTH and IRSN. The test results show that under the given conditions the conversion of CO into CO{sub 2} has no negative impact on the parallel hydrogen conversion. The efficiency of the CO recombination in terms of molar rates is significantly smaller (by a factor of ∼2) than the corresponding H{sub 2} conversion efficiency. Due to the exothermal reaction, the parallel CO conversion may also have an impact on the possible ignition of the flammable gases at hot PAR surfaces. The authors have used three different numerical codes for the simulation of the parallel CO

  18. Molecular Self-Assembly Strategy for Generating Catalytic Hybrid Polypeptides

    Science.gov (United States)

    Ikezoe, Yasuhiro; Pike, Douglas H.; Nanda, Vikas; Matsui, Hiroshi

    2016-01-01

    Recently, catalytic peptides were introduced that mimicked protease activities and showed promising selectivity of products even in organic solvents where protease cannot perform well. However, their catalytic efficiency was extremely low compared to natural enzyme counterparts presumably due to the lack of stable tertiary fold. We hypothesized that assembling these peptides along with simple hydrophobic pockets, mimicking enzyme active sites, could enhance the catalytic activity. Here we fused the sequence of catalytic peptide CP4, capable of protease and esterase-like activities, into a short amyloidogenic peptide fragment of Aβ. When the fused CP4-Aβ construct assembled into antiparallel β-sheets and amyloid fibrils, a 4.0-fold increase in the hydrolysis rate of p-nitrophenyl acetate (p-NPA) compared to neat CP4 peptide was observed. The enhanced catalytic activity of CP4-Aβ assembly could be explained both by pre-organization of a catalytically competent Ser-His-acid triad and hydrophobic stabilization of a bound substrate between the triad and p-NPA, indicating that a design strategy for self-assembled peptides is important to accomplish the desired functionality. PMID:27116246

  19. Surface Structure and Catalytic Performance of Ni-Fe Catalyst for Low-Temperature CO Hydrogenation

    Directory of Open Access Journals (Sweden)

    Fanhui Meng

    2014-01-01

    Full Text Available Catalysts 16NixFe/Al2O3 (x is 0, 1, 2, 4, 6, 8 were prepared by incipient wetness impregnation method and the catalytic performance for the production of synthetic natural gas (SNG from CO hydrogenation in slurry-bed reactor were studied. The catalysts were characterized by BET, XRD, UV-Vis DRS, H2-TPR, CO-TPD, and XPS, and the results showed that the introduction of iron improved the dispersion of Ni species, weakened the interaction between Ni species and support and decreased the reduction temperature and that catalyst formed Ni-Fe alloy when the content of iron exceeded 2%. Experimental results revealed that the addition of iron to the catalyst can effectively improve the catalytic performance of low-temperature CO methanation. Catalyst 16Ni4Fe/Al2O3 with the iron content of 4% exhibited the best catalytic performance, the conversion of CO and the yield of CH4 reached 97.2% and 84.9%, respectively, and the high catalytic performance of Ni-Fe catalyst was related to the property of formed Ni-Fe alloy. Further increase of iron content led to enhancing the water gas shift reaction.

  20. PREPARATION AND CATALYTIC BEHAVIOUR OF POLYMER-BOUND METALLOPORPHYRIN IN HYDROGENATION OF OLEFIN

    Institute of Scientific and Technical Information of China (English)

    1998-01-01

    The meso-tetraarylporphyrin has been anchored to styrene-divinylbenzene copolymers by reaction of meso-tetra(4-hydroxylphenyl) porphyrin with chloromethylated resin under mild condition. A number of polymer transition metal complexes have been prepared with the polymer ligand and metal salts. The polymeric ligand and its complexes have been characterized by electronic spectra, and vibrational spectra. Cyclohexene can be hydrogenated with the polymeric porphyrin palladium complex(P-THPPPd) as catalyst, and its catalytic activity was influenced by the polarity of solvents, the contents of water in ethanol or reaction temperature. However, its catalytic activity was lower for nitro groups, carbonyl groups and olefins with steric hindrance substituents, and showed no activity for aromatic rings under these conditions.

  1. Effect of hydrogen combustion reaction on the dehydrogenation of ethane in a fixed-bed catalytic membrane reactor

    Institute of Scientific and Technical Information of China (English)

    Masoud Hasany; Mohammad Malakootikhah; Vahid Rahmanian; Soheila Yaghmaei

    2015-01-01

    A two-dimensional non-isothermal mathematical model has been developed for the ethane dehydrogenation reaction in a fixed-bed catalytic membrane reactor. Since ethane dehydrogenation is an equilibrium reaction, removal of produced hydrogen by the membrane shifts the thermodynamic equilibrium to ethylene production. For further displacement of the dehydrogenation reaction, oxidative dehydrogenation method has been used. Since ethane dehydrogenation is an endothermic reaction, the energy produced by the oxidative dehydrogena-tion method is consumed by the dehydrogenation reaction. The results show that the oxidative dehydrogenation method generated a substantial improvement in the reactor performance in terms of high conversions and significant energy saving. It was also established that the sweep gas velocity in the shell side of the reactor is one of the most important factors in the effectiveness of the reactor.

  2. Room temperature hydrogen generation from hydrolysis of ammonia-borane over an efficient NiAgPd/C catalyst

    KAUST Repository

    Hu, Lei

    2014-12-01

    NiAgPd nanoparticles are successfully synthesized by in-situ reduction of Ni, Ag and Pd salts on the surface of carbon. Their catalytic activity was examined in ammonia borane (NH3BH3) hydrolysis to generate hydrogen gas. This nanomaterial exhibits a higher catalytic activity than those of monometallic and bimetallic counterparts and a stoichiometric amount of hydrogen was produced at a high generation rate. Hydrogen production rates were investigated in different concentrations of NH3BH3 solutions, including in the borates saturated solution, showing little influence of the concentrations on the reaction rates. The hydrogen production rate can reach 3.6-3.8 mol H2 molcat -1 min-1 at room temperature (21 °C). The activation energy and TOF value are 38.36 kJ/mol and 93.8 mol H2 molcat -1 min-1, respectively, comparable to those of Pt based catalysts. This nanomaterial catalyst also exhibits excellent chemical stability, and no significant morphology change was observed from TEM after the reaction. Using this catalyst for continuously hydrogen generation, the hydrogen production rate can be kept after generating 6.2 L hydrogen with over 10,000 turnovers and a TOF value of 90.3 mol H2 molcat -1 min-1.

  3. An investigation of turbulent catalytically stabilized channel flow combustion of lean hydrogen - air mixtures

    Energy Technology Data Exchange (ETDEWEB)

    Mantzaras, I.; Benz, P.; Schaeren, R.; Bombach, R. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

    1999-08-01

    The catalytically stabilised thermal combustion (CST) of lean hydrogen-air mixtures was investigated numerically in a turbulent channel flow configuration using a two-dimensional elliptic model with detailed heterogeneous and homogeneous chemical reactions. Comparison between turbulent and laminar cases having the same incoming mean properties shows that turbulence inhibits homogeneous ignition due to increased heat transport away from the near-wall layer. The peak root-mean-square temperature and species fluctuations are always located outside the extent of the homogeneous reaction zone indicating that thermochemical fluctuations have no significant influence on gaseous combustion. (author) 4 figs., 6 refs.

  4. IDCOR approach to hydrogen generation, combustion, and burn control

    International Nuclear Information System (INIS)

    The IDCOR Program is developing the appropriate information and methodology to predict the following phenomena during severe accidents: 1) hydrogen generation, both in-vessel and ex-vessel, primarily from metal-water reactions; 2) hydrogen distribution in reactor containments; and 3) potential hazards of overpressurization or combustion of hydrogen. The information is being assembled into reports describing the phenomenology and incorporated into the IDCOR Modular Accident Analysis Program, in order to determine the behavior of hydrogen during accident sequences on four reference plants. From these analyses, conditions will be determined so that hydrogen burn control measures can be evaluated. A review is being made of various approaches for suppression of combustion or controlled burning to limit hydrogen to concentrations below the detonation range. The review considers the advantages and disadvantages of various hydrogen control systems concepts for reactor and containment combinations and, in addition, addresses the various concepts for eventual removal of hydrogen from containment

  5. Process concept for hydrogen production by catalytic conversion of defined kerosene fractions; Verfahrenskonzept zur Wasserstofferzeugung durch katalytische Umwandlung definierter Kerosinfraktionen

    Energy Technology Data Exchange (ETDEWEB)

    Frick, Viktoria

    2011-06-15

    The innovative process concept presented in this thesis for on-board hydrogen generation from kerosene for power generation aboard aircrafts by fuel cell systems exhibits significant advantages on reaction and process level compared to the hydrogen production via reforming. It includes the separation of a defined low-sulphur fraction from kerosene via rectification or crystallization which is subsequently converted catalytically to hydrogen. To investigate thermal management and process integration of the overall system four possible process concepts have been identified and their overall efficiency has been compared to a reference concept by process simulation. The key process parameters for fractionation were derived from experimental investigations. The processes with dehydrogenation resulted in the highest hydrogen yield and an overall electrical efficiency of 43 % could be achieved in combination with crystallization, which is a significant increase against the reference concept. Taking aircraft specific boundary conditions into account this process concept has been derived as the lead concept. Moreover, it avoids the unsolved until now problems connected to undesirable production of NO{sub x} and CO. [German] Das im Rahmen dieser Arbeit erarbeitete innovative Prozesskonzept zur on-board Wasserstofferzeugung aus Kerosin fuer den Betrieb von Brennstoffzellensystemen zur Energieversorgung im Flugzeug weist erhebliche reaktions- und verfahrenstechnische Vorteile gegenueber der Wasserstofferzeugung mittels Reformierung auf. Es beinhaltet die Abtrennung, einer definierten schwefelarmen Fraktion des Kerosins mittels Rektifikation oder Kristallisation. Diese wird in einem nachfolgenden Schritt katalytisch zu Wasserstoff umgewandelt. Zur Untersuchung der Waermeintegration und Prozessfuehrung im Gesamtsystem wurden vier moegliche Verfahrenskonzepte identifiziert und deren Systemwirkungsgrade mittels Prozesssimulation mit einem Referenzkonzept verglichen. Die

  6. Development of a para-orthohydrogen catalytic converter for a solid hydrogen cooler

    Science.gov (United States)

    Nast, T. C.; Hsu, I. C.

    1984-01-01

    Design features of a tested catalytic converter for altering vented cryogenic parahydrogen used as a coolant on spacecraft into a para-ortho equilibrium for channeling to other cooling functions are described. The hydrogen is expected to be stored in either liquid or solid form. A high surface area Ni-on-Si catalyst was selected for tests at an operating pressure of 2 torr at a ratio of 1000 gr catalyst for a gr/sec hydrogen flow. Cylindrical and radial flow geometries were tried and measurements centered on the converter efficiencies at different operating temperatures when the converter was placed in the vent line of the H2 cooler. Efficiencies ranging from 10-100 percent were obtained for varying flow rates. Further testing is necessary to characterize the converter performance under a wider range of operating temperatures and environments.

  7. Hydrogen Production From Crude Bio-oil and Biomass Char by Electrochemical Catalytic Reforming

    Institute of Scientific and Technical Information of China (English)

    Xing-long Li; Shen Ning; Li-xia Yuan; Quan-xin Li

    2011-01-01

    We reports an efficient approach for production of hydrogen from crude bio-oil and biomass char in the dual fixed-bed system by using the electrochemical catalytic reforming method.The maximal absolute hydrogen yield reached 110.9 g H2/kg dry biomass.The product gas was a mixed gas containing 72%H2,26%CO2,1.9%CO,and a trace amount of CH4.It was observed that adding biomass char (a by-product of pyrolysis of biomass) could remarkably increase the absolute H2 yield (about 20%-50%).The higher reforming temperature could enhance the steam reforming reaction of organic compounds in crude bio-oil and the reaction of CO and H2O.In addition,the CuZn-Al2O3 catalyst in the water-gas shift bed could also increase the absolute H2 yield via shifting CO to CO2.

  8. Dynamic\tmodelling of catalytic three-phase reactors for hydrogenation and oxidation processes

    Directory of Open Access Journals (Sweden)

    Salmi T.

    2000-01-01

    Full Text Available The dynamic modelling principles for typical catalytic three-phase reactors, batch autoclaves and fixed (trickle beds were described. The models consist of balance equations for the catalyst particles as well as for the bulk phases of gas and liquid. Rate equations, transport models and mass balances were coupled to generalized heterogeneous models which were solved with respect to time and space with algorithms suitable for stiff differential equations. The aspects of numerical solution strategies were discussed and the procedure was illustrated with three case studies: hydrogenation of aromatics, hydrogenation of aldehydes and oxidation of ferrosulphate. The case studies revealed the importance of mass transfer resistance inside the catalyst pallets as well as the dynamics of the different phases being present in the reactor. Reliable three-phase reactor simulation and scale-up should be based on dynamic heterogeneous models.

  9. On-site hydrogen generation from biodiesel and diesel

    OpenAIRE

    Martin, Stefan

    2015-01-01

    The lack of hydrogen infrastructure and distribution poses an obstacle for the introduction of fuel cell vehicles to the market. Therefore it is reasonable to consider using liquid fuels for on-board or on-site hydrogen generation. Within the FP7 project NEMESIS2+ (01/2012-06/2015, www.nemesis-project.eu) a small-scale hydrogen generator capable of producing 50 Nm3h-1 from biodiesel and diesel is currently being developed. Reduction of hydrogen production costs (< 5.0 € per kg), high overall...

  10. Biomass-to-hydrogen via fast pyrolysis and catalytic steam reforming

    Energy Technology Data Exchange (ETDEWEB)

    Chornet, E.; Wang, D.; Czernik, S. [National Renewable Energy Lab., Golden, CO (United States)] [and others

    1996-10-01

    Pyrolysis of lignocellulosic biomass and reforming the pyroligneous oils is being studied as a strategy for producing hydrogen. Novel technologies for the rapid pyrolysis of biomass have been developed in the past decade. They provide compact and efficient systems to transform biomass into vapors that are condensed to oils, with yields as high as 75-80 wt.% of the anhydrous biomass. This {open_quotes}bio-oil{close_quotes} is a mixture of aldehydes, alcohols, acids, oligomers from the constitutive carbohydrates and lignin, and some water derived from the dehydration reactions. Hydrogen can be produced by reforming the bio-oil or its fractions with steam. A process of this nature has the potential to be cost competitive with conventional means of producing hydrogen. The reforming facility can be designed to handle alternate feedstocks, such as natural gas and naphtha, if necessary. Thermodynamic modeling of the major constituents of the bio-oil has shown that reforming is possible within a wide range of temperatures and steam-to-carbon ratios. Existing catalytic data on the reforming of oxygenates have been studied to guide catalyst selection. Tests performed on a microreactor interfaced with a molecular beam mass spectrometer showed that, by proper selection of the process variables: temperature, steam-to-carbon ratio, gas hourly space velocity, and contact time, almost total conversion of carbon in the feed to CO and CO{sub 2} could be obtained. These tests also provided possible reaction mechanisms where thermal cracking competes with catalytic processes. Bench-scale, fixed bed reactor tests demonstrated high hydrogen yields from model compounds and carbohydrate-derived pyrolysis oil fractions. Reforming bio-oil or its fractions required proper dispersion of the liquid to avoid vapor-phase carbonization of the feed in the inlet to the reactor. A special spraying nozzle injector was designed and successfully tested with an aqueous fraction of bio-oil.

  11. Stereo-Specific Hydrogen Exchange Accompanying Catalytic Hydrogenation of Methyl β, β-Dimethylacrylate

    International Nuclear Information System (INIS)

    During platinum or palladium-catalysed hydrogenation in which, in solution, methyl β, β-dimethylacrylate is converted into the corresponding ester of isovaleric acid by the equation CH3CH3>C = CH-COOCH3 H2, cat. sol. --> CH3CH3>C = CH-CH2-COOCH3' an isotopic exchange of hydrogen between the gas and the solvent on the one hand and the substrate on the other is superposed upon the process of saturation of the double bond. This was studied by carrying out, at 20°C, hydrogenations which were interrupted after saturation of half the starting product and by employing D2 or esters deuterated either totally or at specific positions, different positions being used from experiment to experiment. The isotopic composition of the hydrogen at each of the positions of the molecules, both saturated and non-saturated, was determined, after separation of the molecules by chromatography in the gaseous phase, by combined mass spectrometry and nuclear magnetic resonance. A separate study was made of behaviour in respect of exchange of substrate in the non-saturated and saturated state, in the absence of hydrogen or the catalyst or both. Among the factors examined were, in particular, the effects of the solvent and the catalyst - which were very pronounced - on all the phenomena observed. These can be summarized as follows, (a) Molecules of the substrate no longer exchange once they are saturated, (b) With non-saturated molecules, restricted exchange takes place in which only the β-methyls are involved. This exchange is symmetric in the presence of rhodium and palladium, and stereo-specific in the presence of platinum - on an average 2.2 times greater in the cis-group than in the trans-group. This fact in the latter case excludes the hypothesis of double bond migration from the α-β position to the β-γ position as an exchange mechanism; which is confirmed by the absence of exchange at the exposition, (c) All the isotopic varieties from -d0 to -d6 or -d8 are present in the

  12. Effects of acido-basic support properties on the catalytic hydrogenation of acetylene on gold nano-particles

    Science.gov (United States)

    Manda, Abdullah Ahmed

    Metallic gold nanoparticles supported on gamma-Al2O 3 and magnesia-alumina mixed oxide, with different magnesia content have been prepared by sol-gel method and characterized by different techniques (inductive coupled plasma-mass spectroscopy (ICP-MS), XRD, BET surface area analysis, transmission electron microscopy (TEM), CO2 and NH 3 temperature programmed desorption (TPD), H2 temperature programmed reduction (TPR) and FTIR of adsorbed CO2). Such systems were found to produce catalysts with controllable acidity, varying from catalyst possessing large density of acidic and low density of basic sites, others with acidic and basic sites of equal strength and density, and others with large basic and low acid sites densities, respectively. The catalytic assessment of the generated acidity was carried out using 2-propanol decomposition as a test reaction. The results obtained indicate that the presence of magnesia and reduced gold nanopartilces has imparted the catalysts, 1%Au/4%Mg-Al 2O3 and 1%Au/8%Mg-Al2O3, with significant base-catalytic properties. Acetylene hydrogenation and formation of coke deposits were investigated on a gold catalyst supported on gamma-Al2O3 and gold supported on alumina-magnisia mixed oxide with different gold content; 1%Au/gamma-Al 2O3, 1%Au/15%Mg-Al2O3, 2%Au/15%Mg-Al 2O3 and 4%Au/15%Mg-Al2O3. The effect of the H2/C2H2 ratio was studied over a range of values. The catalytic activity and selectivity towards ethylene and other products were investigated at different reaction temperatures. Acetylene hydrogenation was investigated in the presence and absence of ethylene in stream. It is investigated that the adsorption of the triple bond is preferred over the double bond and during selective catalytic (SCR) of C2H2 the two hydrocarbons do not compete for the same adsorption sites. The deactivation of catalysts was studied by temperature programmed oxidation (TPO). Higher content of coke over 1%Au/Al2O3 catalyst was investigated in contrast to

  13. A Study of Hydrogen Generation with Doubly-Fed Adjustable Speed Wind Generator

    Science.gov (United States)

    Kinoshita, Hirotaka; Takahashi, Rion; Murata, Toshiaki; Tamura, Junji; Sugimasa, Masatoshi; Komura, Akiyoshi; Futami, Motoo; Ichinose, Masaya; Ide, Kazumasa

    This paper presents a combination system of wind power generator and hydrogen generator. In the proposed system, Doubly-Fed Synchronous Generator (DFSG) is used as an adjustable speed wind generator, and an electrolyzer is connected to its terminal for hydrogen generation, which is controlled by power electronic converters. Output power from the wind generator is smoothed and supplied to the power system as well as to the electrolyzer to generate hydrogen under a cooperative control of the wind generator and the electrolyzer. The performance of the proposed system is investigated by simulation analyses, in which simulations are performed by using PSCAD/EMTDC.

  14. Production of natural antioxidants from vegetable oil deodorizer distillates: effect of catalytic hydrogenation.

    Science.gov (United States)

    Pagani, María Ayelén; Baltanás, Miguel A

    2010-02-01

    Natural tocopherols are one of the main types of antioxidants found in living creatures, but they also have other critical biological functions. The biopotency of natural (+)-alpha-tocopherol (RRR) is 36% higher than that of the synthetic racemic mixture and 300% higher than the SRR stereoisomer. Vegetable oil deodorizer distillates (DD) are an excellent source of natural tocopherols. Catalytic hydrogenation of DD preconcentrates has been suggested as a feasible route for recovery of tocopherols in high yield. However, it is important to know whether the hydrogenation operation, as applied to these tocopherol-rich mixtures, is capable of preserving the chiral (RRR) character, which is critical to its biopotency. Fortified (i.e., (+)-alpha-tocopherol enriched) sunflower oil and methyl stearate, as well as sunflower oil DD, were fully hydrogenated using commercial Ni and Pd catalysts (120-180 degrees C; 20-60 psig). Products were analyzed by chiral HPLC. Results show that the desired chiral configuration (RRR) is fully retained. Thus, the hydrogenation route can be safely considered as a valid alternative for increasing the efficiency of tocopherol recovery processes from DDs while preserving their natural characteristics.

  15. Biomass to hydrogen-rich syngas via catalytic steam gasification of bio-oil/biochar slurry.

    Science.gov (United States)

    Chen, Guanyi; Yao, Jingang; Liu, Jing; Yan, Beibei; Shan, Rui

    2015-12-01

    The catalytic steam gasification of bio-oil/biochar slurry (bioslurry) for hydrogen-rich syngas production was investigated in a fixed-bed reactor using LaXFeO3 (X=Ce, Mg, K) perovskite-type catalysts. The effects of elemental substitution in LaFeO3, temperature, water to carbon molar ratio (WCMR) and bioslurry weight hourly space velocity (WbHSV) were examined. The results showed that La0.8Ce0.2FeO3 gave the best performance among the prepared catalysts and had better catalytic activity and stability than the commercial 14 wt.% Ni/Al2O3. The deactivation caused by carbon deposition and sintering was significantly depressed in the case of La0.8Ce0.2FeO3 catalyst. Both higher temperature and lower WbHSV contributed to more H2 yield. The optimal WCMR was found to be 2, and excessive introducing of steam reduced hydrogen yield. The La0.8Ce0.2FeO3 catalyst gave a maximum H2 yield of 82.01% with carbon conversion of 65.57% under the optimum operating conditions (temperature=800°C, WCMR=2 and WbHSV=15.36h(-1)). PMID:26378962

  16. A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater

    Institute of Scientific and Technical Information of China (English)

    LI XiaoNian; ZHANG QunFeng; KONG LingNiao; XIANG YiZhi; JU YaoMing; WU XiaoQiong; FENG Feng; YUAN JunFeng; MA Lei; LU ChunShan

    2008-01-01

    A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater by aqueous phase reforming (APR) has been proposed. It is worthy of noting that this technique may be a potential way for the purification of refractory and highly toxic organics in water for hydrogen production. Hazardous organics (such as phenol, aniline, nitrobenzene, tetrahydrofuran (THF), toluene, N,N-dimethylformamide (DMF) and cyclohexanol) in water could be completely de-graded into H2 and CO2 with high selectivity over Raney Ni, and Sn-modified Raney Ni (Sn-Raney-Ni) or Pd/C catalyst under mild conditions. The experimental results operated in tubular and autoclave reactors, indicated that the degradation degree of organics and H2 selectivity could reach 100% under the optimal reaction conditions. The Sn-Raney-Ni (Sn/Ni=0.06) and Pd/C catalysts show better catalytic performances than the Raney Ni catalyst for the degradation of organics in water into H2 and CO2 by the aqueous phase reforming process.

  17. Simulation of hydrogen mitigation in catalytic recombiner: Part-I: Surface chemistry modelling

    Energy Technology Data Exchange (ETDEWEB)

    Prabhudharwadkar, Deoras M. [Department of Mechanical Engineering, Indian Institute of Technology-Bombay, Powai, Mumbai 400076, Maharashtra (India); Aghalayam, Preeti A. [Department of Chemical Engineering, Indian Institute of Technology-Bombay, Powai, Mumbai 400076 (India); Iyer, Kannan N., E-mail: kiyer@iitb.ac.i [Department of Mechanical Engineering, Indian Institute of Technology-Bombay, Powai, Mumbai 400076, Maharashtra (India)

    2011-05-15

    This paper aims at accurate modelling of a Passive Catalytic Recombiner used for hydrogen mitigation in the nuclear power plant containments. In order to assess the performance of the recombiner through numerical simulations, it is required to accurately predict the catalytic reactions. There are various detailed reaction mechanisms available in the literature for prediction of hydrogen-oxygen reaction over a platinum surface. While a single step reaction rate expression is always sought in order to obtain numerical predictions economically, a detailed reaction mechanism that includes several elementary reactions and intermediate species is likely to produce more accurate predictions. The paper compares the solution from two of competing models, one a single step reaction and the other a multiple reaction model. A new single step rate expression is also derived from the detailed mechanism after simplifying it for the present problem. The paper also considers the diffusion controlled model that assumes rapid reaction rates for which the surface chemistry is not required at all. In order to find the best suited approach to model the surface chemistry, CFD simulations were performed with FLUENT code using available experimental data from the literature. The current study reports comparison up to 4% H{sub 2} mole fraction in dry air with catalyst temperature varying from 300 K to 800 K. It is demonstrated that the new single step model is able to satisfactorily predict the data as well as the detailed chemistry model. The diffusion controlled model is shown to over-predict the data.

  18. Simulation of hydrogen mitigation in catalytic recombiner. Part-II: Formulation of a CFD model

    Energy Technology Data Exchange (ETDEWEB)

    Prabhudharwadkar, Deoras M. [Department of Mechanical Engineering, Indian Institute of Technology-Bombay, Powai, Mumbai 400076 (India); Iyer, Kannan N., E-mail: kiyer@me.iitb.ac.i [Department of Mechanical Engineering, Indian Institute of Technology-Bombay, Powai, Mumbai 400076 (India)

    2011-05-15

    Research highlights: Hydrogen transport in containment with recombiners is a multi-scale problem. A novel methodology worked out to lump the recombiner characteristics. Results obtained using commercial code FLUENT are cast in the form of correlations. Hence, coarse grids can obtain accurate distribution of H{sub 2} in containment. Satisfactory working of the methodology is clearly demonstrated. - Abstract: This paper aims at formulation of a model compatible with CFD code to simulate hydrogen distribution and mitigation using a Passive Catalytic Recombiner in the Nuclear power plant containments. The catalytic recombiner is much smaller in size compared to the containment compartments. In order to fully resolve the recombination processes during the containment simulations, it requires the geometric details of the recombiner to be modelled and a very fine mesh size inside the recombiner channels. This component when integrated with containment mixing calculations would result in a large number of mesh elements which may take large computational times to solve the problem. This paper describes a method to resolve this simulation difficulty. In this exercise, the catalytic recombiner alone was first modelled in detail using the best suited option to describe the reaction rate. A detailed parametric study was conducted, from which correlations for the heat of reaction (hence the rate of reaction) and the heat transfer coefficient were obtained. These correlations were then used to model the recombiner channels as single computational cells providing necessary volumetric sources/sinks to the energy and species transport equations. This avoids full resolution of these channels, thereby allowing larger mesh size in the recombiners. The above mentioned method was successfully validated using both steady state and transient test problems and the results indicate very satisfactory modelling of the component.

  19. Thermo-Catalytic Methane Decomposition for Hydrogen Production: Effect of Palladium Promoter on Ni-based Catalysts

    OpenAIRE

    Irene Lock Sow Mei; S.S.M. Lock; Dai-Viet N. Vo; Bawadi Abdullah

    2016-01-01

    Hydrogen production from the direct thermo-catalytic decomposition of methane is a promising alternative for clean fuel production. However, thermal decomposition of methane can hardly be of any practical and empirical interest in the industry unless highly efficient and effective catalysts, in terms of both catalytic activity and operational lifetime have been developed. In this study, the effect of palladium (Pd) as a promoter onto Ni supported on alumina catalyst has been investigated by u...

  20. Size-Dependent Catalytic Activity of Palladium Nanoparticles Fabricated in Porous Organic Polymers for Alkene Hydrogenation at Room Temperature.

    Science.gov (United States)

    Mondal, John; Trinh, Quang Thang; Jana, Avijit; Ng, Wilson Kwok Hung; Borah, Parijat; Hirao, Hajime; Zhao, Yanli

    2016-06-22

    Ultrafine palladium nanoparticles (Pd NPs) with 8 and 3 nm sizes were effectively fabricated in triazine functionalized porous organic polymer (POP) TRIA that was developed by nonaqueous polymerization of 2,4,6-triallyoxy-1,3,5-triazine. The Pd NPs encapsulated POP (Pd-POP) was fully characterized using several techniques. Further studies revealed an excellent capability of Pd-POP for catalytic transfer hydrogenation of alkenes at room temperature with superior catalytic performance and high selectivity of desired products. Highly flammable H2 gas balloon at high pressure and temperature used in conventional hydrogenation reactions was not needed in the present synthetic system. Catalytic activity is strongly dependent on the size of encapsulated Pd NPs in the POP. The Pd-POP catalyst with Pd NPs of 8 nm in diameter exhibited higher catalytic activity for alkene hydrogenation as compared with the Pd-POP catalyst encapsulating 3 nm Pd NPs. Computational studies were undertaken to gain insights into different catalytic activities of these two Pd-POP catalysts. High reusability and stability as well as no Pd leaching of these Pd-POP catalysts make them highly applicable for hydrogenation reactions at room temperature. PMID:27258184

  1. On-site production of electrolytic hydrogen for generator cooling

    Science.gov (United States)

    Mehta, B. R.

    Hydrogen produced by water electrolysis could be cost effective over the merchant hydrogen used for generator cooling. Advanced water electrolyzers are being developed specifically for this utility application. These designs are based on solid-polymer-electrolyte and alkaline water electrolysis technologies. This paper describes the status of electrolyzer development and demonstration projects.

  2. Catalytic hydrogenation of carbon monoxide. Progress report, December 15, 1991--December 14, 1992

    Energy Technology Data Exchange (ETDEWEB)

    Wayland, B.B.

    1992-12-01

    This project is focused on developing strategies to accomplish the reduction and hydrogenation of carbon monoxide to produce organic oxygenates at mild conditions. Our approaches to this issue are based on the recognition that rhodium macrocycles have unusually favorable thermodynamic values for producing a series of intermediate implicated in the catalytic hydrogenation of CO. Observations of metalloformyl complexes produced by reactions of H{sub 2} and CO, and reductive coupling of CO to form metallo {alpha}-diketone species have suggested a multiplicity of routes to organic oxygenates that utilize these species as intermediates. Thermodynamic and kinetic-mechanistic studies are used in constructing energy profiles for a variety of potential pathways, and these schemes are used in guiding the design of new metallospecies to improve the thermodynamic and kinetic factors for individual steps in the overall process. Variation of the electronic and steric effects associated with the ligand arrays along with the influences of the reaction medium provide the chemical tools for tuning these factors. Emerging knowledge of the factors that contribute to M-H, M-C and M-O bond enthalpies is directing the search for ligand arrays that will expand the range of metal species that have favorable thermodynamic parameters to produce the primary intermediates for CO hydrogenation. Studies of rhodium complexes are being extended to non-macrocyclic ligand complexes that emulate the favorable thermodynamic features associated with rhodium macrocycles, but that also manifest improved reaction kinetics. Multifunctional catalyst systems designed to couple the ability of rhodium complexes to produce formyl and diketone intermediates with a second catalyst that hydrogenates these imtermediates are promising approaches to accomplish CO hydrogenation at mild conditions.

  3. Efficient Electrochemical Hydrogen Peroxide Generation in Water Project

    Data.gov (United States)

    National Aeronautics and Space Administration — An electrochemical cell is proposed for the efficient generation of 3% hydrogen peroxide (H2O2) in pure water using only power, oxygen and water. H2O2 is an...

  4. Cold weather hydrogen generation system and method of operation

    Energy Technology Data Exchange (ETDEWEB)

    Dreier, Ken Wayne (Madison, CT); Kowalski, Michael Thomas (Seymour, CT); Porter, Stephen Charles (Burlington, CT); Chow, Oscar Ken (Simsbury, CT); Borland, Nicholas Paul (Montpelier, VT); Goyette, Stephen Arthur (New Hartford, CT)

    2010-12-14

    A system for providing hydrogen gas is provided. The system includes a hydrogen generator that produces gas from water. One or more heat generation devices are arranged to provide heating of the enclosure during different modes of operation to prevent freezing of components. A plurality of temperature sensors are arranged and coupled to a controller to selectively activate a heat source if the temperature of the component is less than a predetermined temperature.

  5. Co-production of hydrogen and carbon nanotubes on nickel foam via methane catalytic decomposition

    Science.gov (United States)

    Ping, Dan; Wang, Chaoxian; Dong, Xinfa; Dong, Yingchao

    2016-04-01

    The co-production of COx-free hydrogen and carbon nanotubes (CNTs) was achieved on 3-dimensional (3D) macroporous nickel foam (NF) via methane catalytic decomposition (MCD) over nano-Ni catalysts using chemical vapor deposition (CVD) technique. By a simple coating of a NiO-Al2O3 binary mixture sol followed by a drying-calcination-reduction treatment, NF supported composite catalysts (denoted as NiyAlOx/NF) with Al2O3 transition-layer incorporated with well-dispersed nano-Ni catalysts were successfully prepared. The effects of Ni loading, calcination temperature and reaction temperature on the performance for simultaneous production of COx-free hydrogen and CNTs were investigated in detail. Catalysts before and after MCD were characterized by XRD, TPR, SEM, TEM, TG and Raman spectroscopy technology. Results show that increasing Ni loading, lowering calcination temperature and optimizing MCD reaction temperature resulted in high production efficiency of COx-free H2 and carbon, but broader diameter distribution of CNTs. Through detailed parameter optimization, the catalyst with a Ni/Al molar ratio of 0.1, calcination temperature of 550 °C and MCD temperature of 650 °C was favorable to simultaneously produce COx-free hydrogen with a growth rate as high as 10.3% and CNTs with uniform size on NF.

  6. Graphene sheets/cobalt nanocomposites as low-cost/high-performance catalysts for hydrogen generation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Fei; Hou, Chengyi; Zhang, Qinghong [State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620 (China); Wang, Hongzhi, E-mail: wanghz@dhu.edu.cn [State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620 (China); Li, Yaogang, E-mail: yaogang_li@dhu.edu.cn [College of Materials Science and Engineering, Donghua University, Shanghai 201620 (China)

    2012-08-15

    The production of clean and renewable hydrogen through the hydrolysis of sodium borohydride has received much attention owing to increasing global energy demands. Graphene sheets/cobalt (GRs/Co) nanocomposites, which are highly efficient catalysts, have been prepared using a one-step solvothermal method in ethylene glycol. Co{sup 2+} salts were converted to Co nanoparticles, which were simultaneously inserted into the graphene layers with the reduction of graphite oxide sheets to GRs. The as-synthesized samples were characterized by X-ray diffraction, Fourier transform infrared spectra, Raman spectroscopy, field emission scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy and vibrating sample magnetometer. The maximum saturation magnetization value reached 80.8 emu g{sup -1}, meaning they are more suitable for magnet-controlled generation of H{sub 2} than noble metal catalysts. The catalytic activity of the composite was investigated by the hydrolysis of sodium borohydride in aqueous solution both with and without a GRs support. It was found that the high electronic conductive GRs support increased the hydrogen generation rate (about two times) compared with pure cobalt. The improved hydrogen generation rate, low cost and uncomplicated recycling makes the GRs/Co nanocomposites promising candidates as catalysts for hydrogen generation. Highlights: Black-Right-Pointing-Pointer Graphene sheets/cobalt nanocomposites were prepared by a one-step solvothermal method. Black-Right-Pointing-Pointer The maximum saturation magnetization value of the composites reached 80.8 emu g{sup -1}. Black-Right-Pointing-Pointer The graphene support greatly increased the catalytic activity of cobalt. Black-Right-Pointing-Pointer An easily removed, recycled and controlled functional filter was obtained.

  7. Studies on Hydrogen Selective Silica Membranes and the Catalytic Reforming of CH4 with CO2 in a Membrane Reactor

    OpenAIRE

    Lee, Doohwan

    2003-01-01

    In this work the synthesis, characterization, and gas transport properties of hydrogen selective silica membranes were studied along with the catalytic reforming of CH4 with CO2 (CH4 + CO z 2 CO + 2 H2) in a hydrogen separation membrane reactor. The silica membranes were prepared by chemical vapor deposition (CVD) of a thin SiO2 layer on porous supports (Vycor glass and alumina) using thermal decomposition of tetraethylorthosilicate (TEOS) in an inert atmosphere. These membranes displayed h...

  8. Cobalamin Catalytic Centers for Stable Fuels Generation from Carbon Dioxide

    Science.gov (United States)

    Robertson, Wesley D.; Jawdat, Benmaan I.; Ennist, Nathan M.; Warncke, Kurt

    2010-03-01

    Our aim is to design and construct protein-based artificial photosynthetic systems that reduce carbon dioxide (CO2) to stable fuel forms within the robust and adaptable (βα)8 TIM-barrel protein structure. The EutB subunit of the adenosylcobalamin-dependent enzyme, ethanolamine ammonia-lyase, from Salmonella typhimurium, was selected as the protein template. This system was selected because the Co^I forms of the native cobalamin (Cbl) cofactor, and the related cobinamide (Cbi), possess redox properties that are commensurate with reduction of CO2. The kinetics of photo- (excited 5'-deazariboflavin electron donor) and chemical [Ti(III)] reduction, and subsequent reaction, of the Cbl and Cbi with CO2 are measured by time-resolved UV/visible absorption spectroscopy. Products are quantified by NMR spectroscopy. The results address the efficacy of the organocobalt catalytic centers for CO2 reduction to stable fuels, towards protein device integration.

  9. Effect of Catalytic Cylinders on Autothermal Reforming of Methane for Hydrogen Production in a Microchamber Reactor

    Directory of Open Access Journals (Sweden)

    Yunfei Yan

    2014-01-01

    Full Text Available A new multicylinder microchamber reactor is designed on autothermal reforming of methane for hydrogen production, and its performance and thermal behavior, that is, based on the reaction mechanism, is numerically investigated by varying the cylinder radius, cylinder spacing, and cylinder layout. The results show that larger cylinder radius can promote reforming reaction; the mass fraction of methane decreased from 26% to 21% with cylinder radius from 0.25 mm to 0.75 mm; compact cylinder spacing corresponds to more catalytic surface and the time to steady state is decreased from 40 s to 20 s; alteration of staggered and aligned cylinder layout at constant inlet flow rates does not result in significant difference in reactor performance and it can be neglected. The results provide an indication and optimize performance of reactor; it achieves higher conversion compared with other reforming reactors.

  10. Hazelnut shell to hydrogen-rich gaseous products via catalytic gasification process

    Energy Technology Data Exchange (ETDEWEB)

    Demirbas, A. [Selcuk Univ., Dept. of Chemical Engineering, Konya (Turkey)

    2004-01-15

    The gasification of biomass is a thermal treatment, which results in a high production of gaseous products and small quantities of char and ash. Steam reforming of hydrocarbons, partial oxidation of heavy oil residues, selected steam reforming of aromatic compounds, and gasification of coals and solid wastes to yield a mixture of H{sub 2} and CO (syngas), followed by a water-gas shift reaction to produce H{sub 2} and CO{sub 2}, are well-established processes. The samples, both untreated and impregnated with a catalyst, were pyrolyzed and gasified at 770, 925, 975, and 1025 K, and 975, 1075, 1175, and 1225 K temperatures, respectively. K{sub 2}CO{sub 3} was used as a catalyst, 10.0, 20.0, 30.0, and 50.0 wt% of the shell sample, in the catalytic-pyrolysis runs. The ratios of water-to-hazelnut shell were 0.7 and 1.9 in steam gasification runs. The total volume and the yield of gas from both pyrolysis and gasification increase with increasing temperature. The highest hydrogen-rich gas yield was obtained from the catalytic gasification run (water/hazelnut shell = 1.9) at 1225 K. (Author)

  11. Wax: A benign hydrogen-storage material that rapidly releases H2-rich gases through microwave-assisted catalytic decomposition

    Science.gov (United States)

    Gonzalez-Cortes, S.; Slocombe, D. R.; Xiao, T.; Aldawsari, A.; Yao, B.; Kuznetsov, V. L.; Liberti, E.; Kirkland, A. I.; Alkinani, M. S.; Al-Megren, H. A.; Thomas, J. M.; Edwards, P. P.

    2016-01-01

    Hydrogen is often described as the fuel of the future, especially for application in hydrogen powered fuel-cell vehicles (HFCV’s). However, its widespread implementation in this role has been thwarted by the lack of a lightweight, safe, on-board hydrogen storage material. Here we show that benign, readily-available hydrocarbon wax is capable of rapidly releasing large amounts of hydrogen through microwave-assisted catalytic decomposition. This discovery offers a new material and system for safe and efficient hydrogen storage and could facilitate its application in a HFCV. Importantly, hydrogen storage materials made of wax can be manufactured through completely sustainable processes utilizing biomass or other renewable feedstocks. PMID:27759014

  12. Ab initio molecular dynamics simulations for the role of hydrogen in catalytic reactions of furfural on Pd(111)

    Science.gov (United States)

    Xue, Wenhua; Dang, Hongli; Liu, Yingdi; Jentoft, Friederike; Resasco, Daniel; Wang, Sanwu

    2014-03-01

    In the study of catalytic reactions of biomass, furfural conversion over metal catalysts with the presence of hydrogen has attracted wide attention. We report ab initio molecular dynamics simulations for furfural and hydrogen on the Pd(111) surface at finite temperatures. The simulations demonstrate that the presence of hydrogen is important in promoting furfural conversion. In particular, hydrogen molecules dissociate rapidly on the Pd(111) surface. As a result of such dissociation, atomic hydrogen participates in the reactions with furfural. The simulations also provide detailed information about the possible reactions of hydrogen with furfural. Supported by DOE (DE-SC0004600). This research used the supercomputer resources of the XSEDE, the NERSC Center, and the Tandy Supercomputing Center.

  13. High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to gamma-valerolactone

    NARCIS (Netherlands)

    Luo, Wenhao; Meenakshisundaram, Sankar; Beale, Andrew M.; He, Qian; Kiely, Christopher J.; Bruijnincx, Pieter C. A.; Weckhuysen, Bert M.

    2015-01-01

    The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into gamma-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, s

  14. SYNTHESIS OF POLYMER-STABILIZED PLATINUM/RUTHENIUM BIMETALLIC COLLOIDS AND THEIR CATALYTIC PROPERTIES FOR SELECTIVE HYDROGENATION OF CROTONALDEHYDE

    Institute of Scientific and Technical Information of China (English)

    Wei-xia Tu; Han-fan Liu

    2005-01-01

    Polymer-stabilized platinum/ruthenium bimetallic colloids (Pt/Ru) were synthesized by polyol reduction with microwave irradiation and characterized by TEM and XPS. The colloidal nanoparticles have small and narrow size distributions. Catalytic performance of the Pt/Ru colloidal catalysts was investigated on the selective hydrogenation of crontonaldehyde (CRAL). A suitable amount of the added metal ions and base can improve the selectivity of CRAL to crotylalcohol (CROL) remarkably. The catalytic activity and the selectivity are dependent on the compositions of bimetallic colloids. Thereinto, PVP-stabilized 9Pt/1Ru colloid with a molar ratio of metals Pt:Ru = 9:1 shows the highest catalytic selectivity 77.3% to CROL at 333 K under 4.0 MPa of hydrogen.

  15. Short term hydrogen generation following LOCA and loss of ECCS

    International Nuclear Information System (INIS)

    The purpose of the present study is to estimate the amount of hydrogen that can be generated due to metal water reaction following LOCA and loss of ECCS in a 500 MWe PHWR. A computer code HYGEN (Hydrogen Generation) written in FORTRAN calculates time-dependent fuel temperature during the post blowdown period and the amount of hydrogen generated as a result of metal water reaction. It is seen from the analyses that metal water reaction depends on fuel bundle power, its initial temperature and steam flow conditions. At present, four groups of channels have been analysed for different steam flow conditions, and it is found that, for an about 5 gm/sec steam flow condition, the maximum of amount of hydrogen is generated (5.76 x 104 gm-mole) due to the zircaloy - steam reaction. This amount of hydrogen, when considered mixed in volume V1 (drywell) of the reactor building, means that the global concentration reaches about 2.76% by volume. So, it is seen that in the short term, the global hydrogen concentration in the reactor building is well below the flammability limit of 4% by volume. (author) 4 refs., 1 tab., 10 figs

  16. Pretreated Landfill Gas Conversion Process via a Catalytic Membrane Reactor for Renewable Combined Fuel Cell-Power Generation

    Directory of Open Access Journals (Sweden)

    Zoe Ziaka

    2013-01-01

    Full Text Available A new landfill gas-based reforming catalytic processing system for the conversion of gaseous hydrocarbons, such as incoming methane to hydrogen and carbon oxide mixtures, is described and analyzed. The exit synthesis gas (syn-gas is fed to power effectively high-temperature fuel cells such as SOFC types for combined efficient electricity generation. The current research work is also referred on the description and design aspects of permreactors (permeable reformers carrying the same type of landfill gas-reforming reactions. Membrane reactors is a new technology that can be applied efficiently in such systems. Membrane reactors seem to perform better than the nonmembrane traditional reactors. The aim of this research includes turnkey system and process development for the landfill-based power generation and fuel cell industries. Also, a discussion of the efficient utilization of landfill and waste type resources for combined green-type/renewable power generation with increased processing capacity and efficiency via fuel cell systems is taking place. Moreover, pollution reduction is an additional design consideration in the current catalytic processors fuel cell cycles.

  17. Hydrogen production in a zigzag and straight catalytic wall coated micro channel reactor by CFD modeling

    Energy Technology Data Exchange (ETDEWEB)

    Fazeli, Ali; Behnam, Mohsen [Gas Research Division, Research Institute of Petroleum Industry (RIPI), P.O. Box 14665-137, Tehran (Iran)

    2010-09-15

    Hydrogen production from steam reforming of methanol for fuel cell application was modeled in a wall coated micro channel reactor by CFD approach. Heat of steam reforming (SR) was supplied from catalytic total oxidation (TOX) of methanol on Cu/ZnO/Al{sub 2}O{sub 3} catalyst and Heat conducts from TOX to SR zone through Steel divider wall between two channels. Heat integration was compared in zigzag and straight geometry of microreactor by CFD modeling. The model is two dimensional, steady state and containing five zones: TOX fluid, TOX catalyst layer, steel wall of the channel, SR catalyst layer and SR fluid. Set of partial differential equations (PDEs) including x and y momentum balance, continuity, partial mass balances and energy balance was solved by finite volume method. Stiff reaction rates were considered for methanol total oxidation (TOX), methanol steam reforming (SR), water gas shift (WGS) and methanol decomposition (MD) reactions. The results show that zigzag geometry is better than straight one because heat and mass transfer in zigzag reactor are more than straight. Conversion of methanol in zigzag geometry is greater than straight one. In the outlet of zigzag micro channels, carbon monoxide selectivity is less and hydrogen mole fraction is more than straight one. (author)

  18. Application of microscopy technology in thermo-catalytic methane decomposition to hydrogen

    Energy Technology Data Exchange (ETDEWEB)

    Mei, Irene Lock Sow, E-mail: irene.sowmei@gmail.com; Lock, S. S. M., E-mail: serenelock168@gmail.com; Abdullah, Bawadi, E-mail: bawadi-abdullah@petronas.com.my [Chemical Engineering Department, Universiti Teknologi PETRONAS, Bandar Sri Iskandar, 31750, Perak (Malaysia)

    2015-07-22

    Hydrogen production from the direct thermo-catalytic decomposition of methane is a promising alternative for clean fuel production because it produces pure hydrogen without any CO{sub x} emissions. However, thermal decomposition of methane can hardly be of any practical and empirical interest in the industry unless highly efficient and effective catalysts, in terms of both specific activity and operational lifetime have been developed. In this work, bimetallic Ni-Pd on gamma alumina support have been developed for methane cracking process by using co-precipitation and incipient wetness impregnation method. The calcined catalysts were characterized to determine their morphologies and physico-chemical properties by using Brunauer-Emmett-Teller method, Field Emission Scanning Electron Microscopy, Energy-dispersive X-ray spectroscopy and Thermogravimetric Analysis. The results suggested that that the catalyst which is prepared by the co-precipitation method exhibits homogeneous morphology, higher surface area, have uniform nickel and palladium dispersion and higher thermal stability as compared to the catalyst which is prepared by wet impregnation method. This characteristics are significant to avoid deactivation of the catalysts due to sintering and carbon deposition during methane cracking process.

  19. An FTIR study on the catalytic effect of water molecules on the reaction of CO successive hydrogenation at 3 K

    International Nuclear Information System (INIS)

    Graphical abstract: This work highlights a selective catalytic action of water molecules on the reaction of CO hydrogenation at 3 K. Research highlights: → [CO/H2O] and [H/H2] are coinjected at 3 K. → H2 molecules condense rapidly at 3 K and screen the reaction mostly at the 1st step. → The observed catalytic effects on CO hydrogenation increase with water concentration. - Abstract: The reaction of successive CO hydrogenation has been performed at 3 K by coinjecting CO molecules and H atoms. The concentration of CO has been progressively reduced and replaced by water molecules to create two different environments where CO and H2O are successively the dominant species in the binary (CO/H2O) mixture. The catalytic effect of water molecules on CO hydrogenation appears clearly since the early times of the experiment and evolves with the formation of the CO/H2/H2O mixed-matrix. The process of CO hydrogenation, initially frozen at the first step of the reaction, is brought to completion through water influence. Water molecules guide the reaction toward the formation of CH3OH and promote different reaction steps depending on water concentration. Water molecules increase the probability of reactive to encounter H atoms either physically, by introducing structural changes in the matrix, or chemically, by raising the number of chemical pathways.

  20. Hydrogen generation via anaerobic fermentation of paper mill wastes.

    Science.gov (United States)

    Valdez-Vazquez, Idania; Sparling, Richard; Risbey, Derek; Rinderknecht-Seijas, Noemi; Poggi-Varaldo, Héctor M

    2005-11-01

    The objective of this work was to determine the hydrogen production from paper mill wastes using microbial consortia of solid substrate anaerobic digesters. Inocula from mesophilic, continuous solid substrate anaerobic digestion (SSAD) reactors were transferred to small lab scale, batch reactors. Milled paper (used as a surrogate paper waste) was added as substrate and acetylene or 2-bromoethanesulfonate (BES) was spiked for methanogenesis inhibition. In the first phase of experiments it was found that acetylene at 1% v/v in the headspace was as effective as BES in inhibiting methanogenic activity. Hydrogen gas accumulated in the headspace of the bottles, reaching a plateau. Similar final hydrogen concentrations were obtained for reactors spiked with acetylene and BES. In the second phase of tests the headspace of the batch reactors was flushed with nitrogen gas after the first plateau of hydrogen was reached, and subsequently incubated, with no further addition of inhibitor nor substrate. It was found that hydrogen production resumed and reached a second plateau, although somewhat lower than the first one. This procedure was repeated a third time and an additional amount of hydrogen was obtained. The plateaux and initial rates of hydrogen accumulation decreased in each subsequent incubation cycle. The total cumulative hydrogen harvested in the three cycles was much higher (approx. double) than in the first cycle alone. We coined this procedure as IV-SSAH (intermittently vented solid substrate anaerobic hydrogen generation). Our results point out to a feasible strategy for obtaining higher hydrogen yields from the fermentation of industrial solid wastes, and a possible combination of waste treatment processes consisting of a first stage IV-SSAH followed by a second SSAD stage. Useful products of this approach would be hydrogen, organic acids or methane, and anaerobic digestates that could be used as soil amenders after post-treatment.

  1. Hydrogen generation via anaerobic fermentation of paper mill wastes

    Energy Technology Data Exchange (ETDEWEB)

    Valdez Vazquez, I.; Poggi Varaldo, H.M. [CINVESTAV-IPN, Mexico D.F. (Mexico). Dept. of Biotechnology and Bioengineering; Sparling, R.; Risbey, D. [Manitoba Univ., Winnipeg (Canada). Dept. of Microbiology; Rinderknecht Seijas, N. [ESIQUIE-IPN, Mexico D.F. (Mexico). Division Base Sciences

    2005-11-15

    The objective of this work was to determine the hydrogen production from paper mill wastes using microbial consortia of solid substrate anaerobic digesters. Inocula from mesophilic, continuous solid substrate anaerobic digestion (SSAD) reactors were transferred to small lab scale, batch reactors. Milled paper (used as a surrogate paper waste) was added as substrate and acetylene or 2-bromoethanesulfonate (BES) was spiked for methanogenesis inhibition. In the first phase of experiments it was found that acetylene at 1% v/v in the headspace was as effective as BES in inhibiting methanogenic activity. Hydrogen gas accumulated in the headspace of the bottles, reaching a plateau. Similar final hydrogen concentrations were obtained for reactors spiked with acetylene and BES. In the second phase of tests the headspace of the batch reactors was flushed with nitrogen gas after the first plateau of hydrogen was reached, and subsequently incubated, with no further addition of inhibitor nor substrate. It was found that hydrogen production resumed and reached a second plateau, although somewhat lower than the first one. This procedure was repeated a third time and an additional amount of hydrogen was obtained. The plateaux and initial rates of hydrogen accumulation decreased in each subsequent incubation cycle. The total cumulative hydrogen harvested in the three cycles was much higher (approx. double) than in the first cycle alone. We coined this procedure as IV-SSAH (intermittently vented solid substrate anaerobic hydrogen generation). Our results point out to a feasible strategy for obtaining higher hydrogen yields from the fermentation of industrial solid wastes, and a possible combination of waste treatment processes consisting of a first stage IV-SSAH followed by a second SSAD stage. Useful products of this approach would be hydrogen, organic acids or methane, and anaerobic digestates that could be used as soil amenders after post-treatment. (author)

  2. Acetaldehyde behavior over platinum based catalyst in hydrogen stream generated by ethanol reforming

    Energy Technology Data Exchange (ETDEWEB)

    de Lima, Adriana F.F. [Laboratorio de Catalise, Instituto Nacional de Tecnologia, Av. Venezuela 82/507, 20081-310 Rio de Janeiro, RJ (Brazil); Instituto de Quimica e INOG (Instituto Nacional de Oleo Gas), UERJ-CNPq, FAPERJ, Universidade do Estado do Rio de Janeiro, Rua Sao Francisco Xavier, 524, 20550-900 Rio de Janeiro, RJ (Brazil); Colman, Rita C. [Departamento de Engenharia Quimica e de Petroleo, Universidade Federal Fluminense, Av. Passos da Patria, 156/bl E/240, 24210-240 Niteroi, RJ (Brazil); Zotin, Fatima M.Z. [Instituto de Quimica e INOG (Instituto Nacional de Oleo Gas), UERJ-CNPq, FAPERJ, Universidade do Estado do Rio de Janeiro, Rua Sao Francisco Xavier, 524, 20550-900 Rio de Janeiro, RJ (Brazil); CETEM-MCT, Av. Pedro Calmon, 900, Cidade Universitaria, 21941-908 Rio de Janeiro, RJ (Brazil); Appel, Lucia G. [Laboratorio de Catalise, Instituto Nacional de Tecnologia, Av. Venezuela 82/507, 20081-310 Rio de Janeiro, RJ (Brazil)

    2010-12-15

    Due to the greenhouse effect, hydrogen production from bioethanol reforming is a very important subject in heterogeneous catalysis research. Pt based catalysts are employed in H{sub 2} purification processes and also as electrocatalysts of PEM (''Proton Exchange Membrane'') fuel cells. Hydrogen obtained from ethanol reforming may contain, as contaminants, acetaldehyde and small amounts of CO. This aldehyde can be decarbonylated on Pt based catalysts generating carbon monoxide and methane, rendering the hydrogen purification more challenging. Moreover, acetaldehyde might also change the electrocatalyst behavior. Therefore, this contribution aims at studying the acetaldehyde behavior in the presence of platinum based catalysts in hydrogen atmosphere. The Pt/SiO{sub 2}, Pt/USY catalysts and an electrocatalyst were characterized by n-butylamine, H{sub 2} and CO{sub 2} adsorption, ATG/DTG measurements and cyclohexane dehydrogenation reaction. It was observed that the acid-basic properties of the supports promote condensation reactions. When in contact with Pt based catalysts, acetaldehyde undergoes C-C and C=O bond scissions. The former occurs at a wide range of temperatures, whereas the latter only at low temperatures (<200 C). The C-C bond scission (decarbonylation) produces methane and CO. The C=O bond scission generates carbon residues on the catalyst as well as oxygen species, which in turn is able to eliminate CO from the catalytic surface. The data also show that decarbonylation is not a structure-sensitive reaction. (author)

  3. Hydrogen generation from methanolysis of sodium borohydride over Co/Al2O3 catalyst

    Institute of Scientific and Technical Information of China (English)

    Dongyan Xu; Lin Zhao; Ping Dai; Shengfu Ji

    2012-01-01

    Co/Al2O3 catalyst is prepared with an impregnation-chemical reduction method and used to catalyze the methanolysis of sodium borohydride (NaBH4) for hydrogen generation.At solution temperature of 0℃,the methanolysis reaction can be effectively accelerated using Co/Al2O3 catalyst and provide a desirable hydrogen generation rate,which makes it suitable for apphcations under the circumstance of low environmental temperature.The byproduct of methanolysis reaction is analyzed by X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR).The characterization results indicate that methanol can be easily recovered after methanolysis reaction by hydrolysis of the methanolysis byproduct,NaB(OCH3)4.The catalytic activity of Co/Al2O3 towards NaBH4 methanolysis can be further improved by appropriate calcination treatment.The catalytic methanolysis kinetics and catalyst reusability are also studied over the Co/Al2O3 catalyst calcined at the optimized temperature.

  4. Hydrogenation-controlled phase transition on two-dimensional transition metal dichalcogenides and their unique physical and catalytic properties

    Science.gov (United States)

    Qu, Yuanju; Pan, Hui; Kwok, Chi Tat

    2016-09-01

    Two-dimensional (2D) transition metal dichalcogenides (TMDs) have been widely used from nanodevices to energy harvesting/storage because of their tunable physical and chemical properties. In this work, we systematically investigate the effects of hydrogenation on the structural, electronic, magnetic, and catalytic properties of 33 TMDs based on first-principles calculations. We find that the stable phases of TMD monolayers can transit from 1T to 2H phase or vice versa upon the hydrogenation. We show that the hydrogenation can switch their magnetic and electronic states accompanying with the phase transition. The hydrogenation can tune the magnetic states of TMDs among non-, ferro, para-, and antiferro-magnetism and their electronic states among semiconductor, metal, and half-metal. We further show that, out of 33 TMD monolayers, 2H-TiS2 has impressive catalytic ability comparable to Pt in hydrogen evolution reaction in a wide range of hydrogen coverages. Our findings would shed the light on the multi-functional applications of TMDs.

  5. Hydrogenation-controlled phase transition on two-dimensional transition metal dichalcogenides and their unique physical and catalytic properties

    Science.gov (United States)

    Qu, Yuanju; Pan, Hui; Kwok, Chi Tat

    2016-01-01

    Two-dimensional (2D) transition metal dichalcogenides (TMDs) have been widely used from nanodevices to energy harvesting/storage because of their tunable physical and chemical properties. In this work, we systematically investigate the effects of hydrogenation on the structural, electronic, magnetic, and catalytic properties of 33 TMDs based on first-principles calculations. We find that the stable phases of TMD monolayers can transit from 1T to 2H phase or vice versa upon the hydrogenation. We show that the hydrogenation can switch their magnetic and electronic states accompanying with the phase transition. The hydrogenation can tune the magnetic states of TMDs among non-, ferro, para-, and antiferro-magnetism and their electronic states among semiconductor, metal, and half-metal. We further show that, out of 33 TMD monolayers, 2H-TiS2 has impressive catalytic ability comparable to Pt in hydrogen evolution reaction in a wide range of hydrogen coverages. Our findings would shed the light on the multi-functional applications of TMDs. PMID:27686869

  6. The generation of electricity by gas turbines using the catalytic combustion of low-Btu gases

    DEFF Research Database (Denmark)

    Frederiksen, O.P.; Qvale, Einar Bjørn

    1989-01-01

    Various systems for the generation of electricity by gas turbines using catalytic combustion of low-Btu gases have been investigated. Parametric studies of three configurations that are deemed to be practically feasible have been completed. It is shown that thermodynamic efficiency of these systems...

  7. Selective Catalytic Synthesis Using the Combination of Carbon Dioxide and Hydrogen: Catalytic Chess at the Interface of Energy and Chemistry.

    Science.gov (United States)

    Klankermayer, Jürgen; Wesselbaum, Sebastian; Beydoun, Kassem; Leitner, Walter

    2016-06-20

    The present Review highlights the challenges and opportunities when using the combination CO2 /H2 as a C1 synthon in catalytic reactions and processes. The transformations are classified according to the reduction level and the bond-forming processes, covering the value chain from high volume basic chemicals to complex molecules, including biologically active substances. Whereas some of these concepts can facilitate the transition of the energy system by harvesting renewable energy into chemical products, others provide options to reduce the environmental impact of chemical production already in today's petrochemical-based industry. Interdisciplinary fundamental research from chemists and chemical engineers can make important contributions to sustainable development at the interface of the energetic and chemical value chain. The present Review invites the reader to enjoy this exciting area of "catalytic chess" and maybe even to start playing some games in her or his laboratory. PMID:27237963

  8. Generation of correlated photons in hydrogenated amorphous-silicon waveguides

    OpenAIRE

    Clemmen, S.; Perret, A; Selvaraja, Shankar Kumar; Bogaerts, Wim; Van Thourhout, Dries; Baets, Roel; Emplit, Ph.; Massar, S.

    2011-01-01

    We report the first (to our knowledge) observation of correlated photon emission in hydrogenated amorphous- silicon waveguides. We compare this to photon generation in crystalline silicon waveguides with the same geome- try. In particular, we show that amorphous silicon has a higher nonlinearity and competes with crystalline silicon in spite of higher loss.

  9. Supercontinuum generation in hydrogenated amorphous silicon waveguides at telecommunication wavelengths.

    Science.gov (United States)

    Safioui, Jassem; Leo, François; Kuyken, Bart; Gorza, Simon-Pierre; Selvaraja, Shankar Kumar; Baets, Roel; Emplit, Philippe; Roelkens, Gunther; Massar, Serge

    2014-02-10

    We report supercontinuum (SC) generation centered on the telecommunication C-band (1550 nm) in CMOS compatible hydrogenated amorphous silicon waveguides. A broadening of more than 550 nm is obtained in 1cm long waveguides of different widths using as pump picosecond pulses with on chip peak power as low as 4 W.

  10. Catalytic Transfer Hydrogenation of Furfural to Furfuryl Alcohol over Nitrogen-Doped Carbon-Supported Iron Catalysts.

    Science.gov (United States)

    Li, Jiang; Liu, Jun-Ling; Zhou, Hong-Jun; Fu, Yao

    2016-06-01

    Iron-based heterogeneous catalysts, which were generally prepared by pyrolysis of iron complexes on supports at elevated temperature, were found to be capable of catalyzing the transfer hydrogenation of furfural (FF) to furfuryl alcohol (FFA). The effects of metal precursor, nitrogen precursor, pyrolysis temperature, and support on catalytic performance were examined thoroughly, and a comprehensive study of the reaction parameters was also performed. The highest selectivity of FFA reached 83.0 % with a FF conversion of 91.6 % under the optimal reaction condition. Catalyst characterization suggested that iron cations coordinated by pyridinic nitrogen functionalities were responsible for the enhanced catalytic activity. The iron catalyst could be recycled without significant loss of catalytic activity for five runs, and the destruction of the nitrogen-iron species, the presence of crystallized Fe2 O3 phase, and the pore structure change were the main reasons for catalyst deactivation. PMID:27144965

  11. SYNTHESIS AND CHARACTERIZATION OF A SILICA-SUPPORTED CARBOXYMETHYLCELLULOSE PLATINUM COMPLEX AND ITS CATALYTIC BEHAVIORS FOR HYDROGENATION OF AROMATICS

    Institute of Scientific and Technical Information of China (English)

    TANG Liming; HUANG Meiyu; JIANG Yingyan

    1996-01-01

    A silica-supported carboxymethylcellulose platinum complex (abbreviated as SiO2-CMC-Pt) has been prepared and characterized by XPS. Its catalytic properties for hydrogenation of aromatic compounds were studied. The results showed that this catalyst could catalyze the hydrogenation of phenol, anisol, p-cresol, benzene and toluene to cyclohexanol, cyclohexyl methyl ether, p-methyl cyclohexanol, cyclohexane and methylcyclohexane, respectively in 100% yield at 30℃ and 1 atm. In the hydrogenation of phenol,COO/Pt ratio in SiO2-CMC-Pt has much influence on the initial hydrogenation rate and the selectivity for the intermediate product, cyclohexanone. The highest initial rate and the highest yield of cyclohexanone both occur at COO/Pt ratio of 6. The complex is stable during the reaction and can be used repeatedly.

  12. Hydrogen production from catalytic reforming of the aqueous fraction of pyrolysis bio-oil with modified Ni-Al catalysts

    OpenAIRE

    D. Yao; Wu, C.; Yang, H; Hu, Q.; Nahil, MA; H Chen; Williams, PT

    2014-01-01

    Hydrogen production from renewable resources has received extensive attention recently for a sustainable and renewable future. In this study, hydrogen was produced from catalytic steam reforming of the aqueous fraction of crude bio-oil, which was obtained from pyrolysis of biomass. Five Ni-Al catalysts modified with Ca, Ce, Mg, Mn and Zn were investigated using a fixed-bed reactor. Optimized process conditions were obtained with a steam reforming temperature of 800 °C and a steam to carbon ra...

  13. Supported catalysts based on layered double hydroxides for catalytic oxidation and hydrogenation: general functionality and promising application prospects.

    Science.gov (United States)

    Feng, Junting; He, Yufei; Liu, Yanan; Du, Yiyun; Li, Dianqing

    2015-08-01

    Oxidation and hydrogenation catalysis plays a crucial role in the current chemical industry for the production of key chemicals and intermediates. Because of their easy separation and recyclability, supported catalysts are widely used in these two processes. Layered double hydroxides (LDHs) with the advantages of unique structure, composition diversity, high stability, ease of preparation and low cost have shown great potential in the design and synthesis of novel supported catalysts. This review summarizes the recent progress in supported catalysts by using LDHs as supports/precursors for catalytic oxidation and hydrogenation. Particularly, partial hydrogenation of acetylene, hydrogenation of dimethyl terephthalate, methanation, epoxidation of olefins, elimination of NOx and SOx emissions, and selective oxidation of biomass have been chosen as representative reactions in the petrochemical, fine chemicals, environmental protection and clean energy fields to highlight the potential application and the general functionality of LDH-based catalysts in catalytic oxidation and hydrogenation. Finally, we concisely discuss some of the scientific challenges and opportunities of supported catalysts based on LDH materials. PMID:25962432

  14. Field-controlled electron transfer and reaction kinetics of the biological catalytic system of microperoxidase-11 and hydrogen peroxide

    OpenAIRE

    Yongki Choi; Siu-Tung Yau

    2011-01-01

    Controlled reaction kinetics of the bio-catalytic system of microperoxidase-11 and hydrogen peroxide has been achieved using an electrostatic technique. The technique allowed independent control of 1) the thermodynamics of the system using electrochemical setup and 2) the quantum mechanical tunneling at the interface between microperoxidase-11 and the working electrode by applying a gating voltage to the electrode. The cathodic currents of electrodes immobilized with microperoxidase-11 showed...

  15. Graphene Porous Foam Loaded with Molybdenum Carbide Nanoparticulate Electrocatalyst for Effective Hydrogen Generation.

    Science.gov (United States)

    Wang, Jie; Xia, Han; Peng, Zhen; Lv, Cuncai; Jin, Lihuang; Zhao, Yaoxing; Huang, Zhipeng; Zhang, Chi

    2016-04-21

    A facile method is developed for the synthesis of graphene porous foam (Gr PF) loaded with dispersed molybdenum carbide (Mo2 C) nanoparticles; the material exhibits effective catalytic activity in the hydrogen evolution reaction (HER). Mo2 C/Gr PF is synthesized by the carbonization of glucose and the carbothermal reduction of hexaammonium molybdate in a confined space defined by the intervals between sodium chloride nanoparticles. The synthesis in the confined space results in thin Gr PF (≈8 nm) loaded with aggregation-free small Mo2 C nanoparticles [(13±2) nm]. The overpotential required for a current density of 20 mA cm(-2) in the electrochemical hydrogen generation is as small as 199 mV in acidic solution and 380 mV in basic solution. The performance is superior to that of a Mo2 C/C composite and compares favorably to those reported for Mo2 C nanostructures. The Mo2 C/Gr PF affords stable water electrolysis in both acidic and basic solution and exhibits nearly 100 % faradaic efficiency. The prominent performance, long-term stability, and high faradic efficiency make Mo2 C/Gr PF a promising HER catalyst for practical hydrogen generation from water electrolysis.

  16. Hydrogen Peroxide Gas Generator Cycle with a Reciprocating Pump

    Energy Technology Data Exchange (ETDEWEB)

    Whitehead, J C

    2002-06-11

    A four-chamber piston pump is powered by decomposed 85% hydrogen peroxide. The performance envelope of the evolving 400 gram pump has been expanded to 172 cc/s water flow at discharge pressures near 5 MPa. A gas generator cycle system using the pump has been tested under similar conditions of pressure and flow. The powerhead gas is derived from a small fraction of the pumped hydrogen peroxide, and the system starts from tank pressures as low as 0.2 MPa. The effects of steam condensation on performance have been evaluated.

  17. Wind energy-hydrogen storage hybrid power generation

    Energy Technology Data Exchange (ETDEWEB)

    Wenjei Yang; Orhan Aydin [University of Michigan, Ann Arbor, MI (United States). Dept. of Mechanical Engineering and Applied Mechanics

    2001-07-01

    In this theoretical investigation, a hybrid power generation system utilizing wind energy and hydrogen storage is presented. Firstly, the available wind energy is determined, which is followed by evaluating the efficiency of the wind energy conversion system. A revised model of windmill is proposed from which wind power density and electric power output are determined. When the load demand is less than the output of the generation, the excess electric power is relayed to the electrolytic cell where it is used to electrolyse the de-ionized water. Hydrogen thus produced can be stored as hydrogen compressed gas or liquid. Once the hydrogen is stored in an appropriate high-pressure vessel, it can be used in a combustion engine, fuel cell, or burned in a water-cooled burner to produce a very high-quality steam for space heating, or to drive a turbine to generate electric power. It can also be combined with organic materials to produce synthetic fuels. The conclusion is that the system produces no harmful waste and depletes no resources. Note that this system also works well with a solar collector instead of a windmill. (author)

  18. Development of catalytic systems for selective hydrogenation and hydrogenolysis based on statistical planning methods coupled with kinetic studies

    Energy Technology Data Exchange (ETDEWEB)

    Zhorov, Yu.M.; Morozova, E.V.; Panchenkov, G.M.

    1979-01-01

    An efficient catalyst design methodology is described, which was used in developing an active and stable mixed oxide catalytic composition for selective hydrogenation of m-bonds under conditions excluding hydrogenolysis of C-C bonds. Catalysts of optimum composition, i.e., 40-50Vertical Bar3< CuO/25-30Vertical Bar3< NiO/20-35Vertical Bar3< SiO/sub 2/, and structure (20-30 A. average pore radius) can be prepared by coprecipitation of copper and nickel salts with silica gel powder in a sodium silicate solution at 90/sup 0/C. By using these catalysts, crotonaldehyde (CA) was hydrogenated to n-butanol in one stage with over 99Vertical Bar3< yields at 180/sup 0/C. The same catalyst was efficient in selective hydrogenation of acetylene (contained in relatively high concentrations in pyrolysis gases) to ethylene at 130/sup 0/C, hydrogenation of piperylene (a by-product in isoprene manufacture) to n-pentenes at 160/sup 0/C, with almost 100Vertical Bar3< selectivity, and in hydrogenolysis of C-S and C-N bonds at 290/sup 0/-370/sup 0/C. Catalytic hydrorefining of a gasoline fraction (105/sup 0/-180/sup 0/C bp) at 350/sup 0/C and 40 atm, reduced its sulfur content from 0.03Vertical Bar3< to 0.00001Vertical Bar3<, and completely removed nitrogen.

  19. Pt nanoparticles modified by rare earth oxides: Electronic effect and influence to catalytic hydrogenation of 3-phenoxybenzaldehyde

    International Nuclear Information System (INIS)

    Graphical abstract: - Highlights: • The rare earths modified Pt/Al2O3 were prepared by colloidal deposition method. • Modification of Pt by the rare earth enhanced catalytic hydrogenation activity. • The activity improvement is due to electron interaction between Pt and rare earth. • The hydrogenation mechanism of rare earth modified Pt catalyst was proposed. - Abstract: The rare earth elements (La, Ce, Nd, Sm, Pr, and Gd) modified Pt/Al2O3 catalysts were prepared by the colloidal deposition and chemical reduction methods, respectively. Pt nanoparticles with average size 3 ± 0.5 nm were uniformly dispersed on the surface of Al2O3 for the samples prepared by the colloidal deposition method, which exhibited higher activities in the hydrogenation of 3-phenoxybenzadehyde than the corresponding samples prepared by chemical reduction method. Moreover, except Gd, the catalysts modified by rare earth elements showed better catalytic performance than unmodified Pt/Al2O3. For Pt–Ce/Al2O3 catalyst, when the weight percent of Pt and Ce was 0.5 and 0.25, respectively, the hydrogenation conversion of 3-phenoxybenzaldehyde was 97.3% after 6 h reaction. This activity improvement is due to the electronic interaction between Pt and rare earth elements, which was investigated by X-ray photoelectron spectroscopy

  20. Solar powered hydrogen generating facility and hydrogen powered vehicle fleet. Final technical report, August 11, 1994--January 6, 1997

    Energy Technology Data Exchange (ETDEWEB)

    Provenzano, J.J.

    1997-04-01

    This final report describes activities carried out in support of a demonstration of a hydrogen powered vehicle fleet and construction of a solar powered hydrogen generation system. The hydrogen generation system was permitted for construction, constructed, and permitted for operation. It is not connected to the utility grid, either for electrolytic generation of hydrogen or for compression of the gas. Operation results from ideal and cloudy days are presented. The report also describes the achievement of licensing permits for their hydrogen powered trucks in California, safety assessments of the trucks, performance data, and information on emissions measurements which demonstrate performance better than the Ultra-Low Emission Vehicle levels.

  1. Energy Efficient Catalytic Activation of Hydrogen peroxide for Green Chemical Processes: Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Collins, Terrence J.; Horwitz, Colin

    2004-11-12

    A new, highly energy efficient approach for using catalytic oxidation chemistry in multiple fields of technology has been pursued. The new catalysts, called TAML® activators, catalyze the reactions of hydrogen peroxide and other oxidants for the exceptionally rapid decontamination of noninfectious simulants (B. atrophaeus) of anthrax spores, for the energy efficient decontamination of thiophosphate pesticides, for the facile, low temperature removal of color and organochlorines from pulp and paper mill effluent, for the bleaching of dyes from textile mill effluents, and for the removal of recalcitrant dibenzothiophene compounds from diesel and gasoline fuels. Highlights include the following: 1) A 7-log kill of Bacillus atrophaeus spores has been achieved unambiguously in water under ambient conditions within 15 minutes. 2) The rapid total degradation under ambient conditions of four thiophosphate pesticides and phosphonate degradation intermediates has been achieved on treatment with TAML/peroxide, opening up potential applications of the decontamination system for phosphonate structured chemical warfare agents, for inexpensive, easy to perform degradation of stored and aged pesticide stocks (especially in Africa and Asia), for remediation of polluted sites and water bodies, and for the destruction of chemical warfare agent stockpiles. 3) A mill trial conducted in a Pennsylvanian bleached kraft pulp mill has established that TAML catalyst injected into an alkaline peroxide bleach tower can significantly lower color from the effluent stream promising a new, more cost effective, energy-saving approach for color remediation adding further evidence of the value and diverse engineering capacity of the approach to other field trials conducted on effluent streams as they exit the bleach plant. 4) Dibenzothiophenes (DBTs), including 4,6-dimethyldibenzothiophene, the most recalcitrant sulfur compounds in diesel and gasoline, can be completely removed from model gasoline

  2. Generator cooling hydrogen purity improvement system using hydrogen absorbing alloy; Suiso kyuzo gokin riyo hatsudenkinai suiso jundo kojo system

    Energy Technology Data Exchange (ETDEWEB)

    Takeda, H.; Kabutomori, T.; Wakisaka, Y. [Japan Steel Works, Ltd., Tokyo (Japan); Nishimura, Y.; Kogi, T.; Sato, J.; Haruki, N. [Kansai Electric Power Co. Inc., Osaka (Japan); Fujita, T. [Mitsubishi Electric Corp., Tokyo (Japan)

    1998-09-15

    Described herein is a system which uses a hydrogen-absorbing alloy to purify a hydrogen gas stream used as a coolant for power generator. Hydrogen in the stream containing impurities such as nitrogen can be selectively absorbed by sufficiently cooled hydrogen-absorbing alloy. Impurity gases concentrated in the alloy pores are released, and then the alloy is heated to release hydrogen. This purifies hydrogen to at least 99.99%. This system essentially consists of an hydrogen-absorbing unit, hot water production/supply system which circulates hot water of 80 to 90degC to release hydrogen out of the alloy, pretreatment unit, and temperature and pressure sensors. It is confirmed, by the test in which the system is connected to a commercial power generator of 600MW, that the system can be continuously operated to purify hydrogen to at least 99.9% for an extended period. 4 refs., 18 figs., 1 tab.

  3. Modelling studies to proper size a hydrogen generator for fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Maggio, G.; Recupero, V.; Di Leonardo, R.; Lagana, M. [Istituto CNR-TAE, Lucia, Messina (Italy)

    1996-12-31

    Based upon an extensive survey of literature a mathematical model has been developed to study the temperature profile along the catalytic bed of a reactor for the methane partial oxidation. The model allowed a preliminary design of a 5 Nm{sup 3} syngas/h prototype to be integrated with second generation fuel cells as hydrogen generator (in the framework of the EC-JOU2 contract). This design was based on some target features, including the choice of a GHSV (gas hour space velocity) equal to 80000 h{sup -1}, a catalyst particle size of 1/8inches, a molar air/methane ratio of 2.7 (i.e. O{sub 2}/CH{sub 4}=0.53), a linear velocity in the catalytic bed of about 2 m/sec, and an inert/catalyst ratio 3:1. Starting from this data, the work has been concerned with the identification of the controlling regime (kinetic or diffusional), and then with the estimation of the gas composition and temperature profiles along the reactor. A comparison between experimental and model results has also been accomplished.

  4. Generation of hydrogen from photocatalytic cleavage of water

    Energy Technology Data Exchange (ETDEWEB)

    Mallinson, R.G.; Resasco, D.E.; Lobban, L.L.; Nicholas, K.M. [Univ. of Oklahoma, Norman, OK (United States)

    1998-08-01

    This paper describes the objectives, methods and early results on the US Department of Energy sponsored project to generate hydrogen from splitting of water using photocatalysts. The approach uses organometallic photosensitizers adsorbed onto platinated titania. Platinized titania is a photocatalyst for water splitting, but does not absorb sunlight in the visible range, where most of the sun`s energy is contained. Organometallic photosensitizers are synthesized, attached to platinized titania and characterized by UV-Vis spectroscopy, cyclic voltammetry, action spectra and hydrogen generation ability. Thus far, Copper, Iron and Ruthenium catalyst systems have been produced and characterized in this manner. Suitable sensitized systems that have the desirable properties have not yet been found.

  5. Fluid-Bed Testing of Greatpoint Energy's Direct Oxygen Injection Catalytic Gasification Process for Synthetic Natural Gas and Hydrogen Coproduction Year 6 - Activity 1.14 - Development of a National Center for Hydrogen Technology

    Energy Technology Data Exchange (ETDEWEB)

    Swanson, Michael; Henderson, Ann

    2012-04-01

    The GreatPoint Energy (GPE) concept for producing synthetic natural gas and hydrogen from coal involves the catalytic gasification of coal and carbon. GPE’s technology “refines” coal by employing a novel catalyst to “crack” the carbon bonds and transform the coal into cleanburning methane (natural gas) and hydrogen. The GPE mild “catalytic” gasifier design and operating conditions result in reactor components that are less expensive and produce pipeline-grade methane and relatively high purity hydrogen. The system operates extremely efficiently on very low cost carbon sources such as lignites, subbituminous coals, tar sands, petcoke, and petroleum residual oil. In addition, GPE’s catalytic coal gasification process eliminates troublesome ash removal and slagging problems, reduces maintenance requirements, and increases thermal efficiency, significantly reducing the size of the air separation plant (a system that alone accounts for 20% of the capital cost of most gasification systems) in the catalytic gasification process. Energy & Environmental Research Center (EERC) pilot-scale gasification facilities were used to demonstrate how coal and catalyst are fed into a fluid-bed reactor with pressurized steam and a small amount of oxygen to “fluidize” the mixture and ensure constant contact between the catalyst and the carbon particles. In this environment, the catalyst facilitates multiple chemical reactions between the carbon and the steam on the surface of the coal. These reactions generate a mixture of predominantly methane, hydrogen, and carbon dioxide. Product gases from the process are sent to a gas-cleaning system where CO{sub 2} and other contaminants are removed. In a full-scale system, catalyst would be recovered from the bottom of the gasifier and recycled back into the fluid-bed reactor. The by-products (such as sulfur, nitrogen, and CO{sub 2}) would be captured and could be sold to the chemicals and petroleum industries, resulting in

  6. Hydrogen generation during molten-fuel-coolant interactions

    International Nuclear Information System (INIS)

    Given the absence of adequate cooling water to the core of a light-water reactor, the fission product decay heat would eventually cause the reactor fuel and cladding to melt. This could lead to slumping of the molten core materials into the lower plenum of the reactor vessel, possibly followed by failure of the vessel wall and pouring of the molten materials into the reactor cavity. Recent analyses have indicated that residual water is likely to be present both in the lower plenum and in the reactor cavity. Therefore, when the molten core materials enter either region, there is a strong probability of molten core contacting water. The physical process by which the molten core contacts and mixes with the water is important for two reasons: (1) because of its potential for rapid steam generation from a fuel-coolant interaction (FCI) either energetic or non-energetic; and (2) because it is a source of combustible hydrogen from the oxidation of the metallic components of the molten core. In this paper the rate of hydrogen generation due to fuel-coolant mixing is the major topic. To predict this one must understand two physical processes. The first is the degree of fuel breakup during the mixing phase and during the FCI. By understanding this process one is able to calculate the surface area available during the chemical reaction. The second is the rate of hydrogen generation per unit area when the fuel is molten and as it cools and solidifies

  7. DESIGN NOTE: A compact catalytic converter for the production of para-hydrogen

    Science.gov (United States)

    Juarez, A. M.; Cubric, D.; King, G. C.

    2002-05-01

    The design and operation of a compact converter to produce a constant flow of para-hydrogen from normal hydrogen is described. The converter features a paramagnetic compound (nickel sulfate) that catalyses the conversion of ortho- to para-hydrogen at temperatures of 14-21 K. The converter has been tested by measuring rotationally resolved photoelectron spectra in the para-hydrogen produced. The percentage of the para-hydrogen species in the converted gas was determined to be >97%.

  8. Molecular hydrogen and catalytic combustion in the production of hyperpolarized 83Kr and 129Xe MRI contrast agents

    Science.gov (United States)

    Rogers, Nicola J.; Hill-Casey, Fraser; Stupic, Karl F.; Six, Joseph S.; Lesbats, Clémentine; Rigby, Sean P.; Fraissard, Jacques; Pavlovskaya, Galina E.; Meersmann, Thomas

    2016-03-01

    Hyperpolarized (hp) 83Kr is a promising MRI contrast agent for the diagnosis of pulmonary diseases affecting the surface of the respiratory zone. However, the distinct physical properties of 83Kr that enable unique MRI contrast also complicate the production of hp 83Kr. This work presents a previously unexplored approach in the generation of hp 83Kr that can likewise be used for the production of hp 129Xe. Molecular nitrogen, typically used as buffer gas in spin-exchange optical pumping (SEOP), was replaced by molecular hydrogen without penalty for the achievable hyperpolarization. In this particular study, the highest obtained nuclear spin polarizations were P = 29% for 83Kr and P = 63% for 129Xe. The results were reproduced over many SEOP cycles despite the laser-induced on-resonance formation of rubidium hydride (RbH). Following SEOP, the H2 was reactively removed via catalytic combustion without measurable losses in hyperpolarized spin state of either 83Kr or 129Xe. Highly spin-polarized 83Kr can now be purified for the first time, to our knowledge, to provide high signal intensity for the advancement of in vivo hp 83Kr MRI. More generally, a chemical reaction appears as a viable alternative to the cryogenic separation process, the primary purification method of hp 129Xe for the past 2 1/2 decades. The inherent simplicity of the combustion process will facilitate hp 129Xe production and should allow for on-demand continuous flow of purified and highly spin-polarized 129Xe.

  9. Room-Temperature and Aqueous-Phase Synthesis of Plasmonic Molybdenum Oxide Nanoparticles for Visible-Light-Enhanced Hydrogen Generation.

    Science.gov (United States)

    Shi, Jiayuan; Kuwahara, Yasutaka; Wen, Meicheng; Navlani-García, Miriam; Mori, Kohsuke; An, Taicheng; Yamashita, Hiromi

    2016-09-01

    A straightforward aqueous synthesis of MoO3-x nanoparticles at room temperature was developed by using (NH4 )6 Mo7 O24 ⋅4 H2 O and MoCl5 as precursors in the absence of reductants, inert gas, and organic solvents. SEM and TEM images indicate the as-prepared products are nanoparticles with diameters of 90-180 nm. The diffuse reflectance UV-visible-near-IR spectra of the samples indicate localized surface plasmon resonance (LSPR) properties generated by the introduction of oxygen vacancies. Owing to its strong plasmonic absorption in the visible-light and near-infrared region, such nanostructures exhibit an enhancement of activity toward visible-light catalytic hydrogen generation. MoO3-x nanoparticles synthesized with a molar ratio of Mo(VI) /Mo(V) 1:1 show the highest yield of H2 evolution. The cycling catalytic performance has been investigated to indicate the structural and chemical stability of the as-prepared plasmonic MoO3-x nanoparticles, which reveals its potential application in visible-light catalytic hydrogen production. PMID:27555123

  10. Hydrogen production from simulated hot coke oven gas by catalytic reforming over Ni/Mg(A1)O catalysts

    Institute of Scientific and Technical Information of China (English)

    Hongwei Cheng; Baohua Yue; Xueguang Wang; Xionggang Lu; Weizhong Ding

    2009-01-01

    Hydrogen production by catalytic reforming of simulated hot coke oven gas (HCOG) with toluene as a model tar compound was investigated in a fixed bed reactor over Ni/Mg(Al)O catalysts. The catalysts were prepared by a homogeneous precipitation method using urea hydrolysis and characterized by ICP,BET, XRD, TPR, TEM and TG. XRD showed that the hydrotalcite type precursor after calcination formed (Ni,Mg)Al2O4 spinel and Ni-Mg-O solid solution structure. TPR results suggested that the increase in Ni/Mg molar ratio gave rise to the decrease in the reduction temperature of Ni2+ to Ni0 on Ni/Mg(Al)O catalysts. The reaction results indicated that toluene and CH4 could completely be converted to H2 and CO in the catalytic reforming of the simulated HCOG under atmospheric pressure and the amount of H2 in the reaction effluent gas was about 4 times more than that in original HCOG. The catalysts with lower Ni/Mg molar ratio showed better catalytic activity and resistance to ceking, which may become promising catalysts in the catalytic reforming of HCOG.

  11. HIGH EFFICIENCY GENERATION OF HYDROGEN FUELS USING NUCLEAR POWER

    Energy Technology Data Exchange (ETDEWEB)

    BROWN,LC; BESENBRUCH,GE; LENTSCH,RD; SCHULTZ,KR; FUNK,JF; PICKARD,PS; MARSHALL,AC; SHOWALTER,SK

    2003-06-01

    OAK B202 HIGH EFFICIENCY GENERATION OF HYDROGEN FUELS USING NUCLEAR POWER. Combustion of fossil fuels, used to power transportation, generate electricity, heat homes and fuel industry provides 86% of the world's energy. Drawbacks to fossil fuel utilization include limited supply, pollution, and carbon dioxide emissions. Carbon dioxide emissions, thought to be responsible for global warming, are now the subject of international treaties. Together, these drawbacks argue for the replacement of fossil fuels with a less-polluting potentially renewable primary energy such as nuclear energy. Conventional nuclear plants readily generate electric power but fossil fuels are firmly entrenched in the transportation sector. Hydrogen is an environmentally attractive transportation fuel that has the potential to displace fossil fuels. Hydrogen will be particularly advantageous when coupled with fuel cells. Fuel cells have higher efficiency than conventional battery/internal combustion engine combinations and do not produce nitrogen oxides during low-temperature operation. Contemporary hydrogen production is primarily based on fossil fuels and most specifically on natural gas. When hydrogen is produced using energy derived from fossil fuels, there is little or no environmental advantage. There is currently no large scale, cost-effective, environmentally attractive hydrogen production process available for commercialization, nor has such a process been identified. The objective of this work is to find an economically feasible process for the production of hydrogen, by nuclear means, using an advanced high-temperature nuclear reactor as the primary energy source. Hydrogen production by thermochemical water-splitting (Appendix A), a chemical process that accomplishes the decomposition of water into hydrogen and oxygen using only heat or, in the case of a hybrid thermochemical process, by a combination of heat and electrolysis, could meet these goals. Hydrogen produced from

  12. Cellular graphene aerogel combines ultralow weight and high mechanical strength: A highly efficient reactor for catalytic hydrogenation.

    Science.gov (United States)

    Zhang, Bingxing; Zhang, Jianling; Sang, Xinxin; Liu, Chengcheng; Luo, Tian; Peng, Li; Han, Buxing; Tan, Xiuniang; Ma, Xue; Wang, Dong; Zhao, Ning

    2016-05-12

    The construction of three-dimensional graphene aerogels (GAs) is of great importance owing to their outstanding properties for various applications. Up to now, the combination of ultralow weight and super mechanical strength for GA remains a great challenge. Here we demonstrate the fabrication of cellular GAs by a facile, easily controlled and versatile route, i.e. the chemical reduction of graphene oxide assemblies at oil-water interface under a mild condition (70 °C). The GA is ultralight (with density <3 mg cm(-3)) yet mechanically resilient because the walls of the cell closely pack in a highly ordered manner to maximize mechanical strength. The GA has been utilized as an appealing reactor for catalytic hydrogenation, which exhibited great advantages such as large oil absorption capability, exceptional catalytic activity, ease of product separation and high stability.

  13. Cellular graphene aerogel combines ultralow weight and high mechanical strength: A highly efficient reactor for catalytic hydrogenation

    Science.gov (United States)

    Zhang, Bingxing; Zhang, Jianling; Sang, Xinxin; Liu, Chengcheng; Luo, Tian; Peng, Li; Han, Buxing; Tan, Xiuniang; Ma, Xue; Wang, Dong; Zhao, Ning

    2016-05-01

    The construction of three-dimensional graphene aerogels (GAs) is of great importance owing to their outstanding properties for various applications. Up to now, the combination of ultralow weight and super mechanical strength for GA remains a great challenge. Here we demonstrate the fabrication of cellular GAs by a facile, easily controlled and versatile route, i.e. the chemical reduction of graphene oxide assemblies at oil-water interface under a mild condition (70 °C). The GA is ultralight (with density resilient because the walls of the cell closely pack in a highly ordered manner to maximize mechanical strength. The GA has been utilized as an appealing reactor for catalytic hydrogenation, which exhibited great advantages such as large oil absorption capability, exceptional catalytic activity, ease of product separation and high stability.

  14. Cellular graphene aerogel combines ultralow weight and high mechanical strength: A highly efficient reactor for catalytic hydrogenation.

    Science.gov (United States)

    Zhang, Bingxing; Zhang, Jianling; Sang, Xinxin; Liu, Chengcheng; Luo, Tian; Peng, Li; Han, Buxing; Tan, Xiuniang; Ma, Xue; Wang, Dong; Zhao, Ning

    2016-01-01

    The construction of three-dimensional graphene aerogels (GAs) is of great importance owing to their outstanding properties for various applications. Up to now, the combination of ultralow weight and super mechanical strength for GA remains a great challenge. Here we demonstrate the fabrication of cellular GAs by a facile, easily controlled and versatile route, i.e. the chemical reduction of graphene oxide assemblies at oil-water interface under a mild condition (70 °C). The GA is ultralight (with density <3 mg cm(-3)) yet mechanically resilient because the walls of the cell closely pack in a highly ordered manner to maximize mechanical strength. The GA has been utilized as an appealing reactor for catalytic hydrogenation, which exhibited great advantages such as large oil absorption capability, exceptional catalytic activity, ease of product separation and high stability. PMID:27174450

  15. Thermo-Catalytic Methane Decomposition for Hydrogen Production: Effect of Palladium Promoter on Ni-based Catalysts

    Directory of Open Access Journals (Sweden)

    Irene Lock Sow Mei

    2016-08-01

    Full Text Available Hydrogen production from the direct thermo-catalytic decomposition of methane is a promising alternative for clean fuel production. However, thermal decomposition of methane can hardly be of any practical and empirical interest in the industry unless highly efficient and effective catalysts, in terms of both catalytic activity and operational lifetime have been developed. In this study, the effect of palladium (Pd as a promoter onto Ni supported on alumina catalyst has been investigated by using co-precipitation technique. The introduction of Pd promotes better catalytic activity, operational lifetime and thermal stability of the catalyst. As expected, highest methane conversion was achieved at reaction temperature of 800 °C while the bimetallic catalyst (1 wt.% Ni -1wt.% Pd/Al2O3 gave the highest methane conversion of 70% over 15 min of time-on-stream (TOS. Interestingly, the introduction of Pd as promoter onto Ni-based catalyst also has a positive effect on the operational lifetime and thermal stability of the catalyst as the methane conversion has improved significantly over 240 min of TOS. Copyright © 2016 BCREC GROUP. All rights reserved Received: 21st January 2016; Revised: 6th February 2016; Accepted: 6th March 2016 How to Cite: Mei, I.L.S., Lock, S.S.M., Vo, D.V.N., Abdullah, B. (2016. Thermo-Catalytic Methane Decomposition for Hydrogen Production: Effect of Palladium Promoter on Ni-based Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 11 (2: 191-199 (doi:10.9767/bcrec.11.2.550.191-199 Permalink/DOI: http://dx.doi.org/10.9767/bcrec.11.2.550.191-199

  16. Selective catalytic reduction of nitrogen oxides from industrial gases by hydrogen or methane; Reduction catalytique selective des oxydes d'azote (NO{sub x}) provenant d'effluents gazeux industriels par l'hydrogene ou le methane

    Energy Technology Data Exchange (ETDEWEB)

    Engelmann Pirez, M

    2004-12-15

    This work deals with the selective catalytic reduction of nitrogen oxides (NO{sub x}), contained in the effluents of industrial plants, by hydrogen or methane. The aim is to replace ammonia, used as reducing agent, in the conventional process. The use of others reducing agents such as hydrogen or methane is interesting for different reasons: practical, economical and ecological. The catalyst has to convert selectively NO into N{sub 2}, in presence of an excess of oxygen, steam and sulfur dioxide. The developed catalyst is constituted by a support such as perovskites, particularly LaCoO{sub 3}, on which are dispersed noble metals (palladium, platinum). The interaction between the noble metal and the support, generated during the activation of the catalyst, allows to minimize the water and sulfur dioxide inhibitor phenomena on the catalytic performances, particularly in the reduction of NO by hydrogen. (O.M.)

  17. Sum Frequency Generation Studies of Hydrogenation Reactions on Platinum Nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Krier, James M. [Univ. of California, Berkeley, CA (United States)

    2013-08-31

    Sum Frequency Generation (SFG) vibrational spectroscopy is used to characterize intermediate species of hydrogenation reactions on the surface of platinum nanoparticle catalysts. In contrast to other spectroscopy techniques which operate in ultra-high vacuum or probe surface species after reaction, SFG collects information under normal conditions as the reaction is taking place. Several systems have been studied previously using SFG on single crystals, notably alkene hydrogenation on Pt(111). In this thesis, many aspects of SFG experiments on colloidal nanoparticles are explored for the first time. To address spectral interference by the capping agent (PVP), three procedures are proposed: UV cleaning, H2 induced disordering and calcination (core-shell nanoparticles). UV cleaning and calcination physically destroy organic capping while disordering reduces SFG signal through a reversible structural change by PVP.

  18. A New Method for Generating Hydrogen from Water

    Institute of Scientific and Technical Information of China (English)

    MENG Qing-Bo; LI Ke-Xin; LI Hong; FAN Yu-Zun; YU Zhe-Xun; LI Dong-Mei; LUO Yan-Hong; CHEN Li-Quan

    2008-01-01

    A new method for generating hydrogen by the reaction of A1 powder with water using iodine as additive is developed. 12 can penetrate through the surface oxide layer on atuminium to form AlI3. High solubility of AlI3 in water is benefited to activate Al surface. It is found that the production of hydrogen becomes significant above 60℃ and obeys a logarithm rule. The pH value varies from 5 to 3 then back to 4.5 during the reaction,which is determined mainly by the kinetics of hydration reaction of AlI3 and the reaction of Al and HI produced spontaneously.

  19. DWPF Hydrogen Generation Study-Form of Noble Metal SRAT Testing

    Energy Technology Data Exchange (ETDEWEB)

    Bannochie, C

    2005-09-01

    The Defense Waste Processing Facility, DWPF, has requested that the Savannah River National Laboratory, SRNL, investigate the factors that contribute to hydrogen generation to determine if current conservatism in setting the DWPF processing window can be reduced. A phased program has been undertaken to increase understanding of the factors that influence hydrogen generation in the DWPF Chemical Process Cell, CPC. The hydrogen generation in the CPC is primarily due to noble metal catalyzed decomposition of formic acid with a minor contribution from radiolytic processes. Noble metals have historically been added as trim chemicals to process simulations. The present study investigated the potential conservatism that might be present from adding the catalytic species as trim chemicals to the final sludge simulant versus co-precipitating the noble metals into the insoluble sludge solids matrix. Two sludge simulants were obtained, one with co-precipitated noble metals and one without noble metals. Co-precipitated noble metals were expected to better match real waste behavior than using trimmed noble metals during CPC simulations. Portions of both sludge simulants were held at 97 C for about eight hours to qualitatively simulate the effects of long term storage on particle morphology and speciation. The two original and two heat-treated sludge simulants were then used as feeds to Sludge Receipt and Adjustment Tank, SRAT, process simulations. Testing was done at relatively high acid stoichiometries, {approx}175%, and without mercury in order to ensure significant hydrogen generation. Hydrogen generation rates were monitored during processing to assess the impact of the form of noble metals. The following observations were made on the data: (1) Co-precipitated noble metal simulant processed similarly to trimmed noble metal simulant in most respects, such as nitrite to nitrate conversion, formate destruction, and pH, but differently with respect to hydrogen generation: (A

  20. Atomistic Modelling of Materials for Clean Energy Applications : hydrogen generation, hydrogen storage, and Li-ion battery

    OpenAIRE

    Qian, Zhao

    2013-01-01

    In this thesis, a number of clean-energy materials for hydrogen generation, hydrogen storage, and Li-ion battery energy storage applications have been investigated through state-of-the-art density functional theory. As an alternative fuel, hydrogen has been regarded as one of the promising clean energies with the advantage of abundance (generated through water splitting) and pollution-free emission if used in fuel cell systems. However, some key problems such as finding efficient ways to prod...

  1. Ruthenium(0) nanoclusters stabilized by a Nanozeolite framework: isolable, reusable, and green catalyst for the hydrogenation of neat aromatics under mild conditions with the unprecedented catalytic activity and lifetime.

    Science.gov (United States)

    Zahmakiran, Mehmet; Tonbul, Yalçin; Ozkar, Saim

    2010-05-12

    The hydrogenation of aromatics is a ubiquitous chemical transformation used in both the petrochemical and specialty industry and is important for the generation of clean diesel fuels. Reported herein is the discovery of a superior heterogeneous catalyst, superior in terms of catalytic activity, selectivity, and lifetime in the hydrogenation of aromatics in the solvent-free system under mild conditions (at 25 degrees C and 42 +/- 1 psig initial H(2) pressure). Ruthenium(0) nanoclusters stabilized by a nanozeolite framework as a new catalytic material is reproducibly prepared from the borohydride reduction of a colloidal solution of ruthenium(III)-exchanged nanozeolites at room temperature and characterized by using ICP-OES, XRD, XPS, DLS, TEM, HRTEM, TEM/EDX, mid-IR, far-IR, and Raman spectroscopy. The resultant ruthenium(0) nanoclusters hydrogenate neat benzene to cyclohexane with 100% conversion under mild conditions (at 25 degrees C and 42 +/- 1 psig initial H(2) pressure) with record catalytic activity (initial TOF = 5430 h(-1)) and lifetime (TTO = 177 200). They provide exceptional catalytic activity not only in the hydrogenation of neat benzene but also in the solvent-free hydrogenation of methyl substituted aromatics such as toluene, o-xylene, and mesitylene under otherwise identical conditions. Moreover, they are an isolable, bottleable, and reusable catalyst in the hydrogenation of neat aromatics. When the isolated ruthenium(0) nanoclusters are reused, they retain 92% of their initial catalytic activity even for the third run in the hydrogenation of neat benzene under the same conditions as those of the first run. The work reported here also includes (i) far-infrared spectroscopic investigation of nanozeolite, ruthenium(III)-exchanged-nanozeolite, and ruthenium(0) nanoclusters stabilized by a nanozeolite framework, indicating that the host framework remains intact after the formation of a nanozeolite framework stabilized ruthenium(0) nanoclusters; (ii) the

  2. Catalytic Glycerol Hydrodeoxygenation under Inert Atmosphere: Ethanol as a Hydrogen Donor

    Directory of Open Access Journals (Sweden)

    Efterpi S. Vasiliadou

    2014-12-01

    Full Text Available Glycerol hydrodeoxygenation to 1,2-propanediol (1,2-PDO is a reaction of high interest. However, the need for hydrogen supply is a main drawback of the process. According to the concept investigated here, 1,2-propanediol is efficiently formed using bio-glycerol feedstock with H2 formed in situ via ethanol aqueous phase reforming. Ethanol is thought to be a promising H2 source, as it is alcohol that can be used instead of methanol for transesterification of oils and fats. The H2 generated is consumed in the tandem reaction of glycerol hydrodeoxygenation. The reaction cycle proceeds in liquid phase at 220–250 °C and 1.5–3.5 MPa initial N2 pressure for a 2 and 4-h reaction time. Pt-, Ni- and Cu-based catalysts have been synthesized, characterized and evaluated in the reaction. Among the materials tested, Pt/Fe2O3-Al2O3 exhibited the most promising performance in terms of 1,2-propanediol productivity, while reusability tests showed a stable behavior. Structural integrity and no formation of carbonaceous deposits were verified via Temperature Programmed Desorption of hydrogen (TPD-H2 and thermogravimetric analysis of the fresh and used Pt/FeAl catalyst. A study on the effect of various operating conditions (reaction time, temperature and pressure indicated that in order to maximize 1,2-propanediol productivity and yield, milder reaction conditions should be applied. The highest 1,2-propanediol yield, 53% (1.1 g1,2-PDO gcat−1·h−1, was achieved at a lower reaction temperature of 220 °C.

  3. A compact process for the treatment of olive mill wastewater by combining wet hydrogen peroxide catalytic oxidation and biological techniques

    Energy Technology Data Exchange (ETDEWEB)

    Azabou, Samia [Laboratoire des BioProcedes, Centre de Biotechnologie de Sfax, BP 1177, 3018 Sfax (Tunisia); Najjar, Wahiba [Laboratoire de Chimie des Materiaux et Catalyse, Faculte des Sciences de Tunis, Campus Universitaire, 2092 Tunis (Tunisia); Bouaziz, Mohamed [Laboratoire des BioProcedes, Centre de Biotechnologie de Sfax, BP 1177, 3018 Sfax (Tunisia); Ghorbel, Abdelhamid [Laboratoire de Chimie des Materiaux et Catalyse, Faculte des Sciences de Tunis, Campus Universitaire, 2092 Tunis (Tunisia); Sayadi, Sami, E-mail: sami.sayadi@cbs.rnrt.tn [Laboratoire des BioProcedes, Centre de Biotechnologie de Sfax, BP 1177, 3018 Sfax (Tunisia)

    2010-11-15

    A system based on combined actions of catalytic wet oxidation and microbial technologies for the treatment of highly polluted OMW containing polyphenols was studied. The wet hydrogen peroxide catalytic oxidation (WHPCO) process has been investigated in the semi-batch mode at atmospheric pressure, using aluminium-iron-pillared inter layer clay ((Al-Fe)PILC), under two different catalytic processes: ((Al-Fe)PILC/H{sub 2}O{sub 2}/ultraviolet radiations) at 25 deg. C and ((Al-Fe)PILC/H{sub 2}O{sub 2}) at 50 deg. C. The results show that raw OMW was resistant to the photocatalytic process. However ((Al-Fe)PILC/H{sub 2}O{sub 2}), system operating at 50 deg. C reduced considerably the COD, colour and total phenolic contents, and thus decreased the inhibition of the marine photobacteria Vibrio fischeri luminescence by 70%. This study also examined the feasibility of coupling WHPCO and anaerobic digestion treatment. Biomethanisation experiments performed with raw OMW or pre-treated OMW proved that pre-treatments with ((Al-Fe)PILC/H{sub 2}O{sub 2}) system, for more than 2 h, resulted in higher methane production. Both untreated OMW as well as 2-h pre-treated OMW revealed as toxic to anaerobic bacteria.

  4. A General Catalytic Enantioselective Transfer Hydrogenation Reaction of β,β-Disubstituted Nitroalkenes Promoted by a Simple Organocatalyst.

    Science.gov (United States)

    Bernardi, Luca; Fochi, Mariafrancesca

    2016-01-01

    Given its synthetic relevance, the catalytic enantioselective reduction of β,β-disubstituted nitroalkenes has received a great deal of attention. Several bio-, metal-, and organo-catalytic methods have been developed, which however are usually applicable to single classes of nitroalkene substrates. In this paper, we present an account of our previous work on this transformation, which implemented with new disclosures and mechanistic insights results in a very general protocol for nitroalkene reductions. The proposed methodology is characterized by (i) a remarkably broad scope encompassing various nitroalkene classes; (ii) Hantzsch esters as convenient (on a preparative scale) hydrogen surrogates; (iii) a simple and commercially available thiourea as catalyst; (iv) user-friendly procedures. Overall, the proposed protocol gives a practical dimension to the catalytic enantioselective reduction of β,β-disubstituted nitroalkenes, offering a useful and general platform for the preparation of nitroalkanes bearing a stereogenic center at the β-position in a highly enantioenriched form. A transition state model derived from control kinetic experiments combined with literature data is proposed and discussed. This model accounts and justifies the observed experimental results. PMID:27483233

  5. A compact process for the treatment of olive mill wastewater by combining wet hydrogen peroxide catalytic oxidation and biological techniques

    International Nuclear Information System (INIS)

    A system based on combined actions of catalytic wet oxidation and microbial technologies for the treatment of highly polluted OMW containing polyphenols was studied. The wet hydrogen peroxide catalytic oxidation (WHPCO) process has been investigated in the semi-batch mode at atmospheric pressure, using aluminium-iron-pillared inter layer clay ((Al-Fe)PILC), under two different catalytic processes: ((Al-Fe)PILC/H2O2/ultraviolet radiations) at 25 deg. C and ((Al-Fe)PILC/H2O2) at 50 deg. C. The results show that raw OMW was resistant to the photocatalytic process. However ((Al-Fe)PILC/H2O2), system operating at 50 deg. C reduced considerably the COD, colour and total phenolic contents, and thus decreased the inhibition of the marine photobacteria Vibrio fischeri luminescence by 70%. This study also examined the feasibility of coupling WHPCO and anaerobic digestion treatment. Biomethanisation experiments performed with raw OMW or pre-treated OMW proved that pre-treatments with ((Al-Fe)PILC/H2O2) system, for more than 2 h, resulted in higher methane production. Both untreated OMW as well as 2-h pre-treated OMW revealed as toxic to anaerobic bacteria.

  6. Mapping the Hydrogen Bond Networks in the Catalytic Subunit of Protein Kinase A Using H/D Fractionation Factors.

    Science.gov (United States)

    Li, Geoffrey C; Srivastava, Atul K; Kim, Jonggul; Taylor, Susan S; Veglia, Gianluigi

    2015-07-01

    Protein kinase A is a prototypical phosphoryl transferase, sharing its catalytic core (PKA-C) with the entire kinase family. PKA-C substrate recognition, active site organization, and product release depend on the enzyme's conformational transitions from the open to the closed state, which regulate its allosteric cooperativity. Here, we used equilibrium nuclear magnetic resonance hydrogen/deuterium (H/D) fractionation factors (φ) to probe the changes in the strength of hydrogen bonds within the kinase upon binding the nucleotide and a pseudosubstrate peptide (PKI5-24). We found that the φ values decrease upon binding both ligands, suggesting that the overall hydrogen bond networks in both the small and large lobes of PKA-C become stronger. However, we observed several important exceptions, with residues displaying higher φ values upon ligand binding. Notably, the changes in φ values are not localized near the ligand binding pockets; rather, they are radiated throughout the entire enzyme. We conclude that, upon ligand and pseudosubstrate binding, the hydrogen bond networks undergo extensive reorganization, revealing that the open-to-closed transitions require global rearrangements of the internal forces that stabilize the enzyme's fold. PMID:26030372

  7. Catalytic oxidative desulfurization of diesel utilizing hydrogen peroxide and functionalized-activated carbon in a biphasic diesel-acetonitrile system

    Energy Technology Data Exchange (ETDEWEB)

    Haw, Kok-Giap; Bakar, Wan Azelee Wan Abu; Ali, Rusmidah; Chong, Jiunn-Fat [Department of Chemistry, Faculty of Science, Universiti Teknologi Malaysia, 81310 UTM Skudai, Johor (Malaysia); Kadir, Abdul Aziz Abdul [Department of Petroleum Engineering, Faculty of Chemical and Natural Resources Engineering, Universiti Teknologi Malaysia, 81310 UTM Skudai, Johor (Malaysia)

    2010-09-15

    This paper presents the development of granular functionalized-activated carbon as catalysts in the catalytic oxidative desulfurization (Cat-ODS) of commercial Malaysian diesel using hydrogen peroxide as oxidant. Granular functionalized-activated carbon was prepared from oil palm shell using phosphoric acid activation method and carbonized at 500 C and 700 C for 1 h. The activated carbons were characterized using various analytical techniques to study the chemistry underlying the preparation and calcination treatment. Nitrogen adsorption/desorption isotherms exhibited the characteristic of microporous structure with some contribution of mesopore property. The Fourier Transform Infrared Spectroscopy results showed that higher activation temperature leads to fewer surface functional groups due to thermal decomposition. Micrograph from Field Emission Scanning Electron Microscope showed that activation at 700 C creates orderly and well developed pores. Furthermore, X-ray Diffraction patterns revealed that pyrolysis has converted crystalline cellulose structure of oil palm shell to amorphous carbon structure. The influence of the reaction temperature, the oxidation duration, the solvent, and the oxidant/sulfur molar ratio were examined. The rates of the catalytic oxidative desulfurization reaction were found to increase with the temperature, and H{sub 2}O{sub 2}/S molar ratio. Under the best operating condition for the catalytic oxidative desulfurization: temperature 50 C, atmospheric pressure, 0.5 g activated carbon, 3 mol ratio of hydrogen peroxide to sulfur, 2 mol ratio of acetic acid to sulfur, 3 oxidation cycles with 1 h for each cycle using acetonitrile as extraction solvent, the sulfur content in diesel was reduced from 2189 ppm to 190 ppm with 91.3% of total sulfur removed. (author)

  8. Photo-catalytic hydrogen production over Fe{sub 2}O{sub 3} based catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Boudjemaa, A. [Technical and Scientific Research Centre of Physico-chemistry Analysis (CRAPC), BP 248, RP 16004, Algiers (Algeria); Laboratory of Chemistry of Natural Gas, Faculty of Chemistry (USTHB) BP 32, 16111 Algiers (Algeria); Trari, M. [Laboratory of Storage and Valorization of Renewable Energies, Faculty of Chemistry (USTHB) BP 32, 16111 Algiers (Algeria)

    2010-08-15

    The hydrogen photo-evolution was successfully achieved in aqueous (Fe{sub 1-x}Cr{sub x}){sub 2}O{sub 3} suspensions (0 {<=} x {<=} 1). The solid solution has been prepared by incipient wetness impregnation and characterized by X-ray diffraction, BET, transport properties and photo-electrochemistry. The oxides crystallize in the corundum structure, they exhibit n-type conductivity with activation energy of {proportional_to}0.1 eV and the conduction occurs via adiabatic polaron hops. The characterization of the band edges has been studied by the Mott Schottky plots. The onset potential of the photo-current is {proportional_to}0.2 V cathodic with respect to the flat band potential, implying a small existence of surface states within the gap region. The absorption of visible light promotes electrons into (Fe{sub 1-x}Cr{sub x}){sub 2}O{sub 3}-CB with a potential ({proportional_to}-0.5 V{sub SCE}) sufficient to reduce water into hydrogen. As expected, the quantum yield increases with decreasing the electro affinity through the substitution of iron by the more electropositive chromium which increases the band bending at the interface and favours the charge separation. The generated photo-voltage was sufficient to promote simultaneously H{sub 2}O reduction and SO{sub 3}{sup 2-} oxidation in the energetically downhill reaction (H{sub 2}O + SO{sub 3}{sup 2-} {yields} H{sub 2} + SO{sub 4}{sup 2-}, {delta}G = -17.68 kJ mol{sup -1}). The best activity occurs over Fe{sub 1.2}Cr{sub 0.8}O{sub 3} in SO{sub 3}{sup 2-} (0.1 M) solution with H{sub 2} liberation rate of 21.7 {mu}mol g{sup -1} min{sup -1} and a quantum yield 0.06% under polychromatic light. Over time, a pronounced deceleration occurs, due to the competitive reduction of the end product S{sub 2}O{sub 6}{sup 2-}. (author)

  9. In situ generation of electron acceptor for photoelectrochemical biosensing via hemin-mediated catalytic reaction.

    Science.gov (United States)

    Zang, Yang; Lei, Jianping; Zhang, Lei; Ju, Huangxian

    2014-12-16

    A novel photoelectrochemical sensing strategy is designed for DNA detection on the basis of in situ generation of an electron acceptor via the catalytic reaction of hemin toward H2O2. The photoelectrochemical platform was established by sequential assembly of near-infrared CdTe quantum dots, capture DNA, and a hemin-labeled DNA probe to form a triple-helix molecular beacon (THMB) structure on an indium tin oxide electrode. According to the highly catalytic capacity of hemin toward H2O2, a photoelectrochemical mechanism was then proposed, in which the electron acceptor of O2 was in situ-generated on the electrode surface, leading to the enhancement of the photocurrent response. The utilization of CdTe QDs can extend the absorption edge to the near-infrared band, resulting in an increase in the light-to-electricity efficiency. After introducing target DNA, the THMB structure is disassembled and releases hemin and, thus, quenches the photocurrent. Under optimized conditions, this biosensor shows high sensitivity with a linear range from 1 to 1000 pM and detection limit of 0.8 pM. Moreover, it exhibits good performance of excellent selectivity, high stability, and acceptable fabrication reproducibility. This present strategy opens an alternative avenue for photoelectrochemical signal transduction and expands the applications of hemin-based materials in photoelectrochemical biosensing and clinical diagnosis. PMID:25393151

  10. Catalytic Lignin Valorization Process for the Production of Aromatic Chemicals and Hydrogen

    NARCIS (Netherlands)

    Zakzeski, J.; Jongerius, A.L.; Bruijnincx, P.C.A.; Weckhuysen, B.M.

    2012-01-01

    With dwindling reserves of fossil feedstock as a resource for chemicals production, the fraction of chemicals and energy supplied by alternative, renewable resources, such as lignin, can be expected to increase in the foreseeable future. Here, we demonstrate a catalytic process to valorize lignin (e

  11. Maximizing renewable hydrogen production from biomass in a bio/catalytic refinery

    DEFF Research Database (Denmark)

    Westermann, Peter; Jørgensen, Betina; Lange, L.;

    2007-01-01

    concept is the high versatility with respect to input of different types of biological wastes, which are abundant and cheap residues from agricultural production. Also the concept leaves the opportunity to optimize the microbiological and catalytic processes to meet specific needs for fuel flexibility....

  12. Pyrolysis of de-oiled seed cake of Jatropha Curcas and catalytic steam reforming of pyrolytic bio-oil to hydrogen.

    Science.gov (United States)

    Renny, Andrew; Santhosh, Viswanathan; Somkuwar, Nitin; Gokak, D T; Sharma, Pankaj; Bhargava, Sanjay

    2016-11-01

    The aim of this work was to study the pyrolysis of de-oiled seed cake of Jatropha Curcas and catalytic steam reforming of pyrolytic bio-oil to hydrogen. As per literature, presence of heavy nitrogenous and oxygenated compounds leads to catalyst deactivation. Here, an attempt has been made to tune pyrolytic reactions to optimize the N and O content of the pyrolytic bio-oil. Bio-oil conversion and hydrogen yield decreased as reaction progressed, which attributes to temporary loss of catalytic activity by blockage of catalyst pores by carbon deposition. Further, retention of steam reforming activity after repetitive steam activation suggests long-term catalyst usage. PMID:27566523

  13. Pyrolysis of de-oiled seed cake of Jatropha Curcas and catalytic steam reforming of pyrolytic bio-oil to hydrogen.

    Science.gov (United States)

    Renny, Andrew; Santhosh, Viswanathan; Somkuwar, Nitin; Gokak, D T; Sharma, Pankaj; Bhargava, Sanjay

    2016-11-01

    The aim of this work was to study the pyrolysis of de-oiled seed cake of Jatropha Curcas and catalytic steam reforming of pyrolytic bio-oil to hydrogen. As per literature, presence of heavy nitrogenous and oxygenated compounds leads to catalyst deactivation. Here, an attempt has been made to tune pyrolytic reactions to optimize the N and O content of the pyrolytic bio-oil. Bio-oil conversion and hydrogen yield decreased as reaction progressed, which attributes to temporary loss of catalytic activity by blockage of catalyst pores by carbon deposition. Further, retention of steam reforming activity after repetitive steam activation suggests long-term catalyst usage.

  14. Chemistry and catalysis of coal liquefaction: catalytic and thermal upgrading of coal liquid and hydrogenation of CO to produce fuels. Quarterly progress report, January-March 1980

    Energy Technology Data Exchange (ETDEWEB)

    Wiser, W.H.

    1980-08-01

    Analysis of a group of coal liquids produced by catalytic hydrogenation of Utah coals with ZnCl/sub 2/ catalyst was begun. Carbon-13 nuclear magnetic resonance and liquid chromatography techniques will be used to correlate chemical properties with hydrogenation reactivity. Equipment previously used for downflow measurements of heat and momentum transfer in a gas-coal suspension was modified for upflow measurements. The catalytic hydrodeoxygenation of methyl benzoate has been studied to elucidate the reactions of ester during upgrading of coal-derived liquids. The kinetics of hydrogenation of phenanthrene have also been determined. The catalytic cracking mechanism of octahydroanthracene is reported in detail. Studies of the hydrodesulfurization of thiophene indicate that some thiophene is strongly adsorbed as a hydrogen-deficient polymer on cobalt-molybdate catalyst. Part of the polymer can be desorbed as thiophene by hydrogenation. Poisoning of the catalyst inhibits the hydrosulfurization activity to a greater degree than the hydrogenation activity. Iron-manganese catalysts for carbon monoxide hydrogenation is studied to determine the role of iron carbide formation on selectivity. Pure iron catalyst forms a Hagg iron carbide phase under reaction conditions.

  15. HYDROGEN GENERATION FROM ELECTROLYSIS - REVISED FINAL TECHNICAL REPORT

    Energy Technology Data Exchange (ETDEWEB)

    IBRAHIM, SAMIR; STICHTER, MICHAEL

    2008-07-31

    DOE GO13028-0001 DESCRIPTION/ABSTRACT This report is a summary of the work performed by Teledyne Energy Systems to understand high pressure electrolysis mechanisms, investigate and address safety concerns related to high pressure electrolysis, develop methods to test components and systems of a high pressure electrolyzer, and produce design specifications for a low cost high pressure electrolysis system using lessons learned throughout the project. Included in this report are data on separator materials, electrode materials, structural cell design, and dissolved gas tests. Also included are the results of trade studies for active area, component design analysis, high pressure hydrogen/oxygen reactions, and control systems design. Several key pieces of a high pressure electrolysis system were investigated in this project and the results will be useful in further attempts at high pressure and/or low cost hydrogen generator projects. An important portion of the testing and research performed in this study are the safety issues that are present in a high pressure electrolyzer system and that they can not easily be simplified to a level where units can be manufactured at the cost goals specified, or operated by other than trained personnel in a well safeguarded environment. The two key objectives of the program were to develop a system to supply hydrogen at a rate of at least 10,000 scf/day at a pressure of 5000psi, and to meet cost goals of $600/ kW in production quantities of 10,000/year. On these two points TESI was not successful. The project was halted due to concerns over safety of high pressure gas electrolysis and the associated costs of a system which reduced the safety concerns.

  16. Catalytic Hydrogenation of Methanol-Containing Eflfuent from Epoxidation of Propylene

    Institute of Scientific and Technical Information of China (English)

    Cheng Ke

    2015-01-01

    This paper describes the hydrogenation of impurities in the methanol-containing eflfuent from the propylene epoxidation process with hydrogen peroxide. The effects of reaction temperature, pressure, weight hourly space velocity (WHSV) and H2/methanol ratio on the concentration of various impurities in methanol solvent were investigated. It was found out that the aldehyde, hydrogen peroxide and nitro compounds in the methanol solvent could be completely hydroge-nated over the Ni catalyst under proper reaction conditions. 90%of acetone and up to 50%of acetals (ketals) existing in the methanol solvent could be hydrogenated. No signiifcant change was observed for the rest of the impurities that were present in the methanol solvent (i. e., 1-methoxy-2-propanol, 2-methoxy-1-propanol and 1,2-propanediol). The H2O2 decomposition reaction was enhanced using Ni catalyst, through the formation of NioOH, but no oxygen was found in the off-gas of hy-drogenation reaction since NioH could react on NioOH formed via dissociative adsorption of hydrogen peroxide, or on NioO formed via adsorption of oxygen.

  17. Selective Catalytic Oxidation of Hydrogen Sulfide to Elemental Sulfur from Coal-Derived Fuel Gases

    Energy Technology Data Exchange (ETDEWEB)

    Gardner, Todd H.; Berry, David A.; Lyons, K. David; Beer, Stephen K.; Monahan, Michael J.

    2001-11-06

    The development of low cost, highly efficient, desulfurization technology with integrated sulfur recovery remains a principle barrier issue for Vision 21 integrated gasification combined cycle (IGCC) power generation plants. In this plan, the U. S. Department of Energy will construct ultra-clean, modular, co-production IGCC power plants each with chemical products tailored to meet the demands of specific regional markets. The catalysts employed in these co-production modules, for example water-gas-shift and Fischer-Tropsch catalysts, are readily poisoned by hydrogen sulfide (H{sub 2}S), a sulfur contaminant, present in the coal-derived fuel gases. To prevent poisoning of these catalysts, the removal of H{sub 2}S down to the parts-per-billion level is necessary. Historically, research into the purification of coal-derived fuel gases has focused on dry technologies that offer the prospect of higher combined cycle efficiencies as well as improved thermal integration with co-production modules. Primarily, these concepts rely on a highly selective process separation step to remove low concentrations of H{sub 2}S present in the fuel gases and produce a concentrated stream of sulfur bearing effluent. This effluent must then undergo further processing to be converted to its final form, usually elemental sulfur. Ultimately, desulfurization of coal-derived fuel gases may cost as much as 15% of the total fixed capital investment (Chen et al., 1992). It is, therefore, desirable to develop new technology that can accomplish H{sub 2}S separation and direct conversion to elemental sulfur more efficiently and with a lower initial fixed capital investment.

  18. Noble metal catalyzed hydrogen generation from formic acid in nitrite-containing simulated nuclear waste media

    International Nuclear Information System (INIS)

    The Hanford Waste Vitrification Plant (HWVP) is being designed by the U.S. Department of Energy to immobilize high-level nuclear waste. Simulants for the HWVP feed containing the major nonradioactive components Al, Cd, Fe, Mn, Nd, Ni, Si, Zr, Na, CO32-, NO3- and NO2- were used as media to evaluate the stability of formic acid towards hydrogen evolution by the reaction HCO2H→H2+/CO2 catalyzed by the noble metals Ru, Rh, and/or Pd found in significant quantities in uranium fission products. Small-scale experiments using 40-50 mL of feed simulant in closed glass reactors (250-550 mL total volume) at 80-100 degree C were used to study the effect of nitrite and nitrate ion on the catalytic activities of the noble metals for formic acid decomposition. Reactions were monitored using gas chromatography to analyze the CO2, H2, NO, and N2O in the gas phase as a function of time. Rhodium, which was introduced as soluble RhCl3.3H2O, was found to be the most active catalyst for hydrogen generation from formic acid above nearly 80 degree C in the presence of nitrite ion in accord with earlier observations. The apparent homogeneous nature of the nitrite-promoted Rh-catalyzed formic acid decomposition is consistent with the approximate pseudo-first-order dependence of the hydrogen production rate on Rh concentration. 24 refs., 7 figs., 2 tabs

  19. Investigation of a catalytic gas generator for the Space Shuttle APU. [hydrazine Auxiliary Propulsion Unit

    Science.gov (United States)

    Emmons, D. L.; Huxtable, D. D.; Blevins, D. R.

    1974-01-01

    An investigation was conducted to establish the capability of a monopropellant hydrazine catalytic gas generator to meet the requirements specified for the Space Shuttle APU. Detailed analytical and experimental studies were conducted on potential problem areas including long-term nitriding effects on materials, design variables affecting catalyst life, vehicle vibration effects, and catalyst oxidation/contamination. A full-scale gas generator, designed to operate at a chamber pressure of 750 psia and a flow rate of 0.36 lbm/sec, was fabricated and subjected to three separate life test series. The objective of the first test series was to demonstrate the capability of the gas generator to successfully complete 20 simulated Space Shuttle missions in steady-state operation. The gas generator was then refurbished and subjected to a second series of tests to demonstrate the pulse-mode capability of the gas generator during 20 simulated missions. The third series of tests was conducted with a refurbished reactor to further demonstrate pulse-mode capability with a modified catalyst bed.

  20. Broad Spectrum Photoelectrochemical Diodes for Solar Hydrogen Generation

    Energy Technology Data Exchange (ETDEWEB)

    Grimes, Craig A.

    2014-11-26

    Under program auspices we have investigated material chemistries suitable for the solar generation of hydrogen by water photoelectrolysis. We have built upon, and extended, our knowledge base on the synthesis and application of TiO2 nanotube arrays, a material architecture that appears ideal for water photoelectrolysis. To date we have optimized, refined, and greatly extended synthesis techniques suitable for achieving highly ordered TiO2 nanotube arrays of given length, wall thickness, pore diameter, and tube-to-tube spacing for use in water photoelectrolysis. We have built upon this knowledge based to achieve visible light responsive, photocorrosion stable n-type and p-type ternary oxide nanotube arrays for use in photoelectrochemical diodes.

  1. Photocatalytic Hydrogen Generation by CdSe/CdS Nanoparticles.

    Science.gov (United States)

    Qiu, Fen; Han, Zhiji; Peterson, Jeffrey J; Odoi, Michael Y; Sowers, Kelly L; Krauss, Todd D

    2016-09-14

    The photocatalytic hydrogen (H2) production activity of various CdSe semiconductor nanoparticles was compared including CdSe and CdSe/CdS quantum dots (QDs), CdSe quantum rods (QRs), and CdSe/CdS dot-in-rods (DIRs). With equivalent photons absorbed, the H2 generation activity orders as CdSe QDs ≫ CdSe QRs > CdSe/CdS QDs > CdSe/CdS DIRs, which is surprisingly the opposite of the electron-hole separation efficiency. Calculations of photoexcited surface charge densities are positively correlated with the H2 production rate and suggest the size of the nanoparticle plays a critical role in determining the relative efficiency of H2 production. PMID:27478995

  2. Progress in Catalytic Membrane Reactors for High Purity Hydrogen Production%膜催化反应器及其制氢技术的研究进展

    Institute of Scientific and Technical Information of China (English)

    闫云飞; 张力; 李丽仙; 唐强

    2011-01-01

    As a kind of ideal fuel for fuel cell, hydrogen must be satisfied with the enough high purity. To produce high purity hydrogen at a low cost and large scale method has become a key research focus in the industrialization of fuel-cell technology. The membrane catalytic technology with catalysis and separation dual functions has been developed in recent years, which is a good method to produce high purity hydrogen. Based on the latest developments in the membrane catalytic reaction fields, the advantages, composition and type of membrane catalytic reactor are summarized. The preparation techniques, advantages and classification of inorganic membrane materials are described. Especially, the progress and application for high purity hydrogen production are reviewed in three kinds of catalytic membrane reactors, including oxygen-permeable membrane reactor, hydrogen-permeation membrane reactor and double-membranes reactor. The existing problems of catalytic membrane and membrane catalytic reactor in the industrialization process of hydrogen production using the membrane catalytic technology are also discussed. Additionally, the prospects of membrane catalytic reactors for hydrogen production is proposed.%燃料电池对其理想燃料氢气的纯度要求极高,如何低成本、大规模制取高纯氢气己成为燃料电池技术实现工业化的一个关键问题和研究热点.近年发展起来的兼具催化与分离双重功能的膜催化反应技术是实现制取高纯氢气的一个有效途径.本文结合膜催化反应领域的最新进展,综述了膜催化反应器的优点、组成、类型;介绍了无机膜材料的优点、分类及制备技术;详细综述了透氧膜催化反应器、透氢膜催化反应器及双膜催化反应器在制氢过程中的研究进展和应用,指出了膜催化反应制氢技术在工业化发展过程中存在的问题及应用前景.

  3. H2CAP - Hydrogen assisted catalytic biomass pyrolysis for green fuels

    DEFF Research Database (Denmark)

    Arndal, Trine Marie Hartmann; Høj, Martin; Jensen, Peter Arendt;

    2014-01-01

    Pyrolysis of biomass produces a high yield of condensable oil at moderate temperature and low pressure.This bio-oil has adverse properties such as high oxygen and water contents, high acidity and immiscibility with fossil hydrocarbons. Catalytic hydrodeoxygenation (HDO) is a promising technology...... that can be used to upgrade the crude bio-oil to fuel-grade oil. The development of the HDO process is challenged by rapid catalyst deactivation, instability of the pyrolysis oil, poorly investigated reaction conditions and a high complexity and variability of the input oil composition. However, continuous...... catalytic hydropyrolysis coupled with downstream HDO of the pyrolysis vapors before condensation shows promise (Figure 1). A bench scale experimental setup will be constructed for the continuous conversion of solid biomass (100g /h) to low oxygen, fuel-grade bio-oil. The aim is to provide a proof...

  4. A thermal hydraulic analysis model for catalytic hydrogen recombiners in the containment vessel of a BWR

    Energy Technology Data Exchange (ETDEWEB)

    Fujii, Tadashi; Fujimoto, Kiyoshi [Power and Industrial Systems Rand D Division, Hitachi LTD., HItachi Ibaraki (Japan); Yamanari, Shouzou; Yoshinari, Yasuo

    1999-07-01

    Passive catalytic recombiners have been developed as a safety system to lower flammable gases concentrations in a nuclear power plant accident. Passive catalytic recombiners are of very simple construction and free of active components, which hold the promise of better plant economy, maintainability and reliability. In evaluation of the performance of the recombiners, the clarification of the diffusion and mixing behaviors of flammable gases in the primary containment vessel (PCV) is desirable. The diffusion/mixing behaviors of flammable gases are affected by natural circulation flow induced by the exothermic reaction of the recombiner, forced flow due to the PCV spray and interference by the obstacles in the PCV (such as pipings and components). As an analytical tool to deal with thermal hydraulic behaviors for passive catalytic recombiners, the authors have studied applicability of a three-dimensional analysis code. From the viewpoint of analytical capabilities, the authors selected the STAR-CD code. This paper describes the applicability of the code, including verification analysis and preliminary evaluation for a BWR plant. (author)

  5. Size Control of Iron Oxide Nanoparticles Using Reverse Microemulsion Method: Morphology, Reduction, and Catalytic Activity in CO Hydrogenation

    Directory of Open Access Journals (Sweden)

    Mohammad Reza Housaindokht

    2013-01-01

    Full Text Available Iron oxide nanoparticles were prepared by microemulsion method and evaluated in Fischer-Tropsch synthesis. The precipitation process was performed in a single-phase microemulsion operating region. Different HLB values of surfactant were prepared by mixing of sodium dodecyl sulfate (SDS and Triton X-100. Transmission electron microscopy (TEM, surface area, pore volume, average pore diameter, pore size distribution, and XRD patterns were used to analyze size distribution, shape, and structure of precipitated hematite nanoparticles. Furthermore, temperature programmed reduction (TPR and catalytic activity in CO hydrogenation were implemented to assess the performance of the samples. It was found that methane and CO2 selectivity and also the syngas conversion increased as the HLB value of surfactant decreased. In addition, the selectivity to heavy hydrocarbons and chain growth probability (α decreased by decreasing the catalyst crystal size.

  6. Synthesis and Catalytic Performance of Ni/SiO2 for Hydrogenation of 2-Methylfuran to 2-Methyltetrahydrofuran

    Directory of Open Access Journals (Sweden)

    Fu Ding

    2015-01-01

    Full Text Available A series of Ni/SiO2 catalysts with different Ni content were prepared by sol-gel method for application in the synthesis of 2-methyltetrahydrofuran (2-MTHF by hydrogenation of 2-methylfuran (2-MF. The catalyst structure was investigated by X-ray diffraction (XRD, transmission electron microscopy (TEM, X-ray photoelectron spectroscopy (XPS, and temperature programmed reduction (TPR. It is found that structures and catalytic performance of the catalysts were highly affected by the Ni content. The catalyst with a 25% Ni content had an appropriate size of the Ni species and larger BET surface area and produced a higher 2-MF conversion with enhanced selectivity in 2-MTHF.

  7. Preparation and Characterization of A New Dinuclear Ruthenium Complex with BDPX Ligand and Its Catalytic Hydrogenation Reactions for Cinnamaldehyde

    Institute of Scientific and Technical Information of China (English)

    TANG,Yuan-You(唐元友); LI,Rui-Xiang(李瑞祥); LI,Xian-Jun(李贤均); WONG,Ning-Bew(黄宁表); TIN,Kim-Chung(田金忠); ZHANG,Zhe-Ying(张哲英); MAK,Thomas C.W.(麦松威)

    2004-01-01

    A new anionic dinuclear ruthenium complex bearing 1,2-bis(diphenylphosphinomethyl)benzene (BDPX)[NH2Et2][{RuCl (BDPX)}2(μ-Cl)3] (1) was synthesized and its structure was determined by an X-ray crystallographic analysis. This result indicated that complex 1 consisted of an anion dinuclear BDPX-Ru and a cationic diethylammonium. The crystal belonged to monoclinic system, C2/c space group with a=3.3552(7) nm, b= 1.8448(4)nm, c=2.4265(5) nm, β= 101.89(3)° and Z=8. The catalytic hydrogenation activities and selectivities of complex 1 for cinnamaldehyde were investigated.

  8. Hydrogen production by catalytic decomposition of methane using a Fe-based catalyst in a fluidized bed reactor

    Institute of Scientific and Technical Information of China (English)

    D.Torres; S.de Llobet; J.L.Pinilla; M.J.Lázaro; I.Suelves; R.Moliner

    2012-01-01

    Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work.A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed reactor (FBR).A parametric study of the effects of some process variables,including reaction temperature and space velocity,is undertaken.The operating conditions strongly affect the catalyst performance.Methane conversion was increased by increasing the temperature and lowering the space velocity.Using temperatures between 700 and 900 ℃ and space velocities between 3 and 6 LN/(gcat·h),a methane conversion in the range of 25%-40% for the gas exiting the reactor could be obtained during a 6 h run.In addition,carbon was deposited in the form of nanofilaments (chain like nanofibers and multiwall nanotubes) with similar properties to those obtained in a fixed bed reactor.

  9. Effects of hydrophobic carrier and packing on the mass transfer capabilities in hydrogen-water liquid phase catalytic exchange bed

    International Nuclear Information System (INIS)

    Hydrogen-water liquid phase catalytic exchange bed was packed with 'sandwich' layers of the catalyst and the packing, and the effects of catalyst carrier, inert packing and their filled ratio on the overall mass transfer coefficient (Kya) were investigated experimentally. The results show that C-PTFE is suitable for hydrophobic catalyst. Kya of the bed with catalyst-stainless steel mini-spiral packing is better than that with stainless steel θ-packing, and the active Al2O3 is not suitable for the exchange bed. Moreover, if the stainless steel mini-spiral packing is etched in aqua regia, the operating flexibility and overall mass transfer capability of exchange bed are improved notably. The preferable packing ratio (catalyst/packing) is 1:4. (authors)

  10. Development of a new hydrogen purification system by using hydrogen absorbing alloy for generator cooling; Suiso kyuzo gokin riyo hatsudenkinai suiso jundo kojo system no kaihatsu

    Energy Technology Data Exchange (ETDEWEB)

    Haruki, N.; Sato, J.; Kogi, T.; Nishimura, Y. [Kansai Electric Power Co., Inc., Osaka (Japan); Takeda, H. [Japan Steel works Ltd., Tokyo (Japan)] Fujita, T. [Mitsubishi Electric Corp., Tokyo (Japan)

    1997-05-20

    Hydrogen absorbing alloys have a number of useful functions, such as energy conversion, hydrogen storage and purification. As an application to separation and purification of hydrogen, we have developed a new hydrogen purification system by using a hydrogen absorbing alloy for generator cooling. For demonstration testing with an actual machine, a hydrogen recovery and purification device using 120kg of alloy was manufactured and installed on No.5 turbine-synchronous generator at Himeji No.2 power station. This device is designed to improve the purity of the hydrogen gas in generator containing impurities such as nitrogen and oxygen. The test results tell that the purity of the hydrogen gas in the generator can be enhanced from 98% to 99.9% and maintained at this level under continuous operation. An application of the hydrogen purification system is expected to decrease the generator`s windage loss, resulting higher generator efficiency. 2 refs., 18 figs.

  11. Modeling and Simulation of the Hydrogenation of α-Methylstyrene on Catalytically Active Metal Foams as Tubular Reactor Packing

    Directory of Open Access Journals (Sweden)

    Farzad Lali

    2016-01-01

    Full Text Available This work presents a one-dimensional reactor model for a tubular reactor packed with a catalytically active foam packing with a pore density of 30 PPI in cocurrent upward flow in the example of hydrogenation reaction of α-methylstyrene to cumene. This model includes material, enthalpy, and momentum balances as well as continuity equations. The model was solved within the parameter space applied for experimental studies under assumption of a bubbly flow. The method of orthogonal collocation on finite elements was applied. For isothermal and polytropic processes and steady state conditions, axial profiles for concentration, temperature, fluid velocities, pressure, and liquid holdup were computed and the conversions for various gas and liquid flow rates were validated with experimental results. The obtained results were also compared in terms of space time yield and catalytic activity with experimental results and stirred tank and also with random packed bed reactor. The comparison shows that the application of solid foams as reactor packing is advantageous compared to the monolithic honeycombs and random packed beds.

  12. Improvement of hydrogen isotope exchange reactions on Li4SiO4 ceramic pebble by catalytic metals

    Institute of Scientific and Technical Information of China (English)

    Cheng Jian Xiao; Chun Mei Kang; Xiao Jun Chen; Xiao Ling Gao; Yang Ming Luo; Sheng Hu; Xiao Lin Wang

    2012-01-01

    Li4SiO4 ceramic pebble is considered as a candidate tritium breeding material of Chinese Helium Cooled Solid Breeder Test Blanket Module (CH HCSB TBM) for the International Thermonuclear Experimental Reactor (ITER).In this paper,Li4SiO4 ceramic pebbles deposited with catalytic metals,including Pt,Pd,Ru and Ir,were prepared by wet impregnation method.The metal particles on Li4SiO4 pebble exhibit a good promotion of hydrogen isotope exchange reactions in H2-DzO gas system,with conversion equilibrium temperature reduction of 200-300 ℃.The out-of-pile tritium release experiments were performed using 1.0 wt% Pt/Li4SiO4 and Li4SiO4 pebbles irradiated in a thermal neutron reactor.The thermal desorption spectroscopy shows that Pt was effective to increase the tritium release rate at lower temperatures,and the ratio of tritium molecule (HT) to tritiated water (HTO) of 1.0 wt% Pt/Li4SiO4 was much more than that of Li4SiO4,which released mainly as HTO.Thus,catalytic metals deposited on Li4SiO4 pebble may help to accelerate the recovery of bred tritium particularly in low temperature region,and increase the tritium molecule form released from the tritium breeding materials.

  13. Spark Discharge Generated Nanoparticles for Hydrogen Storage Applications

    NARCIS (Netherlands)

    Vons, V.A.

    2010-01-01

    One of the largest obstacles to the large scale application of hydrogen powered fuel cell vehicles is the absence of hydrogen storage methods suitable for application on-board of these vehicles. Metal hydrides are materials in which hydrogen is reversibly absorbed by one or more metals or combinatio

  14. Selective Catalytic Hydrogenations of Nitriles, Ketones, and Aldehydes by Well-Defined Manganese Pincer Complexes.

    Science.gov (United States)

    Elangovan, Saravanakumar; Topf, Christoph; Fischer, Steffen; Jiao, Haijun; Spannenberg, Anke; Baumann, Wolfgang; Ludwig, Ralf; Junge, Kathrin; Beller, Matthias

    2016-07-20

    Hydrogenations constitute fundamental processes in organic chemistry and allow for atom-efficient and clean functional group transformations. In fact, the selective reduction of nitriles, ketones, and aldehydes with molecular hydrogen permits access to a green synthesis of valuable amines and alcohols. Despite more than a century of developments in homogeneous and heterogeneous catalysis, efforts toward the creation of new useful and broadly applicable catalyst systems are ongoing. Recently, Earth-abundant metals have attracted significant interest in this area. In the present study, we describe for the first time specific molecular-defined manganese complexes that allow for the hydrogenation of various polar functional groups. Under optimal conditions, we achieve good functional group tolerance, and industrially important substrates, e.g., for the flavor and fragrance industry, are selectively reduced. PMID:27219853

  15. Catalytic reduction of nitrate and nitrite ions by hydrogen : investigation of the reaction mechanism over Pd and Pd-Cu catalysts

    NARCIS (Netherlands)

    Ilinitch, OM; Nosova, LV; Gorodetskii, VV; Ivanov, VP; Trukhan, SN; Gribov, EN; Bogdanov, SV; Cuperus, FP

    2000-01-01

    The catalytic behavior of mono- and bimetallic catalysts with Pd and/or Cu supported over gamma-Al2O3 in the reduction of aqueous nitrate and nitrite ions by hydrogen was investigated. The composition of the supported metal catalysts was analysed using secondary ion mass spectroscopy (SIMS) and X-ra

  16. Molybdatophosphoric acid as an efficient catalyst for the catalytic and chemoselective oxidation of sulfides to sulfoxides using urea hydrogen peroxide as a commercially available oxidant

    Directory of Open Access Journals (Sweden)

    ALIREZA HASANINEJAD

    2010-03-01

    Full Text Available An efficient procedure for the chemoselective oxidation of alkyl (aryl sulfides to the corresponding sulfoxides using urea hydrogen peroxide (UHP in the presence of a catalytic amount of molybdatophosphoric acid at room temperature is described. The advantages of described method are: generality, high yield and chemoselectivity, short reaction time, low cost and compliment with green chemistry protocols.

  17. Catalytic enantioselective addition of hydrogen cyanide to benzaldehyde and p-methoxybenzaldehyde using cyclo-His-(αMe)Phe as catalyst

    NARCIS (Netherlands)

    Hulst, Ron; Broxterman, Quirinus B.; Kamphuis, Johan; Formaggio, Fernando; Crisma, Marco; Toniolo, Claudio; Kellogg, Richard M.

    1997-01-01

    Two cyclo-dipeptides based on His and the unnatural (αMe)Phe have been examined as catalysts in the enantioselective addition of hydrogen cyanide to benzaldehyde and p-methoxy-benzaldehyde. The synthesis, catalytic activity and NMR study towards the mechanism of this reaction are presented.

  18. Catalytic enantioselective addition of hydrogen cyanide to benzaldehyde and p-methoxybenzaldehyde using cyclo-His-(alpha-Me)Phe as catalyst

    NARCIS (Netherlands)

    Hulst, R; Broxterman, QB; Kamphuis, J; Formaggio, F; Crisma, M; Toniolo, C; Kellogg, RM

    1997-01-01

    Two cyclo-dipeptides based on His and the unnatural (alpha Me)Phe have been examined as catalysts in the enantioselective addition of hydrogen cyanide to benzaldehyde and p-methoxy-benzaldehyde. The synthesis, catalytic activity and NMR study towards the mechanism of this reaction are presented. (C)

  19. Generation mechanism of hydrogen gas from hardened cement paste by γ-irradiation

    International Nuclear Information System (INIS)

    Hydrogen gas is generated from cementitious waste forms by radiolysis of water. In the case of low level radioactive waste, gas yields have been confirmed to be sufficiently low by irradiation experiments. However, studies have suggested that the hydrogen generation rate in cementitious waste forms is larger than the rate calculated form the g-value (H2 yields for 100eV absorbed). In this paper, the factors that increase the gas generation were investigated quantitatively. Two factors were identified, the effect of an organic diethylene glycol which reacts with hydrogen radicals to produce hydrogen, and the effect of electrons generated in the cementitious matrix which decompose water to hydrogen. The hydrogen generation rate was confirmed to drop less than the rate calculated from the g-value when these factors were eliminated

  20. Justification procedure of hydrogen safety of RU BN compartments as exemplified by steam generator box

    International Nuclear Information System (INIS)

    Basic proposals on completing calculational procedures of sodium cooled reactors hydrogen safety justification, particularly steam generator (SG) box, are presented. It is pointed out that hydrogen appearance in SG box is possible only in accidents with multiple failures. The data presented shows that hydrogen safety and explosion-proofness of fast reactor facility SG box are provided without any special complex and expensive means

  1. Controllable hydrogen generation performance from Al/NaBH4 composite activated by La metal and CoCl2 salt in pure water

    Institute of Scientific and Technical Information of China (English)

    LIU Jianbo; FEI Yong; PAN Hua; FAN Meiqiang; WANG Liangliang; YAO Jun

    2012-01-01

    A novel composition of Al/NaBH4 mixture activated by La and CoCl2 in water for hydrogen generation was investigated.The composition had good stability at 298 K with high La content and low CoCl2 content,but presented good hydrogen generation performance with increasing global temperature.For example,The Al-15 wt.%La-5 wr.%CoCl2/NaBH4 mixture (mass ratio of 1∶1)yielded 1664 ml hydrogen/1 g mixture with 100% efficiency within 60 min at 333 K.The hydrogen generation rate and amount could be regulated by changing composition design,hydrolytic condition,etc.There existed a synergistic effect of La and CoCl2.Increasing La content was helpful to decrease crystal size of the mixture,but its hydrolysis byproduct La(OH)3 deposited on Al surface and had side effect on Al hydrolysis.Increased CoCl2 content was attributed to the producing of more actively catalytic sites Co2B/Al(OH)3 formed in the hydrolytic process.Co2B had dual catalytic effect on Al/NaBH4 hydrolysis.It deposited on Al surface and acted as a cathode of a micro galvanic cell.Co2B/Al(OH)3 was also a good promoter to NaBH4 hydrolysis.Therefore,the Al/NaBH4 mixture activated by La and CoCl2 may be applied as hydrogen generation material and the experimental data lays a foundation for designing practical hydrogen generators.

  2. New Ruthenium Complexes Based on Tetradentate Bipyridine Ligands for Catalytic Hydrogenation of Esters.

    Science.gov (United States)

    Wang, Fangyuan; Tan, Xuefeng; Lv, Hui; Zhang, Xumu

    2016-08-01

    New bipyridinemethanamine-containing tetradentate ligands and their corresponding ruthenium complexes have been synthesized. The synthesized complexes performed well in the hydrogenation of a variety of esters with high efficiency (TON up to 9700) giving alcohols in good yields. PMID:27385062

  3. Non-catalytic plasma-arc reforming of natural gas with carbon dioxide as the oxidizing agent for the production of synthesis gas or hydrogen - HTR2008-58023

    International Nuclear Information System (INIS)

    The world's energy consumption is increasing constantly due to the growing population of the world. The increasing energy consumption has a negative effect on the fossil fuel reserves of the world. Hydrogen has the potential to provide energy for all our needs by making use of fossil fuel such as natural gas and nuclear-based electricity. Hydrogen can be produced by reforming methane with carbon dioxide as the oxidizing agent. Hydrogen can be produced in a Plasma-arc reforming unit making use of the heat energy generated by a 500 MWt Pebble Bed Modular Reactor (PBMR). The reaction in the unit takes place stoichiometrically in the absence of a catalyst. Steam can be added to the feed stream together with the Carbon Dioxide, which make it possible to control the H2/CO ratio in the synthesis gas between 1/1 and 3/1. This ratio of H2/CO in the synthesis gas is suitable to be used as feed gas to almost any chemical and petrochemical process. To increase the hydrogen production further, the Water-Gas Shift Reaction can be applied. A techno-economic analysis was performed on the non-catalytic plasma-arc reforming process. The capital cost of the plant is estimated at $463 million for the production of 1 132 million Nm3/year of hydrogen. The production cost of hydrogen is in the order of $12.81 per GJ depending on the natural gas cost and the price of electricity. (authors)

  4. Catalytic decomposition of methane to COx-free hydrogen and carbon nanotubes over Co–W/MgO catalysts

    Directory of Open Access Journals (Sweden)

    Ahmed E. Awadallah

    2015-09-01

    Full Text Available Bimetallic catalysts containing a series of Co/W at 40/10, 30/20, 20/30 and 10/40 wt% supported on MgO with a total metal content of 50 wt% were prepared and used for the catalytic decomposition of methane to COx-free hydrogen and multi-walled carbon nanotubes (MWCNTs. The solid fresh and exhausted catalysts were characterized structurally and chemically through XRD, TPR, BET, TGA, TEM and Raman spectroscopy. The 40%Co–10%W/MgO catalyst exhibited the highest activity for the production of both hydrogen and MWCNTs. The formation of a large amount of non-interacted Co3O4 species is considered as the main reason for the catalyst superiority in its activity. On the contrary, catalysts formulations of 20%Co–30%W and 10%Co–40%W demonstrated the formation of a large amount of hardly reducible CoWO4 and MgWO4 particles causing lower activity of these catalysts toward methane decomposition as evidenced through the XRD and TPR results.

  5. Catalytic conversion of biomass-derived feedstocks into olefins and aromatics with ZSM-5: the hydrogen to carbon effective ratio

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Huiyan; Cheng, Yu-Ting; Vispute, Tushar; Xiao, R; Huber, George W.

    2011-01-01

    Catalytic conversion of ten biomass-derived feedstocks, i.e.glucose, sorbitol, glycerol, tetrahydrofuran, methanol and different hydrogenated bio-oil fractions, with different hydrogen to carbon effective (H/C{sub eff}) ratios was conducted in a gas-phase flow fixed-bed reactor with a ZSM-5 catalyst. The aromatic + olefin yield increases and the coke yield decreases with increasing H/C{sub eff} ratio of the feed. There is an inflection point at a H/C{sub eff} ratio = 1.2, where the aromatic + olefin yield does not increase as rapidly as it does prior to this point. The ratio of olefins to aromatics also increases with increasing H/C{sub eff} ratio. CO and CO₂ yields go through a maximum with increasing H/C{sub eff} ratio. The deactivation rate of the catalyst decreases significantly with increasing H/C{sub eff} ratio. Coke was formed from both homogeneous and heterogeneous reactions. Thermogravimetric analysis (TGA) for the ten feedstocks showed that the formation of coke from homogeneous reactions decreases with increasing H/C{sub eff} ratio. Feedstocks with a H/C{sub eff} ratio less than 0.15 produce large amounts of undesired coke (more than 12 wt%) from homogeneous decomposition reactions. This paper shows that the conversion of biomass-derived feedstocks into aromatics and olefins using zeolite catalysts can be explained by the H/C{sub eff} ratio of the feed.

  6. Experimental studies on catalytic hydrogen recombiners for light water reactors; Experimentelle Untersuchungen zu katalytischen Wasserstoffkombinatoren fuer Leichtwasserreaktoren

    Energy Technology Data Exchange (ETDEWEB)

    Drinovac, P.

    2006-06-19

    In the course of core melt accidents in nuclear power plants a large amount of hydrogen can be produced and form an explosive or even detonative gas mixture with aerial oxygen in the reactor building. In the containment atmosphere of pressurized water reactors hydrogen combines a phlogistically with the oxygen present to form water vapor even at room temperature. In the past, experimental work conducted at various facilities has contributed little or nothing to an understanding of the operating principles of catalytic recombiners. Hence, the purpose of the present study was to conduct detailed investigations on a section of a recombiner essentially in order to deepen the understanding of reaction kinetics and heat transport processes. The results of the experiments presented in this dissertation form a large data base of measurements which provides an insight into the processes taking place in recombiners. The reaction-kinetic interpretation of the measured data confirms and deepens the diffusion theory - proposed in an earlier study. Thus it is now possible to validate detailed numeric models representing the processes in recombiners. Consequently the present study serves to broaden and corroborate competence in this significant area of reactor technology. In addition, the empirical knowledge thus gained may be used for a critical reassessment of previous numeric model calculations. (orig.)

  7. Sub-10 nm Platinum Nanocrystals with Size and Shape Control: Catalytic Study for Ethylene and Pyrrole Hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Tsung, Chia-Kuang; Kuhn, John N.; Huang, Wenyu; Aliaga, Cesar; Hung, Ling-I; Somorjai, Gabor A.; Yang, Peidong

    2009-03-02

    Platinum nanocubes and nanopolyhedra with tunable size from 5 to 9 nm were synthesized by controlling the reducing rate of metal precursor ions in a one-pot polyol synthesis. A two-stage process is proposed for the simultaneous control of size and shape. In the first stage, the oxidation state of the metal ion precursors determined the nucleation rate and consequently the number of nuclei. The reaction temperature controlled the shape in the second stage by regulation of the growth kinetics. These well-defined nanocrystals were loaded into MCF-17 mesoporous silica for examination of catalytic properties. Pt loadings and dispersions of the supported catalysts were determined by elemental analysis (ICP-MS) and H2 chemisorption isotherms, respectively. Ethylene hydrogenation rates over the Pt nanocrystals were independent of both size and shape and comparable to Pt single crystals. For pyrrole hydrogenation, the nanocubes enhanced ring-opening ability and thus showed a higher selectivity to n-butylamine as compared to nanopolyhedra.

  8. Dependable Hydrogen and Industrial Heat Generation from the Next Generation Nuclear Plant

    Energy Technology Data Exchange (ETDEWEB)

    Charles V. Park; Michael W. Patterson; Vincent C. Maio; Piyush Sabharwall

    2009-03-01

    The Department of Energy is working with industry to develop a next generation, high-temperature gas-cooled nuclear reactor (HTGR) as a part of the effort to supply the US with abundant, clean and secure energy. The Next Generation Nuclear Plant (NGNP) project, led by the Idaho National Laboratory, will demonstrate the ability of the HTGR to generate hydrogen, electricity, and high-quality process heat for a wide range of industrial applications. Substituting HTGR power for traditional fossil fuel resources reduces the cost and supply vulnerability of natural gas and oil, and reduces or eliminates greenhouse gas emissions. As authorized by the Energy Policy Act of 2005, industry leaders are developing designs for the construction of a commercial prototype producing up to 600 MWt of power by 2021. This paper describes a variety of critical applications that are appropriate for the HTGR with an emphasis placed on applications requiring a clean and reliable source of hydrogen. An overview of the NGNP project status and its significant technology development efforts are also presented.

  9. Electrospun polyacrylonitrile nanofibers supported Ag/Pd nanoparticles for hydrogen generation from the hydrolysis of ammonia borane

    Science.gov (United States)

    Tong, Yan; Lu, Xiaofeng; Sun, Weining; Nie, Guangdi; Yang, Liu; Wang, Ce

    2014-09-01

    A high-performance hydrogen generation system based on the electrospun polyacrylonitrile (PAN)/Ag/Pd composite nanofibers, which were prepared by microwave reducing the electrospun PAN/AgNO3 nanofibers and followed by a replacement reaction has been demonstrated. The morphology of the as-prepared PAN/Ag/Pd composite nanofibers and the metal nanoparticles on the fibers were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution TEM (HRTEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) measurements. It has been demonstrated that the obtained PAN/Ag/Pd composite nanofibers possess fine morphology and high catalytic activities for H2 generation from aqueous solution of ammonia borane (NH3BH3, AB). The H2 generation test exhibited that the catalyst had excellent catalytic activity (with turnover frequency (TOF) of 377.2 mol H2 h-1 (mol Pd)-1), good recycle stability and easy-separation from the reaction system. This new kind of nanofibers possesses great potential application for the new clean energy development.

  10. Hydrogen Plasma Generation with 200 MHz RF Ion Source

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jeongtae; Park, Kwangmook; Seo, Dong Hyuk; Kim, Han-Sung; Kwon, Hyeok-Jung; Cho, Yong-Sub [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2014-10-15

    The ion source for the system is required to be rugged with 2000 hours maintenance free operation time because it is installed in the vessel filled with SF6 gas at the pressure of 10 bar. A 200 MHz RF ion source is considered as an ion source. It is a simple construction and provides long life operation. The specifications of the ion source are 5 kV extraction voltage and 1 mA beam current referenced to the proton. RF ion source has been developed and undergone a performance test. Results of the test are presented. 200 MHz RF ion source is designated and manufactured. First of all test stand test of ion source are set up for a performance test of ion source. It includes a RF ion source, a 200-MHz RF system, beam extraction system, vacuum system, beam extraction system, and beam diagnostic system. At pressure of 1.2E-5 torr, hydrogen plasma is generated with net RF power 70 W. Pyrex tube surrounded by an inductive coil takes the role of vessel and discharge is enhanced with field of permanent magnets.

  11. Integrated photoelectrochemical energy storage: solar hydrogen generation and supercapacitor.

    Science.gov (United States)

    Xia, Xinhui; Luo, Jingshan; Zeng, Zhiyuan; Guan, Cao; Zhang, Yongqi; Tu, Jiangping; Zhang, Hua; Fan, Hong Jin

    2012-01-01

    Current solar energy harvest and storage are so far realized by independent technologies (such as solar cell and batteries), by which only a fraction of solar energy is utilized. It is highly desirable to improve the utilization efficiency of solar energy. Here, we construct an integrated photoelectrochemical device with simultaneous supercapacitor and hydrogen evolution functions based on TiO(2)/transition metal hydroxides/oxides core/shell nanorod arrays. The feasibility of solar-driven pseudocapacitance is clearly demonstrated, and the charge/discharge is indicated by reversible color changes (photochromism). In such an integrated device, the photogenerated electrons are utilized for H(2) generation and holes for pseudocapacitive charging, so that both the reductive and oxidative energies are captured and converted. Specific capacitances of 482 F g(-1) at 0.5 A g(-1) and 287 F g(-1) at 1 A g(-1) are obtained with TiO(2)/Ni(OH)(2) nanorod arrays. This study provides a new research strategy for integrated pseudocapacitor and solar energy application.

  12. Numerical study of methanol–steam reforming and methanol–air catalytic combustion in annulus reactors for hydrogen production

    International Nuclear Information System (INIS)

    Highlights: ► Performance of mini-scale integrated annulus reactors for hydrogen production. ► Flow rates fed to combustor and reformer control the reactor performance. ► Optimum performance is found from balance of flow rates to combustor and reformer. ► Better performance can be found when shell side is designed as combustor. -- Abstract: This study presents the numerical simulation on the performance of mini-scale reactors for hydrogen production coupled with liquid methanol/water vaporizer, methanol/steam reformer, and methanol/air catalytic combustor. These reactors are designed similar to tube-and-shell heat exchangers. The combustor for heat supply is arranged as the tube or shell side. Based on the obtained results, the methanol/air flow rate through the combustor (in terms of gas hourly space velocity of combustor, GHSV-C) and the methanol/water feed rate to the reformer (in terms of gas hourly space velocity of reformer, GHSV-R) control the reactor performance. With higher GHSV-C and lower GHSV-R, higher methanol conversion can be achieved because of higher reaction temperature. However, hydrogen yield is reduced and the carbon monoxide concentration is increased due to the reversed water gas shift reaction. Optimum reactor performance is found using the balance between GHSV-C and GHSV-R. Because of more effective heat transfer characteristics in the vaporizer, it is found that the reactor with combustor arranged as the shell side has better performance compared with the reactor design having the combustor as the tube side under the same operating conditions.

  13. Effect of Catalytic Cylinders on Autothermal Reforming of Methane for Hydrogen Production in a Microchamber Reactor

    OpenAIRE

    Yunfei Yan; Hongliang Guo; Li Zhang; Junchen Zhu; Zhongqing Yang; Qiang Tang; Xin Ji

    2014-01-01

    A new multicylinder microchamber reactor is designed on autothermal reforming of methane for hydrogen production, and its performance and thermal behavior, that is, based on the reaction mechanism, is numerically investigated by varying the cylinder radius, cylinder spacing, and cylinder layout. The results show that larger cylinder radius can promote reforming reaction; the mass fraction of methane decreased from 26% to 21% with cylinder radius from 0.25 mm to 0.75 mm; compact cylinder spaci...

  14. Development of New Chiral Bicyclic Ligands : Applications in Catalytic Asymmetric Transfer Hydrogenation, Epoxidations, and Epoxide Rearrangements

    OpenAIRE

    Gayet, Arnaud

    2005-01-01

    This thesis describes the synthesis and application of new chiral bicyclic ligands and their application in asymmetric catalysis. The studies involved: [i] The development of novel chiral bicyclic amino sulfur ligands and their use in transfer hydrogenation. [ii] The development of the kinetic resolution of racemic epoxide through the use of chiral lithium amides. [iii] The synthesis and application of chiral bicyclic amine in the organocatalysed epoxidation of alkenes. [iv] Development and a...

  15. Polyacrylonitrile Fibers Anchored Cobalt/Graphene Sheet Nanocomposite: A Low-Cost, High-Performance and Reusable Catalyst for Hydrogen Generation.

    Science.gov (United States)

    Zhang, Fei; Huang, Guoji; Hou, Chengyi; Wang, Hongzhi; Zhang, Qinghong; Li, Yaogang

    2016-06-01

    Cobalt and its composites are known to be active and inexpensive catalysts in sodium borohydride (NaBH4) hydrolysis to generate clean and renewable hydrogen energy. A novel fiber catalyst, cobalt/graphene sheet nanocomposite anchored on polyacrylonitrile fibers (Co/GRs-PANFs), which can be easily recycled and used in any reactor with different shapes, were synthesized by anchoring cobalt/graphene (Co/GRs) on polyacrylonitrile fibers coated with graphene (GRs-PANFs) at low temperature. The unique structure design effectively prevents the inter-sheet restacking of Co/GRs and fully exploits the large surface area of novel hybrid material for generate hydrogen. And the extra electron transfer path supplied by GRs on the surface of GRs-PANFs can also enhance their catalysis performances. The catalytic activity of the catalyst was investigated by the hydrolysis of NaBH4 in aqueous solution with GRs-PANFs. GRs powders and Co powders were used as control groups. It was found that both GRs and fiber contributed to the hydrogen generation rate of Co/GRs-PANFs (3222 mL x min(-1) x g(-1)), which is much higher than that of cobalt powders (915 mL x min(-1) x g(-1)) and Co/GRs (995 mL x min(-1) x g(-1)). The improved hydrogen generation rate, low cost and uncomplicated recycling make the Co/GRs-PANFs promising candidate as catalysts for hydrogen generation. PMID:27427607

  16. Lipocalin 2 alleviates iron toxicity by facilitating hypoferremia of inflammation and limiting catalytic iron generation.

    Science.gov (United States)

    Xiao, Xia; Yeoh, Beng San; Saha, Piu; Olvera, Rodrigo Aguilera; Singh, Vishal; Vijay-Kumar, Matam

    2016-06-01

    Iron is an essential transition metal ion for virtually all aerobic organisms, yet its dysregulation (iron overload or anemia) is a harbinger of many pathologic conditions. Hence, iron homeostasis is tightly regulated to prevent the generation of catalytic iron (CI) which can damage cellular biomolecules. In this study, we investigated the role of iron-binding/trafficking innate immune protein, lipocalin 2 (Lcn2, aka siderocalin) on iron and CI homeostasis using Lcn2 knockout (KO) mice and their WT littermates. Administration of iron either systemically or via dietary intake strikingly upregulated Lcn2 in the serum, urine, feces, and liver of WT mice. However, similarly-treated Lcn2KO mice displayed elevated CI, augmented lipid peroxidation and other indices of organ damage markers, implicating that Lcn2 responses may be protective against iron-induced toxicity. Herein, we also show a negative association between serum Lcn2 and CI in the murine model of dextran sodium sulfate (DSS)-induced colitis. The inability of DSS-treated Lcn2KO mice to elicit hypoferremic response to acute colitis, implicates the involvement of Lcn2 in iron homeostasis during inflammation. Using bone marrow chimeras, we further show that Lcn2 derived from both immune and non-immune cells participates in CI regulation. Remarkably, exogenous rec-Lcn2 supplementation suppressed CI levels in Lcn2KO serum and urine. Collectively, our results suggest that Lcn2 may facilitate hypoferremia, suppress CI generation and prevent iron-mediated adverse effects. PMID:27007712

  17. Biomedical and Forensic Applications of Combined Catalytic Hydrogenation-Stable Isotope Ratio Analysis

    Directory of Open Access Journals (Sweden)

    Mark A. Sephton

    2007-01-01

    Full Text Available Studies of biological molecules such as fatty acids and the steroid hormones have the potential to benefit enormously from stable carbon isotope ratio measurements of individual molecules. In their natural form, however, the body’s molecules interact too readily with laboratory equipment designed to separate them for accurate measurements to be made.Some methods overcome this problem by adding carbon to the target molecule, but this can irreversibly overprint the carbon source ‘signal’. Hydropyrolysis is a newly-applied catalytic technique that delicately strips molecules of their functional groups but retains their carbon skeletons and stereochemistries intact, allowing precise determination of the carbon source. By solving analytical problems, the new technique is increasing the ability of scientists to pinpoint molecular indicators of disease, elucidate metabolic pathways and recognise administered substances in forensic investigations.

  18. CFD simulation of hydrogen mixing and mitigation by means of passive auto-catalytic recombiners

    Energy Technology Data Exchange (ETDEWEB)

    Kelm, S.; Reinecke, E-A.; Jahn, W., E-mail: s.kelm@fz-juelich.de [Forschungszentrum Juelich GmbH, Juelich (Germany); Allelein, H-J. [RWTH Aachen Univ.. Aachen (Germany)

    2011-07-01

    Modeling of passive auto-catalytic recombiners (PARs) operation in containment geometries involves a large variety of scales; thus, a CFD calculation resolving all these scales would be much too expensive. Therefore, the mechanistic PAR model REKO-DIREKT, developed at Forschungszentrum Juelich, has been coupled with the commercial CFD code ANSYS CFX in order to simulate PAR operation as well as the induced flow and transport phenomena. Based on a short introduction of REKO-DIREKT, its interface to CFX and the explicit coupling scheme is discussed. The paper is finalized by a first demonstration of simulation capabilities on the basis of the ThAI PAR-4 experiment (Becker Technologies GmbH, Eschborn, Germany). (author)

  19. Construction and biofunctional evaluation of electrospun vascular graft loaded with selenocystamine for in situ catalytic generation of nitric oxide

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Siyuan; An, Jun; Weng, Lei [State Key Laboratory of Medicinal Chemical Biology, Key Laboratory of Bioactive Materials for Ministry of Education, College of Life Sciences, Nankai University, Tianjin 300071 (China); Li, Yandong [Institute of Polymer Chemistry, College of Chemistry, Nankai University, Tianjin 300071 (China); Xu, Han; Wang, Yaping; Ding, Dan; Kong, Deling [State Key Laboratory of Medicinal Chemical Biology, Key Laboratory of Bioactive Materials for Ministry of Education, College of Life Sciences, Nankai University, Tianjin 300071 (China); Wang, Shufang, E-mail: wangshufang@nankai.edu.cn [State Key Laboratory of Medicinal Chemical Biology, Key Laboratory of Bioactive Materials for Ministry of Education, College of Life Sciences, Nankai University, Tianjin 300071 (China)

    2014-12-01

    Construction and biofunctional evaluation of a novel vascular graft with in situ catalytic generation of nitric oxide were described in this paper. Poly α-lysine and poly (γ-glutamic acid) were deposited alternately onto the surface of an electrospun poly ε-caprolactone matrix via electrostatic layer-by-layer self-assembly, and then selenocystamine was loaded as a catalyst. Measurement of in vitro catalytic generation of nitric oxide demonstrated that this catalyst-loaded material could considerably accelerate the release of nitric oxide from S-nitrosoglutathione. A fibroblast proliferation assay showed that the material possessed satisfactory cellular compatibility. The catalyst-loaded material could inhibit the spread of smooth muscle cells in the presence of nitric oxide donors. In arteriovenous-shunt experiment, the catalyst-loaded graft exhibited good anti-thrombotic property where it could prevent acute thrombosis by decreasing the adhesion and activation of platelets and other blood cells. These data suggest a new method of building vascular grafts with improved hemocompatibility and biological functions. - Highlights: • A porous small-diameter vascular graft was prepared by electrospinning. • Selenocystamine was loaded for in situ catalytic and sustained NO generation. • There was a significant catalytic NO generation on the catalyst-loaded sample. • The spread of smooth muscle cells was inhibited on the catalyst-loaded sample. • The catalyst-loaded sample showed anti-thrombotic property in AV-shunt experiment.

  20. Effective hydrogen generation and resource circulation based on sulfur cycle system

    Energy Technology Data Exchange (ETDEWEB)

    Takahashi, Hideyuki; Mabuchi, Takashi; Hayashi, Tsugumi; Yokoyama, Shun; Tohji, Kazuyuki [Graduate School of Environmental Studies, Tohoku University 6-6-20, Aramaki, Aoba-ku, Sendai, 980-8579 (Japan)

    2013-12-10

    For the effective hydrogen generation from H{sub 2}S, it should be compatible that the increscent of the photocatalytic (or electrochemical) activities and the development of effective utilization method of by-products (poly sulfide ion). In this study, “system integration” to construct the sulfur cycle system, which is compatible with the increscent of the hydrogen and or electron energy generation ratio and resource circulation, is investigated. Photocatalytic hydrogen generation rate can be enhanced by using stratified photocatalysts. Photo excited electron can be transpired to electrode to convert the electron energy to hydrogen energy. Poly sulfide ion as the by-products can be transferred into elemental sulfur and/or industrial materials such as rubber. Moreover, elemental sulfur can be transferred into H{sub 2}S which is the original materials for hydrogen generation. By using this “system integration”, the sulfur cycle system for the new energy generation can be constructed.

  1. Production of activated carbon and its catalytic application for oxidation of hydrogen sulphide

    Science.gov (United States)

    Azargohar, Ramin

    Hydrogen sulphide is an environmentally hazardous gas which is present in many gas streams associated with oil and gas industry. Oxidation of H 2S to sulphur in air produces no bulky or waste material and requires no further purification. Activated carbon is known as a catalyst for this reaction. In this research, a coal-based precursor (luscar char) and a biomass-based precursor (biochar) were used for production of activated carbons by two common methods of activation: physical and chemical activation in which steam and potassium hydroxide (KOH), respectively, were used. Experiments were designed by the statistical central composite design method. Two models were developed for the BET surface area and reaction yield of each activation process. These models showed the effects of operating conditions, such as activation temperature, mass ratio of activating agent to precursor, activation time, and nitrogen flowrate on the BET surface area and reaction yield for each activation method for each precursor. The optimum operating conditions were calculated using these models to produce activated carbons with relatively large BET surface area (> 500 m2/g) and high reaction yield (> 50 wt %). The BET surface area and reaction yield for activated carbons produced at optimum operating conditions showed maximum 7 and 7.4% difference, respectively, comparing to the values predicted by models. The activated carbons produced at optimum operating conditions were used as the base catalysts for the direct oxidation of 1 mol % hydrogen sulphide in nitrogen to sulphur at the temperature range of 160-205°C and pressure of 700 kPa. Originally activated carbons showed a good potential for oxidation of hydrogen sulphide by their selectivity for sulphur product and low amount of sulphur dioxide production. To improve the performance of steam-activated carbons, the catalysts were modified by acid-treatment followed by thermal desorption. This method increased the break-through times for

  2. Catalytic asymmetric synthesis of a tertiary benzylic carbon center via phenol-directed alkene hydrogenation.

    Science.gov (United States)

    Caille, Seb; Crockett, Rich; Ranganathan, Krishnakumar; Wang, Xiang; Woo, Jacqueline C S; Walker, Shawn D

    2011-07-01

    An expeditious synthetic approach to chiral phenol 1, a key building block in the preparation of a series of drug candidates, is reported. The strategy includes a cost-effective and readily scalable route to cyclopentanone 3 from isobutyronitrile (10). The sterically hindered and enolizable ketone 3 was subsequently employed in a challenging Grignard addition mediated by LaCl(3)·2LiCl. A novel preparation of the lanthanide reagent required for this transformation is described. To complete the process, a highly enantioselective hydrogenation step afforded the target (1). The importance of the phenol group to the success of this asymmetric transformation is discussed. PMID:21630712

  3. Preparation and catalytic performance of monolayer-dispersed Pd/Ni bimetallic catalysts for hydrogenation

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    Pd/Ni bimetallic catalysts were prepared by replacement reactions,characterized by X-ray diffraction,CO chemisorption and H2 temperature-programmed desorption,and evaluated for hydrogenation of cyclohexene,styrene and acetone.The results show that Pd atoms are monolayer-dispersed on the Ni surface in these Pd/Ni catalysts.Consequently,Pd/Ni catalysts are much more active than Pd/Ni and Pd/γ-Al2O3 with the same Pd loading prepared by the conventional impregnation method.

  4. Method of generating hydrogen-storing hydride complexes

    Science.gov (United States)

    Srinivasan, Sesha S; Niemann, Michael U; Goswami, D. Yogi; Stefanakos, Elias K

    2013-05-14

    A ternary hydrogen storage system having a constant stoichiometric molar ratio of LiNH.sub.2:MgH.sub.2:LiBH.sub.4 of 2:1:1. It was found that the incorporation of MgH.sub.2 particles of approximately 10 nm to 20 nm exhibit a lower initial hydrogen release temperature of 150.degree. C. Furthermore, it is observed that the particle size of LiBNH quaternary hydride has a significant effect on the hydrogen sorption concentration with an optimum size of 28 nm. The as-synthesized hydrides exhibit two main hydrogen release temperatures, one around 160.degree. C. and the other around 300.degree. C., with the main hydrogen release temperature reduced from 310.degree. C. to 270.degree. C., while hydrogen is first reversibly released at temperatures as low as 150.degree. C. with a total hydrogen capacity of 6 wt. % to 8 wt. %. Detailed thermal, capacity, structural and microstructural properties have been demonstrated and correlated with the activation energies of these materials.

  5. Carbon-based catalysts:Opening new scenario to develop next-generation nano-engineered catalytic materials

    Institute of Scientific and Technical Information of China (English)

    Claudio Ampelli; Siglinda Perathoner; Gabriele Centi

    2014-01-01

    This essay analyses some of the recent development in nanocarbons (carbon materials having a defined and controlled nano-scale dimension and functional properties which strongly depend on their nano-scale features and architecture), with reference to their use as advanced catalytic materials. It is remarked how their features open new possibilities for catalysis and that they represent a new class of catalytic materials. Although carbon is used from long time in catalysis as support and electrocatalytic applications, nanocarbons offer unconventional ways for their utilization and to address some of the new challenges deriving from moving to a more sustainable future. This essay comments how nanocarbons are a key element to develop next-generation catalytic materials, but remarking that this goal requires overcoming some of the actual limits in current research. Some aspects are discussed to give a glimpse on new directions and needs for R&D to progress in this direction.

  6. Ammonia Decomposition for Hydrogen Production in Catalytic Microchannels with Slip/Jump Effects

    Directory of Open Access Journals (Sweden)

    Azad Qazi Zade

    2015-01-01

    Full Text Available The rarefaction effects on the catalytic decomposition of NH3 in ruthenium–coated planar microchannels is numerically simulated in the Knudsen number range 0.015-0.03. A colocated finite–volume method is used to solve the governing equations. A concentration jump model derived from the kinetic theory of gases is employed to account for the concentration discontinuity at the reactive walls. A detailed surface reaction mechanism for ammonia decomposition on ruthenium along with a multi-component species diffusion model are used to study the effects of concentration jump coupled with velocity slip and temperature jump on the walls. The velocity-slip, temperature-jump and concentration-jump boundary conditions have miscellaneous effects on flow, temperature and species concentration fields. The results suggest that the velocity-slip boundary condition only slightly influences the species distribution at the edge of the Knudsen layer as well as inside the channel, while the temperature-jump boundary condition affects the heat and mass transfer characteristics the most. The concentration-jump effect, on the other hand, can counter balance the temperature-jump effects in some cases.

  7. Empirical rate equation model of hydrogen generation for Hanford tank waste

    International Nuclear Information System (INIS)

    Hydrogen is the major flammable gas produced from radioactive tank waste at the Hanford Site. Understanding gas generation and the ability to predict the gas generation rates are important for controlling the flammable gas hazard during interim storage and for planning for future activities such as waste transfer, retrieval, and treatment. Several models have been previously proposed to estimate the hydrogen generation rate but were limited by very little waste data. In this work, based on the availability of a large body of tank waste data, empirical rate equation models are developed and validated to simulate the hydrogen generation from thermal chemical reactions, water and organic radiolysis, and corrosion processes

  8. Continuous hydrogen generation from formic acid; Kontinuierliche Wasserstofferzeugung aus Ameisensaeure

    Energy Technology Data Exchange (ETDEWEB)

    Sponholz, Peter; Mellmann, Doerthe; Boddien, Albert; Gaertner, Felix; Junge, Henrik; Beller, Matthias [Rostock Univ. (Germany). Leibniz-Institut fuer Katalyse e.V.

    2011-07-01

    One of the biggest challenges in this century will be the sustainable supply of energy. A major goal is to meet the energy demand without using fossil fuels and to integrate renewable energy into the energy economy. For applications storage systems for hydrogen are needed. One possible storage system for hydrogen is formic acid which is liquid, non-toxic and has a gravimetric hydrogen content of 4.4%. Our aim is to continuously dehydrogenize formic acid and to use the gas mixture (H{sub 2}, CO{sub 2}) in a connected fuel cell. (orig.)

  9. Hydrogen generation systems utilizing sodium silicide and sodium silica gel materials

    Science.gov (United States)

    Wallace, Andrew P.; Melack, John M.; Lefenfeld, Michael

    2015-07-14

    Systems, devices, and methods combine reactant materials and aqueous solutions to generate hydrogen. The reactant materials can sodium silicide or sodium silica gel. The hydrogen generation devices are used in fuels cells and other industrial applications. One system combines cooling, pumping, water storage, and other devices to sense and control reactions between reactant materials and aqueous solutions to generate hydrogen. Multiple inlets of varied placement geometries deliver aqueous solution to the reaction. The reactant materials and aqueous solution are churned to control the state of the reaction. The aqueous solution can be recycled and returned to the reaction. One system operates over a range of temperatures and pressures and includes a hydrogen separator, a heat removal mechanism, and state of reaction control devices. The systems, devices, and methods of generating hydrogen provide thermally stable solids, near-instant reaction with the aqueous solutions, and a non-toxic liquid by-product.

  10. Hydrogen Production by Thermo-catalytic Decomposition of Natural Gas: Carbonaceous Catalysts

    International Nuclear Information System (INIS)

    TCD of CH4 using different kinds of carbon catalyst, activated carbons (AC) and carbon blacks (CB) have been studied. AC showed an acceptable initial reaction rate but they become rapidly deactivated, while CB with high surface area provided more stable and sustainable hydrogen production. Regeneration of the carbonaceous catalysts after deactivation, using CO2 as activating agent has been studied. A commercial active carbon has been selected for the regeneration tests. The optimum operation conditions for the catalysts regeneration have been studied, attending to the burn off of the catalysts during the regeneration, which is important for the self-consistence of the process, and the recovering in the surface area, which is one of the most important factors affecting the activity of these catalysts. (authors)

  11. Catalytic performance of Fe modified K/Mo2C catalyst for CO hydrogenation

    Institute of Scientific and Technical Information of China (English)

    Minglin Xiang; Dudu Wu; Juan Zou; Debao Li; Yuhan Sun; Xichun She

    2011-01-01

    Fe modified and un-modified K/Mo2C were prepared and investigated as catalysts for CO hydrogenation reaction.Compared with K/Mo2C catalyst,the addition of Fe increased the production of alcohols,especially the C2+OH.Meanwhile,considerable amounts of C5+ hydrocarbons and C=2-C=4 were formed,whereas methane selectivity greatly decreased.Also,the activity and selectivity of the catalyst were readily affected by the reaction pressure and temperature employed.According to the XPS results,Mo4+ might be responsible for the production of alcohols,whereas the low valence state of Mo species such as Moo and/or Mo2+ might be account for the high activity and selectivity toward hydrocarbons.

  12. General Tritium Labelling of Gentamicin C by catalytic hydrogen exchange Reaction with Tritiated Water

    International Nuclear Information System (INIS)

    Gentamicin C was labelled with tritium by means of a PtO2 catalyzed hydrogen exchange reaction. Under the conditions of the exchange (100 mg of gentamicin, basic form, 0,3 ml H2O-3H, and 50 mg of prereduced PtO2) the radiochemical yield was 0,24, 0,38 and 0,48 % at 120 degree celsius, for 8, 16 and 24 hours respectively. Chemical yield for purified gentamicin was about 60 %. Purification was accomplished with a cellulose column eluted with the lower phase of chloroform-methanol 17 % ammonium hydroxide (2:1:1, v/v) . Chemical purity, determined by HPLC, was 96,5 % and radiochemical one was 95. Main exchange degradation products show biological activity. (Author) 12 refs

  13. Hydrogen Generator by Methane Pyrolysis with Carbon Capture Project

    Data.gov (United States)

    National Aeronautics and Space Administration — ORBITEC proposes to develop, fabricate, and test a system to provide 99.999% hydrogen by efficiently performing methane pyrolysis. The system has three unique...

  14. NaBH4 generator integrated with energy conversion device based on hydrogen combustion

    Science.gov (United States)

    Netskina, O. V.; Fursenko, R. V.; Komova, O. V.; Odintsov, E. S.; Simagina, V. I.

    2015-01-01

    A thermoelectric energy conversion device operating on the heat generated by a hydrogen diffusion microflame has been developed. For the first time, a NaBH4 hydrogen generator has been employed as a source of fuel for such type of power generator. A 1%Ru-3%Co/Sibunit catalyst ensures hydrogen generation at a rate of 3 cm3 s-1 during 3 h. Power and efficiency characteristics of the integrated system consisting of a hydrogen generator and an energy converter based on combustion technologies have been studied experimentally. The total efficiency and the generated power of the system were measured to achieve values of up to 1.23% and 0.25 W, respectively. Ways to further improve the system's power output and efficiency characteristics have been discussed.

  15. A flameless catalytic combustion-based thermoelectric generator for powering electronic instruments on gas pipelines

    International Nuclear Information System (INIS)

    Highlights: ► MPPT is used to improve the feature that TEG output is sensitive to load variation. ► The improved feature makes TEG suitable to power electronic device on gas pipeline. ► Test shows heat transfer uniformity plays an important role in improving TEG output. ► It can get an optimized TEG by uniformly filling a thermal insulation material. - Abstract: This paper presents a flameless catalytic combustion-based thermoelectric power generator that uses commercial thermoelectric modules. The structure of the thermoelectric generator (TEG) is introduced and the power performance is measured based on a designed circuit system. The open circuit voltage of the TEG is about 7.3 V. The maximum power output can reach up to 6.5 W when the load resistance matches the TEG internal resistance. However, the system output is sensitive to load variation. To improve this characteristic, maximum power point tracking technique is used and results in an open circuit voltage of 13.8 V. The improved characteristic makes the TEG system a good charger to keep the lead acid battery fully charged so as to meet the needs of electronic instruments on gas pipelines. In addition, the combustion features have been investigated based on the temperature measurement. Test results show that the uniformity of combustion heat transfer process and the combustion chamber structure play important roles in improving system power output. It can get an optimized TEG system (maximum power output: 8.3 W) by uniformly filling a thermal insulation material (asbestos) to avoid a non-uniform combustion heat transfer process

  16. Selective Electrochemical Generation of Hydrogen Peroxide from Water Oxidation.

    Science.gov (United States)

    Viswanathan, Venkatasubramanian; Hansen, Heine A; Nørskov, Jens K

    2015-11-01

    Water is a life-giving source, fundamental to human existence, yet over a billion people lack access to clean drinking water. The present techniques for water treatment such as piped, treated water rely on time and resource intensive centralized solutions. In this work, we propose a decentralized device concept that can utilize sunlight to split water into hydrogen and hydrogen peroxide. The hydrogen peroxide can oxidize organics while the hydrogen bubbles out. In enabling this device, we require an electrocatalyst that can oxidize water while suppressing the thermodynamically favored oxygen evolution and form hydrogen peroxide. Using density functional theory calculations, we show that the free energy of adsorbed OH* can be used to determine selectivity trends between the 2e(-) water oxidation to H2O2 and the 4e(-) oxidation to O2. We show that materials which bind oxygen intermediates sufficiently weakly, such as SnO2, can activate hydrogen peroxide evolution. We present a rational design principle for the selectivity in electrochemical water oxidation and identify new material candidates that could perform H2O2 evolution selectively.

  17. Selective electrochemical generation of hydrogen peroxide from water oxidation

    CERN Document Server

    Viswanathan, Venkatasubramanian; Nørskov, Jens K

    2015-01-01

    Water is a life-giving source, fundamental to human existence, yet, over a billion people lack access to clean drinking water. Present techniques for water treatment such as piped, treated water rely on time and resource intensive centralized solutions. In this work, we propose a decentralized device concept that can utilize sunlight to split water into hydrogen and hydrogen peroxide. The hydrogen peroxide can oxidize organics while the hydrogen bubbles out. In enabling this device, we require an electrocatalyst that can oxidize water while suppressing the thermodynamically favored oxygen evolution and form hydrogen peroxide. Using density functional theory calculations, we show that the free energy of adsorbed OH$^*$ can be used as a descriptor to screen for selectivity trends between the 2e$^-$ water oxidation to H$_2$O$_2$ and the 4e$^-$ oxidation to O$_2$. We show that materials that bind oxygen intermediates sufficiently weakly, such as SnO$_2$, can activate hydrogen peroxide evolution. We present a rati...

  18. The hydrogen generation from alkaline NaBH4 solution by using electroplated amorphous Co–Ni–P film catalysts

    International Nuclear Information System (INIS)

    The amorphous Co–Ni–P films were electroplating on Cu sheets. The effects of NiSO4 concentrations on the deposit plating rate and the catalytic activities for NaBH4 hydrolysis were investigated. The surface morphology and phase structure of the deposited Co–Ni–P films were characterized by scanning electron microscopy (SEM) and X-ray diffraction (XRD) analysis. The composition was analyzed by energy dispersive spectrometer (EDX). Experimental results showed that adding NiSO4 in Co–P bath could increase the deposition rate. When 0.01 M of NiSO4 was used, the highest deposition rate and the highest hydrogen generation rate of 3636 mL (min g-catalyst)−1 were obtained. The activation energy (Ea) for the NaBH4 hydrolysis was 38 kJ mol−1, which was comparable to the value of noble metal catalysts.

  19. Influence of rare-earth metal doping on the catalytic performance of CuO-CeO2 for the preferential oxidation of CO in excess hydrogen

    Institute of Scientific and Technical Information of China (English)

    Zhigang Liu; Renxian Zhou; Xiaoming Zheng

    2008-01-01

    Doping of different rare-earth metals(Pr,Nd,Y and La)had an evident influence on the catalytic performance of CuO-CeO2 for the preferential oxidation(PROX)Of CO in excess hydrogen.As for Pr,the doping enhanced the catalytic activity of CuO-CeO2 for PROX.For example,the CO conversion over the above catalyst for PROX was higher than 99%at 120℃.Especially.the doping of Pr widened the temperature window by 20℃ over CuO-CeO2 with 99%CO conversion.For Nd,Y and La,the doping depressed the catalytic activity of CuO-CeO2 for PROX.However,the doping of transition metals markedly improved the selectivity of CuO-CeO2 for PROX.

  20. Promoting effect of Ir on the catalytic property of Ru/ZnO catalysts for selective hydrogenation of crotonaldehyde

    International Nuclear Information System (INIS)

    A series of ZnO supported Ru–Ir bimetal catalysts were prepared and tested for vapor-phase selective hydrogenation of crotonaldehyde. The addition of Ir could effectively promote the catalytic performance, especially the catalyst stability. A Ru–0.5Ir/ZnO catalyst showed the highest activity (a conversion of 63.3%) and selectivity to crotyl alcohol (94.4%) after 30 h reaction. The enhanced stability was attributed to the modified electronic property of Ru by the formation of RuIr alloy as the X-ray photoelectron spectroscopy results showed charge transfer from Ru to Ir, as well as the weakened surface acidity in the Ru–Ir/ZnO catalyst as evidenced by NH3 temperature-programmed desorption technique. Besides, the deactivation of the catalysts was due to the strong chemisorption of CO on the metal surface via decarbonylation reaction and deposition of organic compounds on the catalyst surface, which was characterized by CO poisoning experiment, CO temperature-programmed desorption and temperature-programmed oxidation methods.

  1. Kinetic spectrophotometric determination of Bi(III based on its catalytic effect on the oxidation of phenylfluorone by hydrogen peroxide

    Directory of Open Access Journals (Sweden)

    SOFIJA M. RANČIĆ

    2009-08-01

    Full Text Available A new reaction was suggested and a new kinetic method was elaborated for determination of Bi(III in solution, based on its catalytic effect on the oxidation of phenyl-fluorone (PF by hydrogen peroxide in ammonia buffer. By application of spectrophotometric technique, a limit of quantification (LQ of 128 ng cm-3 was reached, and the limit of detection (LD of 37 ng cm-3 was obtained, where LQ was defined as the ratio signal:noise = 10:1 and LD was defined as signal 3:1 against the blank. The RSD value was found to be in the range 2.8–4.8 % for the investigated concentration range of Bi(III. The influence of some ions upon the reaction rate was tested. The method was confirmed by determining Bi(III in a stomach ulcer drug (“Bicit HP”, Hemofarm A.D.. The obtained results were compared to those obtained by AAS and good agreement of results was obtained.

  2. Effect of water injection on hydrogen generation during severe accident in PWR

    Institute of Scientific and Technical Information of China (English)

    TAO Jun; CAO Xuewu

    2009-01-01

    Effect of water injection on hydrogen generation during severe accident in a 1000 MWe pressurized water reactor was studied.The analyses were carried out with different water injection rates at different core damage stages.The core can be quenched and accident progression can be terminated by water injection at the time before cohesive core debris is formed at lower core region.Hydrogen generation rate decreases with water injection into the core at the peak core temperature of 1700 K,because the core is quenched and reflooded quickly.The water injection at the peak core temperature of 1900 K,the hydrogen generation rate increases at low injection rates of the water,as the core is quenched slowly and the core remains in uncovered condition at high temperatures for a longer time than the situation of high injection rate.At peak core temperature of 2100-2300 K,the Hydrogen generation rate increases by water injection because of the steam serving to the high temperature steam-starved core.Hydrogen generation rate increases significantly after water injection into the core at peak core temperature of 2500 K because of the steam serving to the relocating Zr-U-O mixture.Almost no hydrogen generation can be seen in base case after formation of the molten pool at the lower core region.However,hydrogen is generated if water is injected into the molten pool,because steam serves to the crust supporting the molten pool.Reactor coolant system (RCS) depressurization by opening power operated relief valves has important effect on hydrogen generation.Special attention should be paid to hydrogen generation enhancement caused by RCS depressurization.

  3. Catalytic hydrogen production over RhPd/CeO2 catalysts and CO purification over Au/TiO2 catalysts

    OpenAIRE

    Jiménez Divins, Núria

    2015-01-01

    La consulta íntegra de la tesi, inclosos els articles no comunicats públicament per drets d'autor, es pot realitzar prèvia petició a l'Arxiu UPC This Thesis focuses on the study of the catalytic production of hydrogen from a biofuel, namely the bioethanol. It also studies the subsequent purification of pre-cleaned reformate streams. The end use of the hydrogen produced is to feed fuel cells to power portable and mobile applications. In this Thesis, two types of catalysts have been develope...

  4. Pentlandite rocks as sustainable and stable efficient electrocatalysts for hydrogen generation

    Science.gov (United States)

    Konkena, Bharathi; junge Puring, Kai; Sinev, Ilya; Piontek, Stefan; Khavryuchenko, Oleksiy; Dürholt, Johannes P.; Schmid, Rochus; Tüysüz, Harun; Muhler, Martin; Schuhmann, Wolfgang; Apfel, Ulf-Peter

    2016-01-01

    The need for sustainable catalysts for an efficient hydrogen evolution reaction is of significant interest for modern society. Inspired by comparable structural properties of [FeNi]-hydrogenase, here we present the natural ore pentlandite (Fe4.5Ni4.5S8) as a direct ‘rock' electrode material for hydrogen evolution under acidic conditions with an overpotential of 280 mV at 10 mA cm−2. Furthermore, it reaches a value as low as 190 mV after 96 h of electrolysis due to surface sulfur depletion, which may change the electronic structure of the catalytically active nickel–iron centres. The ‘rock' material shows an unexpected catalytic activity with comparable overpotential and Tafel slope to some well-developed metallic or nanostructured catalysts. Notably, the ‘rock' material offers high current densities (≤650 mA cm−2) without any loss in activity for approximately 170 h. The superior hydrogen evolution performance of pentlandites as ‘rock' electrode labels this ore as a promising electrocatalyst for future hydrogen-based economy. PMID:27461840

  5. Pentlandite rocks as sustainable and stable efficient electrocatalysts for hydrogen generation

    Science.gov (United States)

    Konkena, Bharathi; Junge Puring, Kai; Sinev, Ilya; Piontek, Stefan; Khavryuchenko, Oleksiy; Dürholt, Johannes P.; Schmid, Rochus; Tüysüz, Harun; Muhler, Martin; Schuhmann, Wolfgang; Apfel, Ulf-Peter

    2016-07-01

    The need for sustainable catalysts for an efficient hydrogen evolution reaction is of significant interest for modern society. Inspired by comparable structural properties of [FeNi]-hydrogenase, here we present the natural ore pentlandite (Fe4.5Ni4.5S8) as a direct `rock' electrode material for hydrogen evolution under acidic conditions with an overpotential of 280 mV at 10 mA cm-2. Furthermore, it reaches a value as low as 190 mV after 96 h of electrolysis due to surface sulfur depletion, which may change the electronic structure of the catalytically active nickel-iron centres. The `rock' material shows an unexpected catalytic activity with comparable overpotential and Tafel slope to some well-developed metallic or nanostructured catalysts. Notably, the `rock' material offers high current densities (<=650 mA cm-2) without any loss in activity for approximately 170 h. The superior hydrogen evolution performance of pentlandites as `rock' electrode labels this ore as a promising electrocatalyst for future hydrogen-based economy.

  6. Pentlandite rocks as sustainable and stable efficient electrocatalysts for hydrogen generation.

    Science.gov (United States)

    Konkena, Bharathi; Junge Puring, Kai; Sinev, Ilya; Piontek, Stefan; Khavryuchenko, Oleksiy; Dürholt, Johannes P; Schmid, Rochus; Tüysüz, Harun; Muhler, Martin; Schuhmann, Wolfgang; Apfel, Ulf-Peter

    2016-01-01

    The need for sustainable catalysts for an efficient hydrogen evolution reaction is of significant interest for modern society. Inspired by comparable structural properties of [FeNi]-hydrogenase, here we present the natural ore pentlandite (Fe4.5Ni4.5S8) as a direct 'rock' electrode material for hydrogen evolution under acidic conditions with an overpotential of 280 mV at 10 mA cm(-2). Furthermore, it reaches a value as low as 190 mV after 96 h of electrolysis due to surface sulfur depletion, which may change the electronic structure of the catalytically active nickel-iron centres. The 'rock' material shows an unexpected catalytic activity with comparable overpotential and Tafel slope to some well-developed metallic or nanostructured catalysts. Notably, the 'rock' material offers high current densities (≤650 mA cm(-2)) without any loss in activity for approximately 170 h. The superior hydrogen evolution performance of pentlandites as 'rock' electrode labels this ore as a promising electrocatalyst for future hydrogen-based economy. PMID:27461840

  7. Hydrogen generation monitoring and mass gain analysis during the steam oxidation for Zircaloy using hydrogen and oxygen sensors

    International Nuclear Information System (INIS)

    The oxidation behavior of Zircaloy-4 at high temperatures in a flowing Ar-H2O (saturated at 323 K) mixed gas was investigated using hydrogen and oxygen sensors installed at a gas outlet, and the utility of the gas sensing methods by using both sensors was examined. The generated amount of hydrogen was determined from the hydrogen partial pressure continuously measured by the hydrogen sensor, and the resultant calculated oxygen amount that reacted with the specimen was in close agreement with the mass gain gravimetrically measured after the experiment. This result demonstrated that the hydrogen partial pressure measurement using a hydrogen sensor is an effective method for examining the steam oxidation of this metal as well as monitoring the hydrogen evolution. The advantage of this method is that the oxidation rate of the metal at any time as a differential quantity is able to be obtained, compared to the oxygen amount gravimetrically measured as an integral quantity. When the temperature was periodically changed in the range of 1173 K to 1523 K, highly accurate measurements could be carried out using this gas monitoring method, although reasonable measurements were not gravimetrically performed due to the fluctuating thermo-buoyancy during the experiment. A change of the oxidation rate was clearly detected at a monoclinic tetragonal transition temperature of ZrO2. From the calculation of the water vapor partial pressure during the thermal equilibrium condition using the hydrogen and oxygen partial pressures, it became clear that a thermal equilibrium state is maintained when the isothermal condition is maintained, but is not when the temperature increases or decreases with time. Based on these results, it was demonstrated that the gas monitoring system using hydrogen and oxygen sensors is very useful for investigating the oxidation process of the Zircaloy in steam. (author)

  8. In situ generation of hydrogen from water by aluminum corrosion in solutions of sodium aluminate

    OpenAIRE

    Soler Turu, Lluis; Candela Soto, Angélica Maria; Macanás de Benito, Jorge; Muñoz Tapia, Maria; Casado Giménez, Juan

    2009-01-01

    A new process to obtain hydrogen from water using aluminum in sodium aluminate solutions is described and compared with results obtained in aqueous sodium hydroxide. This process consumes only water and aluminum, which are raw materials much cheaper than other compounds used for in situ hydrogen generation, such as hydrocarbons and chemical hydrides, respectively. As a consequence, our process could be an economically feasible alternative for hydrogen to supply fuel cells. Results showed an i...

  9. Photocatalytic hydrogen generation using glycerol wastewater over Pt/TiO2

    Institute of Scientific and Technical Information of China (English)

    Min LI; Yuexiang LI; Shaoqin PENG; Gongxuan LU; Shuben LI

    2009-01-01

    Using glycerol as electron donor, photocataly-tic hydrogen generation over Pt/TiO2 was investigated.The results show that glycerol can not only improve the efficiency of photocatalytic hydrogen generation but can also be decomposed effectively. The factors which affect photocatalytic hydrogen generation, such as irradiation time, initial concentration of the glycerol solution, pH-value of the suspensions and the coexisting substances were studied. The final oxidation products of glycerol were H2O and CO2. Glyceraldhyde, glycoladehyde, glycolic acid and formaldehyde were identified as the intermedi-ates. A possible reaction mechanism was discussed.

  10. Catalytic Hydrogenation of the Sweet Principles of Stevia rebaudiana, Rebaudioside B, Rebaudioside C, and Rebaudioside D and Sensory Evaluation of Their Reduced Derivatives

    OpenAIRE

    Mary Campbell; Indra Prakash; Venkata Sai Prakash Chaturvedula

    2012-01-01

    Catalytic hydrogenation of rebaudioside B, rebaudioside C, and rebaudioside D; the three ent-kaurane diterpene glycosides isolated from Stevia rebaudiana was carried out using Pd(OH)2. Reduction of steviol glycosides was performed using straightforward synthetic chemistry with the catalyst Pd(OH)2 and structures of the corresponding dihydro derivatives were characterized on the basis of 1D and 2D nuclear magnetic resonance (NMR) spectral data indicating that all are novel compounds being repo...

  11. A new approach for hydrogen generation from sewage sludge.

    Science.gov (United States)

    Zhang, Qiwu; Kano, Junya

    2016-02-01

    A new process to produce hydrogen efficiently from sewage sludge (SWS) was developed with co-grinding operation of the dried SWS with calcium and nickel hydroxides (Ca(OH)2 and Ni(OH)2) and subsequent heating of the ground mixture at relatively low temperature below 600°C. A set of analytical methods were used to characterize the ground samples before heating and the gaseous and solid products after heating. Thermo-mass spectroscopic (TG-MS) analysis showed hydrogen occurrence around 450°C. Hydrogen yield over 70g per kg SWS with concentration of 93.6% was obtained with the hydroxide additions of Ca to C from SWS at 1:1 and Ni to C at 1:6, respectively. X-ray diffraction (XRD) analysis of the solid residues after heating confirmed the existences of calcium carbonate and nickel metal. Based on the obtained results, possible reaction pathway was proposed. PMID:26642224

  12. Green diesel production via catalytic hydrogenation/decarboxylation of triglycerides and fatty acids of vegetable oil and brown grease

    Science.gov (United States)

    Sari, Elvan

    than activated carbon itself for both decarboxylation of oleic acid and hydrogenation of alkenes. In an additional effort to reduce Pd amount in the catalyst, Pd2Co/C catalysts with various Pd content were prepared and the catalytic activity study showed that 0.5 wt% Pd2Co/C catalyst performs even better than a 5 wt% Pd/C catalyst. Pd and Co alloys were very well dispersed and formed fine clusters, which led to a higher active metal surface area and hence favored the decarboxylation of oleic acid. This study showed that an alloy of Pd on carbon with a significantly low Pd content is much more active and selective to diesel hydrocarbons production from an unsaturated fatty acid in super-critical water and may be regarded as a prospective feasible decarboxylation catalyst for the removal of oxygen from vegetable oil/animal fat without the need of additional hydrogen.

  13. Effect of the Sequence of the Thermoelectric Generator and the Three-Way Catalytic Converter on Exhaust Gas Conversion Efficiency

    Science.gov (United States)

    Su, Chuqi; Tong, Naiqiang; Xu, Yuman; Chen, Shan; Liu, Xun

    2013-07-01

    The potential for thermoelectric exhaust heat recovery in vehicles has increased with recent improvements in the efficiency of thermoelectric generators (TEGs). The problem with using thermoelectric generators for vehicle applications is whether the device is compatible with the original vehicle exhaust system, which determines the quality of the exhaust gas treatment and the realization of energy conservation and emission reduction. Based on ANSYS CFX simulation analysis of the impact of two positional relationships between the TEG and three-way catalytic converter in the exhaust system on the working efficiency of both elements, it is concluded that the layout with the front three-way catalytic converter has an advantage over the other layout mode under current conditions. New ideas for an improvement program are proposed to provide the basis for further research.

  14. Hydrogen bonding strength of interfacial water determined with surface sum-frequency generation

    NARCIS (Netherlands)

    M. Sovago; R. Kramer Campen; H.J. Bakker; M. Bonn

    2009-01-01

    We demonstrate that marked variations exist in hydrogen bonding interactions of interfacial water at different aqueous interfaces. The average hydrogen bond strength and its distribution are inferred from surface sum-frequency generation (SFG) spectra through the center frequency and width, respecti

  15. Investment in hydrogen tri-generation for wastewater treatment plants under uncertainties

    Science.gov (United States)

    Gharieh, Kaveh; Jafari, Mohsen A.; Guo, Qizhong

    2015-11-01

    In this article, we present a compound real option model for investment in hydrogen tri-generation and onsite hydrogen dispensing systems for a wastewater treatment plant under price and market uncertainties. The ultimate objective is to determine optimal timing and investment thresholds to exercise initial and subsequent options such that the total savings are maximized. Initial option includes investment in a 1.4 (MW) Molten Carbonate Fuel Cell (MCFC) fed by mixture of waste biogas from anaerobic digestion and natural gas, along with auxiliary equipment. Produced hydrogen in MCFC via internal reforming, is recovered from the exhaust gas stream using Pressure Swing Adsorption (PSA) purification technology. Therefore the expansion option includes investment in hydrogen compression, storage and dispensing (CSD) systems which creates additional revenue by selling hydrogen onsite in retail price. This work extends current state of investment modeling within the context of hydrogen tri-generation by considering: (i) Modular investment plan for hydrogen tri-generation and dispensing systems, (ii) Multiple sources of uncertainties along with more realistic probability distributions, (iii) Optimal operation of hydrogen tri-generation is considered, which results in realistic saving estimation.

  16. Non-catalytic transfer hydrogenation in supercritical CO2 for coal liquefaction

    Science.gov (United States)

    Elhussien, Hussien

    This thesis presents the results of the investigation on developing and evaluating a low temperature (products of coal dissolution were non-polar and polar while the supercritical CO2, which enhanced the rates of hydrogenation and dissolution of the non-polar molecules and removal from the reaction site, was non-polar. The polar modifier (PM) for CO2 was added to the freed to aid in the dissolution and removal of the polar components. The addition of a phase transfer agent (PTA) allowed a seamless transport of the ions and by-product between the aqueous and organic phases. DDAB, used as the PTA, is an effective phase transfer catalyst and showed enhancement to the coal dissolution process. COAL + DH- +H 2O → COAL.H2 + DHO-- This process has a great feature due to the fact that the chemicals were obtained without requir-ing to first convert coal to CO and H2 units as in indirect coal liquefaction. The experiments were conducted in a unique reactor set up that can be connected through two lines. one line to feed the reactor with supercritical CO 2 and the other connected to gas chromatograph. The use of the supercritical CO2 enhanced the solvent option due to the chemical extraction, in addition to the low environmental impact and energy cost. In this thesis the experiment were conducted at five different temperatures from atmos-pheric to 140°C, 3000 - 6000 psi with five component of feed mixture, namely water, HTA, PTA, coal, and PM in semi batch vessels reactor system with a volume of 100 mL. The results show that the chemicals were obtained without requiring to first convert coal to CO and H2 units as in indirect coal liquefaction. The results show that the conversion was found to be 91.8% at opti-mum feed mixtures values of 3, 1.0 and 5.4 for water: PM, HTA: coal, water: coal respectively. With the oil price increase and growing in energy demand, the coal liquefaction remain affordable and available energy alternative.

  17. Hydrogen generation from aluminium corrosion in reactor containment spray solutions

    International Nuclear Information System (INIS)

    The aluminium corrosion experiments in reactor containment spray solutions, under the conditions expected to prevail during LOCA in BWR and PWR, were performed in order to investigate relationships between temperature, pH and hydrogen production rates. In order to simulate the conditions in a BWR containment realistic ratios between aluminium surface and water volume and between aluminium surface and oxygen volume were used. Three different aluminium alloys were exposed to spray solutions: AA 1050, AA 5052 and AA 6082. The corrosion rates were measured for BWR solutions (deaerated and aerated) with pH 5 and 9 at 50, 100 and 1500C. The pressure was constantly 0.8 MPa. The hydrogen production rate was measured by means of gas chromatography. In deionized BWR water the corrosion rates did not exceed about 0.05 mm/year in all cases, i.e. were practically independent of temperature and pH. Hydrogen concentrations were less than 0.1 vol.% in cooled dry gas. Corrosion rates and hydrogen production in PWR alkaline solution measured at pH 9.7 and 1500C were very high. AA 5052 alloy was the best material

  18. Enzymatic generation of hydrogen peroxide shows promising antifouling effect

    DEFF Research Database (Denmark)

    Kristensen, J.B.; Olsen, Stefan Møller; Laursen, B.S.;

    2010-01-01

    The antifouling (AF) potential of hydrogen peroxide (H2O2) produced enzymatically in a coating containing starch, glucoamylase, and hexose oxidase was evaluated in a series of laboratory tests and in-sea field trials. Dissolved H2O2 inhibited bacterial biofilm formation by eight of nine marine Pr...

  19. Combustion of hydrogen-oxygen mixture in electrochemically generated nanobubbles

    NARCIS (Netherlands)

    Svetovoy, Vitaly B.; Sanders, Remco G.P.; Lammerink, Theo S.J.; Elwenspoek, Miko

    2011-01-01

    Ignition of exothermic chemical reactions in small volumes is considered as difficult or impossible due to the large surface-to-volume ratio. Here observation of the spontaneous reaction is reported between hydrogen and oxygen in bubbles whose diameter is smaller than a threshold value around 150 nm

  20. HOGEN{trademark} proton exchange membrane hydrogen generators: Commercialization of PEM electrolyzers

    Energy Technology Data Exchange (ETDEWEB)

    Smith, W.F.; Molter, T.M. [Proton Energy Systems, Inc., Rocky Hill, CT (United States)

    1997-12-31

    PROTON Energy Systems` new HOGEN series hydrogen generators are Proton Exchange Membrane (PEM) based water electrolyzers designed to generate 300 to 1000 Standard Cubic Feet Per Hour (SCFH) of high purity hydrogen at pressures up to 400 psi without the use of mechanical compressors. This paper will describe technology evolution leading to the HOGEN, identify system design performance parameters and describe the physical packaging and interfaces of HOGEN systems. PEM electrolyzers have served US and UK Navy and NASA needs for many years in a variety of diverse programs including oxygen generators for life support applications. In the late 1970`s these systems were advocated for bulk hydrogen generation through a series of DOE sponsored program activities. During the military buildup of the 1980`s commercial deployment of PEM hydrogen generators was de-emphasized as priority was given to new Navy and NASA PEM electrolysis systems. PROTON Energy Systems was founded in 1996 with the primary corporate mission of commercializing PEM hydrogen generators. These systems are specifically designed and priced to meet the needs of commercial markets and produced through manufacturing processes tailored to these applications. The HOGEN series generators are the first step along the path to full commercial deployment of PEM electrolyzer products for both industrial and consumer uses. The 300/1000 series are sized to meet the needs of the industrial gases market today and provide a design base that can transition to serve the needs of a decentralized hydrogen infrastructure tomorrow.

  1. 催化点火气氢气氧推力器试验研究%Experimental Investigation on Catalytic Hydrogen and Oxygen Thruster

    Institute of Scientific and Technical Information of China (English)

    林震; 王长辉; 刘宇

    2012-01-01

    为探索催化点火气氢气氧推力器的点火规律和相关性能,设计并搭建了1N催化点火气氢气氧推力器试验系统,进行了冷热试试验。试验成功实现了不同工况下的多次催化点火。结果表明:供给氧氢混合比控制在100时,推力器预燃室产生的点火温度为700℃,能够满足燃烧室点火要求;催化剂面积体积比对催化氢氧点火具有决定性影响,采用面积体积比大的催化载体可以实现常温(8℃)下的催化点火;另外,试验中氢氧燃烧产生的高温和试验结束后推力器内残留的液态水也对催化组件提出了一定的耐温性和防水性要求。%In order to study the catalytic ignition law of catalytic hydrogen and oxygen thruster, a 1N catalytic thruster and relative experimental system were constructed. A series of tests were conducted. Several catalytic ignition in different working condition was realized. It indicates that when the oxygen and hydrogen mixture ratio is 100, the measured temperature of pre- combustion is 700℃ , which is the most applicable ignition temperature. Catalytic ignition in normal temperature can be real- ized using palladium-carbon as catalyzer which shows the domination of surface-volume ratio for catalytic ignition. In addition, it indicates that the ability of fireproof and waterproof is also the key characteristics of the catalyzer parts for catalytic hydrogen and oxwen thruster.

  2. Ruthenium(0) nanoparticles supported on multiwalled carbon nanotube as highly active catalyst for hydrogen generation from ammonia-borane.

    Science.gov (United States)

    Akbayrak, Serdar; Ozkar, Saim

    2012-11-01

    Ruthenium(0) nanoparticles supported on multiwalled carbon nanotubes (Ru(0)@MWCNT) were in situ formed during the hydrolysis of ammonia-borane (AB) and could be isolated from the reaction solution by filtration and characterized by ICP-OES, XRD, TEM, SEM, EDX, and XPS techniques. The results reveal that ruthenium(0) nanoparticles of size in the range 1.4-3.0 nm are well-dispersed on multiwalled carbon nanotubes. They were found to be highly active catalyst in hydrogen generation from the hydrolysis of AB with a turnover frequency value of 329 min⁻¹. The reusability experiments show that Ru(0)@MWCNTs are isolable and redispersible in aqueous solution; when redispersed they are still active catalyst in the hydrolysis of AB exhibiting a release of 3.0 equivalents of H₂ per mole of NH₃BH₃ and preserving 41% of the initial catalytic activity even after the fourth run of hydrolysis. The lifetime of Ru(0)@MWCNTs was measured as 26400 turnovers over 29 h in the hydrolysis of AB at 25.0 ± 0.1 °C before deactivation. The work reported here also includes the kinetic studies depending on the temperature to determine the activation energy of the reaction (E(a) = 33 ± 2 kJ/mol) and the effect of catalyst concentration on the rate of the catalytic hydrolysis of AB, respectively. PMID:23113804

  3. A composite of borohydride and super absorbent polymer for hydrogen generation

    Science.gov (United States)

    Li, Z. P.; Liu, B. H.; Liu, F. F.; Xu, D.

    To develop a hydrogen source for underwater applications, a composite of sodium borohydride and super absorbent polymer (SAP) is prepared by ball milling sodium borohydride powder with SAP powder, and by dehydrating an alkaline borohydride gel. When sodium polyacrylate (NaPAA) is used as the SAP, the resulting composite exhibits a high rate of borohydride hydrolysis for hydrogen generation. A mechanism of hydrogen evolution from the NaBH 4-NaPAA composite is suggested based on structure analysis by X-ray diffraction and scanning electron microscopy. The effects of water and NiCl 2 content in the precursor solution on the hydrogen evolution behavior are investigated and discussed.

  4. Solar Photo Catalytic Hydrogen Production from water using a dual bed photosystem

    Energy Technology Data Exchange (ETDEWEB)

    Florida Solar Energy Center

    2003-03-30

    A body of work was performed in which the feasibility of photocatalytically decomposing water into its constituent elements using a dual bed, or modular photosystem, under solar radiation was investigated. The system envisioned consists of two modules, each consisting of a shallow, flat, sealed container, in which microscopic photocatalytic particles are immobilized. The photocatalysts absorb light, generating free electrons and lattice vacancy holes, which are capable of performing reductive and oxidative chemistry, respectively. The photocatalysts would be chosen as to whether they specifically promote H{sub 2} or O{sub 2} evolution in their respective containers. An aqueous solution containing a redox mediator is pumped between the two chambers in order to transfer electron equivalents from one reaction to the other.

  5. Ceria-supported ruthenium nanoparticles as highly active and long-lived catalysts in hydrogen generation from the hydrolysis of ammonia borane.

    Science.gov (United States)

    Akbayrak, Serdar; Tonbul, Yalçın; Özkar, Saim

    2016-07-01

    Ruthenium(0) nanoparticles supported on ceria (Ru(0)/CeO2) were in situ generated from the reduction of ruthenium(iii) ions impregnated on ceria during the hydrolysis of ammonia borane. Ru(0)/CeO2 was isolated from the reaction solution by centrifugation and characterized by ICP-OES, BET, XRD, TEM, SEM-EDS and XPS techniques. All the results reveal that ruthenium(0) nanoparticles were successfully supported on ceria and the resulting Ru(0)/CeO2 is a highly active, reusable and long-lived catalyst for hydrogen generation from the hydrolysis of ammonia borane with a turnover frequency value of 361 min(-1). The reusability tests reveal that Ru(0)/CeO2 is still active in the subsequent runs of hydrolysis of ammonia borane preserving 60% of the initial catalytic activity even after the fifth run. Ru(0)/CeO2 provides a superior catalytic lifetime (TTO = 135 100) in hydrogen generation from the hydrolysis of ammonia borane at 25.0 ± 0.1 °C before deactivation. The work reported here includes the formation kinetics of ruthenium(0) nanoparticles. The rate constants for the slow nucleation and autocatalytic surface growth of ruthenium(0) nanoparticles were obtained using hydrogen evolution as a reporter reaction. An evaluation of rate constants at various temperatures enabled the estimation of activation energies for both the reactions, Ea = 60 ± 7 kJ mol(-1) for the nucleation and Ea = 47 ± 2 kJ mol(-1) for the autocatalytic surface growth of ruthenium(0) nanoparticles, as well as the activation energy of Ea = 51 ± 2 kJ mol(-1) for the catalytic hydrolysis of ammonia borane. PMID:27302302

  6. Experimental and modelling evaluation of an ammonia-fuelled microchannel reactor for hydrogen generation / Steven Chiuta

    OpenAIRE

    Chiuta, Steven

    2015-01-01

    In this thesis, ammonia (NH3) decomposition was assessed as a fuel processing technology for producing on-demand hydrogen (H2) for portable and distributed fuel cell applications. This study was motivated by the present lack of infrastructure to generate H2 for proton exchange membrane (PEM) fuel cells. An overview of past and recent worldwide research activities in the development of reactor technologies for portable and distributed hydrogen generation via NH3 decomposition wa...

  7. Solar-Hydrogen-Fuel Cell Prototype as a Source of Renewable Energy Generation

    OpenAIRE

    Andrés Rodríguez-Castellanos; Ernesto López-Torres; Omar Solorza-Feria

    2007-01-01

    A small renewable energy prototype is presented, integrated by a solar photovoltaic module used for electrolysis of water where the resulting hydrogen was fed to a regenerative fuel cell for a clean electricity generation. A photovoltaic module provided DC power to an electrolyzer, to produce 56 cm3/min of hydrogen which is fed to a fuel cell and generate electricity. This prototype was designed and manufactured to show the future energy scenario of renewable energy. For water electrolysis, p...

  8. Methane decomposition under a corona discharge to generate COx-free hydrogen

    International Nuclear Information System (INIS)

    A non-thermal plasma reforming unit operating at atmospheric pressure has been developed for converting methane to COx-free hydrogen. Argon was used to provide additional electrons and photons for higher reaction rates. A series of experiments was performed for positive corona discharge at a fixed inter-electrode distance (15 mm) to study the effects of discharge power (range of 14–20 W) and residence time (60, 120, 180 and 240 s). A second series of experiments studied the effect of inter-electrode distance on hydrogen production, with distances of 15, 20, 25, 30 and 35 mm tested. The analysis of the results shows that both discharge power and residence time, have a positive influence on methane conversion, hydrogen selectivity and energy conversion efficiency. Longer discharge gaps favour hydrogen production. A final series of experiments on corona polarity showed that a positive discharge was preferable. - Highlights: • We examine plasma-assisted COx-free hydrogen generation from methane. • Higher powers and residence times favour hydrogen production. • Positive polarity and higher inter-electrode distances favour hydrogen production. • Energy conversion efficiency is mainly governed by hydrogen selectivity. • Corona discharges are a promising approach for hydrogen generation from methane

  9. Hydrogen production by steam reforming of bio-alcohols. The use of conventional and membrane-assisted catalytic reactors

    Energy Technology Data Exchange (ETDEWEB)

    Seelam, P. K.

    2013-11-01

    The energy consumption around the globe is on the rise due to the exponential population growth and urbanization. There is a need for alternative and non-conventional energy sources, which are CO{sub 2}-neutral, and a need to produce less or no environmental pollutants and to have high energy efficiency. One of the alternative approaches is hydrogen economy with the fuel cell (FC) technology which is forecasted to lead to a sustainable society. Hydrogen (H{sub 2}) is recognized as a potential fuel and clean energy carrier being at the same time a carbon-free element. Moreover, H{sub 2} is utilized in many processes in chemical, food, metallurgical, and pharmaceutical industry and it is also a valuable chemical in many reactions (e.g. refineries). Non-renewable resources have been the major feedstock for H{sub 2} production for many years. At present, {approx}50% of H{sub 2} is produced via catalytic steam reforming of natural gas followed by various down-stream purification steps to produce {approx}99.99% H{sub 2}, the process being highly energy intensive. Henceforth, bio-fuels like biomass derived alcohols (e.g. bio-ethanol and bio-glycerol), can be viable raw materials for the H{sub 2} production. In a membrane based reactor, the reaction and selective separation of H{sub 2} occur simultaneously in one unit, thus improving the overall reactor efficiency. The main motivation of this work is to produce H{sub 2} more efficiently and in an environmentally friendly way from bio-alcohols with a high H{sub 2} selectivity, purity and yield. In this thesis, the work was divided into two research areas, the first being the catalytic studies using metal decorated carbon nanotube (CNT) based catalysts in steam reforming of ethanol (SRE) at low temperatures (<450 deg C). The second part was the study of steam reforming (SR) and the water-gas-shift (WGS) reactions in a membrane reactor (MR) using dense and composite Pd-based membranes to produce high purity H{sub 2}. CNTs

  10. Generation of Hydrogen from Photolysis of Organic Acids by Photosynthetic Bacteria

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    Photodecomposition of ten kinds of organic acids by Rhodopseudomonas palustris for producing hydrogen has been investigated. By using acetate as hydrogen donor, dynamics of hydrogen production and cell growth has been determined; the influences of acetate concentration, temperature, light intensity and the effects of the interaction among metal ions (Fe3+, Ni2+), acetate and glutamate in aqueous solution on hydrogen production have been examined for optimizing the conditions of H2 generation. The results show that H2 production is partially correlated with cell growth; Ni2+ inhibits hydrogen production, but enhances cell growth; Fe3+ promotes hydrogen production evidently. The highest rate of H2 production is 22.1 mL L-1 h-1 under the conditions of 35 ~ 37℃, 6000 ~ 8000 lx, 30 mmolL-1 of acetate, 9 mmolL-1 of glutamate, and 50 (molL-1 of Fe3+.

  11. Catalytic activity of iron hexacyanoosmate(II) towards hydrogen peroxide and nicotinamide adenine dinucleotide and its use in amperometric biosensors

    Energy Technology Data Exchange (ETDEWEB)

    Kotzian, Petr; Janku, Tereza [Department of Analytical Chemistry, University of Pardubice, Nam. Cs. Legii 565, CZ-532 10 Pardubice (Czech Republic); Kalcher, Kurt [Institute of Chemistry - Analytical Chemistry, Karl-Franzens University, Universitaetsplatz 1, A-8010 Graz (Austria); Vytras, Karel [Department of Analytical Chemistry, University of Pardubice, Nam. Cs. Legii 565, CZ-532 10 Pardubice (Czech Republic)], E-mail: karel.vytras@upce.cz

    2007-09-19

    Hydrogen peroxide and nicotinamide adenine dinucleotide (NADH) may be determined amperometrically using screen-printed electrodes chemically modified with iron(III) hexacyanoosmate(II) (Osmium purple) in flow injection analysis (FIA). The determination is based on the exploitation of catalytic currents resulting from the oxidation/reduction of the modifier. The performance of the sensor was characterized and optimized by controlling several operational parameters (applied potential, pH and flow rate of the phosphate buffer). Comparison has been made with analogous complexes of ruthenium (Ruthenium purple) and iron (Prussian blue). Taking into account the sensitivity and stability of corresponding sensors, the best results were obtained with the use of Osmium purple. The sensor exhibited a linear increase of the amperometric signal with the concentration of hydrogen peroxide in the range of 0.1-100 mg L{sup -1} with a detection limit (evaluated as 3{sigma}) of 0.024 mg L{sup -1} with a R.S.D. 1.5% for 10 mg L{sup -1} H{sub 2}O{sub 2} under optimized flow rate of 0.4 mL min{sup -1} in 0.1 M phosphate buffer carrier (pH 6) and a working potential of +0.15 V versus Ag/AgCl. Afterwards, a biological recognition element - either glucose oxidase or ethanol dehydrogenase - was incorporated to achieve a sensor facilitating the determination of glucose or ethanol, respectively. The glucose sensor gave linearity between current and concentration in the range from 1 to 250 mg L{sup -1} with a R.S.D. 2.4% for 100 mg L{sup -1} glucose, detection limit 0.02 mg L{sup -1} (3{sigma}) and retained its original activity after 3 weeks when stored at 6 deg. C. Optimal parameters in the determination of ethanol were selected as: applied potential +0.45 V versus Ag/AgCl, flow rate 0.2 mL min{sup -1} in 0.1 M phosphate buffer carrier (pH 7). Different structural designs of the ethanol sensor were tested and linearity obtained was up to 1000 mg L{sup -1} with a maximum R.S.D. of 5

  12. Hydrogen generation through massive corrosion of deformed aluminum in water

    Energy Technology Data Exchange (ETDEWEB)

    Czech, E.; Troczynski, T. [Materials Engineering Department, University of British Columbia, 309-6350 Stores Rd., Vancouver, BC V6T 1Z4 (Canada)

    2010-02-15

    Aluminum, one of most reactive metals, rapidly corrodes in strong acidic or alkaline solutions but passivates at pH of about 5-9. We have determined that the passivation of aluminum in this range of pH, and in particular in regular tap water, can be substantially prevented after milling of aluminum with water-soluble inorganic salts (referred to as ''WIS''), such as KCl or NaCl. Ensuing corrosion of Al in tap water, with accompanying release of hydrogen and precipitation of aluminum hydroxide, at normal pressure and moderate temperatures ({proportional_to}55 C) is rapid and substantial. For example, {proportional_to}92% of the Al in the Al-WIS system when milled for 1 h and {proportional_to}81% when milled for 15 min, corrodes in 1 h, with the release of 1.5 mol of hydrogen per each mole of Al consumed in the reaction. Besides gaseous hydrogen, only solid aluminum hydroxides were formed as the reaction byproducts, opening up the possibility of straightforward recycling of the system. The effects of WIS concentration, chemistry of other additives, powder particle size, temperature, and milling conditions on the reaction kinetics are reported. (author)

  13. Near-Monodisperse Ni-Cu Bimetallic Nanocrystals of Variable Composition: Controlled Synthesis and Catalytic Activity for H2 Generation

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Yawen; Huang, Wenyu; Habas, Susan E.; Kuhn, John N.; Grass, Michael E.; Yamada, Yusuke; Yang, Peidong; Somorjai, Gabor A.

    2008-07-22

    Near-monodisperse Ni{sub 1-x}Cu{sub x} (x = 0.2-0.8) bimetallic nanocrystals were synthesized by a one-pot thermolysis approach in oleylamine/1-octadecene, using metal acetylacetonates as precursors. The nanocrystals form large-area 2D superlattices, and display a catalytic synergistic effect in the hydrolysis of NaBH{sub 4} to generate H{sub 2} at x = 0.5 in a strongly basic medium. The Ni{sub 0.5}Cu{sub 0.5} nanocrystals show the lowest activation energy, and also exhibit the highest H{sub 2} generation rate at 298 K.

  14. Hydrogen production from catalytic decomposition of methane; Produccion de hidrogeno a partir de la descomposicion termica catalitica del biogas de digestion anaerobia

    Energy Technology Data Exchange (ETDEWEB)

    Belsue Echevarria, M.; Etxebeste Juarez, O.; Perez Gil, S.

    2002-07-01

    The need of substitution of part of the energy obtained from fossil fuels instead of energy from renewable sources, together with the minimal emissions of CO{sub ''} and CO that are expected with these technologies, make renewable sources a very attractive predecessor for the production of hydrogen. In this situation, a usable source for hydrogen production is the biogas achieved by means of technologies like the anaerobic digestion of different kinds of biomass (MSW, sewage sludge, stc.). In this article we suggest the Thermal Catalytic Decomposition of the methane contained in this biogas, after separation of pollutants like CO{sub ''}, H{sub 2}S. steam. This technology will give hydrogen, usable in fuel cells, and nanoestructured carbon as products. (Author) 7 refs.

  15. Autothermal hydrogen storage and delivery systems

    Science.gov (United States)

    Pez, Guido Peter; Cooper, Alan Charles; Scott, Aaron Raymond

    2011-08-23

    Processes are provided for the storage and release of hydrogen by means of dehydrogenation of hydrogen carrier compositions where at least part of the heat of dehydrogenation is provided by a hydrogen-reversible selective oxidation of the carrier. Autothermal generation of hydrogen is achieved wherein sufficient heat is provided to sustain the at least partial endothermic dehydrogenation of the carrier at reaction temperature. The at least partially dehydrogenated and at least partially selectively oxidized liquid carrier is regenerated in a catalytic hydrogenation process where apart from an incidental employment of process heat, gaseous hydrogen is the primary source of reversibly contained hydrogen and the necessary reaction energy.

  16. Hydrogen generation systems and methods utilizing sodium silicide and sodium silica gel materials

    Science.gov (United States)

    Wallace, Andrew P.; Melack, John M.; Lefenfeld, Michael

    2015-08-11

    Systems, devices, and methods combine thermally stable reactant materials and aqueous solutions to generate hydrogen and a non-toxic liquid by-product. The reactant materials can sodium silicide or sodium silica gel. The hydrogen generation devices are used in fuels cells and other industrial applications. One system combines cooling, pumping, water storage, and other devices to sense and control reactions between reactant materials and aqueous solutions to generate hydrogen. Springs and other pressurization mechanisms pressurize and deliver an aqueous solution to the reaction. A check valve and other pressure regulation mechanisms regulate the pressure of the aqueous solution delivered to the reactant fuel material in the reactor based upon characteristics of the pressurization mechanisms and can regulate the pressure of the delivered aqueous solution as a steady decay associated with the pressurization force. The pressure regulation mechanism can also prevent hydrogen gas from deflecting the pressure regulation mechanism.

  17. Development of generator-cooling hydrogen purity improvement system using hydrogen absorbing alloy; Suiso kyuzo gokin ni yoru hatsudenkinai suiso jundo kojo system no kaihatsu

    Energy Technology Data Exchange (ETDEWEB)

    Nishimura, Y.; Sato, J.; Haruki, N.; Kogi, T.; Okuno, Y. [The Kansai Electric Power Co. Inc., Osaka (Japan); Takeda, H.; Wakisaka, Y. [The Japan Steel Works, Ltd., Tokyo (Japan); Fujita, T. [Mitsubishi Electric Corp., Tokyo (Japan)

    1997-01-31

    A generator-cooling hydrogen purity improvement system was developed by utilizing hydrogen absorbing and discharging functions of hydrogen storage alloy. For demonstration test with an actual machine, four elements, Ca, Ni, Mm and Al, were used as hydrogen storage alloys. To treat hydrogen gas with a wide range of purity and reduce hydrogen gas feed, flow operation for hydrogen purity improvement, batch operation, and recycle operation for maintaining the hydrogen purity were performed. As a result of the generator-cooling hydrogen purity improvement demonstration test, it was found that the hydrogen purity can be enhanced from 97.69% before operation to 99.9% after operation for 104 hours and to 99.95% after operation for 140 hours. The hydrogen recovery rates during flow test and batch test were between 92 and 95%. For the hydrogen purity maintaining test, it was confirmed that the high hydrogen purity of 99.9% has been continuously maintained for 140 days, and that the hydrogen recovery rate was over 99%. 2 refs., 15 figs., 3 tabs.

  18. Catalytic De/hydrogenation in Mg by co-doped Ni and VO{sub x} on active carbon: extremely fast kinetics at low temperatures and high hydrogen capacity

    Energy Technology Data Exchange (ETDEWEB)

    Jia, Yi; Cheng, Lina [ARC Centre of Excellence for Functional Nanomaterials, University of Queensland, Brisbane (Australia); School of Mechanical and Mining Engineering, University of Queensland, Brisbane (Australia); Pan, Nan [Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, Hefei (China); Zou, Jin [School of Mechanical and Mining Engineering, University of Queensland, Brisbane (Australia); Lu, Gaoqing (Max) [ARC Centre of Excellence for Functional Nanomaterials, University of Queensland, Brisbane (Australia); Yao, Xiangdong [ARC Centre of Excellence for Functional Nanomaterials, University of Queensland, Brisbane (Australia); Queensland Micro- and Nanotechnology Centre (QMNC), Griffith University, Brisbane (Australia)

    2011-05-15

    A multi-component catalyst Ni-VO{sub x}/AC (VO{sub x} is comprised of V{sub 2}O{sub 5} and VO{sub 2}, x = 2.18) was synthesized by a wet impregnation method. The synthesized Ni-VO{sub x}/AC shows a superior catalytic effect on de/hydrogenation of Mg. The MgH{sub 2}+Ni-VO{sub x}/AC composites can absorb 6.2 wt.-% hydrogen within only 1 min at 150 C under a hydrogen pressure of 2 MPa and desorb 6.5 wt.-% hydrogen within 10 min at 300 C under an initial hydrogen pressure of 1 KPa, which overcomes a critical barrier for practical use of Mg as a hydrogen storage material. A significant decrease of activation energy (E{sub a}) indicates that Ni-VO{sub x}/AC catalyst is highly efficient for Mg de/hydrogenation, which may be ascribed to the synergistic effect of bimetals (metal oxides) and nanocarbon. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  19. Selective Electrochemical Generation of Hydrogen Peroxide from Water Oxidation

    DEFF Research Database (Denmark)

    Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Nørskov, Jens K.

    2015-01-01

    Water is a life-giving source, fundamental to human existence, yet over a billion people lack access to clean drinking water. The present techniques for water treatment such as piped, treated water rely on time and resource intensive centralized solutions. In this work, we propose a decentralized...... sufficiently weakly, such as SnO2, can activate hydrogen peroxide evolution. We present a rational design principle for the selectivity in electrochemical water oxidation and identify new material candidates that could perform H2O2 evolution selectively....

  20. Zircaloy-oxidation and hydrogen-generation rates in degraded-core accident situations

    International Nuclear Information System (INIS)

    Oxidation of Zircaloy cladding is the primary source of hydrogen generated during a degraded-core accident. In this paper, reported Zircaloy oxidation rates, either measured at 1500 to 18500C or extrapolated from the low-temperature data obtained at 0C, are critically reviewed with respect to their applicability to a degraded-core accident situation in which the high-temperature fuel cladding is likely to be exposed to and oxidized in mixtures of hydrogen and depleted steam, rather than in an unlimited flux of pure steam. New results of Zircaloy oxidation measurements in various mixtures of hydrogen and steam are reported for >15000C. The results show significantly smaller oxidation and, hence, hydrogen-generation rates in the mixture, compared with those obtained in pure steam. It is also shown that a significant fraction of hydrogen, generated as a result of Zircaloy oxidation, is dissolved in the cladding material itself, which prevents that portion of hydrogen from reaching the containment building space. Implications of these findings are discussed in relation to a more realistic method of quantifying the hydrogen source term for a degraded-core accident analysis

  1. Control of microbially generated hydrogen sulfide in produced waters

    Energy Technology Data Exchange (ETDEWEB)

    Burger, E.D.; Vance, I.; Gammack, G.F.; Duncan, S.E.

    1995-12-31

    Production of hydrogen sulfide in produced waters due to the activity of sulfate-reducing bacteria (SRB) is a potentially serious problem. The hydrogen sulfide is not only a safety and environmental concern, it also contributes to corrosion, solids formation, a reduction in produced oil and gas values, and limitations on water discharge. Waters produced from seawater-flooded reservoirs typically contain all of the nutrients required to support SRB metabolism. Surface processing facilities provide a favorable environment in which SRB flourish, converting water-borne nutrients into biomass and H{sub 2}S. This paper will present results from a field trial in which a new technology for the biochemical control of SRB metabolism was successfully applied. A slip stream of water downstream of separators on a produced water handling facility was routed through a bioreactor in a side-steam device where microbial growth was allowed to develop fully. This slip stream was then treated with slug doses of two forms of a proprietary, nonbiocidal metabolic modifier. Results indicated that H{sub 2}S production was halted almost immediately and that the residual effect of the treatment lasted for well over one week.

  2. Influence of different preparation conditions on catalytic activity of ag /gama-al/sub 2/o/sub 3/ for hydrogenation of coal slime pyrolysis

    International Nuclear Information System (INIS)

    This paper, introducing variable conditional factors with Ag/AL/sub 2/O/sub 3/ as catalyst, selects five variables to investigate the influences of experimental conditions on Ag/Al2O/sub 3/ catalytic activity and define the optimal process conditions. These variables include Ag loading amount, calcinations temperature, calcinations time, reduction temperature, reduction time. X ray diffraction (XRD), hydrogen temperature-programmed reduction (TPR), X ray photoelectron spectrum (XPS) and scanning electron microscopy (SEM) were utilized to characterize the catalytic activity of Ag/-Al/sub 2/O/sub 3/, active center structure and state and those of carrier were emphatically studied, In the meantime the effects of active center and carrier on catalytic activity are studied. The results showed that: (1) In the range of 600 degree C-900 degree C, the catalytic activity of Ag/-Al/sub 2/O/sub 3/ with different loading showed little difference when changing loading amount, in the range of 900 degree C-1100 degree C, when the loading was 5%, the catalytic activity was very high; From the XRD and SEM characterizations, when the loading was 5%, it showed strong intensity diffraction peak of Ag crystal, crystal Ag is the most important activity center to promote hydrogen yield. (2) the catalytic activity of Ag/-Al/sub 2/O/sub 3/ at 450 degree C was considerably higher than that at 400 degree C and 500 degree C. By BET, XRD and SEM characterization, it can be seen, the diffraction peaks intensity of Ag crystal at 450 degree C is higher and sharper than that at 400 degree C and 500 degree C and with the increase of calcinations temperature, the specific surface area of catalysts also increased. (3) In the range of 600 degree C - 1000 degree C, the effects of calcinations time can be negligible, while, with temperature higher than 1000 degree C, 4-hour-calcinations-time catalyst exhibits a more noticeable catalytic activity than 3-hour and 5-hour catalyst do; From the XRD

  3. DESIGN, SYNTHESIS AND STUDY OF MULTI-COMPONENT AND INTEGRATED SYSTEMS FOR LIGHT-DRIVEN HYDROGEN GENERATION

    Energy Technology Data Exchange (ETDEWEB)

    Professor Richard Eisenberg

    2012-07-18

    The research focussed on fundamental problems in the conversion of light to stored chemical energy. Specifically, work was completed on the design, synthesis and study of multi-component super- and supramolecular systems for photoinduced charge separation, one of the key steps in artificial photosynthesis, and on the use of these and related systems for the photochemical generation of H2 from water. At the center of these systems are chromophores comprised of square planar coordinated Pt(II) ions with arylacetylide and either diimine or terpyridyl ligands. Previous work had shown that the chromophores are photoluminescent in fluid solution with long-lived metal-to-ligand charge transfer (3MLCT) excited states that are necessarily directional. An advance which set the stage for a number of proposed studies was the light-driven production of hydrogen from water using a Pt(terpyridyl)(arylacetylide)+ chromophore and a sacrificial electron donor. The reaction is catalytic and appears to rival previously reported ruthenium bipyridyl systems in terms of H2 production. Variation of system components and mechanistic studies were conducted to understand better the individual steps in the overall process and how to improve its efficiency. Success with light driven H2 generation was employed as a key probe as new systems were constructed consisting of triads for photoinduced charge separation placed in close proximity to the H2 generating catalyst - a Pt colloid - through direct linkage or supramolecular interactions with the polymer used to stabilize the colloid. In order to prepare new donor-chromophore-acceptor (D-C-A) triads and associated D-C and C-A dyads, new ligands were synthesized having functional groups for different coupling reactions such as simple amide formation and Pd-catalyzed coupling. In these systems, the donor was attached to the arylacetylide ligands and the acceptor was linked to the diimine or terpyridyl chelate. Research under the contract proved

  4. Electrodeposited synthesis of self-supported Ni-P cathode for efficient electrocatalytic hydrogen generation

    Directory of Open Access Journals (Sweden)

    Ruixian Wu

    2016-06-01

    Full Text Available One of the key challenges for electrochemical water splitting is the development of low-cost and efficient hydrogen evolution cathode. In this work, a self-supported Ni-P cathode was synthesized by a facile electrodeposition method. The composition and morphology were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. The Ni-P cathode performed low onset over-potential, good catalytic activity and long-term stability under neutral and alkaline conditions. The mechanism of Ni-P electrode for hydrogen production was discussed by electrochemical impedance spectroscopy. The excellent performance of Ni-P cathode was mainly attributed to the synergistic effect of phosphate anions and the self-supported feature.

  5. Electrodeposited synthesis of self-supported Ni-P cathode for efficient electrocatalytic hydrogen generation

    Institute of Scientific and Technical Information of China (English)

    Ruixian Wu; Yuming Dong n; Pingping Jiang; Guangli Wang; Yanmei Chen; Xiuming Wu

    2016-01-01

    One of the key challenges for electrochemical water splitting is the development of low-cost and efficient hydrogen evolution cathode. In this work, a self-supported Ni-P cathode was synthesized by a facile electrodeposition method. The composition and morphology were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. The Ni-P cathode performed low onset over-potential, good catalytic activity and long-term stability under neutral and alkaline conditions. The mechanism of Ni-P electrode for hydrogen production was discussed by electrochemical impedance spectroscopy. The excellent performance of Ni-P cathode was mainly attributed to the synergistic effect of phosphate anions and the self-supported feature.

  6. Empirical rate equation model and rate calculations of hydrogen generation for Hanford tank waste; FINAL

    International Nuclear Information System (INIS)

    Empirical rate equations are derived to estimate hydrogen generation based on chemical reactions, radiolysis of water and organic compounds, and corrosion processes. A comparison of the generation rates observed in the field with the rates calculated for twenty eight tanks shows agreement with in a factor of two to three

  7. Hydrogen generation from steam reforming of ethanol in dielectric barrier discharge

    Institute of Scientific and Technical Information of China (English)

    Baowei Wang; Yijun Lü; Xu Zhang; Shuanghui Hu

    2011-01-01

    Dielectric barrier discharge(DBD)was used for the generation of hydrogen from ethanol reforming.Effects of reaction conditions,such as vaporization temperature,ethanol flow rate,water/ethanol ratio,and addition of oxygen,on the ethanol conversion and hydrogen yield,were studied.The results showed that the increase of ethanol flow rate decreased ethanol conversion and hydrogen yield,and high water/ethanol ratio and addition of oxygen were advantageous.Ethanol conversion and hydrogen yield increased with the vaporization room temperature up to the maximum at first,and then decreased slightly.The maximum hydrogen yield of 31.8% was obtained at an ethanol conversion of 88.4% under the optimum operation conditions of vaporization room temperature of 120℃,ethanol flux of 0.18 mL/min,water/ethanol ratio of 7.7 and oxygen volume concentration of 13.3%.

  8. Hydrogen generation by nuclear power for sustainable development in the 21-st century

    International Nuclear Information System (INIS)

    Hydrogen is the main non-polluting fuel. It is produced by natural gas steam reforming, water electrolysis and thermonuclear processes. Currently, 4% of the hydrogen world production is obtained by water electrolysis. The use of nuclear power for hydrogen production avoids the generation of greenhouse gases and the dependence of primary external energy sources. The US is currently developing a modular reactor for hydrogen production and water desalination, STAR - H2 (Secure Transportable Autonomous Reactor for Hydrogen production) with fast neutrons, lead cooling and passive safety systems operating at a temperature of 780 deg C. Also, a Russian reactor of the same type is operated at 540 deg C. China and India joint industrial countries like France, Japan, Russia and US in recognizing that any strategies aiming at a future with clean energy implies the nuclear energy

  9. CHALLENGES IN GENERATING HYDROGEN BY HIGH TEMPERATURE ELECTROLYSIS USING SOLID OXIDE CELLS

    Energy Technology Data Exchange (ETDEWEB)

    M. S. Sohal; J. E. O' Brien; C. M. Stoots; M. G. McKellar; J. S. Herring; E. A. Harvego

    2008-03-01

    Idaho National Laboratory’s (INL) high temperature electrolysis research to generate hydrogen using solid oxide electrolysis cells is presented in this paper. The research results reported here have been obtained in a laboratory-scale apparatus. These results and common scale-up issues also indicate that for the technology to be successful in a large industrial setting, several technical, economical, and manufacturing issues have to be resolved. Some of the issues related to solid oxide cells are stack design and performance optimization, identification and evaluation of cell performance degradation parameters and processes, integrity and reliability of the solid oxide electrolysis (SOEC) stacks, life-time prediction and extension of the SOEC stack, and cost reduction and economic manufacturing of the SOEC stacks. Besides the solid oxide cells, balance of the hydrogen generating plant also needs significant development. These issues are process and ohmic heat source needed for maintaining the reaction temperature (~830°C), high temperature heat exchangers and recuperators, equal distribution of the reactants into each cell, system analysis of hydrogen and associated energy generating plant, and cost optimization. An economic analysis of this plant was performed using the standardized H2A Analysis Methodology developed by the Department of Energy (DOE) Hydrogen Program, and using realistic financial and cost estimating assumptions. The results of the economic analysis demonstrated that the HTE hydrogen production plant driven by a high-temperature helium-cooled nuclear power plant can deliver hydrogen at a cost of $3.23/kg of hydrogen assuming an internal rate of return of 10%. These issues need interdisciplinary research effort of federal laboratories, solid oxide cell manufacturers, hydrogen consumers, and other such stakeholders. This paper discusses research and development accomplished by INL on such issues and highlights associated challenges that need to

  10. Precipitation and calcination synthesis methods forming nano-sized platinum catalytic particles for methanol and hydrogen oxidation

    Science.gov (United States)

    Naidoo, S.; Naidoo, Q.; Musil, E.; Linkov, V.; Vaivars, G.

    2013-03-01

    Under varying experimental conditions of calcination and precipitation reactions, different particle sizes and levels of platinum on carbon supported (Pt/C) catalysts were obtained. Rapid precipitation following a chemical reaction ensured formation of nano-sized catalytic particles using super-saturated concentrations under controlled conditions was a significant contribution in understanding the synthesis process and how it relates to an increased number of catalytic reaction sites ultimately providing superior electrochemical (EC) activity. These conditions influenced nucleation and growth rates of the catalytic particles. The super-saturation concentrations of the reactants in the reaction vessel played a direct role in producing the desired morphology of the crystallites.

  11. Hydrogen Fuel Cell Analysis: Lessons Learned from Stationary Power Generation Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Scott E. Grasman; John W. Sheffield; Fatih Dogan; Sunggyu Lee; Umit O. Koylu; Angie Rolufs

    2010-04-30

    This study considered opportunities for hydrogen in stationary applications in order to make recommendations related to RD&D strategies that incorporate lessons learned and best practices from relevant national and international stationary power efforts, as well as cost and environmental modeling of pathways. The study analyzed the different strategies utilized in power generation systems and identified the different challenges and opportunities for producing and using hydrogen as an energy carrier. Specific objectives included both a synopsis/critical analysis of lessons learned from previous stationary power programs and recommendations for a strategy for hydrogen infrastructure deployment. This strategy incorporates all hydrogen pathways and a combination of distributed power generating stations, and provides an overview of stationary power markets, benefits of hydrogen-based stationary power systems, and competitive and technological challenges. The motivation for this project was to identify the lessons learned from prior stationary power programs, including the most significant obstacles, how these obstacles have been approached, outcomes of the programs, and how this information can be used by the Hydrogen, Fuel Cells & Infrastructure Technologies Program to meet program objectives primarily related to hydrogen pathway technologies (production, storage, and delivery) and implementation of fuel cell technologies for distributed stationary power. In addition, the lessons learned address environmental and safety concerns, including codes and standards, and education of key stakeholders.

  12. Influence of chirality on catalytic generation of nitric oxide and platelet behavior on selenocystine immobilized TiO2 films.

    Science.gov (United States)

    Fan, Yonghong; Pan, Xiaxin; Wang, Ke; Wu, Sisi; Han, Honghong; Yang, Ping; Luo, Rifang; Wang, Hong; Huang, Nan; Tan, Wei; Weng, Yajun

    2016-09-01

    As nitric oxide (NO) plays vital roles in the cardiovascular system, incorporating this molecule into cardiovascular stents is considered as an effective method. In the present study, selenocystine with different chirality (i.e., l- and d-selenocystine) was used as the catalytic molecule immobilized on TiO2 films for decomposing endogenous NO donor. The influences of surface chirality on NO release and platelet behavior were evaluated. Results show that although the amount of immobilized l-selenocystine on the surface was nearly the same as that of immobilized d-selenocystine, in vitro catalytic NO release tests showed that l-selenocystine immobilized surfaces were more capable of catalyzing the decomposition of S-nitrosoglutathione and thus generating more NO. Accordingly, l-selenocystine immobilized surfaces demonstrated significantly increased inhibiting effects on the platelet adhesion and activation, when compared to d-selenocystine immobilized ones. Measurement of the cGMP concentration of platelets further confirmed that surface chirality played an important role in regulating NO generation and platelet behaviors. Additionally, using bovine serum albumin and fibrinogen as model proteins, the protein adsorption determined with quartz crystal microbalance showed that the l-selenocystine immobilized surface enhanced protein adsorption. In conclusion, surface chirality significantly influences protein adsorption and NO release, which may have significant implications in the design of NO-generating cardiovascular stents. PMID:27153116

  13. Effect of hydrogen on generation of lattice defects in shock-loaded Pd

    Energy Technology Data Exchange (ETDEWEB)

    Melikhova, Oksana, E-mail: oksivmel@yahoo.com [Charles University in Prague, Faculty of Mathematics and Physics, V Holešovičkách 2, CZ-180 00 Praha 8 (Czech Republic); Čížek, Jakub [Charles University in Prague, Faculty of Mathematics and Physics, V Holešovičkách 2, CZ-180 00 Praha 8 (Czech Republic); Chen, Yuzeng [State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, 710072 Xi’an (China); Suo, Tao [School of Aeronautics, Northwestern Polytechnical University, 710072 Xi’an (China); Procházka, Ivan [Charles University in Prague, Faculty of Mathematics and Physics, V Holešovičkách 2, CZ-180 00 Praha 8 (Czech Republic); Liu, Feng [State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, 710072 Xi’an (China)

    2015-10-05

    Highlights: • Influence of hydrogen on defect generation during shock-loading of Pd was examined. • Shock-loading introduced dislocations and vacancies. • Deformation-induced vacancies agglomerated into clusters consisting of 2–3 vacancies. • Absorbed hydrogen facilitates generation of both dislocations and vacancies. - Abstract: The effect of hydrogen absorbed in fcc Pd lattice on the generation of dislocations and vacancies during plastic deformation by shock-loading was investigated in this work. Well annealed bulk Pd samples were firstly charged with hydrogen up to various hydrogen concentrations. Subsequently the samples were shock-loaded on a Split-Hopkinson apparatus. Shock-loading yields extremely high strain rate and causes intensive plastic deformation of the samples. Lattice defects of the shock-loaded samples were characterized by positron lifetime spectroscopy combined with X-ray diffraction. It was found that shock-loaded Pd samples exhibit not only high density of dislocations but also small vacancy clusters created by agglomeration of deformation-induced vacancies. Pre-charging of Pd samples with hydrogen increases both the dislocation density and the concentration of vacancy clusters.

  14. Lessons learned from hydrogen generation and burning during the TMI-2 event

    International Nuclear Information System (INIS)

    This document summarizes what has been learned from generation of hydrogen in the reactor core and the hydrogen burn that occurred in the containment building of the Three Mile Island Unit No. 2 (TMI-2) nuclear power plant on March 28, 1979. During the TMI-2 loss-of-coolant accident (LOCA), a large quantity of hydrogen was generated by a zirconium-water reaction. The hydrogen burn that occurred 9 h and 50 min after the initiation of the TMI-2 accident went essentially unnoticed for the first few days. Even through the burn increased the containment gas temperature and pressure to 12000F (6500C) and 29 lb/in2 (200 kPa) gage, there was no serious threat to the containment building. The processes, rates, and quantities of hydrogen gas generated and removed during and following the LOCA are described in this report. In addition, the methods which were used to define the conditions that existed in the containment building before, during, and after the hydrogen burn are described. The results of data evaluations and engineering calculations are presented to show the pressure and temperature histories of the atmosphere in various containment segments during and after the burn. Material and equipment in reactor containment buildings can be protected from burn damage by the use of relatively simple enclosures or insulation

  15. Catalytic dehydrogenation of isobutane in the presence of hydrogen over Cs-modified Ni{sub 2}P supported on active carbon

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Yanli [Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Technology, College of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Sang, Huanxin [Tianjin Academy of Environmental Sciences, Tianjin 300191 (China); Wang, Kang [Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Technology, College of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China); Wang, Xitao, E-mail: wangxt@tju.edu.cn [Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin Key Laboratory of Applied Catalysis Science and Technology, College of Chemical Engineering and Technology, Tianjin University, Tianjin 300072 (China)

    2014-10-15

    Graphical abstract: - Highlights: • Ni{sub 2}P catalyst is tested in dehydrogenation of isobutane for the first time. • The effects of Cs promoter on catalytic performance of Ni2P/AC were investigated. • Cs-Ni2P/AC exhibits high activity and selectivity for isobutane dehydrogenation. - Abstract: In this article, an environmentally friendly non-noble-metal class of Cs-Ni{sub 2}P/active carbon (AC) catalyst was prepared and demonstrated to exhibit enhanced catalytic performance in isobutane dehydrogenation. The results of activity tests reveal that Ni/AC catalyst was highly active for isobutane cracking, which led to the formation of abundant methane and coke. After the introduction of phosphorus through impregnation with ammonium di-hydrogen phosphate and H{sub 2}-temperature programmed reduction, undesired cracking reactions were effectively inhibited, and the selectivity to isobutene and stability of catalyst increased remarkably. The characterization results indicate that, after the addition of phosphorous, the improvement of dehydrogenation selectivity is ascribed to the partial positive charges carried on Ni surface in Ni{sub 2}P particles, which decreases the strength of Ni-C bond between Ni and carbonium-ion intermediates and the possibility of excessive dehydrogenation. In addition, Cs-modified Ni{sub 2}P/AC catalysts display much higher catalytic performance as compared to Ni{sub 2}P/AC catalyst. Cs-Ni{sub 2}P-6.5 catalyst has the highest catalytic performance, and the selectivity to isobutene higher than 93% can be obtained even after 4 h reaction. The enhancement in catalytic performance of the Cs-modified catalysts is mainly attributed to the function of Cs to improve the dispersion of Ni{sub 2}P particles, transfer electron from Cs to Ni, and decrease acid site number and strength.

  16. Application of solid-phase heterogeneous catalytic hydrogenation for preparation of ethanolamine labelled by tritium and ethanolamides of aroachidonic, eicosanepentaenic, docosahexaenic acids labelled by tritium partially

    International Nuclear Information System (INIS)

    Ethanolamine labelled with tritium with 35-40 Ci/mmol molar radioactivity is produced from glycolic acid nitrile by means of solid-phase heterogeneous catalytic hydrogenation on 5% Rh/C. Preparational quantities of labelled ethanolamine are produced with 10-20% yield with the use of 5% of pd?C and 70% of glycolic acid aqueous nitrile, the molar activity of the preparation required is 4-6 Ci/mmol. Ethanolamides of arachidonic, eicosapentaenoic, docosahexaenoic acids are synthesized from the labelled ethanolamine. The compound produced are tested by chromatographic and fermentative methods

  17. Catalytic Hydrogenation of the Sweet Principles of Stevia rebaudiana, Rebaudioside B, Rebaudioside C, and Rebaudioside D and Sensory Evaluation of Their Reduced Derivatives

    Directory of Open Access Journals (Sweden)

    Mary Campbell

    2012-11-01

    Full Text Available Catalytic hydrogenation of rebaudioside B, rebaudioside C, and rebaudioside D; the three ent-kaurane diterpene glycosides isolated from Stevia rebaudiana was carried out using Pd(OH2. Reduction of steviol glycosides was performed using straightforward synthetic chemistry with the catalyst Pd(OH2 and structures of the corresponding dihydro derivatives were characterized on the basis of 1D and 2D nuclear magnetic resonance (NMR spectral data indicating that all are novel compounds being reported for the first time. Also, the taste properties of all reduced compounds were evaluated against their corresponding original steviol glycosides and sucrose.

  18. High Performance, Low Cost Hydrogen Generation from Renewable Energy

    Energy Technology Data Exchange (ETDEWEB)

    Ayers, Katherine [Proton OnSite; Dalton, Luke [Proton OnSite; Roemer, Andy [Proton OnSite; Carter, Blake [Proton OnSite; Niedzwiecki, Mike [Proton OnSite; Manco, Judith [Proton OnSite; Anderson, Everett [Proton OnSite; Capuano, Chris [Proton OnSite; Wang, Chao-Yang [Penn State University; Zhao, Wei [Penn State University

    2014-02-05

    Renewable hydrogen from proton exchange membrane (PEM) electrolysis is gaining strong interest in Europe, especially in Germany where wind penetration is already at critical levels for grid stability. For this application as well as biogas conversion and vehicle fueling, megawatt (MW) scale electrolysis is required. Proton has established a technology roadmap to achieve the necessary cost reductions and manufacturing scale up to maintain U.S. competitiveness in these markets. This project represents a highly successful example of the potential for cost reduction in PEM electrolysis, and provides the initial stack design and manufacturing development for Proton’s MW scale product launch. The majority of the program focused on the bipolar assembly, from electrochemical modeling to subscale stack development through prototyping and manufacturing qualification for a large active area cell platform. Feasibility for an advanced membrane electrode assembly (MEA) with 50% reduction in catalyst loading was also demonstrated. Based on the progress in this program and other parallel efforts, H2A analysis shows the status of PEM electrolysis technology dropping below $3.50/kg production costs, exceeding the 2015 target.

  19. Cobalt-Nanocrystal-Assembled Hollow Nanoparticles for Electrocatalytic Hydrogen Generation from Neutral-pH Water.

    Science.gov (United States)

    Liu, Bingrui; Zhang, Lin; Xiong, Weilin; Ma, Mingming

    2016-06-01

    Highly active and stable electrocatalysts for hydrogen generation from neutral-pH water are highly desired, but very difficult to achieve. Herein we report a facile synthetic approach to cobalt nanocrystal assembled hollow nanoparticles (Co-HNP), which serve as an electrocatalyst for hydrogen generation from neutral-pH water. An electrode composed of Co-HNP on a carbon cloth (CC) produces cathodic current densities of 10 and 100 mA cm(-2) at overpotentials of -85 mV and -237 mV, respectively. The Co-HNP/CC electrode retains its high activity after 20 h hydrogen generation at a high current density of 150 mA cm(-2) , indicating the superior activity and stability of Co-HNP as electrocatalyst. PMID:27125576

  20. Stabilization of Wind Energy Conversion System with Hydrogen Generator by Using EDLC Energy Storage System

    Science.gov (United States)

    Shishido, Seiji; Takahashi, Rion; Murata, Toshiaki; Tamura, Junji; Sugimasa, Masatoshi; Komura, Akiyoshi; Futami, Motoo; Ichinose, Masaya; Ide, Kazumasa

    The spread of wind power generation is progressed hugely in recent years from a viewpoint of environmental problems including global warming. Though wind power is considered as a very prospective energy source, wind power fluctuation due to the random fluctuation of wind speed has still created some problems. Therefore, research has been performed how to smooth the wind power fluctuation. This paper proposes Energy Capacitor System (ECS) for the smoothing of wind power which consists of Electric Double-Layer Capacitor (EDLC) and power electronics devices and works as an electric power storage system. Moreover, hydrogen has received much attention in recent years from a viewpoint of exhaustion problem of fossil fuel. Therefore it is also proposed that a hydrogen generator is installed at the wind farm to generate hydrogen. In this paper, the effectiveness of the proposed system is verified by the simulation analyses using PSCAD/EMTDC.

  1. Carbon and hydrogen isotopic composition and generation pathway of biogenic gas in China

    Institute of Scientific and Technical Information of China (English)

    SHEN Ping; WANG Xiaofeng; XU Yin; SHI Baoguang; XU Yongchang

    2009-01-01

    The carbon and hydrogen isotopic composition of biogenic gas is of great importance for the study of its generation pathway and reservoiring characteristics. In this paper, the formation pathways and reservoiring characteristics of biogenic gas reservoirs in China are described in terms of the carbon and hydrogen isotopic compositions of 31 gas samples from 10 biogenic gas reservoirs. The study shows that the hydrogen isotopic compositions of these biogenic gas reservoirs can be divided into three intervals:δDCH4>-200‰,-250‰<δDCH4<-200‰ and δDCH4<-250‰. The forerunners believed that the main generation pathway of biogenic gas under the condition of continental fresh water is acetic fermentation. Our research results showed that the generation pathway of biogenic gas under the condition of marine facies is typical CO2- reduction, the biogenic gas has heavy hydrogen isotopic composition: its δDCH4 values are higher than -200‰; that the biogenic gas under the condition of continental facies also was generated by the same way, but its hydrogen isotopic composition is lighter than that of biogenetic gas generated under typical marine facies condition: -250‰<δDCH4<-200‰, the δDCH4 values may be related to the salinity of the water medium in ancient lakes. From the relevant data of the Qaidam Basin, it can be seen that the hydrogen isotopic composition of biogenic methane has the same variation trend with increasing salinity of water medium. There are biogenic gas reservoirs formed in transitional regions under the condition of continental facies. These gas reservoirs resulted from both CO2- reduction and acetic fermentation, the formation of which may be related to the non-variant salinity of ancient water medium and the relatively high geothermal gradient, as is the case encountered in the Baoshan Basin. The biogenic gas generating in these regions has light hydrogen isotopic composition: δDCH4<-250‰, and relatively heavy carbon isotopic

  2. Optimal generation scheduling for renewable microgrids using hydrogen storage systems

    OpenAIRE

    Petrollese, Mario

    2015-01-01

    The topic of this thesis is the development of a tool for an optimal energy management strategy (EMS) of the generators and energy storage systems constituent microgrids, both grid-connected or isolated (stand-alone power system) powered by Renewable Energy Sources (RES). In particular, a novel control system is designed based on the resolution of the unit commitment problem. For each time step, the proposed control system compares the expected power produced by the renewabl...

  3. High Surface Area Tungsten Carbides: Synthesis, Characterization and Catalytic Activity towards the Hydrogen Evolution Reaction in Phosphoric Acid at Elevated Temperatures

    DEFF Research Database (Denmark)

    Tomás García, Antonio Luis; Li, Qingfeng; Jensen, Jens Oluf;

    2014-01-01

    Tungsten carbide powders were synthesized as a potential electrocatalyst for the hydrogen evolution reaction in phosphoric acid at elevated temperatures. With ammonium metatungstate as the precursor, two synthetic routes with and without carbon templates were investigated. Through the intermediate...... nitride route and with carbon black as template, the obtained tungsten carbide samples had higher BET area. In 100% H3PO4 at temperatures up to 185°C, the carbide powders showed superior activity towards the hydrogen evolution reaction. A deviation was found in the correlation between the BET area...... and catalytic activity; this was attributed to the presence of excess amorphous carbon in the carbide powder. TEM imaging and TGA-DTA results revealed a better correlation of the activity with the carbide particle size....

  4. Application of STATCOM/BESS for wind power smoothening and hydrogen generation

    Energy Technology Data Exchange (ETDEWEB)

    Muyeen, S.M.; Takahashi, Rion; Murata, Toshiaki; Tamura, Junji [Department of EEE, Kitami Institute of Technology, 165 Koen-cho, Hokkaido, Kitami 090-8507 (Japan); Ali, Mohd. Hasan [Department of Electrical and Computer Engineering, Ryerson University, 245 Church Street, Toronto (Canada)

    2009-02-15

    This paper proposes static synchronous compensator (STATCOM) incorporated with battery energy storage system (STATCOM/BESS) to smooth the line power of wind farm consists of fixed-speed wind generators. Constant output power reference is not a good choice because there may be some cases where wind speed is very low and then sufficient power cannot be obtained. In that case, energy storage device can solve the problem but large energy capacity may be needed. This paper proposes exponential moving average (EMA) to generate the reference output power, and thus the energy capacity of BESS unit can be small. Another salient feature of this study is the generation of hydrogen by using wind energy. At the wind farm terminal, two topologies of hydrogen generators are considered to be connected and their merits and demerits are analyzed. Finally, by taking the advantage of STATCOM/BESS, simple hydrogen generator topology composed of rectifier and electrolyzer is proposed. Detailed modeling and control strategy of hydrogen generator and STATCOM/BESS topologies are discussed and a cooperative control is developed. The effectiveness of the proposed system is verified by the simulation analysis using PSCAD/EMTDC. (author)

  5. Experimental and numerical investigation of the catalytic partial oxidation of methane to synthesis gas for power generation applications[Dissertation 17183

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, A.

    2007-07-01

    The present work addresses the catalytic partial oxidation (CPO) of methane to synthesis gas, with particular emphasis on power generation applications. A combined experimental and numerical investigation of methane partial oxidation to synthesis gas (H{sub 2}, CO) over rhodium-based catalysts has been carried out at pressures of up to 10 bar. The reactivity of the produced hydrogen and the suitably-low light-off temperatures of the CPO reactor, greatly facilitate operation of power generation gas turbines with reduced NO{sub x} emissions, stable operation with low calorific value fuels, and new combustion strategies for efficient CO{sub 2} capture. Those strategies utilize CPO of methane with oxygen (separated from air) and large exhaust gas recycle (H{sub 2}O and CO{sub 2}). An optically accessible catalytic channel-flow reactor was used to carry out Raman spectroscopy of major gas-phase species and laser induced fluorescence (LIF) of formaldehyde, in order to gain fundamental information on the catalytic and gas-phase chemical pathways. Transverse concentration profiles measured by the spontaneous Raman scattering technique determined the catalytic reactivity, while the LIF provided flame shapes and anchoring positions that, in turn, characterized the gaseous reactivity. Comparison between measurements and 2-D CFD computations, led to the validation of detailed catalytic and gas-phase reaction mechanisms. Experiments in a subscale gas-turbine honeycomb catalytic reactor have shown that the foregoing reaction mechanisms were also appropriate under gas-turbine relevant conditions with short reactant residence times. The light-off behavior of the subscale honeycomb reactor was reproduced by transient 2-D CFD computations. Ignition and extinction in CPO was studied. It was shown that, despite the chemical impact of the H{sub 2}O diluent during the transient catalytic ignition event, the light-off times themselves were largely unaffected by the exhaust gas dilution

  6. Development status of solid polymer electrolyte water electrolysis for large scale hydrogen generation

    Science.gov (United States)

    Russell, J. H.

    1981-03-01

    Solid polymer water electrolysis technology for large scale hydrogen generation is reviewed. A hydrogen generator module, capable of producing 2000 SCFH, was operated successfully for over 700 hours in the 200 kW system. Test results and further information are presented. Technology development was continued in support of improving both capital cost and conversion efficiency. Progress made in the development of the 10 sq ft active area cell included completion of the initial design, the beginning of fabrication development, and installation of new facilities for cell manufacture.

  7. Generating hydrogen for mobile devices; Wasserstofferzeugung fuer die mobile Anwendung

    Energy Technology Data Exchange (ETDEWEB)

    Schuetz, W. [Vodafone Pilotentwicklung GmbH, Muenchen (Germany)

    2001-10-01

    In future vehicles, more and more functions will be powered by electricity. These are for example ''steer by wire'', ''break by wire'', air conditioning and infotainment. This growing demand for electricity is a new challenge for the automotive industry. The so called APU (auxilliary power unit) is a convincing solution. This power generating unit based on fuel cell technology will provide electrical power in all operation situations. The article deals with the main focus of P{sup 21}-power for the 21st century, the Mannesmann Fuel Cell Product Center of the Vodafone Pilotentwicklung. (orig.)

  8. Effect of torrefaction pretreatment and catalytic pyrolysis on the pyrolysis poly-generation of pine wood.

    Science.gov (United States)

    Chen, Dengyu; Li, Yanjun; Deng, Minsi; Wang, Jiayang; Chen, Miao; Yan, Bei; Yuan, Qiqiang

    2016-08-01

    Torrefaction of pine wood was performed in a tube furnace at three temperatures (220, 250, and 280°C) for 30min. Then catalytic pyrolysis of raw and torrefied pine wood was performed using HZSM-5 catalyst in a fixed-bed pyrolysis reactor at 550°C for 15min. Torrefaction pretreatment and catalytic pyrolysis have an very important effect on the yield, property, and energy distribution of pyrolysis products. The results showed that the yield of biochar rapidly increased, while that of bio-oil decreased with increasing torrefaction temperature. The oxy-compound content of bio-oil, such as acids and aldehydes, sharply decreased. However, the aromatic hydrocarbon content not only increased but also further promoted by HZSM-5 catalyst. With highest mass yields and energy yields, biochar was also the very important product of pyrolysis. The oxygen content in biomass was mainly removed in the form of CO2 and H2O, leading to increasing CO2 content in non-condensable gas.

  9. Effect of torrefaction pretreatment and catalytic pyrolysis on the pyrolysis poly-generation of pine wood.

    Science.gov (United States)

    Chen, Dengyu; Li, Yanjun; Deng, Minsi; Wang, Jiayang; Chen, Miao; Yan, Bei; Yuan, Qiqiang

    2016-08-01

    Torrefaction of pine wood was performed in a tube furnace at three temperatures (220, 250, and 280°C) for 30min. Then catalytic pyrolysis of raw and torrefied pine wood was performed using HZSM-5 catalyst in a fixed-bed pyrolysis reactor at 550°C for 15min. Torrefaction pretreatment and catalytic pyrolysis have an very important effect on the yield, property, and energy distribution of pyrolysis products. The results showed that the yield of biochar rapidly increased, while that of bio-oil decreased with increasing torrefaction temperature. The oxy-compound content of bio-oil, such as acids and aldehydes, sharply decreased. However, the aromatic hydrocarbon content not only increased but also further promoted by HZSM-5 catalyst. With highest mass yields and energy yields, biochar was also the very important product of pyrolysis. The oxygen content in biomass was mainly removed in the form of CO2 and H2O, leading to increasing CO2 content in non-condensable gas. PMID:27183238

  10. Hydrogen generation in microbial reverse-electrodialysis electrolysis cells using a heat-regenerated salt solution.

    Science.gov (United States)

    Nam, Joo-Youn; Cusick, Roland D; Kim, Younggy; Logan, Bruce E

    2012-05-01

    Hydrogen gas can be electrochemically produced in microbial reverse-electrodialysis electrolysis cells (MRECs) using current derived from organic matter and salinity-gradient energy such as river water and seawater solutions. Here, it is shown that ammonium bicarbonate salts, which can be regenerated using low-temperature waste heat, can also produce sufficient voltage for hydrogen gas generation in an MREC. The maximum hydrogen production rate was 1.6 m(3) H(2)/m(3)·d, with a hydrogen yield of 3.4 mol H(2)/mol acetate at a salinity ratio of infinite. Energy recovery was 10% based on total energy applied with an energy efficiency of 22% based on the consumed energy in the reactor. The cathode overpotential was dependent on the catholyte (sodium bicarbonate) concentration, but not the salinity ratio, indicating high catholyte conductivity was essential for maximizing hydrogen production rates. The direction of the HC and LC flows (co- or counter-current) did not affect performance in terms of hydrogen gas volume, production rates, or stack voltages. These results show that the MREC can be successfully operated using ammonium bicarbonate salts that can be regenerated using conventional distillation technologies and waste heat making the MREC a useful method for hydrogen gas production from wastes.

  11. Hydrogen Generation in Microbial Reverse-Electrodialysis Electrolysis Cells Using a Heat-Regenerated Salt Solution

    KAUST Repository

    Nam, Joo-Youn

    2012-05-01

    Hydrogen gas can be electrochemically produced in microbial reverse-electrodialysis electrolysis cells (MRECs) using current derived from organic matter and salinity-gradient energy such as river water and seawater solutions. Here, it is shown that ammonium bicarbonate salts, which can be regenerated using low-temperature waste heat, can also produce sufficient voltage for hydrogen gas generation in an MREC. The maximum hydrogen production rate was 1.6 m3 H2/m3·d, with a hydrogen yield of 3.4 mol H2/mol acetate at a salinity ratio of infinite. Energy recovery was 10% based on total energy applied with an energy efficiency of 22% based on the consumed energy in the reactor. The cathode overpotential was dependent on the catholyte (sodium bicarbonate) concentration, but not the salinity ratio, indicating high catholyte conductivity was essential for maximizing hydrogen production rates. The direction of the HC and LC flows (co- or counter-current) did not affect performance in terms of hydrogen gas volume, production rates, or stack voltages. These results show that the MREC can be successfully operated using ammonium bicarbonate salts that can be regenerated using conventional distillation technologies and waste heat making the MREC a useful method for hydrogen gas production from wastes. © 2012 American Chemical Society.

  12. Understanding oscillatory phenomena in molecular hydrogen generation via sodium borohydride hydrolysis.

    Science.gov (United States)

    Budroni, M A; Biosa, E; Garroni, S; Mulas, G R C; Marchettini, N; Culeddu, N; Rustici, M

    2013-11-14

    The hydrolysis of borohydride salts represents one of the most promising processes for the generation of high purity molecular hydrogen under mild conditions. In this work we show that the sodium borohydride hydrolysis exhibits a fingerprinting periodic oscillatory transient in the hydrogen flow over a wide range of experimental conditions. We disproved the possibility that flow oscillations are driven by supersaturation phenomena of gaseous bubbles in the reactive mixture or by a nonlinear thermal feedback according to a thermokinetic model. Our experimental results indicate that the NaBH4 hydrolysis is a spontaneous inorganic oscillator, in which the hydrogen flow oscillations are coupled to an "oscillophor" in the reactive solution. The discovery of this original oscillator paves the way for a new class of chemical oscillators, with fundamental implications not only for testing the general theory on oscillations, but also with a view to chemical control of borohydride systems used as a source of hydrogen based green fuel. PMID:24084866

  13. Coupling a PEM fuel cell and the hydrogen generation from aluminum waste cans

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, Susana Silva; Albanil Sanchez, Loyda; Alvarez Gallegos, Alberto A. [Centro de Investigacion en Ingenieria y Ciencias Aplicadas, Av. Universidad 1001, Col. Chamilpa, Cuernavaca, Mor. CP 62210 (Mexico); Sebastian, P.J. [Centro de Investigacion en Energia-UNAM, 62580 Temixco, Morelos (Mexico); Cuerpo Academico de Energia y Sustentabilidad, UPCH, Tuxtla Gutierrez, Chiapas (Mexico)

    2007-10-15

    High purity hydrogen was generated from the chemical reaction of aluminum and sodium hydroxide. The aluminum used in this study was obtained from empty soft drink cans and treated with concentrated sulfuric acid to remove the paint and plastic film. One gram of aluminum was reacted with a solution of 2moldm{sup -3} of sodium hydroxide to produce hydrogen. The hydrogen produced from aluminum cans and oxygen obtained from a proton exchange membrane electrolyzer or air, was fed to a proton exchange membrane (PEM) fuel cell to produce electricity. Yields of 44 mmol of hydrogen contained in a volume of 1.760dm{sup 3} were produced from one gram of aluminum in a time period of 20 min. (author)

  14. Hydrogen-generating reactions in LWR severe accidents

    International Nuclear Information System (INIS)

    The available data on the reactions of Zircaloys, stainless steels, uranium metal and uranium dioxide with steam at temperatures above about 10000C and the reactions of core melts during concrete penetration have been reviewed and assessed for the IDCOR Program. The uranium metal is included because small quantities can be formed from the high temperature interaction between Zircaloy and uranium dioxide and because the uranium data adds insight into the nature of the reactions of core materials with steam. Thermodynamic analyses and comparisons of reaction rate data have been made. One of the purposes of this assessment was to develop fully the information generated in the early studies of oxidation processes, particularly the extensive program carried out at ANL from about 1960 to 1968

  15. Research Progress in Catalytic Hydrogenation of CO2 to Ethanol%CO2催化加氢制乙醇研究进展

    Institute of Scientific and Technical Information of China (English)

    王慧敏; 杨绪壮; 张兵兵; 苏海全

    2012-01-01

    燃料乙醇是可再生的清洁燃料,具有替代汽油的应用前景.以CO2气体为碳源并通过催化加氢制燃料乙醇具有环境保护和节约能源的现实意义.主要介绍了CO2催化加氢的反应机理以及催化剂活性组分、前驱物、助剂及载体对催化活性、产物选择性的影响,同时介绍了反应条件对催化过程的影响.%Fuel ethanol is often regarded as a potential renewable clean alternative fuel to gasoline. It has practical significance of environmental protection and energy conservation to synthesize fuel ethanol by the hydrogenation of CO2. The reaction mechanism of catalytic hydrogenation of CO2 to ethanol as well as the effects of active sites,precursors,promoters and supports on the catalytic activity and product selectivity are reviewed. Moreover,the effects of reaction conditions on the catalysis are also introduced.

  16. Hydrogen generation in SRAT with nitric acid and late washing flowsheets

    International Nuclear Information System (INIS)

    Melter feed preparation processes, incorporating a final wash of the precipitate slurry feed to Defense Waste Processing Facility (DWPF) and a partial substitution of the SRAT formic acid requirement with nitric acid, should not produce peak hydrogen generation rates during Cold Chemical Runs (CCR's) and radioactive operation greater than their current, respective hydrogen design bases of 0.024 lb/hr and 1.5 lb/hr. A single SRAT bench-scale process simulation for CCR-s produced a DWPF equivalent peak hydrogen generation rate of 0.004 lb/hr. During radioactive operation, the peak hydrogen generation rate will be dependent on the extent DWPF deviates from the nominal precipitate hydrolysis and melter feed preparation process operating parameters. Two actual radioactive sludges were treated according to the new flowsheets. The peak hydrogen evolution rates were equivalent to 0.038 and 0.20 lb/hr (DWPF scale) respectively. Compared to the formic acid -- HAN hydrolysis flowsheets, these peak rates were reduced by a factor of 2.5 and 3.4 for Tank 15 and Tank 11 sludges, respectively

  17. Immobilization of the [FeFe]-hydrogenase CrHydA1 on a gold electrode: design of a catalytic surface for the production of molecular hydrogen.

    Science.gov (United States)

    Krassen, Henning; Stripp, Sven; von Abendroth, Gregory; Ataka, Kenichi; Happe, Thomas; Heberle, Joachim

    2009-06-01

    Hydrogenase-modified electrodes are a promising catalytic surface for the electrolysis of water with an overpotential close to zero. The [FeFe]-hydrogenase CrHydA1 from the photosynthetic green alga Chlamydomonas reinhardtii is the smallest [FeFe]-hydrogenase known and exhibits an extraordinary high hydrogen evolution activity. For the first time, we immobilized CrHydA1 on a gold surface which was modified by different carboxy-terminated self-assembled monolayers. The immobilization was in situ monitored by surface-enhanced infrared spectroscopy. In the presence of the electron mediator methyl viologen the electron transfer from the electrode to the hydrogenase was detected by cyclic voltammetry. The hydrogen evolution potential (-290 mV vs NHE, pH 6.8) of this protein modified electrode is close to the value for bare platinum (-270 mV vs NHE). The surface coverage by CrHydA1 was determined to 2.25 ng mm(-2) by surface plasmon resonance, which is consistent with the formation of a protein monolayer. Hydrogen evolution was quantified by gas chromatography and the specific hydrogen evolution activity of surface-bound CrHydA1 was calculated to 1.3 micromol H(2)min(-1)mg(-1) (or 85 mol H(2)min(-1)mol(-1)). In conclusion, a viable hydrogen-evolving surface was developed that may be employed in combination with immobilized photosystems to provide a platform for hydrogen production from water and solar energy with enzymes as catalysts. PMID:19480942

  18. WTP Waste Feed Qualification: Hydrogen Generation Rate Measurement Apparatus Testing Report

    Energy Technology Data Exchange (ETDEWEB)

    Stone, M. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Newell, J. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Smith, T. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Pareizs, J. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-06-01

    The generation rate of hydrogen gas in the Hanford tank waste will be measured during the qualification of the staged tank waste for processing in the Hanford Tank Waste Treatment and Immobilization Plant. Based on a review of past practices in measurement of the hydrogen generation, an apparatus to perform this measurement has been designed and tested for use during waste feed qualification. The hydrogen generation rate measurement apparatus described in this document and shown in Figure 0-1 utilized a 100 milliliter sample in a continuously-purged, continuously-stirred vessel, with measurement of hydrogen concentration in the vent gas. The vessel and lid had a combined 220 milliliters of headspace. The vent gas system included a small condenser to prevent excessive evaporative losses from the sample during the test, as well as a demister and filter to prevent particle migration from the sample to the gas chromatography system. The gas chromatograph was an on line automated instrument with a large-volume sample-injection system to allow measurement of very low hydrogen concentrations. This instrument automatically sampled the vent gas from the hydrogen generation rate measurement apparatus every five minutes and performed data regression in real time. The fabrication of the hydrogen generation rate measurement apparatus was in accordance with twenty three (23) design requirements documented in the conceptual design package, as well as seven (7) required developmental activities documented in the task plan associated with this work scope. The HGRMA was initially tested for proof of concept with physical simulants and a remote demonstration of the system was performed in the Savannah River National Laboratory Shielded Cells Mockup Facility. Final verification testing was performed using non-radioactive simulants of the Hanford tank waste. Three different simulants were tested to bound the expected rheological properties expected during waste feed qualification

  19. WTP Waste Feed Qualification: Hydrogen Generation Rate Measurement Apparatus Testing Report

    Energy Technology Data Exchange (ETDEWEB)

    Stone, M. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Newell, J. D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Smith, T. E. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Pareizs, J. M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2016-06-01

    The generation rate of hydrogen gas in the Hanford tank waste will be measured during the qualification of the staged tank waste for processing in the Hanford Tank Waste Treatment and Immobilization Plant. Based on a review of past practices in measurement of the hydrogen generation, an apparatus to perform this measurement has been designed and tested for use during waste feed qualification. The hydrogen generation rate measurement apparatus (HGRMA) described in this document utilized a 100 milliliter sample in a continuously-purged, continuously-stirred vessel, with measurement of hydrogen concentration in the vent gas. The vessel and lid had a combined 220 milliliters of headspace. The vent gas system included a small condenser to prevent excessive evaporative losses from the sample during the test, as well as a demister and filter to prevent particle migration from the sample to the gas chromatography system. The gas chromatograph was an on line automated instrument with a large-volume sample-injection system to allow measurement of very low hydrogen concentrations. This instrument automatically sampled the vent gas from the hydrogen generation rate measurement apparatus every five minutes and performed data regression in real time. The fabrication of the hydrogen generation rate measurement apparatus was in accordance with twenty three (23) design requirements documented in the conceptual design package, as well as seven (7) required developmental activities documented in the task plan associated with this work scope. The HGRMA was initially tested for proof of concept with physical simulants, and a remote demonstration of the system was performed in the Savannah River National Laboratory Shielded Cells Mockup Facility. Final verification testing was performed using non-radioactive simulants of the Hanford tank waste. Three different simulants were tested to bound the expected rheological properties expected during waste feed qualification testing. These

  20. Fuel processor and method for generating hydrogen for fuel cells

    Science.gov (United States)

    Ahmed, Shabbir; Lee, Sheldon H. D.; Carter, John David; Krumpelt, Michael; Myers, Deborah J.

    2009-07-21

    A method of producing a H.sub.2 rich gas stream includes supplying an O.sub.2 rich gas, steam, and fuel to an inner reforming zone of a fuel processor that includes a partial oxidation catalyst and a steam reforming catalyst or a combined partial oxidation and stream reforming catalyst. The method also includes contacting the O.sub.2 rich gas, steam, and fuel with the partial oxidation catalyst and the steam reforming catalyst or the combined partial oxidation and stream reforming catalyst in the inner reforming zone to generate a hot reformate stream. The method still further includes cooling the hot reformate stream in a cooling zone to produce a cooled reformate stream. Additionally, the method includes removing sulfur-containing compounds from the cooled reformate stream by contacting the cooled reformate stream with a sulfur removal agent. The method still further includes contacting the cooled reformate stream with a catalyst that converts water and carbon monoxide to carbon dioxide and H.sub.2 in a water-gas-shift zone to produce a final reformate stream in the fuel processor.

  1. Start up system for hydrogen generator used with an internal combustion engine

    Science.gov (United States)

    Houseman, J.; Cerini, D. J. (Inventor)

    1977-01-01

    A hydrogen generator provides hydrogen rich product gases which are mixed with the fuel being supplied to an internal combustion engine for the purpose of enabling a very lean mixture of that fuel to be used, whereby nitrous oxides emitted by the engine are minimized. The hydrogen generator contains a catalyst which must be heated to a pre-determined temperature before it can react properly. To simplify the process of heating up the catalyst at start-up time, either some of the energy produced by the engine such as engine exhaust gas, or electrical energy produced by the engine, or the engine exhaust gas may be used to heat up air which is then used to heat the catalyst.

  2. Chemiluminescence assay for catechin based on generation of hydrogen peroxide in basic solution

    International Nuclear Information System (INIS)

    We have determined that the catechin group in basic solution efficiently produces hydrogen peroxide; moreover, a highly sensitive analysis methodology was developed to measure catechin employing a peroxalate chemiluminescence detection system. Identification of hydrogen peroxide generated by catechin was determined by ESR as well as peroxalate chemiluminescence using catalase and SOD. As a result, catechin-generated superoxide by electron reduction to dissolved oxygen in basic solution, followed by production of hydrogen peroxide through dismutation reaction. This method could measure several tea catechins, (+)-catechin (CC), (-)-epigallocatechin-3-gallate (EGCg), (-)-epicatechin-3-gallate (ECG) and gallic acid, with measurement range from 10-7 to 10-3 mol/l and sensitivity of 10-8 mol/l. This method was also applied to the determination of total catechin levels in green tea, black tea and roasted green tea

  3. Catalytic Hydrolysis of Borohydride for Fuel Cells

    Institute of Scientific and Technical Information of China (English)

    WANG Lianbang; ZHAN Xingyue; YANG Zhenzhen; MA Chun'an

    2011-01-01

    Borohydrides present interesting options for the electrochemical power generation acting either as hydrogen source or anodic fuel for direct borohydride fuel cells(DBFC).In this work,Mg-Ni composite synthesized by mechanically alloying method,used as the catalyst for the hydrolysis of borohydride,has been investigated.Co-doping treatment has been carried out for the purpose of improving the hydrolysis rate further.The as-prepared and Co-doped Mg-Ni composites with low cost showed high catalytic activity to the hydrolysis of borohydride for hydrogen generation.After Co-doping,the hydrogen generation rate was around 280 ml·g-1·min-1.Borohydride would be a promising hydrogen source for fuel cells.

  4. Enhanced Intrinsic Catalytic Activity of λ-MnO2 by Electrochemical Tuning and Oxygen Vacancy Generation.

    Science.gov (United States)

    Lee, Sanghan; Nam, Gyutae; Sun, Jie; Lee, Jang-Soo; Lee, Hyun-Wook; Chen, Wei; Cho, Jaephil; Cui, Yi

    2016-07-18

    Chemically prepared λ-MnO2 has not been intensively studied as a material for metal-air batteries, fuel cells, or supercapacitors because of their relatively poor electrochemical properties compared to α- and δ-MnO2 . Herein, through the electrochemical removal of lithium from LiMn2 O4 , highly crystalline λ-MnO2 was prepared as an efficient electrocatalyst for the oxygen reduction reaction (ORR). The ORR activity of the material was further improved by introducing oxygen vacancies (OVs) that could be achieved by increasing the calcination temperature during LiMn2 O4 synthesis; a concentration of oxygen vacancies in LiMn2 O4 could be characterized by its voltage profile as the cathode in a lithiun-metal half-cell. λ-MnO2-z prepared with the highest OV exhibited the highest diffusion-limited ORR current (5.5 mA cm(-2) ) among a series of λ-MnO2-z electrocatalysts. Furthermore, the number of transferred electrons (n) involved in the ORR was >3.8, indicating a dominant quasi-4-electron pathway. Interestingly, the catalytic performances of the samples were not a function of their surface areas, and instead depended on the concentration of OVs, indicating enhancement in the intrinsic catalytic activity of λ-MnO2 by the generation of OVs. This study demonstrates that differences in the electrochemical behavior of λ-MnO2 depend on the preparation method and provides a mechanism for a unique catalytic behavior of cubic λ-MnO2 . PMID:27254822

  5. Prostaglandins attenuate cardiac contractile dysfunction produced by free radical generation but not by hydrogen peroxide.

    Science.gov (United States)

    Zimmer, K M; Karmazyn, M

    1997-11-01

    The aim of this study was to examine and compare the potential influence of cyclooxygenase or lipoxygenase derived metabolites of arachidonic acid on myocardial injury produced either by a free radical generating system consisting of purine plus xanthine oxidase or that produced by hydrogen peroxide. A free radical generating system consisting of purine (2.3 mM) and xanthine oxidase (10 U/L) as well as hydrogen peroxide (75 microM) produced significant functional changes in the absence of either significant deficits in high energy phosphates or ultrastructural damage. Prostaglandin F2 alpha (30 nM) significantly attenuated both the negative inotropic effect of purine plus xanthine oxidase as well as the ability of the free radical generator to elevate diastolic pressure. An identical concentration of prostaglandin 12 (prostacyclin) significantly reduced diastolic pressure elevation only and had no effect on contractile depression. The salutary effects of the two PGs occurred in the absence of any inhibitory influence on superoxide anion generation produced by the purine and xanthine oxidase reaction. None of prostaglandins modulated the response to hydrogen peroxide. In addition, neither prostaglandin E2 nor leukotrienes exerted any effect on changes produced by either type of oxidative stress. A 5 fold elevation in the concentrations of free radical generators or hydrogen peroxide produced extensive injury as characterized by a virtual total loss in contractility, 400% elevation in diastolic pressure, ultrastructural damage and significant depletions in high energy phosphate content. None of these effects were modulated by eicosanoid treatment. Our results therefore demonstrate a selective ability of both prostaglandin F2 alpha and to a lesser extent prostacyclin, to attenuate dysfunction produced by purine plus xanthine oxidase but not hydrogen peroxide. It is possible that these eicosanoids may represent endogenous protective factors under conditions of enhanced

  6. Experimental and numerical investigation of the catalytic partial oxidation of methane to synthesis gas for power generation applications[Dissertation 17183

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, A.

    2007-07-01

    The present work addresses the catalytic partial oxidation (CPO) of methane to synthesis gas, with particular emphasis on power generation applications. A combined experimental and numerical investigation of methane partial oxidation to synthesis gas (H{sub 2}, CO) over rhodium-based catalysts has been carried out at pressures of up to 10 bar. The reactivity of the produced hydrogen and the suitably-low light-off temperatures of the CPO reactor, greatly facilitate operation of power generation gas turbines with reduced NO{sub x} emissions, stable operation with low calorific value fuels, and new combustion strategies for efficient CO{sub 2} capture. Those strategies utilize CPO of methane with oxygen (separated from air) and large exhaust gas recycle (H{sub 2}O and CO{sub 2}). An optically accessible catalytic channel-flow reactor was used to carry out Raman spectroscopy of major gas-phase species and laser induced fluorescence (LIF) of formaldehyde, in order to gain fundamental information on the catalytic and gas-phase chemical pathways. Transverse concentration profiles measured by the spontaneous Raman scattering technique determined the catalytic reactivity, while the LIF provided flame shapes and anchoring positions that, in turn, characterized the gaseous reactivity. Comparison between measurements and 2-D CFD computations, led to the validation of detailed catalytic and gas-phase reaction mechanisms. Experiments in a subscale gas-turbine honeycomb catalytic reactor have shown that the foregoing reaction mechanisms were also appropriate under gas-turbine relevant conditions with short reactant residence times. The light-off behavior of the subscale honeycomb reactor was reproduced by transient 2-D CFD computations. Ignition and extinction in CPO was studied. It was shown that, despite the chemical impact of the H{sub 2}O diluent during the transient catalytic ignition event, the light-off times themselves were largely unaffected by the exhaust gas dilution

  7. High Efficiency Generation of Hydrogen Fuels using Nuclear Power Annual Report August, 2000 - July 2001

    Energy Technology Data Exchange (ETDEWEB)

    Brown, L.C.

    2002-11-01

    OAK B188 High Efficiency Generation of Hydrogen Fuels using Nuclear Power Annual Report August 2000 - July 2001. Currently no large scale, cost-effective, environmentally attractive hydrogen production process is available for commercialization nor has such a process been identified. Hydrogen is a promising energy carrier, which potentially could replace the fossil fuels used in the transportation sector of our economy. Carbon dioxide emissions from fossil fuel combustion are thought to be responsible for global warming. The purpose of this work is to determine the potential for efficient, cost-effective, large-scale production of hydrogen utilizing high temperature heat from an advanced nuclear power station. The benefits of this work will include the generation of a low-polluting transportable energy feedstock in an efficient method that has little or no implication for greenhouse gas emissions from a primary energy source whose availability and sources are domestically controlled. This will help to ensure energy for a future transportation/energy infrastructure that is not influenced/controlled by foreign governments. This report describes work accomplished during the second year (Phase 2) of a three year project whose objective is to ''define an economically feasible concept for production of hydrogen, by nuclear means, using an advanced high temperature nuclear reactor as the energy source.'' The emphasis of the first year (Phase 1) was to evaluate thermochemical processes which offer the potential for efficient, cost-effective, large-scale production of hydrogen from water, in which the primary energy input is high temperature heat from an advanced nuclear reactor and to select one (or, at most, three) for further detailed consideration. Phase 1 met its goals and did select one process, the sulfur-iodine process, for investigation in Phases 2 and 3. The combined goals of Phases 2 and 3 were to select the advanced nuclear reactor best

  8. Modeling the reaction kinetics of a hydrogen generator onboard a fuel cell -- Electric hybrid motorcycle

    Science.gov (United States)

    Ganesh, Karthik

    Owing to the perceived decline of the fossil fuel reserves in the world and environmental issues like pollution, conventional fuels may be replaced by cleaner alternative fuels. The potential of hydrogen as a fuel in vehicular applications is being explored. Hydrogen as an energy carrier potentially finds applications in internal combustion engines and fuel cells because it is considered a clean fuel and has high specific energy. However, at 6 to 8 per kilogram, not only is hydrogen produced from conventional methods like steam reforming expensive, but also there are storage and handling issues, safety concerns and lack of hydrogen refilling stations across the country. The purpose of this research is to suggest a cheap and viable system that generates hydrogen on demand through a chemical reaction between an aluminum-water slurry and an aqueous sodium hydroxide solution to power a 2 kW fuel cell on a fuel cell hybrid motorcycle. This reaction is essentially an aluminum-water reaction where sodium hydroxide acts as a reaction promoter or catalyst. The Horizon 2000 fuel cell used for this purpose has a maximum hydrogen intake rate of 28 lpm. The study focuses on studying the exothermic reaction between the reactants and proposes a rate law that best describes the rate of generation of hydrogen in connection to the surface area of aluminum available for the certain reaction and the concentration of the sodium hydroxide solution. Further, the proposed rate law is used in the simulation model of the chemical reactor onboard the hybrid motorcycle to determine the hydrogen flow rate to the fuel cell with time. Based on the simulated rate of production of hydrogen from the chemical system, its feasibility of use on different drive cycles is analyzed. The rate of production of hydrogen with a higher concentration of sodium hydroxide and smaller aluminum powder size was found to enable the installation of the chemical reactor on urban cycles with frequent stops and starts

  9. High performance photoelectrochemical hydrogen generation and solar cells with a double type II heterojunction

    NARCIS (Netherlands)

    Lai, Lai-Hung; Gomulya, Widianta; Protesescu, Loredana; Kovalenko, Maksym V.; Loi, Maria A.

    2014-01-01

    We report on the fabrication of CdSe quantum dot (QD) sensitized electrodes by direct adsorption of colloidal QDs on mesoporous TiO2 followed by 3-mercaptopropionic acid (MPA) ligand exchange. High efficiency photoelectrochemical hydrogen generation is demonstrated by means of these electrodes. The

  10. Hydrogen generation by water radiolysis with immersion of oxidation products of Zircaloy-4

    International Nuclear Information System (INIS)

    In order to predict the hydrogen gas generation from seawater or water in which debris would be included by the severe accident of nuclear power plant, we investigated the effect of ZrO2 and the oxidation products of Zircaloy-4 on hydrogen gas generation by radiolysis of water since the radiolytic generation could be affected by materials immersed in water. Powders of well-characterized oxides and oxidation products were immersed in either seawater or distilled water, and irradiated by gamma ray from a Co-60 source. The observed hydrogen yield, G(H2), was measured as a function of the weight fraction of oxide in water up to 50 wt%. The enhancement of the hydrogen generation by radiolysis of water with the commercial oxides and the oxidation products of Zircaloy-4 was quite small or absent in seawater. But the enhancement was observed in the presence of the oxides or the oxidation products at low weight fraction in distilled water. This enhancement in distilled water seemed to be dependent on specific surface area or particle size, but its dependence on the crystal structure was not apparent in the experimental results. The enhancement was saturated at higher ZrO2 weight fractions and it was not apparent in the seawater. (author)

  11. The Effects of CO2 Addition on the Partial Oxidation of Heptane for Hydrogen Generation

    Institute of Scientific and Technical Information of China (English)

    Ran RAN; Guo Xing XIONG; Shi Shan SHENG; Wei Shen YANG

    2004-01-01

    The effects of CO2 on the partial oxidation of heptane for hydrogen generation have been studied. Based on the experimental results and thermodynamic equilibrium calculations, the validity of CO2 addition to weaken the hot spots, and the feasibility of the autothermal operation are discussed.

  12. Status of the development of solid polymer electrolyte water electrolysis for large scale hydrogen generation

    Science.gov (United States)

    Russell, J. H.

    1982-02-01

    Solid polymer electrolyte water electrolysis for large scale hydrogen generation is reported. The program was aimed at performance improvement. Reductions in cell impedance were demonstrated which improve cell performance by over 100 mV. A prototype 500 SCFH system for field evaluation was developed.

  13. Early-time photodynamics of ruthenium-based photocatalysts for light-induced hydrogen generation

    NARCIS (Netherlands)

    Pan, Qing

    2016-01-01

    This thesis aims to provide a fundamental understanding of the early-time photodynamics of a series of Ru/M (M = Pd or Pt) bimetallic photocatalysts for light-induced hydrogen generation. This class of complexes adopts a general structure involving a Ru(II) center coordinated to two peripheral ligan

  14. Biomass & Natural Gas Based Hydrogen Fuel For Gas Turbine (Power Generation)

    Science.gov (United States)

    Significant progress has been made by major power generation equipment manufacturers in the development of market applications for hydrogen fuel use in gas turbines in recent years. Development of a new application using gas turbines for significant reduction of power plant CO2 e...

  15. Liquid Phase Hydrogenation of Benzalacetophenone:Effect of Solvent,Catalyst Support,Catalytic Metal and Reaction Conditions%Liquid Phase Hydrogenation of Benzalacetophenone: Effect of Solvent, Catalyst Support, Catalytic Metal and Reaction Conditions

    Institute of Scientific and Technical Information of China (English)

    Achim STOLLE; Christine SCHMOGER; Bernd ONDRUSCHKA; Werner BONRATH; Thomas F. KELLER; Klaus D. JANDT

    2011-01-01

    Innovative catalysts based on a “porous glass” support material were developed and investigated for the reduction of benzalacetophenone.The easy preparation conditions and possibility to use different metals (e.g.Pd,Pt,Rh) for impregnation gave a broad variety of these catalysts.Hydrogenation experiments with these supported catalysts were carried out under different hydrogen pressures and temperatures.Porous glass catalysts with Pd as the active component gave chemoselective hydrogenation of benzalacetophenone,while Pt- and Rh-catalysts tended to further reduce the carbonyl group,especially at elevated hydrogen pressures and temperatures.Kinetic analysis of the reactions revealed these had zero order kinetics,which was independent of the type of porous glass support and solvent used.

  16. ONO-pincer ruthenium complex-bound norvaline for efficient catalytic oxidation of methoxybenzenes with hydrogen peroxide.

    Science.gov (United States)

    Yoshida, Ryota; Isozaki, Katsuhiro; Yokoi, Tomoya; Yasuda, Nobuhiro; Sadakane, Koichiro; Iwamoto, Takahiro; Takaya, Hikaru; Nakamura, Masaharu

    2016-08-21

    The enhanced catalytic activity of ruthenium complex-bound norvaline Boc-l-[Ru]Nva-OMe 1, in which the ONO-pincer ruthenium complex Ru(pydc)(terpy) 2 is tethered to the α-side chain of norvaline, has been demonstrated for the oxidation of methoxybenzenes to p-benzoquinones with a wide scope of substrates and unique chemoselectivity. PMID:27314504

  17. Calpain-Mediated Processing of Adenylate Cyclase Toxin Generates a Cytosolic Soluble Catalytically Active N-Terminal Domain.

    Directory of Open Access Journals (Sweden)

    Kepa B Uribe

    Full Text Available Bordetella pertussis, the whooping cough pathogen, secretes several virulence factors among which adenylate cyclase toxin (ACT is essential for establishment of the disease in the respiratory tract. ACT weakens host defenses by suppressing important bactericidal activities of the phagocytic cells. Up to now, it was believed that cell intoxication by ACT was a consequence of the accumulation of abnormally high levels of cAMP, generated exclusively beneath the host plasma membrane by the toxin N-terminal catalytic adenylate cyclase (AC domain, upon its direct translocation across the lipid bilayer. Here we show that host calpain, a calcium-dependent Cys-protease, is activated into the phagocytes by a toxin-triggered calcium rise, resulting in the proteolytic cleavage of the toxin N-terminal domain that releases a catalytically active "soluble AC". The calpain-mediated ACT processing allows trafficking of the "soluble AC" domain into subcellular organella. At least two strategic advantages arise from this singular toxin cleavage, enhancing the specificity of action, and simultaneously preventing an indiscriminate activation of cAMP effectors throughout the cell. The present study provides novel insights into the toxin mechanism of action, as the calpain-mediated toxin processing would confer ACT the capacity for a space- and time-coordinated production of different cAMP "pools", which would play different roles in the cell pathophysiology.

  18. Research on Integration of an Automotive Exhaust-Based Thermoelectric Generator and a Three-Way Catalytic Converter

    Science.gov (United States)

    Deng, Y. D.; Chen, Y. L.; Chen, S.; Xianyu, W. D.; Su, C. Q.

    2015-06-01

    A key research topic related to thermoelectric generators (TEGs) for automotive applications is to improve their compatibility with the original vehicle exhaust system, which determines the quality of the exhaust gas treatment and the realization of energy conservation and emission reduction. A new TEG integrated with a three-way catalytic converter (CTEG) by reshaping the converter as the heat exchanger is proposed. A heat-flux coupling simulation model of the integrated TEG is established at the light-off stage of the original three-way catalytic converter (TWC). Temperature distribution maps of the integrated heat exchanger, thermoelectric modules, and cooling-water tank are obtained to present the process of energy flow among the parts of the CTEG. Based on the simulation results, the output power of the CTEG is calculated by a mathematical model. A minimum output power of 31.93 W can be obtained by conversion when the TWC starts working at steady conditions. Theoretically, this case study demonstrates the great potential for use of CTEGs in vehicles.

  19. 对苯二甲酸催化加氢的Ru-Sn-B/丝光沸石催化性能%Catalytic performance of Ru-Sn-B/mordenite for terephthalic acid catalytic hydrogenation

    Institute of Scientific and Technical Information of China (English)

    赵葛新; 靳海波; 何广湘; 郭志武; 杨索和

    2012-01-01

    采用分步浸渍和化学还原的方法制备以丝光沸石分子筛为载体的Ru-Sn-B催化剂,研究了在负载型催化剂Ru-Sn-B/丝光沸石上对苯二甲酸催化加氢制备1,4-环己烷二甲醇的加氢催化性能,并利用XRD和BET等分析手段对Ru-Sn-B/丝光沸石催化剂进行表征.结果 表明,RuB和Sn在丝光沸石上具有较好的分散性,Ru-Sn-B/丝光沸石催化剂具有较高的催化活性和选择性;催化加氢过程中采用两段升温升压的方法,对苯二甲酸转化率约100%,产物1,4-环己烷二甲醇的收率为73.5%,反式与顺式之比为2.42.%Ru-Sn-B/mordenite catalysts were prepared by sequential impregnation and chemical reduction methods and using mordenite zeolite as the carrier. The catalytic performance of Ru-Sn-B/mordenite catalysts for terephthalic acid hydrogenation to 1,4-cyclohexanedimethanol was investigated. The as-prepared catalysts were characterized by XRD, BET, EDS and ICP. The results showed that RuB and Sn had better dispersion on the mordenite, and Ru-Sn-B/mordenite catalyst possessed high catalytic activity and selectivity. The catalytic hydrogenation process used two stage enhancement method of temperature and pressure. Terephthalic acid conversion rate of about 100% ,the yield of the product 1,4-cyclohexanedimethanol of 73.5% ,and the ratio of trans and cis of the product of 2.42 were attained,respectively.

  20. A third-generation dispersion and third-generation hydrogen bonding corrected PM6 method

    DEFF Research Database (Denmark)

    Kromann, Jimmy Charnley; Christensen, Anders Steen; Svendsen, Casper Steinmann;

    2014-01-01

    We present new dispersion and hydrogen bond corrections to the PM6 method, PM6-D3H+, and its implementation in the GAMESS program. The method combines the DFT-D3 dispersion correction by Grimme et al. with a modified version of the H+ hydrogen bond correction by Korth. Overall, the interaction en...... vibrational free energies. While the GAMESS implementation is up to 10 times slower for geometry optimizations of proteins in bulk solvent, compared to MOPAC, it is sufficiently fast to make geometry optimizations of small proteins practically feasible....... energy of PM6-D3H+ is very similar to PM6-DH2 and PM6-DH+, with RMSD and MAD values within 0.02 kcal/mol of one another. The main difference is that the geometry optimizations of 88 complexes result in 82, 6, 0, and 0 geometries with 0, 1, 2, and 3 or more imaginary frequencies using PM6-D3H+ implemented...

  1. Evaluation of the pressure loads generated by hydrogen explosion in auxiliary nuclear building

    International Nuclear Information System (INIS)

    Full text of publication follows: In the framework of nuclear safety, a hydrogen leaks in the auxiliary nuclear building would raise a explosion hazard. A local ignition of the combustible mixture would give birth initially to a slow flame, rapidly accelerated by obstacles. This flame acceleration is responsible for high pressure loads that can damage the auxiliary building and destroy safety equipments in it. In this paper, we evaluate the pressure loads generated by an hydrogen explosion for both bounding and realistic explosion scenarios. The bounding scenarios use stoichiometric hydrogen-air mixtures and the realistic scenarios correspond to hydrogen leaks with mass flow rate varying between 1 g/s and 9 g/s. For every scenario, the impact of the ignition location and ignition time are investigated. The hydrogen dispersion and explosion are computed using the TONUS code. The dispersion model used is based on a finite element solver and the explosion is simulated by a structured finite volumes EULER equation solver and the combustion model CREBCOM which simulates the hydrogen/air turbulent flame propagation, taking into account 3D complex geometry and reactants concentration gradients. The pressure loads computed are then used to investigate the occurrence of a mechanical failure of the tanks located in the auxiliary nuclear building and containing radioactive fluids. The EUROPLEXUS code is used to perform 3D mechanical calculations because the loads are non uniform and of rather short deviation. (authors)

  2. A polymer electrolyte fuel cell stack for stationary power generation from hydrogen fuel

    Energy Technology Data Exchange (ETDEWEB)

    Gottesfeld, S. [Los Alamos National Lab., NM (United States)

    1995-09-01

    The fuel cell is the most efficient device for the conversion of hydrogen fuel to electric power. As such, the fuel cell represents a key element in efforts to demonstrate and implement hydrogen fuel utilization for electric power generation. The low temperature, polymer electrolyte membrane fuel cell (PEMFC) has recently been identified as an attractive option for stationary power generation, based on the relatively simple and benign materials employed, the zero-emission character of the device, and the expected high power density, high reliability and low cost. However, a PEMFC stack fueled by hydrogen with the combined properties of low cost, high performance and high reliability has not yet been demonstrated. Demonstration of such a stack will remove a significant barrier to implementation of this advanced technology for electric power generation from hydrogen. Work done in the past at LANL on the development of components and materials, particularly on advanced membrane/electrode assemblies (MEAs), has contributed significantly to the capability to demonstrate in the foreseeable future a PEMFC stack with the combined characteristics described above. A joint effort between LANL and an industrial stack manufacturer will result in the demonstration of such a fuel cell stack for stationary power generation. The stack could operate on hydrogen fuel derived from either natural gas or from renewable sources. The technical plan includes collaboration with a stack manufacturer (CRADA). It stresses the special requirements from a PEMFC in stationary power generation, particularly maximization of the energy conversion efficiency, extension of useful life to the 10 hours time scale and tolerance to impurities from the reforming of natural gas.

  3. Adsorption-parallel catalytic waves of cinnamic acid in hydrogen peroxide-tetra-n-butylammonium bromide-acetate system

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    The mechanism of the adsorption-parallel catalytic wave of cinnamic acid (C6H5-CH == CH-COOH) in acetate buffer (pH = 4.0)-H2O2-tetra-n-butylammonium bromide (Bu4N.Br) solution was studied by the linear-sweep polarography, cyclic voltammetry and digital simulation approach. Experimental results indicate that the reduction mechanism of cinnamic acid is ECdimE'process, in which the C == C double bond of cinnamic acid first undergoes 1e, 1H+ reduction to produce an intermediate free radical C6H5-C.H-CH2-COOH(E'), then the further reduction of the free radical in 1e,1H+ addition (E') occurs simultaneously with a dimerization reaction between two free radicals (Cdim). Bu4N.Br enhances the polarographic current of cinnamic acid and shifts the peak potential to positive direction. The enhancement action of Bu4N.Br is due to the adsorption of cinnamic acid induced by Bu4N+ species. In addition, H2O2 causes the parallel catalytic wave of cinnamic acid. The mechanism of the catalytic wave is EC'process because H2O2 oxidizes the free radical of cinnamic acid to regenerate the original C == C bond(C'), preventing both the further reduction and the dimerization of the free radicals. The apparent rate constant kf of the oxidation reaction is 1.35×102 mol.L-1.s-1. A new class of catalytic waves for organic compounds, the adsorption-parallel catalytic waves upon the dual enhancement action of both the surfactant and oxidant, has been presented.

  4. Catalytic Asymmetric Reduction of a 3,4-Dihydroisoquinoline for the Large-Scale Production of Almorexant: Hydrogenation or Transfer Hydrogenation?

    OpenAIRE

    Verzijl, Gerard K.M.; Vries, André H.M. de; Vries, Johannes G. de; Kapitan, Peter; Dax, Thomas; Helms, Matthias; Nazir, Zarghun; Skranc, Wolfgang; Imboden, Christoph; Stichler, Juergen; Ward, Richard A.; Abele, Stefan; Lefort, Laurent

    2013-01-01

    Several methods are presented for the enantioselective synthesis of the tetrahydroisoquinoline core of almorexant (ACT-078573A), a dual orexin receptor antagonist. Initial clinical supplies were secured by the Noyori Ru-catalyzed asymmetric transfer hydrogenation (Ru-Noyori ATH) of the dihydroisoquinoline precursor. Both the yield and enantioselectivity eroded upon scale-up. A broad screening exercise identified TaniaPhos as ligand for the iridium-catalyzed asymmetric hydrogenation with a ded...

  5. Hydrogen and methoxy coadsorption in the computation of the catalytic conversion of methanol on the ceria (111) surface

    Science.gov (United States)

    Beste, Ariana; Overbury, Steven H.

    2016-06-01

    Methanol decomposition to formaldehyde catalyzed by the ceria (111) surface was investigated using the DFT + U method. Our results rationalize experimental temperature programmed desorption experiments on the fully oxidized surface. Particular attention was paid to the effect of coadsorption of methoxy and hydrogen on various aspects of the conversion process. This issue had been raised by the experimental observation of water desorption at low temperature removing hydrogen from the system. Within this context, we also investigated hydrogen diffusion on the ceria surface. The hydrogen/methoxy interaction on ceria was shown to be ionic regardless of separation distance. The barrier for dehydrogenation of methoxy using the ionic model system, where hydrogen is coadsorbed, is above 1 eV. This barrier becomes negligible if an incorrect neutral model without coadsorbed hydrogen is employed. While water formation from isolated surface hydrogen is unlikely at low temperature, the presence of coadsorbed methoxy reduces the reaction energy for water formation considerably. For the dehydrated surface, we observed that the preference of the electron to locate at the methoxy oxygen instead of the cerium atom results in a surface that does not contain Ce3 + ions, despite the existence of a vacancy.

  6. Catalytic Hydrogenation of Levulinic Acid in Water into g-Valerolactone over Bulk Structure of Inexpensive Intermetallic Ni-Sn Alloy Catalysts

    Directory of Open Access Journals (Sweden)

    Rodiansono Rodiansono

    2015-07-01

    Full Text Available A bulk structure of inexpensive intermetallic nickel-tin (Ni-Sn alloys catalysts demonstrated highly selective in the hydrogenation of levulinic acid in water into g-valerolactone. The intermetallic Ni-Sn catalysts were synthesized via a very simple thermochemical method from non-organometallic precursor at low temperature followed by hydrogen treatment at 673 K for 90 min. The molar ratio of nickel salt and tin salt was varied to obtain the corresponding Ni/Sn ratio of 4.0, 3.0, 2.0, 1.5, and 0.75. The formation of Ni-Sn alloy species was mainly depended on the composition and temperature of H2 treatment. Intermetallics Ni-Sn that contain Ni3Sn, Ni3Sn2, and Ni3Sn4 alloy phases are known to be effective heterogeneous catalysts for levulinic acid hydrogenation giving very excellence g-valerolactone yield of >99% at 433 K, initial H2 pressure of 4.0 MPa within 6 h. The effective hydrogenation was obtained in H2O without the formation of by-product. Intermetallic Ni-Sn(1.5 that contains Ni3Sn2 alloy species demonstrated very stable and reusable catalyst without any significant loss of its selectivity. © 2015 BCREC UNDIP. All rights reserved. Received: 26th February 2015; Revised: 16th April 2015; Accepted: 22nd April 2015  How to Cite: Rodiansono, R., Astuti, M.D., Ghofur, A., Sembiring, K.C. (2015. Catalytic Hydrogenation of Levulinic Acid in Water into g-Valerolactone over Bulk Structure of Inexpensive Intermetallic Ni-Sn Alloy Catalysts. Bulletin of Chemical Reaction Engineering & Catalysis, 10 (2: 192-200. (doi:10.9767/bcrec.10.2.8284.192-200Permalink/DOI: http://dx.doi.org/10.9767/bcrec.10.2.8284.192-200  

  7. NOBLE METAL CHEMISTRY AND HYDROGEN GENERATION DURING SIMULATED DWPF MELTER FEED PREPARATION

    Energy Technology Data Exchange (ETDEWEB)

    Koopman, D

    2008-06-25

    Simulations of the Defense Waste Processing Facility (DWPF) Chemical Processing Cell vessels were performed with the primary purpose of producing melter feeds for the beaded frit program plus obtaining samples of simulated slurries containing high concentrations of noble metals for off-site analytical studies for the hydrogen program. Eight pairs of 22-L simulations were performed of the Sludge Receipt and Adjustment Tank (SRAT) and Slurry Mix Evaporator (SME) cycles. These sixteen simulations did not contain mercury. Six pairs were trimmed with a single noble metal (Ag, Pd, Rh, or Ru). One pair had all four noble metals, and one pair had no noble metals. One supporting 4-L simulation was completed with Ru and Hg. Several other 4-L supporting tests with mercury have not yet been performed. This report covers the calculations performed on SRNL analytical and process data related to the noble metals and hydrogen generation. It was originally envisioned as a supporting document for the off-site analytical studies. Significant new findings were made, and many previous hypotheses and findings were given additional support as summarized below. The timing of hydrogen generation events was reproduced very well within each of the eight pairs of runs, e.g. the onset of hydrogen, peak in hydrogen, etc. occurred at nearly identical times. Peak generation rates and total SRAT masses of CO{sub 2} and oxides of nitrogen were reproduced well. Comparable measures for hydrogen were reproduced with more variability, but still reasonably well. The extent of the reproducibility of the results validates the conclusions that were drawn from the data.

  8. Hydrogenation of nitriles on a well-characterized nickel surface: From surface science studies to liquid phase catalytic activity measurements

    Energy Technology Data Exchange (ETDEWEB)

    Gardin, D.E.

    1993-12-01

    Nitrile hydrogenation is the most commonly used method for preparing diverse amines. This thesis is aimed at the mechanism and factors affecting the performance of Ni-based catalysts in nitrile hydrogenations. Surface science techniques are used to study bonding of nitriles and amines to a Ni(111) surface and to identify surface intermediates. Liquid-phase hydrogenations of cyclohexene and 1-hexene on a Pt foil were carried out successfully. Finally, knowledge about the surface structure, surface chemical bond, dynamics of surface atoms (diffusion, growth), and reactivity of metal surfaces from solid-gas interface studies, is discussed.

  9. Oxidation of diesel-generated volatile organic compounds in the selective catalytic reduction process

    Energy Technology Data Exchange (ETDEWEB)

    Koebel, M.; Elsener, M. [Paul Scherrer Inst., Villigen (Switzerland). Combustion Research

    1998-10-01

    The main part of the VOCs (volatile organic compounds) contained in diesel exhaust ({approx}80%) is oxidized to CO and CO{sub 2} over an SCR (selective catalytic reduction) catalyst. CO is the major product of this oxidation, representing about 50--70% of the formed products (CO + CO{sub 2}). This preferential formation of CO leads to a pronounced increase of CO emissions when an SCR process is added to a diesel engine. A small fraction of the VOCs is selectively oxidized to carboxylic acids over the SCR catalyst. This selectivity is due to the acidic properties of the catalyst causing the preferential desorption at the oxidation state of the acid. The main products of these oxidation reactions are the lower monocarboxylic acids and some dicarboxylic acids forming stable anhydrides, especially maleic and phthalic acid. The highest emissions of these acids are found at low temperatures; they decrease at higher temperatures. Formic acid is preferentially decomposed into carbon monoxide and water. It must therefore be assumed that the strong increase of CO mentioned above is due to a mechanism involving the thermal decomposition of formic acid formed from various primary VOCs.

  10. Two-chamber hydrogen generation and application: access to pressurized deuterium gas.

    Science.gov (United States)

    Modvig, Amalie; Andersen, Thomas L; Taaning, Rolf H; Lindhardt, Anders T; Skrydstrup, Troels

    2014-06-20

    Hydrogen and deuterium gas were produced and directly applied in a two-chamber system. These gaseous reagents were generated by the simple reaction of metallic zinc with HCl in water for H2 and DCl in deuterated water for D2. The setup proved efficient in classical Pd-catalyzed reductions of ketones, alkynes, alkenes, etc. in near-quantitative yields. The method was extended to the synthesis and isotope labeling of quinoline and 1,2,3,4-tetrahydroquinoline derivatives. Finally, CX-546 and Olaparib underwent efficient Ir-catalyzed hydrogen isotope exchange reactions. PMID:24870212

  11. Comparative study of the hydrogen generation during short term station blackout (STSBO) in a BWR

    International Nuclear Information System (INIS)

    Highlights: • Comparative study of generation in a simulated STSBO severe accident. • MELCOR and SCDAP/RELAP5 codes were used to understanding the main phenomena. • Both codes present similar thermal-hydraulic behavior for pressure and boil off. • SCDAP/RELAP5 predicts 15.8% lower hydrogen production than MELCOR. - Abstract: The aim of this work is the comparative study of hydrogen generation and the associated parameters in a simulated severe accident of a short-term station blackout (STSBO) in a typical BWR-5 with Mark-II containment. MELCOR (v.1.8.6) and SCDAP/RELAP5 (Mod.3.4) codes were used to understand the main phenomena in the STSBO event through the results comparison obtained from simulations with these codes. Due that the simulation scope of SCDAP/RELAP5 is limited to failure of the vessel pressure boundary, the comparison was focused on in-vessel severe accident phenomena; with a special interest in the vessel pressure, boil of cooling, core temperature, and hydrogen generation. The results show that at the beginning of the scenario, both codes present similar thermal-hydraulic behavior for pressure and boil off of cooling, but during the relocation, the pressure and boil off, present differences in timing and order of magnitude. Both codes predict in similar time the beginning of melting material drop to the lower head. As far as the hydrogen production rate, SCDAP/RELAP5 predicts 15.8% lower production than MELCOR

  12. Brewery wastewaters in photobiological hydrogen generation in presence of Rhodobacter sphaeroides O.U. 001

    Energy Technology Data Exchange (ETDEWEB)

    Seifert, K.; Waligorska, M.; Laniecki, M. [Faculty of Chemistry, A. Mickiewicz University, Grunwaldzka 6, 60-780 Poznan (Poland)

    2010-05-15

    Rhodobacter sphaeroides O.U. 001 (concentration of inoculum-0.36 g dry wt/l) and brewery wastewaters were applied in photobiogeneration of hydrogen under illumination of 116 W/m{sup 2}. The best results were obtained with filtered wastewaters sterilized at 120 C for 20 min and maximal concentration of waste in medium equal 10% v/v. The main product in generated biogas was hydrogen (90%). After sterilization the amount of generated hydrogen was tripled (from 0.76 to 2.2 l H{sub 2}/l medium), whereas waste concentration of 10% v/v resulted in the best substrate yield (0.22 l H{sub 2}/l of waste). Under these conditions the amount of generated hydrogen was 2.24 l H{sub 2}/l medium and light conversion efficiency reached value of 1.7%. The modified Gompertz equations served in modeling of the kinetics of the studied process. (author)

  13. Effects of hydrogen bonds in association with flavin and substrate in flavoenzyme d-amino acid oxidase. The catalytic and structural roles of Gly313 and Thr317.

    Science.gov (United States)

    Setoyama, Chiaki; Nishina, Yasuzo; Tamaoki, Haruhiko; Mizutani, Hisashi; Miyahara, Ikuko; Hirotsu, Ken; Shiga, Kiyoshi; Miura, Retsu

    2002-01-01

    According to the three-dimensional structure of a porcine kidney D-amino acid oxidase-substrate (D-leucine) complex model, the G313 backbone carbonyl recognizes the substrate amino group by hydrogen bonding and the side-chain hydroxyl of T317 forms a hydrogen bond with C(2)=O of the flavin moiety of FAD [Miura et al. (1997) J. Biochem. 122, 825-833]. We have designed and expressed the G313A and T317A mutants and compared their enzymatic and spectroscopic properties with those of the wild type. The G313A mutant shows decreased activities to various D-amino acids, but the pattern of substrate specificity is different from that of the wild type. The results imply that the hydrogen bond between the G313 backbone carbonyl and the substrate amino group plays important roles in substrate recognition and in defining the substrate specificity of D-amino acid oxidase. The T317A mutant shows a decreased affinity for FAD. The steady-state kinetic measurements indicate diminished activities of T317A to substrate D-amino acids. The transient kinetic parameters measured by stopped-flow spectroscopy revealed that T317 plays key roles in stabilizing the purple intermediate, a requisite intermediate in the oxidative half-reaction, and in enhancing the release of the product from the active site, thereby optimizing the overall catalytic process of D-amino acid oxidase. PMID:11754736

  14. An efficient route for catalytic activity promotion via hybrid electro-depositional modification on commercial nickel foam for hydrogen evolution reaction in alkaline water electrolysis

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Guanshui; He, Yongwei; Wang, Mei; Zhu, Fuchun; Tang, Bin [Research Institute of Surface Engineering, Taiyuan University of Technology, Yingze West Road 79, Taiyuan 030024 (China); Wang, Xiaoguang, E-mail: wangxiaog1982@163.com [Research Institute of Surface Engineering, Taiyuan University of Technology, Yingze West Road 79, Taiyuan 030024 (China); International Iberian Nanotechnology Laboratory (INL), 4715-330 Braga (Portugal)

    2014-09-15

    Highlights: • Mono-Cu surface modification depress the HER activity of Ni-foam. • Hybrid Ni-foam/Cu0.01/Co0.05 exhibits superior HER performance. • Layer-by-layer structure may contribute to a synergistic promoting effect. - Abstract: In this paper, the single- and hybrid-layered Cu, Ni and Co thin films were electrochemically deposited onto the three-dimensional nickel foam as composite cathode catalyst for hydrogen evolution reaction in alkaline water electrolysis. The morphology, structure and chemical composition of the electrodeposited composite catalysts were investigated using X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive X-ray analysis (EDX). Electrochemical measurement depicted that, for the case of the monometallic layered samples, the general activity for hydrogen evolution reaction followed the sequence: Ni-foam/Ni > Ni-foam/Co > bare Ni-foam > Ni-foam/Cu. It is noteworthy that, the hybrid-layered Ni-foam/Cu0.01/Co0.05 exhibited the highest catalytic activity towards hydrogen evolution reaction with the current density as high as 2.82 times that of the bare Ni-foam. Moreover, both excellent electrochemical and physical stabilities can also be acquired on the Ni-foam/Cu0.01/Co0.05, making this hybrid-layered composite structure as a promising HER electro-catalyst.

  15. Aqueous-phase catalytic hydrogenation of furfural to cyclopentanol over Cu-Mg-Al hydrotalcites derived catalysts:Model reaction for upgrading of bio-oil

    Institute of Scientific and Technical Information of China (English)

    Minghao; Zhou; Zuo; Zeng; Hongyan; Zhu; Guomin; Xiao; Rui; Xiao

    2014-01-01

    A series of Cu-Mg-Al hydrotalcites derived oxides with a(Cu+Mg)/Al mole ratio of 3 and varied Cu/Mg mole ratio(from 0.07 to 0.30) were prepared by co-precipitation and calcination methods, then they were introduced to the hydrogenation of furfural in aqueous-phase. Effects of Cu/Mg mole ratio, reaction temperature, initial hydrogen pressure, reaction time and catalyst amount on the conversion rate of furfural as well as the selectivity toward desired product cyclopentanol were systematically investigated. The conversion of furfural over calcined hydrotalcite catalyst with a Cu/Mg mole ratio of 0.2 was up to 98.5% when the reaction was carried out under 140 ?C and the initial hydrogen pressure of 4 MPa for 10 h, while the selectivity toward cyclopentanol was up to 94.8%. The catalysts were characterized by XRD and SEM. XRD diffraction of all the samples showed characteristic pattern of hydrotalcite with varied peak intensity as a result of different Cu content. The catalytic activity was improved gradually with the increase of Cu component in the hydrotalcite.

  16. On the role of metal particle size and surface coverage for photo-catalytic hydrogen production; a case study of the Au/CdS system

    KAUST Repository

    Majeed, I.

    2015-09-25

    Photo-catalytic hydrogen production has been studied on Au supported CdS catalysts under visible light irradiation in order to understand the effect of Au particle size as well as the reaction medium properties. Au nanoparticles of size about 2-5 nm were deposited over hexagonal CdS particles using a new simple method involving reduction of Au3+ ions with iodide ions. Within the investigated range of Au (between 1 and 5 wt. %) fresh particles with mean size of 4 nm and XPS Au4f/Cd3d surface ratio of 0.07 showed the highest performance (ca. 1 molecule of H2 / Auatom s−1) under visible light irradiation (>420 nm and a flux of 35 mW/cm2). The highest hydrogen production rate was obtained from water (92%)-ethanol (8%) in an electrolyte medium (Na2S-Na2SO3). TEM studies of fresh and used catalysts showed that Au particle size increases (almost 5 fold) with increasing photo-irradiation time due to photo-agglomeration effect yet no sign of deactivation was observed. A mechanism for hydrogen production from ethanol-water electrolyte mixture is presented and discussed.

  17. High Efficiency Generation of Hydrogen Fuels Using Solar Thermochemical Splitting of Water

    Energy Technology Data Exchange (ETDEWEB)

    Heske, Clemens; Moujaes, Samir; Weimer, Alan; Wong, Bunsen; Siegal, Nathan; McFarland, Eric; Miller, Eric; Lewis, Michele; Bingham, Carl; Roth, Kurth; Sabacky, Bruce; Steinfeld, Aldo

    2011-09-29

    The objective of this work is to identify economically feasible concepts for the production of hydrogen from water using solar energy. The ultimate project objective was to select one or more competitive concepts for pilot-scale demonstration using concentrated solar energy. Results of pilot scale plant performance would be used as foundation for seeking public and private resources for full-scale plant development and testing. Economical success in this venture would afford the public with a renewable and limitless source of energy carrier for use in electric power load-leveling and as a carbon-free transportation fuel. The Solar Hydrogen Generation Research (SHGR) project embraces technologies relevant to hydrogen research under the Office of Hydrogen Fuel Cells and Infrastructure Technology (HFCIT) as well as concentrated solar power under the Office of Solar Energy Technologies (SET). Although the photoelectrochemical work is aligned with HFCIT, some of the technologies in this effort are also consistent with the skills and technologies found in concentrated solar power and photovoltaic technology under the Office of Solar Energy Technologies (SET). Hydrogen production by thermo-chemical water-splitting is a chemical process that accomplishes the decomposition of water into hydrogen and oxygen using only heat or a combination of heat and electrolysis instead of pure electrolysis and meets the goals for hydrogen production using only water and renewable solar energy as feed-stocks. Photoelectrochemical hydrogen production also meets these goals by implementing photo-electrolysis at the surface of a semiconductor in contact with an electrolyte with bias provided by a photovoltaic source. Here, water splitting is a photo-electrolytic process in which hydrogen is produced using only solar photons and water as feed-stocks. The thermochemical hydrogen task engendered formal collaborations among two universities, three national laboratories and two private sector

  18. Alkali free hydrolysis of sodium borohydride for hydrogen generation under pressure

    Energy Technology Data Exchange (ETDEWEB)

    Ferreira, M.J.F.; Pinto, A.M.F.R. [Centro de Estudos de Fenomenos de Transporte, Departamento de Engenharia Quimica, Faculdade de Engenharia da Universidade do Porto, Rua Dr. Roberto Frias s/n, 4200-465 Porto (Portugal); Gales, L. [Instituto de Biologia Molecular e Celular, Universidade do Porto, Rua do Campo Alegre 823, 4150-180 Porto and Instituto de Ciencias Biomedicas Abel Salazar, Largo Prof. Abel Salazar 2, 4099-003 Porto (Portugal); Fernandes, V.R.; Rangel, C.M. [Laboratorio Nacional de Energia e Geologia - LNEG, Fuel Cells and Hydrogen Unit Estrada do Paco do Lumiar 22, 1649-038 Lisboa (Portugal)

    2010-09-15

    The present study is related with the production of hydrogen gas (H{sub 2}), at elevated pressures and with high gravimetric storage density, to supply a PEM fuel cell on-demand. To achieve this goal, solid sodium borohydride (NaBH{sub 4}) was mixed with a proper amount of a powder reused nickel-ruthenium based catalyst (Ni-Ru based/NaBH{sub 4}: 0.2 and 0.4 g/g; {approx}150 times reused) inside the bottom of a batch reactor. Then, a stoichiometric amount of pure liquid water (H{sub 2}O/NaBH{sub 4}: 2-8 mol/mol) was added and the catalyzed NaBH{sub 4} hydrolysis evolved, in the absence of an alkali inhibitor. In this way, this research work is designated alkali free hydrolysis of NaBH{sub 4} for H{sub 2} generation. This type of hydrolysis is excellent from an environmental point of view because it does not involve strongly caustic solutions. Experiments were performed in three batch reactors with internal volumes 646, 369 and 229 cm{sup 3}, and having different bottom geometries (flat and conical shapes). The H{sub 2} generated was a function of the added water and completion was achieved with H{sub 2}O/NaBH{sub 4} = 8 mol/mol. The results show that hydrogen yields and rates increase remarkably increasing both system temperature and pressure. Reactor bottom shape influences deeply H{sub 2} generation: the conical bottom shape greatly enhances the rate and practically eliminates the reaction induction time. Our system of compressed hydrogen generation up to 1.26 MPa shows 6.3 wt% and 70 kg m{sup -3}, respectively, for gravimetric and volumetric hydrogen storage capacities (materials-only basis) and therefore is a viable hydrogen storage candidate for portable applications. (author)

  19. Revaluation of hydrogen generation by water radiolysis in SDS vessels at TMI-2 accident

    International Nuclear Information System (INIS)

    Two years after Three Mile Island Unit 2 (TMI-2) loss-of-coolant accident, radioactive contaminated water has been processed by Submerged Demineralizer System (SDS) with two types of zeolite adsorbents to remove radioactive nuclides of Sr-90, Cs-134 and Cs-137. During and after the process, adsorption amount and distribution of nuclides on the zeolites, residual water content and thermal conductivity in the SDS vessels have been measured or estimated for verification of safety in the process, subsequent transportation and disposal. Hydrogen generation has been also evaluated mainly by direct monitoring in the large-scale of vessel after the process. In this work, the revaluation of hydrogen generation was demonstrated on the basis of the open information of vessel, and the latest experimental data obtained in adsorption and radiolysis occurring in small-scale of zeolite-water mixtures. As a property of the zeolites (UOP IE-96, A-51), adsorption and desorption of water vapour on the zeolites were observed as a function of relative pressure corresponding to relative humidity. 10-20 wt% of water was found to be physically and chemically adsorbed on the zeolites within normal humidity of 20 to 90 %RH, reflecting residual water content absorbed on the dominant zeolites in the dewatering of vessels after the process. Hydrogen generated in the radiolysis of zeolite-water mixtures was further measured to obtain the observed yields of hydrogen as functions of water content in the mixtures and of the height of mixtures. It was found that additional water radiolysis took place through the energy dissipation of radiation to the zeolites, and that liquid depth effect on the yield in water was depressed by adding zeolites to water. Based on these experimental results and further estimations, hydrogen generation dependent on decay heat and water content in the SDS vessel was finally revaluated. The procedure and results in this revaluation would be helpful for the decontamination

  20. Novel developments in hydrogen storage, hydrogen activation and ionic liquids

    Energy Technology Data Exchange (ETDEWEB)

    Doroodian, Amir

    2010-12-03

    This dissertation is divided into three chapters. Recently, metal-free hydrogen activation using phosphorous compounds has been reported in science magazine. We have investigated the interaction between hydrogen and phosphorous compounds in presence of strong Lewis acids (chapter one). A new generation of metal-free hydrogen activation, using amines and strong Lewis acids with sterically demanding nature, was already developed in our group. Shortage of high storage capacity using large substitution to improve sterical effect led us to explore the amine borane derivatives, which are explained in chapter two. Due to the high storage capacity of hydrogen in aminoborane derivatives, we have explored these materials to extend hydrogen release. These compounds store hydrogen as proton and hydride on adjacent atoms or ions. These investigations resulted in developing hydrogen storage based on ionic liquids containing methyl guanidinium cation. Then we have continued to develop ionic liquids based on methyl guanidinium cation with different anions, such as tetrafluoro borate (chapter three). We have replaced these anions with transition metal anions to investigate hydrogen bonding and catalytic activity of ionic liquids. This chapter illustrates the world of ionic liquid as a green solvent for organic, inorganic and catalytic reactions and combines the concept of catalysts and solvents based on ionic liquids. The catalytic activity is investigated particularly with respect to the interaction with CO{sub 2}. (orig.)

  1. SLUDGE BATCH 4 FOLLOW-UP QUALIFICATION STUDIES TO EVALUATE HYDROGEN GENERATION

    Energy Technology Data Exchange (ETDEWEB)

    Pareizs, J; David Koopman, D; Dan Lambert, D; Cj Bannochie, C

    2007-08-23

    Follow-up testing was conducted to better understand the excessive hydrogen generation seen in the initial Sludge Batch 4 (SB4) qualification Sludge Receipt and Adjustment Tank/Slurry Mix Evaporator (SRAT/SME) simulation in the Savannah River National Laboratory (SRNL) Shielded Cells. This effort included both radioactive and simulant work. The initial SB4 qualification test produced 0.59 lbs/hr hydrogen in the SRAT, which was just below the DWPF SRAT limit of 0.65 lbs/hr, and the test produced over 0.5 lbs/hr hydrogen in the SME cycle on two separate occasions, which were over the DWPF SME limit of 0.223 lbs/hr.

  2. Adsorption-parallel catalytic waves of cinnamic acid in hydrogen peroxide-tetra-n-butylammonium bromide-acetate system

    Institute of Scientific and Technical Information of China (English)

    亢晓峰; 过玮; 赵川; 宋俊峰

    2000-01-01

    The mechanism of the adsorption-parallel catalytic wave of cinnamic acid (C6H5—CH = CH—COOH) in acetate buffer (pH = 4.0)-H2O2-tetra-n-butylammonium bromide (Bu4N · Br) solution was studied by the linear-sweep polarography, cyclic voltammetry and digital simulation approach. Experimental results indicate that the reduction mechanism of cinnamic acid is ECdimE’ process, in which the C = C double bond of cinnamic acid first undergoes 1 e, 1H+ reduction to produce an intermediate free radical C6H5—CH—CH2—COOH(E), then the further reduction of the free radical in 1e,1H+ addition (E’) occurs simultaneously with a dimerization reaction between two free radicals (Cdim). Bu4N · Br enhances the polarographic current of cinnamic acid and shifts the peak potential to positive direction. The enhancement action of Bu4N · Br is due to the adsorption of cinnamic acid induced by Bu4N+ species. In addition, H2O2 causes the parallel catalytic wave of cinnamic acid. The mechanism of the catalytic wave is EC’ proce

  3. Study on the Dynamics of Catalytic Hydrogenation of Adiponitrile%己二腈催化加氢的动力学研究

    Institute of Scientific and Technical Information of China (English)

    陈聚良; 张华森; 刘国际

    2012-01-01

    对间歇高压釜中进行的雷尼镍催化己二腈加氢的反应动力学进行了研究.通过考察反应过程己二腈、氨基己腈以及己二胺的浓度随时间变化的规律,可计算得到各步反应的反应级数、指前因子和活化能等动力学参数.结果表明,在消除内、外扩散影响的情况下,328 ~358 K的温度范围,2~3.5 MPa 的压力范围内,己二腈加氢成为氨基已腈的过程对己二腈呈一级反应,对氢气呈1.4级反应;氨基己腈继续加氢制备己二胺的过程对氨基己腈为零级反应,对氢气为1.3级反应.在此基础上建立了己二腈催化加氢制备己二胺的各步反应的动力学方程,并对动力学方程进行了验证.%The kinetics for hydrogenation of adiponitrile were studied with Raney nickel as catalyst in a a high-pressure batch reactor. Under the condition of no inside and outside diffusion, the concentration of adiponitrile , aminocaproic nitrile and hexamethylenediamine versus time over the Raney - Ni catalyst were measured. The kinetic parameters of catalytic hydrogenation of adiponitrile to hexamethylenediamine such as reaction order, pre - exponential factor and activated energy in each step were obtained. The results show that, when the temperature kept at 328 -358K and pressure kept at 2 ~3. 5MPa, the order of adiponitrile hydrogenation to adiponitrile was 1, while to hydrogen pressure was 1.4. The intermediate aminocaproic nitrile was hydrogena-ted to hexamethylene diamine, the reaction order to aminocaproic nitrile was 0, to hydrogen pressure was 1.3. Based on these results, the kinetic equations of adiponitrile hydrogenation to hexamethylenediamine in each step were proposed. They are in consistence with the experimental data.

  4. Generation of tubular beams of negative hydrogen ions by a surface plasma source

    International Nuclear Information System (INIS)

    The results of experiments on obtaining a tubular beam of hydrogen negative ions from a surface plasma source with emission ring slit of 100 mm diameter are described in the study. Conditions of burning of a high current ring discharge generating effectively hydrogen negative ions with current density up to 2.1 A/cm2 are investigated. The possibility of generation of intensive tubular beams of hydrogen negative ions by surface plasma sources is shown, the 2.4 A ion beam is obtained. The results of preliminary experiments on accelerating tubular beam up to 135 keV are described. Azymuthally uniform current density distribution of intensive tubular beams generated by discharges with a close electron drift in a surface plasma source with emission ring slit, absence of high-frequency oscillations in optimal conditions of sources operation as well as the possibility of the most complete use of generated by the discharge negative ions flow show the prospects of development of these sources for fast atom injectors

  5. In situ generation of hydrogen from water by aluminum corrosion in solutions of sodium aluminate

    Energy Technology Data Exchange (ETDEWEB)

    Soler, Lluis; Candela, Angelica Maria; Munoz, Maria; Casado, Juan [Centre Grup de Tecniques de Separacio en Quimica (GTS), Unitat de Quimica Analitica, Departament de Quimica, Universitat Autonoma de Barcelona, Campus UAB s/n, 08193 Bellaterra, Barcelona, Catalonia (Spain); Macanas, Jorge [Laboratoire de Genie Chimique, UMR 5503 CNRS-INPT-UPS, Universite de Toulouse, Toulouse (France)

    2009-07-01

    A new process to obtain hydrogen from water using aluminum in sodium aluminate solutions is described and compared with results obtained in aqueous sodium hydroxide. This process consumes only water and aluminum, which are raw materials much cheaper than other compounds used for in situ hydrogen generation, such as hydrocarbons and chemical hydrides, respectively. As a consequence, our process could be an economically feasible alternative for hydrogen to supply fuel cells. Results showed an improvement of the maximum rates and yields of hydrogen production when NaAlO{sub 2} was used instead of NaOH in aqueous solutions. Yields of 100% have been reached using NaAlO{sub 2} concentrations higher than 0.65 M and first order kinetics at concentrations below 0.75 M has been confirmed. Two different heterogeneous kinetic models are verified for NaAlO{sub 2} aqueous solutions. The activation energy (E{sub a}) of the process with NaAlO{sub 2} is 71 kJ mol{sup -1}, confirming a control by a chemical step. A mechanism unifying the behavior of Al corrosion in NaOH and NaAlO{sub 2} solutions is presented. The application of this process could reduce costs in power sources based on fuel cells that nowadays use hydrides as raw material for hydrogen production. (author)

  6. Effect of Copper Nanoparticles Dispersion on Catalytic Performance of Cu/SiO2 Catalyst for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

    Directory of Open Access Journals (Sweden)

    Yajing Zhang

    2013-01-01

    Full Text Available Cu/SiO2 catalysts, for the synthesis of ethylene glycol (EG from hydrogenation of dimethyl oxalate (DMO, were prepared by ammonia-evaporation and sol-gel methods, respectively. The structure, size of copper nanoparticles, copper dispersion, and the surface chemical states were investigated by X-ray diffraction (XRD, transmission electron microscopy (TEM, temperature-programmed reduction (TPR, and X-ray photoelectron spectroscopy (XPS and N2 adsorption. It is found the structures and catalytic performances of the catalysts were highly affected by the preparation method. The catalyst prepared by sol-gel method had smaller average size of copper nanoparticles (about 3-4 nm, better copper dispersion, higher Cu+/C0 ratio and larger BET surface area, and higher DMO conversion and EG selectivity under the optimized reaction conditions.

  7. Preparation, structural characterization and catalytic properties of Co/CeO2 catalysts for the steam reforming of ethanol and hydrogen production

    Science.gov (United States)

    Lovón, Adriana S. P.; Lovón-Quintana, Juan J.; Almerindo, Gizelle I.; Valença, Gustavo P.; Bernardi, Maria I. B.; Araújo, Vinícius D.; Rodrigues, Thenner S.; Robles-Dutenhefner, Patrícia A.; Fajardo, Humberto V.

    2012-10-01

    In this paper, Co/CeO2 catalysts, with different cobalt contents were prepared by the polymeric precursor method and were evaluated for the steam reforming of ethanol. The catalysts were characterized by N2 physisorption (BET method), X-ray diffraction (XRD), UV-visible diffuse reflectance, temperature programmed reduction analysis (TPR) and field emission scanning electron microscopy (FEG-SEM). It was observed that the catalytic behavior could be influenced by the experimental conditions and the nature of the catalyst employed. Physical-chemical characterizations revealed that the cobalt content of the catalyst influences the metal-support interaction which results in distinct catalyst performances. The catalyst with the highest cobalt content showed the best performance among the catalysts tested, exhibiting complete ethanol conversion, hydrogen selectivity close to 66% and good stability at a reaction temperature of 600 °C.

  8. Effect of Copper Nanoparticles Dispersion on Catalytic Performance of Cu/SiO2 Catalyst for Hydrogenation of Dimethyl Oxalate to Ethylene Glycol

    International Nuclear Information System (INIS)

    Cu/SiO2 catalysts, for the synthesis of ethylene glycol (EG) from hydrogenation of dimethyl oxalate (DMO), were prepared by ammonia-evaporation and sol-gel methods, respectively. The structure, size of copper nanoparticles, copper dispersion, and the surface chemical states were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS) and N2 adsorption. It is found the structures and catalytic performances of the catalysts were highly affected by the preparation method. The catalyst prepared by sol-gel method had smaller average size of copper nanoparticles (about 3-4 nm), better copper dispersion, higher Cu+/C0 ratio and larger BET surface area, and higher DMO conversion and EG selectivity under the optimized reaction conditions.

  9. A polymer electrolyte fuel cell stack for stationary power generation from hydrogen fuel

    Energy Technology Data Exchange (ETDEWEB)

    Zawodzinski, C.; Wilson, M.; Gottesfeld, S. [Los Alamos National Lab., NM (United States)

    1996-10-01

    The fuel cell is the most efficient device for the conversion of hydrogen fuel to electric power. As such, the fuel cell represents a key element in efforts to demonstrate and implement hydrogen fuel utilization for electric power generation. A central objective of a LANL/Industry collaborative effort supported by the Hydrogen Program is to integrate PEM fuel cell and novel stack designs at LANL with stack technology of H-Power Corporation (H-Power) in order to develop a manufacturable, low-cost/high-performance hydrogen/air fuel cell stack for stationary generation of electric power. A LANL/H-Power CRADA includes Tasks ranging from exchange, testing and optimization of membrane-electrode assemblies of large areas, development and demonstration of manufacturable flow field, backing and bipolar plate components, and testing of stacks at the 3-5 cell level and, finally, at the 4-5 kW level. The stack should demonstrate the basic features of manufacturability, overall low cost and high energy conversion efficiency. Plans for future work are to continue the CRADA work along the time line defined in a two-year program, to continue the LANL activities of developing and testing stainless steel hardware for longer term stability including testing in a stack, and to further enhance air cathode performance to achieve higher energy conversion efficiencies as required for stationary power application.

  10. Rapid hydrogen gas generation using reactive thermal decomposition of uranium hydride.

    Energy Technology Data Exchange (ETDEWEB)

    Kanouff, Michael P.; Van Blarigan, Peter; Robinson, David B.; Shugard, Andrew D.; Gharagozloo, Patricia E.; Buffleben, George M.; James, Scott Carlton; Mills, Bernice E.

    2011-09-01

    Oxygen gas injection has been studied as one method for rapidly generating hydrogen gas from a uranium hydride storage system. Small scale reactors, 2.9 g UH{sub 3}, were used to study the process experimentally. Complimentary numerical simulations were used to better characterize and understand the strongly coupled chemical and thermal transport processes controlling hydrogen gas liberation. The results indicate that UH{sub 3} and O{sub 2} are sufficiently reactive to enable a well designed system to release gram quantities of hydrogen in {approx} 2 seconds over a broad temperature range. The major system-design challenge appears to be heat management. In addition to the oxidation tests, H/D isotope exchange experiments were performed. The rate limiting step in the overall gas-to-particle exchange process was found to be hydrogen diffusion in the {approx}0.5 {mu}m hydride particles. The experiments generated a set of high quality experimental data; from which effective intra-particle diffusion coefficients can be inferred.

  11. Sewage-sludge-derived carbonaceous materials for catalytic wet hydrogen peroxide oxidation of m-cresol in batch and continuous reactors.

    Science.gov (United States)

    Yu, Yang; Wei, Huangzhao; Yu, Li; Wang, Wei; Zhao, Ying; Gu, Bin; Sun, Chenglin

    2016-01-01

    In this study, four sewage-sludge-derived carbonaceous materials (SWs) were evaluated for their catalytic wet hydrogen peroxide oxidation (CWPO) performance of m-cresol in batch reactor and continuous reactor, respectively. The SWs were produced by carbonization (SW); carbonization with the addition of CaO (CaO-SW); HNO3 pretreatment (HNO3-SW) and steam activation (Activated-SW). The properties of SW catalysts were assessed by thermogravimetric analysis, Brunauer-Emmett-Teller, Fourier Transform Infrared Spectroscopy, X-ray Fluorescence, Scanning electron microscopy, energy dispersive X-ray analysis and zeta potential. The results showed that SW treated by HNO3 (HNO3-SW) had a high conversion of m-cresol in batch reactor and continuous reactor, respectively. Under the conditions of batch reaction (Cm-cresol = 100 mg L(-1), CH2O2 = 15.7 mmol L(-1), initial pH=7.0, 0.5 g L(-1) catalyst, 80°C, 180 min adsorption and 210 min oxidation), the conversion of m-cresol reached 100% and total organic carbon removal was 67.1%. It had a high catalytic activity and stability on the treatment of m-cresol in CWPO for more than 1100 h. Furthermore, a possible reaction mechanism for the oxidation of m-cresol to 2-methyl-p-benzoquinone by CWPO was proposed. PMID:26109374

  12. Nickel-based xerogel catalysts: Synthesis via fast sol-gel method and application in catalytic hydrogenation of p-nitrophenol to p-aminophenol

    Science.gov (United States)

    Feng, Jin; Wang, Qiang; Fan, Dongliang; Ma, Lirong; Jiang, Deli; Xie, Jimin; Zhu, Jianjun

    2016-09-01

    In order to investigate the roles of three-dimensional network structure and calcium on Ni catalysts, the Ni, Ni-Al2O3, Ni-Ca-Al2O3 xerogel catalysts were successfully synthesized via the fast sol-gel process and chemical reduction method. The crystal structure of three different catalysts was observed with X-ray powder diffraction (XRD). Transmission electron microscopy (TEM), scanning electron microscopy (SEM) and nitrogen adsorption-desorption were employed to investigate the role of network structure of xerogel catalysts and the size distribution of Ni nanoparticles. The catalyst composition was determined by inductively coupled plasma-optical emission spectrometry (ICP-OES) measurement and energy-dispersive X-ray spectroscopy (EDS). Temperature-programmed reduction (TPR) experiments were carried out to investigate the reducibility of nickel species and the interaction between nickel species and alumina. The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over the prepared nickel-based xerogel catalysts. The conversion of p-nitrophenol was monitored by UV spectrophotometry and high performance liquid chromatography (HPLC). The results show that the catalysts are highly selective for the conversion of p-nitrophenol to p-aminophenol and the order of catalytic activities of the catalysts is Ni < Ni-Al2O3 < Ni-Ca-Al2O3. The catalysts were recycled and were used to evaluate the reutilization.

  13. Synthesis and Catalytic Performance of Graphene Modified CuO-ZnO-Al2O3 for CO2 Hydrogenation to Methanol

    Directory of Open Access Journals (Sweden)

    Zheng-juan Liu

    2014-01-01

    Full Text Available CuO-ZnO-Al2O3 and graphene nanosheet (GNS were synthesized by coprecipitation route and reduction of exfoliated graphite oxides method, respectively. GNS modified CuO-ZnO-Al2O3 nanocomposites were synthesized by high energy ball milling method. The structure, morphology, and character of the synthesized materials were studied by BET, XRD, TEM, and H2-TPR. It was found that by high energy ball milling method the CuO-ZnO-Al2O3 nanoparticles were uniformly dispersed on GNS surfaces. The catalytic performance for the methanol synthesis from CO2 hydrogenation was also tested. It was shown experimentally that appropriate incorporation of GNS into the CuO-ZnO-Al2O3 could significantly increase the catalyst activity for methanol synthesis. The 10 wt.% GNS modified CuO-ZnO-Al2O3 catalyst gave a methanol space time yield (STY of 92.5% higher than that on the CuO-ZnO-Al2O3 catalyst without GNS. The improved catalytic performance was attributed to the excellent promotion of GNS to dispersion of CuO and ZnO particles.

  14. Preparation, Characterization, and Enhanced Photo catalytic Hydrogen Evolution Activity of Y2Cu2O5-Based Compounds under Simulated Sunlight Irradiation

    International Nuclear Information System (INIS)

    Y2Cu2O5 photo catalyst was successfully prepared via solid state reaction and further combined with TiO2 by a sol-gel method and a solid phase method, respectively. For comparison, Pt Y2Cu2O5particles were loaded to prepare Pt- via a hydrogen reduction method. All the samples were characterized by thermogravimetry and differential thermal analysis (TG/DTA), X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), and scanning electron microscopy (SEM) techniques. Photo catalytic H2 evolution activities of the as-obtained samples were evaluated from aqueous oxalic acid solution under simulated sunlight irradiation. The effects of photo catalyst concentration, TiO2 content, and composite method on the H2 evolution activities of the as-obtained photo catalysts were investigated. The results show that, when the concentration of photo catalyst is 0.8 gL-1, the TiO2 Y2Cu2O5 composite photo catalyst prepared by a sol-gel method exhibits the optimized photo catalytic activity, and the H2 production rate is 4.35 m mol with 30 wt.% content of TiO2

  15. Catalytic Asymmetric Reduction of a 3,4-Dihydroisoquinoline for the Large-Scale Production of Almorexant : Hydrogenation or Transfer Hydrogenation?

    NARCIS (Netherlands)

    Verzijl, Gerard K.M.; Vries, André H.M. de; Vries, Johannes G. de; Kapitan, Peter; Dax, Thomas; Helms, Matthias; Nazir, Zarghun; Skranc, Wolfgang; Imboden, Christoph; Stichler, Juergen; Ward, Richard A.; Abele, Stefan; Lefort, Laurent

    2013-01-01

    Several methods are presented for the enantioselective synthesis of the tetrahydroisoquinoline core of almorexant (ACT-078573A), a dual orexin receptor antagonist. Initial clinical supplies were secured by the Noyori Ru-catalyzed asymmetric transfer hydrogenation (Ru-Noyori ATH) of the dihydroisoqui

  16. Photo-driven autonomous hydrogen generation system based on hierarchically shelled ZnO nanostructures

    International Nuclear Information System (INIS)

    A quantum dot semiconductor sensitized hierarchically shelled one-dimensional ZnO nanostructure has been applied as a quasi-artificial leaf for hydrogen generation. The optimized ZnO nanostructure consists of one dimensional nanowire as a core and two-dimensional nanosheet on the nanowire surface. Furthermore, the quantum dot semiconductors deposited on the ZnO nanostructures provide visible light harvesting properties. To realize the artificial leaf, we applied the ZnO based nanostructure as a photoelectrode with non-wired Z-scheme system. The demonstrated un-assisted photoelectrochemical system showed the hydrogen generation properties under 1 sun condition irradiation. In addition, the quantum dot modified photoelectrode showed 2 mA/cm2 current density at the un-assisted condition

  17. Safety operation of chromatography column system with discharging hydrogen radiolytically generated

    Directory of Open Access Journals (Sweden)

    Watanabe Sou

    2015-01-01

    Full Text Available In the extraction chromatography system, accumulation of hydrogen gas in the chromatography column is suspected to lead to fire or explosion. In order to prevent the hazardous accidents, it is necessary to evaluate behaviors of gas radiolytically generated inside the column. In this study, behaviors of gas inside the extraction chromatography column were investigated through experiments and Computation Fluid Dynamics (CFD simulation. N2 gas once accumulated as bubbles in the packed bed was hardly discharged by the flow of mobile phase. However, the CFD simulation and X-ray imaging on γ-ray irradiated column revealed that during operation the hydrogen gas generated in the column was dissolved into the mobile phase without accumulation and discharged.

  18. Double-side illuminated titania nanotubes for high volume hydrogen generation by water splitting

    International Nuclear Information System (INIS)

    A sonoelectrochemical anodization method is proposed to synthesize TiO2 nanotubular arrays on both sides of a titanium foil (TiO2/Ti/TiO2). Highly ordered TiO2 nanotubular arrays of 16 cm2 area with uniform surface distribution can be obtained using this anodization procedure. These double-sided TiO2/Ti/TiO2 materials are used as both photoanode (carbon-doped titania nanotubes) and cathode (Pt nanoparticles dispersed on TiO2 nanotubes; PtTiO2/Ti/PtTiO2) in a specially designed photoelectrochemical cell to generate hydrogen by water splitting at a rate of 38 ml h-1. The nanomaterials are characterized by FESEM, HRTEM, STEM, EDS, FFT, SAED and XPS techniques. The present approach can be used for large-scale hydrogen generation using renewable energy sources

  19. Enhancement of reaction rates for catalytic benzaldehyde hydrogenation and sorbitol dehydration in water solvent by addition of carbon dioxide

    Indian Academy of Sciences (India)

    Masayuki Shirai; Osamu Sato; Norihito Hiyoshi; Aritomo Yamaguchi

    2014-03-01

    The effect of pressured carbon dioxide on heterogeneous hydrogenation of benzaldehyde and homogeneous dehydration of sorbitol in water solvent was studied. Initial hydrogenation rates of benzaldehyde over a charcoal-supported palladium catalyst in water at 313 K were enhanced by the addition of carbon dioxide. The initial rate increased with an increase in carbon dioxide pressure and became a maximum at 5 MPa. Dehydration of sorbitol proceeded in water phase at 500 K and initial dehydration rates were enhanced by addition of 30 MPa of carbon dioxide.

  20. Hydrogen generation by photoelectrochemical effect of the Cu-doped TiO2 photoanode

    International Nuclear Information System (INIS)

    TiO2 film photoanodes with a size of 1 × 1 cm2 were fabricated by a spin coating method. Cu-doped TiO2 powder with various Cu concentrations (0.2, 0.4, 0.6 and 0.8 at%) and surfactant were used as starting materials in coating Cu-doped TiO2 thin films onto FTO/glass substrate. Crystalline structure of TiO2 material, microstructure of the photoanode films and their thickness were identified by x-ray diffraction and Raman scattering. Hydrogen generation from water by photoelectrochemical effect in the visible light was observed by recording I/V characteristics of the photoanode in dark and light regimes. The obtained results have shown that the hydrogen generation efficiency of photoanode nonlinearly depends on Cu concentration. The nonlinear dependence of the hydrogen generation efficiency may be due to a change of resistivity of the film photoanode that is related with the random distribution of the hetero-junction between interfaces of TiO2 and CuO nanoparticles. (paper)

  1. Easy synthesis of bismuth iron oxide nanoparticles as photocatalyst for solar hydrogen generation from water

    Science.gov (United States)

    Deng, Jinyi

    In this study, high purity bismuth iron oxide (BiFeO3/BFO) nanoparticles of size 50-80 nm have been successfully synthesized by a simple sol-gel method using urea and polyvinyl alcohol at low temperature. X-ray diffraction (XRD) measurement is used to optimize the synthetic process to get highly crystalline and pure phase material. Diffuse reflectance ultraviolet-visible (DRUV-Vis) spectrum indicates that the absorption cut-off wavelength of the nanoparticles is about 620 nm, corresponding to an energy band gap of 2.1 eV. Compared to BaTiO3, BFO has a better degradation of methyl orange under light radiation. Also, photocatalytic tests prove this material to be efficient towards water splitting under simulated solar light to generate hydrogen. The simple synthetic methodology adopted in this paper will be useful in developing low-cost semiconductor materials as effective photocatalysts for hydrogen generation. Photocatalytic tests followed by gas chromatography (GC) analyses show that BiFeO3 generates three times more hydrogen than commercial titania P25 catalyst under the same experimental conditions.

  2. A detailed study of the diastereoselective catalytic hydrogenation of 6-hydroxytetrahydroisoquinoline-(3R)-carboxylic ester intermediates

    NARCIS (Netherlands)

    Lefort, Laurent; Sereinig, Natascha; Straatman, Harrie; Ager, David J.; Vries, Johannes G. de; Werner, John A.; Scherer, Roger B.; Maloney, Todd D.; Argentine, Mark D.; Sullivan, Kevin A.; Fennell, Jared W.

    2012-01-01

    A key step towards a highly-selective antagonist of ionotropic glutamate receptors entails the diastereoselective arene hydrogenation of an enantiopure tetrahydroisoquinoline. An extensive screen using parallel reactors was conducted and led to the discovery of several Pd/C catalysts giving high yie

  3. Influence of preparation method on supported Cu-Ni alloys and their catalytic properties in high pressure CO hydrogenation

    DEFF Research Database (Denmark)

    Wu, Qiongxiao; Eriksen, Winnie L.; Duchstein, Linus Daniel Leonhard;

    2014-01-01

    to impregnation, the coprecipitation and deposition-coprecipitation methods are more efficient for preparation of small and homogeneous Cu-Ni alloy nanoparticles. In order to examine the stability of Cu-Ni alloys in high pressure synthesis gas conversion, they have been tested for high pressure CO hydrogenation...

  4. Mixed Ionic and Electonic Conductors for Hydrogen Generation and Separation: A New Approach

    Energy Technology Data Exchange (ETDEWEB)

    Srikanth Gopalan

    2006-12-31

    Composite mixed conductors comprising one electronic conducting phase, and one ionic conducting phase (MIECs) have been developed in this work. Such MIECs have applications in generating and separating hydrogen from hydrocarbon fuels at high process rates and high purities. The ionic conducting phase comprises of rare-earth doped ceria and the electronic conducting phase of rare-earth doped strontium titanate. These compositions are ideally suited for the hydrogen separation application. In the process studied in this project, steam at high temperatures is fed to one side of the MIEC membrane and hydrocarbon fuel or reformed hydrocarbon fuel to the other side of the membrane. Oxygen is transported from the steam side to the fuel side down the electrochemical potential gradient thereby enriching the steam side flow in hydrogen. The remnant water vapor can then be condensed to obtain high purity hydrogen. In this work we have shown that two-phase MIECs comprising rare-earth ceria as the ionic conductor and doped-strontium titanate as the electronic conductor are stable in the operating environment of the MIEC. Further, no adverse reaction products are formed when these phases are in contact at elevated temperatures. The composite MIECs have been characterized using a transient electrical conductivity relaxation technique to measure the oxygen chemical diffusivity and the surface exchange coefficient. Oxygen permeation and hydrogen generation rates have been measured under a range of process conditions and the results have been fit to a model which incorporates the oxygen chemical diffusivity and the surface exchange coefficient from the transient measurements.

  5. Hydrogen gas generation from refuse-derived fuel (RDF) under wet conditions.

    Science.gov (United States)

    Sakka, Makiko; Kimura, Tetsuya; Sakka, Kazuo; Ohmiya, Kunio

    2004-02-01

    An explosion has recently occurred at a silo containing refuse-derived fuels (RDF) in Japan. There is a possibility that microorganisms are involved in generation of combustible gas from RDF and this study was aimed at showing the presence of bacteria that can ferment RDF pellets. All RDF samples tested contained a relatively high number of viable bacterial cells, 1.4x10(5) to 3.2x10(6) viable cells/g. These bacteria in the RDF samples fermented them to generate heat and hydrogen gas. PMID:14981319

  6. Catalytic activity of hydrophobic Pt/C/PTFE catalysts of different PTFE content for hydrogen-water liquid exchange reaction

    International Nuclear Information System (INIS)

    10%Pt/C catalysts were prepared by liquid reduction method. PTFE and Pt/ C catalysts were adhered to porous metal and hydrophobic Pt/C/PTFE catalysts were prepared. The structure and size of Pt crystal particles of Pt/C catalysts were analyzed by XRD, and their mean size was 3.1 nm. The dispersion state of Pt/C and PTFE was analyzed by SEM, and they had good dispersion mostly, but PTFE membrane could be observed on local parts of Pt/C/PTFE surface. Because of low hydrophobicity, Pt/C/ PTFE catalysts have low activity when the mass ratio of PTFE and Pt/C is 0.5: 1, and their catalytic activity increases markedly when the ratio is 1:1. When the ratio increases again, more Pt active sites would be covered by PTFE and interior diffusion effect would increase, which result in the decrease of catalytic activity of Pt/C/PTFE. By PTFE pretreatment of porous metal carrier, the activity of Pt/C/PTFE catalysts decreases when the mass ratio of PTFE and Pt/C is 0.5:1, and their activity decreases when the mass ratio is 1:1. (authors)

  7. Gas cleaning and hydrogen sulfide removal for COREX coal gas by sorption enhanced catalytic oxidation over recyclable activated carbon desulfurizer.

    Science.gov (United States)

    Sun, Tonghua; Shen, Yafei; Jia, Jinping

    2014-02-18

    This paper proposes a novel self-developed JTS-01 desulfurizer and JZC-80 alkaline adsorbent for H2S removal and gas cleaning of the COREX coal gas in small-scale and commercial desulfurizing devices. JTS-01 desulfurizer was loaded with metal oxide (i.e., ferric oxides) catalysts on the surface of activated carbons (AC), and the catalyst capacity was improved dramatically by means of ultrasonically assisted impregnation. Consequently, the sulfur saturation capacity and sulfur capacity breakthrough increased by 30.3% and 27.9%, respectively. The whole desulfurizing process combined selective adsorption with catalytic oxidation. Moreover, JZC-80 adsorbent can effectively remove impurities such as HCl, HF, HCN, and ash in the COREX coal gas, stabilizing the system pressure drop. The JTS-01 desulfurizer and JZC-80 adsorbent have been successfully applied for the COREX coal gas cleaning in the commercial plant at Baosteel, Shanghai. The sulfur capacity of JTS-01 desulfurizer can reach more than 50% in industrial applications. Compared with the conventional dry desulfurization process, the modified AC desulfurizers have more merit, especially in terms of the JTS-01 desulfurizer with higher sulfur capacity and low pressure drop. Thus, this sorption enhanced catalytic desulfurization has promising prospects for H2S removal and other gas cleaning. PMID:24456468

  8. Gas cleaning and hydrogen sulfide removal for COREX coal gas by sorption enhanced catalytic oxidation over recyclable activated carbon desulfurizer.

    Science.gov (United States)

    Sun, Tonghua; Shen, Yafei; Jia, Jinping

    2014-02-18

    This paper proposes a novel self-developed JTS-01 desulfurizer and JZC-80 alkaline adsorbent for H2S removal and gas cleaning of the COREX coal gas in small-scale and commercial desulfurizing devices. JTS-01 desulfurizer was loaded with metal oxide (i.e., ferric oxides) catalysts on the surface of activated carbons (AC), and the catalyst capacity was improved dramatically by means of ultrasonically assisted impregnation. Consequently, the sulfur saturation capacity and sulfur capacity breakthrough increased by 30.3% and 27.9%, respectively. The whole desulfurizing process combined selective adsorption with catalytic oxidation. Moreover, JZC-80 adsorbent can effectively remove impurities such as HCl, HF, HCN, and ash in the COREX coal gas, stabilizing the system pressure drop. The JTS-01 desulfurizer and JZC-80 adsorbent have been successfully applied for the COREX coal gas cleaning in the commercial plant at Baosteel, Shanghai. The sulfur capacity of JTS-01 desulfurizer can reach more than 50% in industrial applications. Compared with the conventional dry desulfurization process, the modified AC desulfurizers have more merit, especially in terms of the JTS-01 desulfurizer with higher sulfur capacity and low pressure drop. Thus, this sorption enhanced catalytic desulfurization has promising prospects for H2S removal and other gas cleaning.

  9. A catalytic recombiner performance analysis considering fluid dynamics in a containment

    Energy Technology Data Exchange (ETDEWEB)

    Tahara, Mika; Oikawa, Hirohide [Toshiba Corporation, Plant and System Planning Department, Yokohama, Kanagawa (Japan); Arai, Kenji [Toshiba Corporation, Nuclear System Analysis Technology R and D Department, Kawasaki, Kanagawa (Japan)

    2000-10-01

    A severe accident in a light water reactor has the potential to generate hydrogen resulting from metal-water reaction and radiolysis of water. To prevent hydrogen combustion, a flammability gas control system is installed in a reactor containment. Recently passive catalytic recombiners have been developed for the flammability gas control. The catalytic recombiner has advantages over the current heated type recombiner for low costs, easy maintenance, robustness during an accident, and flexible layout. However the hydrogen depletion rate of the catalytic recombiner is affected by the local thermal hydraulic conditions during an accident. To evaluate hydrogen depletion by the catalytic recombiner considering the thermal hydraulic conditions in the containment, a 3-dimensional fluid dynamics analysis is useful. Then a catalytic recombiner model has been developed in which the flammable gas depletion rate is estimated accounting for the flammable gas transfer rate to the catalyst active point from bulk gas. And this model has been incorporated into a 3-dimensional fluid dynamic model, which has been developed using a CFD code STAR-CD. In this paper the 3-dimensional catalytic recombiner model was applied to a catalytic recombiner consisting of plate type catalyst. Confirmation of this model was conducted by using the test result of KALI-H2. The analysis model reasonably predicts the local thermal hydraulic conditions in the containment and the catalytic recombiner performance. (author)

  10. Investigation of the high-order harmonic generation and ionization of model hydrogen atom and real hydrogen atom in intense laser field

    International Nuclear Information System (INIS)

    Solving time-dependent Schroedinger equation numerically, we investigate the high-order harmonic generation and ionization probability of one dimensional, two dimensional and three dimensional hydrogen atom exposed to intense laser field. In the tunneling ionization regime, our results show that the HHG plateau features and cutoff positions of model hydrogen atoms are well agreement with those of real hydrogen atom, and the trend of changing of the ionization probabilities with time is similar, but the values of ionization probabilities for model atoms are different from ones for three dimensional hydrogen atom. We explain the reason for the difference of ionization probabilities between model atoms and real hydrogen atom according to the semiclassical three-step model. (author)

  11. Preparation and Characterization of Polymer-Stabilized Ruthenium-Platinum and Ruthenium-Palladium Bimetallic Colloids and Their Catalytic Properties for Hydrogenation of o-Chloronitrobenzene.

    Science.gov (United States)

    Liu; Yu; Liu; Zheng

    1999-06-15

    Colloidal dispersions of poly(N-vinyl-2-pyrrolidone) (PVP)-stabilized ruthenium-platinum and ruthenium-palladium bimetallic colloids were prepared by NaBH4 reduction of the corresponding mixed-metal salts at room temperature and characterized by TEM, XPS, and XRD. The resulting bimetallic colloids were used as catalysts for the selective hydrogenation of o-chloronitrobenzene (o-CNB) in methanol at 303 K under 0.1 MPa of hydrogen. It was observed that the catalytic performance of PVP-stabilized ruthenium-platinum colloids (PVP-Ru/Pt) and ruthenium-palladium colloids (PVP-Ru/Pd) was dependent on their compositions and could be remarkably affected by some added metal cations. In the presence of cobalt ion, nearly 100% selectivity to o-chloroaniline (o-CAN) was achieved over PVP-Ru/Pt colloids at 100% conversion of o-CNB, with an activity two orders of magnitude higher than that of monometallic PVP-Ru colloid. Copyright 1999 Academic Press. PMID:10339363

  12. EPR spectroscopy of catalytic systems based on nickel complexes of 1,4-diaza-1,3-butadiene (alpha-diimine) ligands in hydrogenation and polymerization reactions

    International Nuclear Information System (INIS)

    The catalytic systems based on .-diimine complexes of Ni(0) and Ni(II) of the general formulas NiBr2(DAD-R) (R = -C3H7 or -CH3) and Ni(DAD-CH3)2 (DAD(-C3H7) = 1,4-bis(2,6-diiso-propylphenyl)-2,3-(dimethyl-1,4-diazabuta-1,3-diene, DAD(-CH3) = 1,4-bis 2,6-dimethylphenyl)-2,3-dimethyl-1,4-diazabuta-1,3-diene), with Lewis acids (AlEt3, AlEt2Cl, AlEtCl2, B(F5C6)3, BF3 centre dot OEt2) in hydrogenation and polymerization reactions were investigated by the EPR spectroscopy method. The Ni(I) complexes of a (DAD-R)NiX2AlXy(C2H5)3-y composition (instead of the aluminum atom may be a boron atom) were identified where R = -CH3 or -C3H7, X = Br, X = Cl or -C2H5. The .-diimines radical-anions are included in the derivatives of aluminum or boron. It is found that there occur oxidation reactions between Ni(DAD-CH3)2 and aluminum organic compounds or boron derivatives, resulting in the formation of paramagnetic complexes. It is shown that there is no direct relationship between activity in polymerization or hydrogenation reactions and concentration of paramagnetic particles.

  13. Study on hydrogen production by catalytic reforming of bio-oil-methanol mixture%生物油-甲醇催化转化制氢

    Institute of Scientific and Technical Information of China (English)

    韩红睿; 张瑞芹; 徐兴敏; 张长森; 刘永刚

    2011-01-01

    Using bio-oil-tnethanol as the raw material, the nickel-based reforming catalyst for hydrogen production prepared in the laboratory was investigated in the fixed micro-reactor. The catalysts before and after reaction were characterized by XRD,BET and SEM. The condensates collected after gasification were analyzed by GC-MS. The results showed that NiCeMg/olivine catalyst exhibited good catalytic activity and good properties of resistance to carbon deposition. The hydrogen yield of 38. 52% and carbon conversion of 68. 29% were attained under the the optimum reaction condition.%以生物油-甲醇为原料,在微型固定反应装置上考察实验室合成镍基催化剂重整制氢的催化效率.对反应前后的催化剂进行XRD、BET和SEM表征分析,并对冷凝液做GC - MS分析.研究发现,实验室自制的NiCeMg/olivine催化剂具有较好的催化活性和一定的抗积炭性能.在选择的最佳反应条件下,氢气产率和碳转化率分别为38.52%和68.29%.

  14. Multi-Generation Concentrating Solar-Hydrogen Power System for Sustainable Rural Development

    Energy Technology Data Exchange (ETDEWEB)

    Krothapalli, A.; Greska, B.

    2007-07-01

    This paper describes an energy system that is designed to meet the demands of rural populations that currently have no access to grid-connected electricity. Besides electricity, it is well recognized that rural populations need at least a centralized refrigeration system for storage of medicines and other emergency supplies, as well as safe drinking water. Here we propose a district system that will employ a multi-generation concentrated solar power (CSP) system that will generate electricity and supply the heat needed for both absorption refrigeration and membrane distillation (MD) water purification. The electricity will be used to generate hydrogen through highly efficient water electrolysis and individual households can use the hydrogen for generating electricity, via affordable proton exchange membrane (PEM) fuel cells, and as a fuel for cooking. The multi-generation system is being developed such that its components will be easy to manufacture and maintain. As a result, these components will be less efficient than their typical counterparts but their low cost-to-efficiency ratio will allow for us to meet our installation cost goal of $1/Watt for the entire system. The objective of this paper is to introduce the system concept and discuss the system components that are currently under development. (auth)

  15. The effect of plutonium dioxide water surface coverage on the generation of hydrogen and oxygen

    Energy Technology Data Exchange (ETDEWEB)

    Veirs, Douglas K. [Los Alamos National Laboratory; Berg, John M. [Los Alamos National Laboratory; Crowder, Mark L. [Savannah River National Laboratory

    2012-06-20

    The conditions for the production of oxygen during radiolysis of water adsorbed onto plutonium dioxide powder are discussed. Studies in the literature investigating the radiolysis of water show that both oxygen and hydrogen can be generated from water adsorbed on high-purity plutonium dioxide powder. These studies indicate that there is a threshold in the amount of water below which oxygen is not generated. The threshold is associated with the number of monolayers of adsorbed water and is shown to occur at approximately two monolayers of molecularly adsorbed water. Material in equilibrium with 50% relative humidity (RH) will be at the threshold for oxygen generation. Using two monolayers of molecularly adsorbed water as the threshold for oxygen production, the total pressure under various conditions is calculated assuming stoichiometric production of hydrogen and oxygen. The specific surface area of the oxide has a strong effect on the final partial pressure. The specific surface areas resulting in the highest pressures within a 3013 container are evaluated. The potential for oxygen generation is mitigated by reduced relative humidity, and hence moisture adsorption, at the oxide surface which occurs if the oxide is warmer than the ambient air. The potential for oxygen generation approaches zero as the temperature difference between the ambient air and the material approaches 6 C.

  16. Broadband, stable and highly coherent supercontinuum generation at telecommunication wavelengths in an hydrogenated amorphous silicon waveguide

    CERN Document Server

    Leo, F; Kuyken, B; Roelkens, G; Gorza, S -P

    2014-01-01

    Hydrogenated amorphous silicon (a:Si-H) has recently been recognized as a highly nonlinear CMOS compatible photonic platform. We experimentally demonstrate the generation of a supercontinuum (SC) spanning over 500 nm in a-Si:H photonic wire waveguide at telecommunication wavelengths using femtosecond input pulse with energy lower than 5 pJ. Numerical modeling of pulse propagation in the waveguide, based on the experimentally characterized dispersion profile, shows that the supercontinuum is the result of soliton fission and dispersive wave generation. It is demonstrated that the SC is highly coherent and that the waveguides do not suffer from material degradation under femtosecond pulse illumination. Finally, a direct comparison of SC generation in c-Si and a-Si:H waveguides confirms the higher performances of a-Si:H over c-Si for broadband low power SC generation at telecommunication wavelengths.

  17. 四氯化碳液相催化加氢反应动力学的研究%KINETIC STUDIES ON THE CATALYTIC HYDROGENATION OF CARBON TETRACHLORIDE TO CHLOROFORM IN LIQUID PHASE

    Institute of Scientific and Technical Information of China (English)

    毛建新; 蒋晓原; 陆维敏; 郑小明

    2001-01-01

    Carbon tetrachloride is an ozone-depleting chemical, while chloroform is not. Therefore it is important for the catalytic hydrodechlorination of CCl4 to CHCl3. In this paper, kinetics on the catalytic hydrogenation of carbon tetrachloride to chloroform in liquid phase was studied. A reaction mechanism was proposed. Hydrogen molecular was activated on the surface of catalyst, the activated hydrogen atom then reacted with CCl4 in the solution and produced CHCl3. A definite kinetic equation could be deduced from the reaction mechanism. The reaction rate constant is concerned with the intial concentration of CCl4 in the solution, pressure, reaction temperature and the concentration of active center. All these factors were investigated over Pt-Pd/C catalyst and fit in with the kinetic equation. The activation energy of the reaction is 86?KJ/mol according to the experimental results.

  18. Hydrogen Generation Through Renewable Energy Sources at the NASA Glenn Research Center

    Science.gov (United States)

    Colozza, Anthony; Prokopius, Kevin

    2007-01-01

    An evaluation of the potential for generating high pressure, high purity hydrogen at the NASA Glenn Research Center (GRC) was performed. This evaluation was based on producing hydrogen utilizing a prototype Hamilton Standard electrolyzer that is capable of producing hydrogen at 3000 psi. The present state of the electrolyzer system was determined to identify the refurbishment requirements. The power for operating the electrolyzer would be produced through renewable power sources. Both wind and solar were considered in the analysis. The solar power production capability was based on the existing solar array field located at NASA GRC. The refurbishment and upgrade potential of the array field was determined and the array output was analyzed with various levels of upgrades throughout the year. The total available monthly and yearly energy from the array was determined. A wind turbine was also sized for operation. This sizing evaluated the wind potential at the site and produced an operational design point for the wind turbine. Commercially available wind turbines were evaluated to determine their applicability to this site. The system installation and power integration were also addressed. This included items such as housing the electrolyzer, power management, water supply, gas storage, cooling and hydrogen dispensing.

  19. Simultaneous Hydrogen Generation and Waste Acid Neutralization in a Reverse Electrodialysis System

    KAUST Repository

    Hatzell, Marta C.

    2014-09-02

    Waste acid streams produced at industrial sites are often co-located with large sources of waste heat (e.g., industrial exhaust gases, cooling water, and heated equipment). Reverse electrodialysis (RED) systems can be used to generate electrical power and hydrogen gas using waste heat-derived solutions, but high electrode overpotentials limit system performance. We show here that an ammonium bicarbonate (AmB) RED system can achieve simultaneous waste acid neutralization and in situ hydrogen production, while capturing energy from excess waste heat. The rate of acid neutralization was dependent on stack flow rate and increased 50× (from 0.06 ± 0.04 to 3.0 ± 0.32 pH units min -1 m-2 membrane), as the flow rate increased 6× (from 100 to 600 mL min-1). Acid neutralization primarily took place due to ammonium electromigration (37 ± 4%) and proton diffusion (60 ± 5%). The use of a synthetic waste acid stream as a catholyte (pH ≈ 2) also increased hydrogen production rates by 65% (from 5.3 ± 0.5 to 8.7 ± 0.1 m3 H2 m-3 catholyte day -1) compared to an AmB electrolyte (pH ≈ 8.5). These findings highlight the potential use of dissimilar electrolytes (e.g., basic anolyte and acidic catholyte) for enhanced power and hydrogen production in RED stacks. © 2014 American Chemical Society.

  20. Molybdenum(VI) network polymers based on anion-π interaction and hydrogen bonding: Synthesis, crystal structures and oxidation catalytic application

    Science.gov (United States)

    Li, Jia; Wang, Ge; Shi, Zhan; Yang, Mu; Luck, Rudy L.

    2009-11-01

    A crystallographic investigation of anion-π interactions and hydrogen bonds on the preferred structural motifs of molybdenum(VI) complexes has been carried out. Two molybdenum(VI) network polymers MoO 2F 4·(Hinca) 2 ( 1) and MoO 2F 3(H 2O)·(Hinpa) ( 2), where inca = isonicotinamide and inpa = isonipecotamide, have been synthesized, crystallographically characterized and successfully applied to alcohol oxidation reaction. Complex 1 crystallizes in the monoclinic space C2/ c: a = 16.832(3) Å, b = 8.8189(15) Å, c = 12.568(2) Å, β = 118.929(3)°, V = 1560.1(5) Å 3, Z = 4. Complex 2 crystallizes in the triclinic space P-1: a = 5.459(2) Å, b = 9.189(4) Å, c = 12.204(5) Å, α = 71.341(6)°, β = 81.712(7)°, γ = 77.705(7)°, V = 564.8(4) Å 3, Z = 2. Complex 1 consists of hydrogen bonding and anion-π interactions, both of which are considered as important factors for controlling the geometric features and packing characteristics of the crystal structure. The geometry of the sandwich complex of [MoO 2F 4] 2- with two pyridine rings indicates that the anion-π interaction is an additive and provides a base for the design and synthesis of new complexes. For complex 2, the anions and the protonated inpa ligands form a 2D supramolecular network by four different types of hydrogen contacts (N-H⋯F, N-H⋯O, O-H⋯F and O-H⋯O). The catalytic ability of complexes 1 and 2 has also been evaluated by applying them to the oxidation of benzyl alcohol with TBHP as oxidant.

  1. Hydrogenation of unactivated enamines to tertiary amines: rhodium complexes of fluorinated phosphines give marked improvements in catalytic activity

    Directory of Open Access Journals (Sweden)

    Sergey Tin

    2015-05-01

    Full Text Available In the hydrogenation of sluggish unactivated enamine substrates, Rh complexes of electron-deficient phosphines are demonstrated to be far more reactive catalysts than those derived from triphenylphosphine. These operate at low catalyst loadings (down to 0.01 mol % and are able to reduce tetrasubstituted enamines. The use of the sustainable and environmentally benign solvent (R-limonene for the reaction is also reported with the amine isolated by acid extraction.

  2. Preparation of Dendritic Carbosilane-supported Palladium Catalyst and Its Catalytic Activity in Hydrogenation of Organic Compounds

    Institute of Scientific and Technical Information of China (English)

    2005-01-01

    The preparation of palladium complex from PdCl2·2H2O and earbosilane dendrimers with peripheral aminopropyl groups was described. The compound obtained was characterized by IR, 1H NMR, X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma atomic emission spectrometric (ICP-AES) spectroscopy respectively. The metal complex was employed as catalyst in hydrogenation of organic compounds. The high activity of the complex was probably due to the formation of the eoordinatively unsaturated palladium.

  3. Ultrathin Co(Ni)-doped MoS2 nanosheets as catalytic promoters enabling efficient solar hydrogen production

    Institute of Scientific and Technical Information of China (English)

    Xiaoyan Ma; Jinquan Li; Changhua An; Juan Feng; Yuhua Chi; Junxue Liu; Jun Zhang

    2016-01-01

    The design of efficient artificial photosynthetic systems that harvest solar energy to drive the hydrogen evolution reaction via water reduction is of great importance from both the theoretical and practical viewpoints.Integrating appropriate co-catalyst promoters with strong light absorbing materials represents an ideal strategy to enhance the conversion efficiency of solar energy in hydrogen production.Herein,we report,for the first time,the synthesis of a class of unique hybrid structures consisting of ultrathin Co(Ni)-doped MoS2 nanosheets (co-catalyst promoter) intimately grown on semiconductor CdS nanorods (light absorber).The as-synthesized one-dimensional CdS@doped-MoS2 heterostructures exhibited very high photocatalytic activity (with a quantum yield of 17.3%) and stability towards H2 evolution from the photoreduction of water.Theoretical calculations revealed that Ni doping can increase the number of uncoordinated atoms at the edge sites of MoS2 nanosheets to promote electron transfer across the CdS/MoS2 interfaces as well as hydrogen reduction,leading to an efficient H2 evolution reaction.

  4. Study of hydrogen generation plant coupled to high temperature gas cooled reactor

    Science.gov (United States)

    Brown, Nicholas Robert

    Hydrogen generation using a high temperature nuclear reactor as a thermal driving vector is a promising future option for energy carrier production. In this scheme, the heat from the nuclear reactor drives an endothermic water-splitting plant, via coupling, through an intermediate heat exchanger. While both high temperature nuclear reactors and hydrogen generation plants have high individual degrees of development, study of the coupled plant is lacking. Particularly absent are considerations of the transient behavior of the coupled plant, as well as studies of the safety of the overall plant. The aim of this document is to contribute knowledge to the effort of nuclear hydrogen generation. In particular, this study regards identification of safety issues in the coupled plant and the transient modeling of some leading candidates for implementation in the Nuclear Hydrogen Initiative (NHI). The Sulfur Iodine (SI) and Hybrid Sulfur (HyS) cycles are considered as candidate hydrogen generation schemes. Several thermodynamically derived chemical reaction chamber models are coupled to a well-known reference design of a high temperature nuclear reactor. These chemical reaction chamber models have several dimensions of validation, including detailed steady state flowsheets, integrated loop test data, and bench scale chemical kinetics. Eight unique case studies are performed based on a thorough literature review of possible events. The case studies are: (1) feed flow failure from one section of the chemical plant to another, (2) product flow failure (recycle) within the chemical plant, (3) rupture or explosion within the chemical plant, (4) nuclear reactor helium inlet overcooling due to a process holding tank failure, (5) helium inlet overcooling as an anticipated transient without SCRAM, (6) total failure of the chemical plant, (7) parametric study of the temperature in an individual reaction chamber, and (8) control rod insertion in the nuclear reactor. Various parametric

  5. Co-generation of acetylene and hydrogen for a carbide-based fuel system

    Energy Technology Data Exchange (ETDEWEB)

    Carreiro, Louis G.; Burke, A. Alan [Naval Undersea Warfare Center Division Newport, Code 8231, 1176 Howell Street, Newport, RI 02841 (United States); Dubois, Lily [Stonehill College, Department of Chemistry, 320 Washington Street, Easton, MA 02357 (United States)

    2010-09-15

    The co-generation of acetylene and hydrogen from the hydrolysis of calcium carbide and calcium hydride was investigated as part of a unique carbide-based fuel system intended for high-temperature fuel cells. To gain better control of this highly energetic reaction, glycerin was used to coat the reactant particles to form slurry prior to their reaction with water. This process was shown to moderate the rate of gas production, as well as to provide a means for preparing slurry that could be pumped into the reactor vessel. It was also observed that the presence of calcium hydroxide, a by-product of hydrolysis, lowered the solubility of acetylene resulting in a higher initial flow rate due to less acetylene being dissolved in solution. However, the buildup of calcium hydroxide with time inhibited the hydrolysis of both calcium carbide and calcium hydride causing the acetylene and hydrogen flow rates to decrease. (author)

  6. Carbon quantum dots coated BiVO{sub 4} inverse opals for enhanced photoelectrochemical hydrogen generation

    Energy Technology Data Exchange (ETDEWEB)

    Nan, Feng; Shen, Mingrong; Fang, Liang, E-mail: zhkang@suda.edu.cn, E-mail: lfang@suda.edu.cn [College of Physics, Optoelectronics and Energy and Jiangsu Key Laboratory of Thin Films, Soochow University, Suzhou 215006 (China); Kang, Zhenhui, E-mail: zhkang@suda.edu.cn, E-mail: lfang@suda.edu.cn [Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-based Functional Materials and Devices, and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China); Wang, Junling [School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798 (Singapore)

    2015-04-13

    Carbon quantum dots (CQDs) coated BiVO{sub 4} inverse opal (io-BiVO{sub 4}) structure that shows dramatic improvement of photoelectrochemical hydrogen generation has been fabricated using electrodeposition with a template. The io-BiVO{sub 4} maximizes photon trapping through slow light effect, while maintaining adequate surface area for effective redox reactions. CQDs are then incorporated to the io-BiVO{sub 4} to further improve the photoconversion efficiency. Due to the strong visible light absorption property of CQDs and enhanced separation of the photoexcited electrons, the CQDs coated io-BiVO{sub 4} exhibit a maximum photo-to-hydrogen conversion efficiency of 0.35%, which is 6 times higher than that of the pure BiVO{sub 4} thin films. This work is a good example of designing composite photoelectrode by combining quantum dots and photonic crystal.

  7. Molecular molybdenum persulfide and related catalysts for generating hydrogen from water

    Science.gov (United States)

    Long, Jeffrey R.; Chang, Christopher J.; Karunadasa, Hemamala I.; Majda, Marcin

    2016-04-19

    New metal persulfido compositions of matter are described. In one embodiment the metal is molybdenum and the metal persulfido complex mimics the structure and function of the triangular active edge site fragments of MoS.sub.2, a material that is the current industry standard for petroleum hydro desulfurization, as well as a promising low-cost alternative to platinum for electrocatalytic hydrogen production. This molecular [(PY5W.sub.2)MoS.sub.2].sup.x+ containing catalyst is capable of generating hydrogen from acidic-buffered water or even seawater at very low overpotentials at a turnover frequency rate in excess of 500 moles H.sub.2 per mole catalyst per second, with a turnover number (over a 20 hour period) of at least 19,000,000 moles H.sub.2 per mole of catalyst.

  8. Performance of laboratory polymer electrolyte membrane hydrogen generator with sputtered iridium oxide anode

    Science.gov (United States)

    Labou, D.; Slavcheva, E.; Schnakenberg, U.; Neophytides, S.

    The continuous improvement of the anode materials constitutes a major challenge for the future commercial use of polymer electrolyte membranes (PEM) electrolyzers for hydrogen production. In accordance to this direction, iridium/titanium films deposited directly on carbon substrates via magnetron sputtering are operated as electrodes for the oxygen evolution reaction interfaced with Nafion 115 electrolyte in a laboratory single cell PEM hydrogen generator. The anode with 0.2 mg cm -2 Ir catalyst loading was electrochemically activated by cycling its potential value between 0 and 1.2 V (vs. RHE). The water electrolysis cell was operated at 90 °C with current density 1 A cm -2 at 1.51 V without the ohmic contribution. The corresponding current density per mgr of Ir catalyst is 5 A mg -1. The achieved high efficiency is combined with sufficient electrode stability since the oxidation of the carbon substrate during the anodic polarization is almost negligible.

  9. Experimental Study of Plasma Under-liquid Electrolysis in Hydrogen Generation

    Institute of Scientific and Technical Information of China (English)

    严宗诚; 陈砺; 王红林

    2006-01-01

    The application and characteristics of relatively big volume plasma produced with cathodic glow discharges taking place across a gaseous envelope over the cathode which was dipped into electrolyte in hydrogen generation were studied. A critical investigation of the influence of methanol concentration and voltage across the circuit on the composition and power consumption per cubic meter of cathode liberating gas was carried out. The course of plasma under-liquid electrolysis has the typical characteristics of glow discharge electrolysis. The cathode liberating gas was in substantial excess of the Faraday law value. When the voltage across the circuit was equal to 550 V, the volume of cathodic gas with sodium carbonate solution was equal to 16.97 times the Faraday law value. The study showed that methanol molecules are more active than water molecules.The methanol molecules were decomposed at the plasma-catholyte interface by the radicals coming out the plasma mantle.Energy consumption per cubic meter of cathodic gases (WV) decreased while methanol concentration of the electrolytes increased. When methanol concentration equaled 5% (ψ), WV was 10.381×103 kJ/m3, less than the corresponding theoretic value of conventional water electrolysis method. The cathodic liberating gas was a mixture of hydrogen, carbon dioxide and carbon monoxide with over 95% hydrogen, if methanol concentration was more than 15% (ψ). The present research work revealed an innovative application of glow discharge and a new highly efficient hydrogen generation method, which depleted less resource and energy than normal electrolysis and is environmentally friendly.

  10. Pd/Graphene catalytic hydrogenation of benzoquinone to hydroquinone%钯/石墨烯催化苯醌加氢制备氢醌

    Institute of Scientific and Technical Information of China (English)

    杨敬贺; 郁清涛; 毛立群

    2015-01-01

    采用微波辅助加热还原法合成了钯/石墨烯(Pd/G)、钯/活性炭(Pd/AC)、钯/石墨(Pd/Graphite)和钯/二氧化硅(Pd/SiO2),并使用透射电子显微镜观测了钯的形貌及在载体上的分散性。将负载型钯催化剂用于苯醌加氢反应,结果显示,Pd/G催化剂的活性最高,苯醌的转化率达到99%,氢醌的选择性为100%,并且循环7次后催化剂仍保持着较高的转化率和选择性。结构表征表明,石墨烯担载的钯纳米粒子的粒径约为5 nm ,无明显团聚。实验进一步考察了反应溶剂(甲醇、乙醇、丙酮、正丙醇、异丙醇、正丁醇)对 Pd/G催化苯醌加氢反应的影响,结果表明该反应对溶剂较为敏感,其中甲醇和丙酮较适宜作为反应溶剂。当以甲醇作为溶剂时,苯醌的转化率为98%,氢醌选择性为99%;以丙酮为溶剂时,苯醌转化率为98%,氢醌选择性为90%。研究工作表明,作为载体,石墨烯对钯催化剂的催化效果起着稳定和增强作用。%In the present study ,we exploited G as a support for palladium nanoparticles by mi‐crowave assisted reduction of palladium acetate with graphene under hydrogen atmosphere .In the same method ,we also employed graphite ,active carbon and silica as carrier for synthesis palladium graphite (Pd/Graphite) ,palladium active carbon (Pd/AC) and palladium silica (Pd/SiO2 ) .The hydrogenation of benzoquinone reaction has been selected as model reaction for e‐valuating G -based palladium catalysts (Pd/G) ,and the morphology and dispersion of palla‐dium on the carrier were observed by TEM .We utilized the supported palladium catalysts for benzoquinone hydrogenation reaction .The results imply that the Pd/G catalyst shows the high‐est activity .T he conversion of benzoquinone reached 99% and the selectivity to hydroquinone was 100% .In addtion ,the catalytic performance of Pd/G catalyst remained

  11. Mitigation of Hydrogen Gas Generation from the Reaction of Water with Uranium Metal in K Basins Sludge

    Energy Technology Data Exchange (ETDEWEB)

    Sinkov, Sergey I.; Delegard, Calvin H.; Schmidt, Andrew J.

    2010-01-29

    Means to decrease the rate of hydrogen gas generation from the chemical reaction of uranium metal with water were identified by surveying the technical literature. The underlying chemistry and potential side reactions were explored by conducting 61 principal experiments. Several methods achieved significant hydrogen gas generation rate mitigation. Gas-generating side reactions from interactions of organics or sludge constituents with mitigating agents were observed. Further testing is recommended to develop deeper knowledge of the underlying chemistry and to advance the technology aturation level. Uranium metal reacts with water in K Basin sludge to form uranium hydride (UH3), uranium dioxide or uraninite (UO2), and diatomic hydrogen (H2). Mechanistic studies show that hydrogen radicals (H·) and UH3 serve as intermediates in the reaction of uranium metal with water to produce H2 and UO2. Because H2 is flammable, its release into the gas phase above K Basin sludge during sludge storage, processing, immobilization, shipment, and disposal is a concern to the safety of those operations. Findings from the technical literature and from experimental investigations with simple chemical systems (including uranium metal in water), in the presence of individual sludge simulant components, with complete sludge simulants, and with actual K Basin sludge are presented in this report. Based on the literature review and intermediate lab test results, sodium nitrate, sodium nitrite, Nochar Acid Bond N960, disodium hydrogen phosphate, and hexavalent uranium [U(VI)] were tested for their effects in decreasing the rate of hydrogen generation from the reaction of uranium metal with water. Nitrate and nitrite each were effective, decreasing hydrogen generation rates in actual sludge by factors of about 100 to 1000 when used at 0.5 molar (M) concentrations. Higher attenuation factors were achieved in tests with aqueous solutions alone. Nochar N960, a water sorbent, decreased hydrogen

  12. [Russian oxygen generation system "Elektron-VM": hydrogen content in electrolytically produced oxygen for breathing by International Space Station crews].

    Science.gov (United States)

    Proshkin, V Yu; Kurmazenko, E A

    2014-01-01

    The article presents the particulars of hydrogen content in electrolysis oxygen produced aboard the ISS Russian segment by oxygen generator "Elektron-VM" (SGK) for crew breathing. Hydrogen content was estimated as in the course of SGK operation in the ISS RS, so during the ground life tests. According to the investigation of hydrogen sources, the primary path of H2 appearance in oxygen is its diffusion through the porous diaphragm separating the electrolytic-cell cathode and anode chambers. Effectiveness of hydrogen oxidation in the SGK reheating unit was evaluated.

  13. Green diesel production via catalytic hydrogenation/decarboxylation of triglycerides and fatty acids of vegetable oil and brown grease

    Science.gov (United States)

    Sari, Elvan

    Increase in the petroleum prices, projected increases in the world's energy demand and environmental awareness have shifted the research interest to the alternative fuel technologies. In particular, green diesel, vegetable oil/animal fat/waste oil and grease derived hydrocarbons in diesel boiling range, has become an attractive alternative to biodiesel---a mixture of fatty acid methyl esters, particularly due to its superior fuel properties that are similar to petroleum diesel. Hence, green diesel can be used as a drop-in fuel in the current diesel engines. The current technology for production of green diesel-hydrodeoxygenation of triglycerides and fatty acids over conventional hydrotreating catalysts suffers from fast catalyst deactivation in the absence of hydrogen combined with high temperatures and high fatty acid content in the feedstock. Additionally, excess hydrogen requirement for hydrodeoxygenation technique leads to high production costs. This thesis proposes a new technology-selective decarboxylation of brown grease, which is a mixture of fats and oils collected from waste water trap and rich in fatty acids, over a supported noble metal catalyst that overcomes the green diesel production challenges. In contrast to other feedstocks used for liquid biofuel production, brown grease is inexpensive and non-food competing feedstock, therefore the process finds solution to waste management issues, reduces the renewable fuel production cost and does not add to the global food shortage problems. Special catalyst formulations were developed to have a high activity and stability in the absence of hydrogen in the fatty acid decarboxylation process. The study shows how catalyst innovations can lead to a new technology that overcomes the process challenges. First, the effect of reaction parameters on the activity and the selectivity of brown grease decarboxylation with minimum hydrogen consumption over an activated carbon supported palladium catalyst were

  14. Classical Dynamics of Harmonic Generation of the Hydrogen Molecular Ion Interacting with Ultrashort Intense Laser Pulses

    Institute of Scientific and Technical Information of China (English)

    LI Chao-Hong; DUAN Yi-Wu; Wing-Ki Liu; Jian-Min Yuan

    2001-01-01

    Within Born-Oppenheimer approximation, by using the classical trajectory theory, a description for the high order harmonic generation of the hydrogen molecular ion interacting with ultrashort laser pulses has been pre sented. The Coulomb singularities have been remedied by the regularization. The action-angle variables have been used to generate the initial inversion symmetry microcanonical distribution. Within a proper intensity range, a harmonic plateau with only odd harmonics appears. For a larger intensity, because of the existence of chaos, the harmonic spectra become noisier. For a large enough intensity, the ionization takes place and the harmonics disappear. So the chaos causes the noises, the ionization suppresses the harmonic generation, and the onset of the ionization follows the onset of chaos.

  15. Improvement of the efficiency of a space oxygen-hydrogen electrochemical generator

    Science.gov (United States)

    Glukhikh, I. N.; Shcherbakov, A. N.; Chelyaev, V. F.

    2014-12-01

    This paper describes the method used for cooling of an on-board oxygen-hydrogen electrochemical generator (ECG). Apart from electric power, such a unit produces water of reaction and heat; the latter is an additional load on the thermal control system of a space vehicle. This load is undesirable in long-duration space flights, when specific energy characteristics of on-board systems are the determining factors. It is suggested to partially compensate the energy consumption by the thermal control system of a space vehicle required for cooling of the electrochemical generator through evaporation of water of reaction from the generator into a vacuum (or through ice sublimation if the pressure in the ambient space is lower than that in the triple point of water.) Such method of cooling of an electrochemical generator improves specific energy parameters of an on-board electric power supply system, and, due to the presence of the negative feedback, it makes the operation of this system more stable. Estimates suggest that it is possible to compensate approximately one half of heat released from the generator through evaporation of its water of reaction at the electrical efficiency of the electrochemical generator equal to 60%. In this case, even minor increase in the efficiency of the generator would result in a considerable increase in the efficiency of the evaporative system intended for its cooling.

  16. 四氯化硅催化氢化合成三氯氢硅机理研究%First Principles Study on the Reaction Mechanism of Catalytic Hydrogenation Process of Silicon Tetrachloride

    Institute of Scientific and Technical Information of China (English)

    岳晓宁; 龙雨谦; 黄韬; 蒋炜; 陈建钧; 梁斌

    2013-01-01

    针对四氯化硅催化氢化过程采用第一性原理机理对其进行模拟研究,结果表明:没有催化剂时,SiCl4与H2反应能垒为464.45 kJ/mol,反应能量为74.94 kJ/mol,与热力学计算结果71.85 kJ/mol一致.负载在HZSM-5分子筛上的氯化钡可催化四氯化硅氢化反应,其最具催化活性表面为(111)面;H2在BaCl2(111)面上表现排斥性;SiCl4表现为吸附性,可在BaCl2(111)表面稳定吸附并生成·SiCl3自由基,过程吸附能为448.33 kJ/mol;在催化剂BaCl2存在条件下,SiCl4与H2反应为自由基反应,反应步骤能垒为400.23 kJ/mol;氢化过程能垒降为184.97kJ/mol;催化氢化反应过程所需能量为64.20 kJ/mol.催化氢化过程反应条件相对无催化剂过程更为温和.%The treatment of silicon tetrachloride is the key problem for the development of polysilicon industries.Catalytic hydrogenation process is a promising alternative technology for current industrial process.However,the reaction mechanism of this process is not clear yet.In this research,hydrogenation process of silicon tetrachloride with and without catalyst was studied to determine the reaction mechanism with the first principle calculation.The calculation demonstrates that the thermo-hydrogenation without catalyst is a molecular reaction.The reaction energy of thermo-hydrogenation reaction of SiCl4 is 74.94 kJ/mol and the energy barrier is 464.45 kJ/mol,which is agreement with the results of thermo dynamic calculation.Employing barium chlorideloaded on the HZSM-5 zeolite,as catalyst,the hydrogenation process transfers into radical reactions.The best active crystal plane of BaCl2 is surface (111).Hydrogen molecular is repulsed by surface (111),meanwhile SiCl4 molecular can be adsorbed steadily to generate silicon trichloridefree radical · SiCl3,and adsorbed chloride.Then,the free radical · SiCl3 reacts with H2 to produce trichlorosilane and free hydrogen atom.The latter combines with the adsorbed chloride atom to yield

  17. Development and performance of bench-scale reactor for the photocatalytic generation of hydrogen

    International Nuclear Information System (INIS)

    In this study, a new novel bench-scale (5 L) tubular photocatalytic reactor was developed and its feasibility studies were conducted for optimizing the operating variables, namely concentration of sulfide ion, concentration of sulfite ion, pH, catalyst concentration, lamp power, volume of wastewater and recycle flow rates at batch recycle mode for the generation of hydrogen from aqueous sodium sulfide using CdS–ZnS/TiO2 core–shell NPs (nanoparticles). The maximum H2 generation was found at 0.05 M concentration of sulfide ion, 0.2 M concentration of sulfite ion, pH 11.3, 0.5 g/L catalyst concentration and recycle flow rate of 18 L/h. Reusability studies were conducted for analyzing stability of photocatalyst. The results showed that the generation of hydrogen depends on light intensity, photoreactor used, nature of photocatalysts and the operating conditions. - Highlights: • Clean fuel production using solar energy. • Bench-scale tubular photocatalytic reactor was developed. • Operating variables have significant effect

  18. Hydrogen

    OpenAIRE

    John O’M. Bockris

    2011-01-01

    The idea of a “Hydrogen Economy” is that carbon containing fuels should be replaced by hydrogen, thus eliminating air pollution and growth of CO2 in the atmosphere. However, storage of a gas, its transport and reconversion to electricity doubles the cost of H2 from the electrolyzer. Methanol made with CO2 from the atmosphere is a zero carbon fuel created from inexhaustible components from the atmosphere. Extensive work on the splitting of water by bacteria shows that if wastes are used as the...

  19. Valorization of Waste Lipids through Hydrothermal Catalytic Conversion to Liquid Hydrocarbon Fuels with in Situ Hydrogen Production

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Dongwook; Vardon, Derek R.; Murali, Dheeptha; Sharma, Brajendra K.; Strathmann, Timothy J.

    2016-03-07

    We demonstrate hydrothermal (300 degrees C, 10 MPa) catalytic conversion of real waste lipids (e.g., waste vegetable oil, sewer trap grease) to liquid hydrocarbon fuels without net need for external chemical inputs (e.g., H2 gas, methanol). A supported bimetallic catalyst (Pt-Re/C; 5 wt % of each metal) previously shown to catalyze both aqueous phase reforming of glycerol (a triacylglyceride lipid hydrolysis coproduct) to H2 gas and conversion of oleic and stearic acid, model unsaturated and saturated fatty acids, to linear alkanes was applied to process real waste lipid feedstocks in water. For reactions conducted with an initially inert headspace gas (N2), waste vegetable oil (WVO) was fully converted into linear hydrocarbons (C15-C17) and other hydrolyzed byproducts within 4.5 h, and H2 gas production was observed. Addition of H2 to the initial reactor headspace accelerated conversion, but net H2 production was still observed, in agreement with results obtained for aqueous mixtures containing model fatty acids and glycerol. Conversion to liquid hydrocarbons with net H2 production was also observed for a range of other waste lipid feedstocks (animal fat residuals, sewer trap grease, dry distiller's grain oil, coffee oil residual). These findings demonstrate potential for valorization of waste lipids through conversion to hydrocarbons that are more compatible with current petroleum-based liquid fuels than the biodiesel and biogas products of conventional waste lipid processing technologies.

  20. Comparison of hydrogen production and electrical power generation for energy capture in closed-loop ammonium bicarbonate reverse electrodialysis systems

    KAUST Repository

    Hatzell, Marta C.

    2014-01-01

    Currently, there is an enormous amount of energy available from salinity gradients, which could be used for clean hydrogen production. Through the use of a favorable oxygen reduction reaction (ORR) cathode, the projected electrical energy generated by a single pass ammonium bicarbonate reverse electrodialysis (RED) system approached 78 W h m-3. However, if RED is operated with the less favorable (higher overpotential) hydrogen evolution electrode and hydrogen gas is harvested, the energy recovered increases by as much ∼1.5× to 118 W h m-3. Indirect hydrogen production through coupling an RED stack with an external electrolysis system was only projected to achieve 35 W h m-3 or ∼1/3 of that produced through direct hydrogen generation.

  1. Engineered materials as potential geocatalysts in deep geological nuclear waste repositories: A case study of the stainless steel catalytic effect on nitrate reduction by hydrogen

    International Nuclear Information System (INIS)

    Highlights: • We demonstrate that stainless steels (316L and Hastelloy) can catalyse nitrate reduction in the presence of hydrogen. • Hydrogen is the sole electron donor. • The reaction proceeds via nitrate sorption at the steel surface up to pH = 9 following Langmuir–Hinshelwood mechanism. • The reaction is inhibited by the presence of phosphate anions which compete with nitrate for the steel sorption sites. - Abstract: The reduction of NO3- in natural waters is commonly promoted by biological activity. In the context of deep geological nuclear waste repositories with potentially high H2 pressure, abiotic redox reactions may be envisaged. Here, the catalytic effect of “inert” metallic surfaces, in part used for nuclear waste canisters, on NO3- reduction under H2 pressure is evaluated. The study is focused on stainless steels by testing the 316L and Hastelloy C276 steels. A parametric kinetic study (0 < P(H2) < 10 bar, 0.1 < [NO3-] < 10 mM, 90 < T° < 150 °C, 4 < pHin situ < 9) reveals that NO3- reduction, in the presence of stainless steel 316L and Hastelloy C276, proceeds via a pH-independent reaction requiring H2 as an electron donor. No corrosion of these steels is observed indicating a true catalytic process. The reaction is inhibited in the presence of PO43-. Activation energies assuming a first-order reaction in the 90–150 °C temperature range are found to be 46 kJ/mol for stainless steel 316L and 186 kJ/mol for Hastelloy C276, making the reaction efficient at lower temperature and on a human time scale. Nitrate sorption at the metallic surface being thought to be the limiting step, sorption and competitive sorption isotherms of several oxyanions were performed at 90 °C on 316L. Nitrate and PO43- are more strongly sorbed than SO42-, likely as inner sphere complexes, and in a large pH range, from acidic to pH 9. The Langmuir–Hinshelwood formalism best fits the kinetic data. The nature of the surface complex, and the competition for

  2. Hydrogen generation arising from the {sup 59}Ni(n,p) reaction and its impact on fission-fusion correlations

    Energy Technology Data Exchange (ETDEWEB)

    Greenwood, L.R.; Garner, A.F.

    1996-04-01

    Whilte the influence of transmutant helium on radiation-induced microstructural evolution has often been studied, there is a tendency to overlook the influence of concurrently-generated hydrogen. There have been some recent speculation and studies, however, that suggest that the influence of hydrogen may be enhanced in the presence of large amounts of helium, especially at lower irradiation temperatures typical of projected ITER operation. The impact of the (n,p) reaction on both hydrogen generation rates and displacement rates are evaluated in this paper for a variety of neutron spectra employed in fission-fusion correlation.

  3. [Isolation of a high hydrogen-producing mutant TB34 generated by transposon insertion and analysis of hydrogen production].

    Science.gov (United States)

    Liu, Hong-Yan; Wang, Guang-Ce; Shi, Liu-Yang; Zhu, Da-Ling

    2012-07-01

    To increase the hydrogen-producing capacity of Pantoea agglomerans BH18, isolated from mangrove sludge, we constructed a stable transposon mutagenesis library of this strain. A Tn7-based transposon was randomly inserted into the genomic DNA. Mutants were screened by kanamycin resistance and identified by amplification of the inserted transposon sequences. A mutant strain TB34 was isolated, whose hydrogen production capacity was significantly improved compared to the wild type strain. In seawater-containing medium supplemented with 10 g x L(-1) glucose and had an initial pH of 7.0, the hydrogen yield (H2/glucose) of the mutant strain was (2.04 +/- 0.04) mol x mol(-1), which was 43% higher than that of the wild type strain. The mutant TB34 showed steady hydrogen production capacity for five consecutive passages. Different carbon sources were tested in the hydrogen production by the mutant TB34 and the results showed that both the mutant strain TB34 and the wild type strain BH18 were able to produce hydrogen on sucrose, glucose and fructose. However, different from the wild type strain, the mutant strain TB34 was also able to produce hydrogen using xylose as substrate, with a hydrogen yield (H2/xylose) of (1.34 +/- 0.09) mol x mol(-1), indicating a broader substrate spectrum in the mutant.

  4. Batch sodium borohydride hydrolysis systems: Effect of sudden valve opening on hydrogen generation rate

    OpenAIRE

    M. J. F. Ferreira; Coelho, F; Rangel, C. M.; Pinto, A. M. F. R.

    2012-01-01

    A study was undertaken in order to investigate the potential of hydrogen (H 2) generation by hydrolysis of sodium borohydride solution (10 wt% NaBH 4 and 7 wt% NaOH), in batch reactors, operating at moderate pressures (up to #8764;1.2 MPa), in the presence of a powdered nickel-ruthenium based catalyst, reused between 311 and 316 times, to feed on-demand a proton exchange membrane fuel cell. A different approach to the testing of the performance of the batch NaBH 4 hydrolysis system is explore...

  5. Investigation of cold cathodes of plasma sources generating of hydrogen ion beams

    CERN Document Server

    Veresov, L P; Dzkuya, M I; Zhukov, Y N; Kuznetsov, G V; Tsekvava, I A

    2001-01-01

    Designs of a hollow cellular cathode (HCC) and of an inverse cylindrical multichamber magnetronic cathode (ICMMC), used as cold cathodes in duoplasmatron for hydrogen ion beam generation, are described. Their service characteristics are compared. It is ascertained that emission ability of both HCC and ICMMC is approximately the same. However, duoplasmatron with ICMMC features a three times higher gas effectiveness compared with HCC. Service life of duoplasmatron with both types of cathodes amounts to several thousand hours. On the basis of test results the choice is made in favour of ICMMC

  6. Role of hydrogen generation by Klebsiella pneumoniae in the oral cavity.

    Science.gov (United States)

    Kanazuru, Tomoko; Sato, Eisuke F; Nagata, Kumiko; Matsui, Hiroshi; Watanabe, Kunihiko; Kasahara, Emiko; Jikumaru, Mika; Inoue, June; Inoue, Masayasu

    2010-12-01

    Some gastrointestinal bacteria synthesize hydrogen (H(2)) by fermentation. Despite the presence of bactericidal factors in human saliva, a large number of bacteria also live in the oral cavity. It has never been shown that oral bacteria also produce H(2) or what role H(2) might play in the oral cavity. It was found that a significant amount of H(2) is synthesized in the oral cavity of healthy human subjects, and that its generation is enhanced by the presence of glucose but inhibited by either teeth brushing or sterilization with povidone iodine. These observations suggest the presence of H(2)-generating bacteria in the oral cavity. The screening of commensal bacteria in the oral cavity revealed that a variety of anaerobic bacteria generate H(2). Among them, Klebsiella pneumoniae (K. pneumoniae) generated significantly large amounts of H(2) in the presence of glucose. Biochemical analysis revealed that various proteins in K. pneumoniae are carbonylated under standard culture conditions, and that oxidative stress induced by the presence of Fe(++) and H(2)O(2) increases the number of carbonylated proteins, particularly when their hydrogenase activity is inhibited by KCN. Inhibition of H(2) generation markedly suppresses the growth of K. pneumoniae. These observations suggest that H(2) generation and/or the reduction of oxidative stress is important for the survival and growth of K. pneumoniae in the oral cavity.

  7. Effective regimes of runaway electron beam generation in helium, hydrogen, and nitrogen

    Science.gov (United States)

    Tarasenko, V. F.; Baksht, E. Kh.; Burachenko, A. G.; Lomaev, M. I.; Sorokin, D. A.; Shut'ko, Yu. V.

    2010-04-01

    Runaway electron beam parameters and current-voltage characteristics of discharge in helium, hydrogen, and nitrogen at pressures in the range of several Torr to several hundred Torr have been studied. It is found that the maximum amplitudes of supershort avalanche electron beams (SAEBs) with a pulse full width at half maximum (FWHM) of ˜100 ps are achieved in helium, hydrogen, and nitrogen at a pressure of ˜60, ˜30, and ˜10 Torr, respectively. It is shown that, as the gas pressure is increased in the indicated range, the breakdown voltage of the gas-filled gap decreases, which leads to a decrease in the SAEB current amplitude. At pressures of helium within 20-60 Torr, hydrogen within 10-30 Torr, and nitrogen within 3-10 Torr, the regime of the runaway electron beam generation changes and, by varying the pressure in the gas-filled diode in the indicated intervals, it is possible to smoothly control the current pulse duration (FWHM) from ˜100 to ˜500 ps, while the beam current amplitude increases by a factor of 1.5-3.

  8. Ultrathin Coating of Confined Pt Nanocatalysts by Atomic Layer Deposition for Enhanced Catalytic Performance in Hydrogenation Reactions.

    Science.gov (United States)

    Wang, Meihua; Gao, Zhe; Zhang, Bin; Yang, Huimin; Qiao, Yan; Chen, Shuai; Ge, Huibin; Zhang, Jiankang; Qin, Yong

    2016-06-13

    Metal-support interfaces play a prominent role in heterogeneous catalysis. However, tailoring the metal-support interfaces to realize full utilization remains a major challenge. In this work, we propose a graceful strategy to maximize the metal-oxide interfaces by coating confined nanoparticles with an ultrathin oxide layer. This is achieved by sequential deposition of ultrathin Al2 O3 coats, Pt, and a thick Al2 O3 layer on carbon nanocoils templates by atomic layer deposition (ALD), followed by removal of the templates. Compared with the Pt catalysts confined in Al2 O3 nanotubes without the ultrathin coats, the ultrathin coated samples have larger Pt-Al2 O3 interfaces. The maximized interfaces significantly improve the activity and the protecting Al2 O3 nanotubes retain the stability for hydrogenation reactions of 4-nitrophenol. We believe that applying ALD ultrathin coats on confined catalysts is a promising way to achieve enhanced performance for other catalysts. PMID:27061428

  9. Simulation Studies of the Hydrogen Production from Methanol Partial Oxidation Steam Reforming by a Tubular Packed-bed Catalytic Reactor*

    Institute of Scientific and Technical Information of China (English)

    蒋元力; 林美淑; 金东显

    2001-01-01

    Hydrogen production by partial oxidation steam reforming of methanol over a Cu/ZnO/Al2O3 cata-lyst has been paid more and more attention. The chemical equilibria involved in the methanol pvxtial oxidation steam reforming reaction network such as methanol partial oxidation, methanol steam reforming, decomposition of methanol and water-gas shift reaction have been examined over the ranges of temperature 473---1073 K under normal pressure. Based on the detailed kinetics of these reactions over a Cu/ZnO/Al2O3 catalyst, and from the basic concept of the effectiveness factor, the intraparticle diffusion limitations were taken into account. The effectiveness factors for each reaction along the bed length were calculated. Then important results were offered for the simulation of this reaction process.

  10. Simulation Studies of the Hydrogen Production from Methanol Partial Oxidation Steam Reforming by a Tubular Packed-bed Catalytic Reactor

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    Hydrogen production by partial oxidation steam reforming of methanol over a Cu/ZnO/Al2 O3 cata lyst has been paid more and more attention. The chemical equilibria involved in the methanol partial oxidation steam reforming reaction network such as methanol partial oxidation, methanol steam reforming, decomposition of methanol and water-gas shift reaction have been examined over the ranges of temperature 473-1073 K under normal pressure. Based on the detailed kinetics of these reactions over a Cu/ZnO/Al2O3 catalyst, and from the basic concept of the effectiveness factor, the intraparticle diffusion limitations were taken into account. The effec tiveness factors for each reaction along the bed length were calculated. Then important results were offered for the simulation of this reaction process.

  11. Ultrasound promoted catalytic liquid-phase dehydrogenation of isopropanol for Isopropanol-Acetone-Hydrogen chemical heat pump.

    Science.gov (United States)

    Xu, Min; Xin, Fang; Li, Xunfeng; Huai, Xiulan; Liu, Hui

    2015-03-01

    The apparent kinetic of the ultrasound assisted liquid-phase dehydrogenation of isopropanol over Raney nickel catalyst was determined in the temperature range of 346-353 K. Comparison of the effects of ultrasound and mechanical agitation on the isopropanol dehydrogenation was investigated. The ultrasound assisted dehydrogenation rate was significantly improved when relatively high power density was used. Moreover, the Isopropanol-Acetone-Hydrogen chemical heat pump (IAH-CHP) with ultrasound irradiation, in which the endothermic reaction is exposure to ultrasound, was proposed. A mathematical model was established to evaluate its energy performance in term of the coefficient of performance (COP) and the exergy efficiency, into which the apparent kinetic obtained in this work was incorporated. The operating performances between IAH-CHP with ultrasound and mechanical agitation were compared. The results indicated that the superiority of the IAH-CHP system with ultrasound was present even if more than 50% of the power of the ultrasound equipment was lost.

  12. Ultrathin Coating of Confined Pt Nanocatalysts by Atomic Layer Deposition for Enhanced Catalytic Performance in Hydrogenation Reactions.

    Science.gov (United States)

    Wang, Meihua; Gao, Zhe; Zhang, Bin; Yang, Huimin; Qiao, Yan; Chen, Shuai; Ge, Huibin; Zhang, Jiankang; Qin, Yong

    2016-06-13

    Metal-support interfaces play a prominent role in heterogeneous catalysis. However, tailoring the metal-support interfaces to realize full utilization remains a major challenge. In this work, we propose a graceful strategy to maximize the metal-oxide interfaces by coating confined nanoparticles with an ultrathin oxide layer. This is achieved by sequential deposition of ultrathin Al2 O3 coats, Pt, and a thick Al2 O3 layer on carbon nanocoils templates by atomic layer deposition (ALD), followed by removal of the templates. Compared with the Pt catalysts confined in Al2 O3 nanotubes without the ultrathin coats, the ultrathin coated samples have larger Pt-Al2 O3 interfaces. The maximized interfaces significantly improve the activity and the protecting Al2 O3 nanotubes retain the stability for hydrogenation reactions of 4-nitrophenol. We believe that applying ALD ultrathin coats on confined catalysts is a promising way to achieve enhanced performance for other catalysts.

  13. Scanning electrochemical microscopy: surface interrogation of adsorbed hydrogen and the open circuit catalytic decomposition of formic acid at platinum.

    Science.gov (United States)

    Rodríguez-López, Joaquín; Bard, Allen J

    2010-04-14

    The surface interrogation mode of scanning electrochemical microscopy (SECM) is extended to the in situ quantification of adsorbed hydrogen, H(ads), at polycrystalline platinum. The methodology consists of the production, at an interrogator electrode, of an oxidized species that is able to react with H(ads) on the Pt surface and report the amounts of this adsorbate through the SECM feedback response. The technique is validated by comparison to the electrochemical underpotential deposition (UPD) of hydrogen on Pt. We include an evaluation of electrochemical mediators for their use as oxidizing reporters for adsorbed species at platinum; a notable finding is the ability of tetramethyl-p-phenylenediamine (TMPD) to oxidize (interrogate) H(ads) on Pt at low pH (0.5 M H(2)SO(4) or 1 M HClO(4)) and with minimal background effects. As a case study, the decomposition of formic acid (HCOOH) in acidic media at open circuit on Pt was investigated. Our results suggest that formic acid decomposes at the surface of unbiased Pt through a dehydrogenation route to yield H(ads) at the Pt surface. The amount of H(ads) depended on the open circuit potential (OCP) of the Pt electrode at the time of interrogation; at a fixed concentration of HCOOH, a more negative OCP yielded larger amounts of H(ads) until reaching a coulomb limiting coverage close to 1 UPD monolayer of H(ads). The introduction of oxygen into the cell shifted the OCP to more positive potentials and reduced the quantified H(ads); furthermore, the system was shown to be chemically reversible, as several interrogations could be run consecutively and reproducibly regardless of the path taken to reach a given OCP. PMID:20225806

  14. Hydrogen Effect on Coke Removal and Catalytic Performance in Pre-Carburization and Methane Dehydro-Aromatization Reaction on Mo/HZSM-5

    Institute of Scientific and Technical Information of China (English)

    Hongtao Ma; Ryoichi Kojima; Satoshi Kikuchi; Masaru Ichikawa

    2005-01-01

    In this study,the effects of pre-carburization of catalyst,hydrogen addition to methane feed and the space velocity of methane on the catalytic performance in methane to benzene (MTB) reaction were discussed in detail over Mo/HZSM-5 catalyst at 1023 K and 0.3 MPa. Compared with the non-precarburized catalyst,the Mo catalyst pre-carburized under the flow of CH4+4H2 at 973 K was found to have the higher activity and better stability. Further 6% H2 addition to the methane feed suppressed the aromatic type of coke formation effectively,and improved the stability of catalyst markedly,moreover gave a much longer reaction life of catalyst (53 h at 1023 K and 5400 ml/(g·h)) and much more formation amounts of benzene and hydrogen. With increase of methane space velocity,both the naphthalene formation selectivity and the coke formation selectivity were decreased by the shortened contact time;the benzene formation selectivity and total formation amount before the complete deactivation of catalyst were increased ly,while the total naphthalene and coke formation amounts did not change much.At high methane space velocity (≥5400 ml/(g·h)),a new middle temperature coke derived from the high temperature aromatic coke was formed on the catalyst; all the coke formed could be burnt off at lower temperature in oxygen,compared with those obtained at low space velocity. Considering the benzene formation amount and catalyst stability together,5400 ml/(g·h) was proved to be the most efficient methane space velocity for benzene production.

  15. Hydrogen Generation from Biomass-Derived Surgar Alcohols via the Aqueous-Phase Carbohydrate Reforming (ACR) Process

    Energy Technology Data Exchange (ETDEWEB)

    Randy Cortright

    2006-06-30

    This project involved the investigation and development of catalysts and reactor systems that will be cost-effective to generate hydrogen from potential sorbitol streams. The intention was to identify the required catalysts and reactors systems as well as the design, construction, and operation of a 300 grams per hour hydrogen system. Virent was able to accomplish this objective with a system that generates 2.2 kgs an hour of gas containing both hydrogen and alkanes that relied directly on the work performed under this grant. This system, funded in part by the local Madison utility, Madison, Gas & Electric (MGE), is described further in the report. The design and development of this system should provide the necessary scale-up information for the generation of hydrogen from corn-derived sorbitol.

  16. Study on the Performance and Commercial Application of New Generation DMMC-1 Type Catalyst for Deep Catalytic Cracking

    Institute of Scientific and Technical Information of China (English)

    Long Jun; Tian Huiping; Liu Yujian; Xie Chaogang; Li Jibing

    2007-01-01

    Over the past decades SINOPEC has been uninterruptedly engaging in the development and upgrading of deep catalytic cracking(DCC)technology for manufacturing propylene from heavy oil.Recently SINOPEC after having made a lot of progress in the area of oil refining at the molecular level has developed a new generation DMMC-1 type catalyst designed for the DCC process.The laboratory evaluation tests have shown that compared to the existing MMC-2 type catalyst that features the best comprehensive performance,the DMMC-1 type catalyst has increased the propylene yield by 2.2% with the propylene selectivity increased by 10%.The saidcatalyst has improved its ability for heavy oil cracking and coke selectivity along with reduction of olefin content in gasoline to achieve a better product distribution and improve the product quality.The resuIts of application of the said catalyst in a 650-kt/a commercial DCC unit at SINOPEC Anqing Branch Company have revealed that the DMMC-1 catalyst demonstrated an enhanced capabilitv for heavy oil cracking and could increase the total liquid yield to 84.56 m%from 83.92 m%,the LPG vield to 38.90 m% from 34.60 m%,the propylene yield to 17.80 m% from 15.37 m% and the propylene concentration to 45.91 m% from 44.91 m%,and reduce the coke yield from 7.61 m% to 7.05 m% and the olefin content in gasoline from 42.3v% to 37.5 v%,resulting in an incremental profit amounting to 52.19 million RMB a year.This technology has further upgradedand developed the DCC technology which has been commanding a leading position among the industry peers.

  17. Hydrogen

    Directory of Open Access Journals (Sweden)

    John O’M. Bockris

    2011-11-01

    Full Text Available The idea of a “Hydrogen Economy” is that carbon containing fuels should be replaced by hydrogen, thus eliminating air pollution and growth of CO2 in the atmosphere. However, storage of a gas, its transport and reconversion to electricity doubles the cost of H2 from the electrolyzer. Methanol made with CO2 from the atmosphere is a zero carbon fuel created from inexhaustible components from the atmosphere. Extensive work on the splitting of water by bacteria shows that if wastes are used as the origin of feed for certain bacteria, the cost for hydrogen becomes lower than any yet known. The first creation of hydrogen and electricity from light was carried out in 1976 by Ohashi et al. at Flinders University in Australia. Improvements in knowledge of the structure of the semiconductor-solution system used in a solar breakdown of water has led to the discovery of surface states which take part in giving rise to hydrogen (Khan. Photoelectrocatalysis made a ten times increase in the efficiency of the photo production of hydrogen from water. The use of two electrode cells; p and n semiconductors respectively, was first introduced by Uosaki in 1978. Most photoanodes decompose during the photoelectrolysis. To avoid this, it has been necessary to create a transparent shield between the semiconductor and its electronic properties and the solution. In this way, 8.5% at 25 °C and 9.5% at 50 °C has been reached in the photo dissociation of water (GaP and InAs by Kainthla and Barbara Zeleney in 1989. A large consortium has been funded by the US government at the California Institute of Technology under the direction of Nathan Lewis. The decomposition of water by light is the main aim of this group. Whether light will be the origin of the post fossil fuel supply of energy may be questionable, but the maximum program in this direction is likely to come from Cal. Tech.

  18. Hydrogen peroxide generation by the Weissberger biogenic oxidative system during hyaluronan degradation.

    Science.gov (United States)

    Valachová, Katarina; Topoľská, Dominika; Mendichi, Raniero; Collins, Maurice N; Sasinková, Vlasta; Šoltés, Ladislav

    2016-09-01

    By applying the enzyme catalase, our study on hyaluronan degradation confirms the generation of hydrogen peroxide using the Weissberger biogenic oxidative system (WBOS), which is composed of ascorbate and cupric ions. Dynamic viscosities of hyaluronan (HA) solutions influenced by WBOS in the absence and presence of catalase were analysed by rotational viscometry. Molar masses of HAs were determined by size-exclusion chromatography with multi-angle laser-light scattering. Our results show that catalase dose-dependently inhibited the degradation of HA macromolecules, which presumably confirms the generation of H2O2 in the reaction system. This has implications in range of biomedical applications such as arthritic joint treatment, tissue engineering, ocular and cosmetic surgery. PMID:27185130

  19. Three-dimensional FeSe2 microflowers assembled by nanosheets: Synthesis, optical properties, and catalytic activity for the hydrogen evolution reaction

    Science.gov (United States)

    Chang, Xiaoying; Jian, Jikang; Cai, Gemei; Wu, Rong; Li, Jin

    2016-03-01

    Three-dimensional FeSe2 microflowers were synthesized for the first time by a facile solvothermal method, using FeCl2·4H2O and selenium powder as raw materials, along with ethanolamine as solvent. The products were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The results show that the FeSe2 microflowers consist of nanosheets with a thickness of about 50 - 80 nm. The Raman spectrum shows the characteristic peaks of Se-Se vibration modes. The optical band gap of the sample was determined to be 1.48 eV by UV-visible absorption spectroscopy. The photoluminescence properties of the FeSe2 microflowers and their catalytic activity for the hydrogen evolution reaction were also assessed. Finally, a possible growth mechanism of the FeSe2 microflowers is proposed. [Figure not available: see fulltext.

  20. Production of bio-hydrogenated diesel by catalytic hydrotreating of palm oil over NiMoS2/γ-Al2O3 catalyst.

    Science.gov (United States)

    Srifa, Atthapon; Faungnawakij, Kajornsak; Itthibenchapong, Vorranutch; Viriya-Empikul, Nawin; Charinpanitkul, Tawatchai; Assabumrungrat, Suttichai

    2014-04-01

    Catalytic hydrotreating of palm oil (refined palm olein type) to produce bio-hydrogenated diesel (BHD) was carried out in a continuous-flow fixed-bed reactor over NiMoS2/γ-Al2O3 catalyst. Effects of dominant hydrotreating parameters: temperature: 270-420°C; H2 pressure: 15-80 bar; LHSV: 0.25-5.0 h(-1); and H2/oil ratio: 250-2000 N(cm(3)/cm(3)) on the conversion, product yield, and a contribution of hydrodeoxygenation (HDO) and decarbonylation/decarboxylation (DCO/DCO2) were investigated to find the optimal hydrotreating conditions. All calculations including product yield and the contribution of HDO and DCO/DCO2 were extremely estimated based on mole balance corresponding to the fatty acid composition in feed to fully understand deoxygenation behaviors at different conditions. These analyses demonstrated that HDO, DCO, and DCO2 reactions competitively occurred at each condition, and had different optimal and limiting conditions. The differences in the hydrotreating reactions, liquid product compositions, and gas product composition were also discussed. PMID:24583218

  1. Effects of potassium on Ni-K/Al2O3 catalysts in the synthesis of carbon nanofibers by catalytic hydrogenation of CO2.

    Science.gov (United States)

    Chen, Ching S; Lin, Jarrn H; You, Jiann H; Yang, Kuo H

    2010-03-25

    Commercially available Ni/Al(2)O(3) samples containing various concentrations of potassium were used to achieve carbon deposition from CO(2) via catalytic hydrogenation. Experimental results show that K additives can induce the formation of carbon nanofibers or carbon deposition on Ni/Al(2)O(3) during the reverse water-gas shift reaction. This work proposes that the formation rate of carbon deposition depends closely on ensemble control, suggesting that the ensemble size necessary to form carbon may be approximately 0.5 potassium atoms. The results of CO(2) temperature-programmed desorption provide strong evidence that the new adsorption sites for CO(2) created on Ni-K/Al(2)O(3) closely depend upon the synthesis of carbon nanofibers. It is found that some potassium-related active phases obtained by calcination and reduction pretreatments can participate in the carbon deposition reaction. The formation pathway for carbon deposition suggests that the main source of carbon deposition is CO(2) and that the pathway is independent of the reaction products CO and CH(4) in the reverse water-gas shift reaction. PMID:19655780

  2. Synthesis and Characterization of K-Ta Mixed Oxides for Hydrogen Generation in Photocatalysis

    Directory of Open Access Journals (Sweden)

    Beata Zielińska

    2012-01-01

    Full Text Available K-Ta mixed oxides photocatalysts have been prepared by impregnation followed by calcination. The influence of the reaction temperature (450°C–900°C on the phase formation, crystal morphology, and photocatalytic activity in hydrogen generation of the produced materials was investigated. The detailed analysis has revealed that all products exhibit high crystallinity and irregular structure. Moreover, two different crystal structures of potassium tantalates such as KTaO3 and K2Ta4O11 were obtained. It was also found that the sample composed of KTaO3 and traces of unreacted Ta2O5 (annealed at 600°C exhibits the highest activity in the reaction of photocatalytic hydrogen generation. The crystallographic phases, optical and vibronic properties were examined by X-ray diffraction (XRD and diffuse reflectance (DR UV-vis and resonance Raman spectroscopic methods, respectively. Morphology and chemical composition of the produced samples were studied using a high-resolution transmission electron microscope (HR-TEM and an energy dispersive X-ray spectrometer (EDX as its mode.

  3. Methanol-steam reforming using a microstructured reactor for hydrogen generation for fuel cell powered vehicles; Methanol-Dampf Reformierung im Mikrostrukturreaktor zur Wasserstofferzeugung fuer Brennstoffzellenfahrzeuge

    Energy Technology Data Exchange (ETDEWEB)

    Pfeifer, P.

    2003-08-01

    On-board hydrogen production in automotive systems is of great interest in order to fulfil the legal requirements of emission control in the near future and to produce zero emission cars. The demand of high dynamics of the on-board hydrogen generation leads to newer technologies like microreaction technology. Excellent heat and mass transfer in microstructured reactors/heat exchangers increase the possibility to reduce the system size and to decrease parasitic heat loss, additionally. The present work describes the development of a coating technology, a catalyst system, catalyst characterisation and the test of these catalysts considering modelling of the reaction and scale-up of metallic microreactors for the catalytic steam reforming of methanol. The appropriateness of the catalyst coatings and of the metallic microreactors for the chosen reaction and dynamic operation has been demonstrated successfully. The coating of the metallic microchannels in the diameter range 100-300 {mu}m was done by the modification of the conventional washcoating process using a solvent-polymer-nanoparticle slurry. Pre-Coating (coating before assembling the foils to a reactor) and Post-Coating (coating after assembling the microstructured foils to a reactor) were shown to be feasible, which is an important fact considering the assembling procedure. Homogeneity of the coating was proven experimentally by hot wire anemometry. (orig.)

  4. Hydrogen sensor

    Science.gov (United States)

    Duan, Yixiang; Jia, Quanxi; Cao, Wenqing

    2010-11-23

    A hydrogen sensor for detecting/quantitating hydrogen and hydrogen isotopes includes a sampling line and a microplasma generator that excites hydrogen from a gas sample and produces light emission from excited hydrogen. A power supply provides power to the microplasma generator, and a spectrometer generates an emission spectrum from the light emission. A programmable computer is adapted for determining whether or not the gas sample includes hydrogen, and for quantitating the amount of hydrogen and/or hydrogen isotopes are present in the gas sample.

  5. Catalytic effect of nano-sized ScH{sub 2} on the hydrogen storage of mechanically milled MgH{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Xuanli, E-mail: Xuanli.Luo@nottingham.ac.uk; Grant, David M., E-mail: David.Grant@nottingham.ac.uk; Walker, Gavin S., E-mail: Gavin.Walker@nottingham.ac.uk

    2015-02-15

    Highlights: • The ScH{sub 2} nanoparticles improved the MgH{sub 2} dehydrogenation kinetics. • Low activation energy of the dehydrogenation reaction (62 ± 5 kJ mol{sup −1}). • Optimal ScH{sub 2} catalyst content was ca. 12 mol.% to achieve lowest activation energy. • High cycling stability at relatively high temperature up to 450 °C. • The ScH{sub 2} nano-structure remained throughout cycling. - Abstract: The hydrogen storage properties of ball milled xMgH{sub 2}/(1 − x)ScH{sub 2} (x = 0.65-1) samples including capacity, kinetics, thermodynamics and cycling stability, were investigated. The effect of ScH{sub 2} catalyst content and ball milling duration on the kinetics of MgH{sub 2} dehydrogenation were studied. It was found that the optimal content of the catalyst ScH{sub 2} was ca. 12 mol.%, which gave an activation energy (E{sub a}) value of 62 ± 5 kJ mol{sup −1} and a hydrogen storage capacity of 5.8 ± 0.1 wt.% for the sample. There was no loss in kinetics in the ScH{sub 2} catalysed MgH{sub 2} system even after cycling at relatively high temperatures up to 450 °C, and the nano-sized ScH{sub 2} (ca. 70 nm) formed during ball milling remained after (de)hydrogenation cycling. Typical MgH{sub 2} dehydrogenation enthalpy (76 ± 1 kJ mol{sup −1} (H{sub 2})) and entropy (138 ± 2 J mol{sup −1} K{sup −1} (H{sub 2})) values observed by the 0.65MgH{sub 2}/0.35ScH{sub 2} sample demonstrated the effect of ScH{sub 2} was purely a catalytic improvement of the kinetics.

  6. Key parameters when developing carbonaceous materials for catalytic wet peroxide oxidation

    OpenAIRE

    Ribeiro, Rui; Silva, Adrián; Pastrana-Martínez, Luisa; Figueiredo, José; Faria, Joaquim; Gomes, Helder

    2014-01-01

    Catalytic wet peroxide oxidation (CWPO) is an advanced oxidation process, operated using simple equipment and mild operating conditians, in which highly oxidizing hydraxyl radicaIs (HO') are generated fram the catalytic decompasition af hydrogen peroxide (H,O,) [L 2). Sinee the report of Lüeking el ai. in 1998 [3], the develapment af suitab-Ie -carbonaceous materials (without any added metal phase) for CWPO has been intensively explored [4). lhe influenee of struetUfal and surr...

  7. Initial Screening of Thermochemical Water-Splitting Cycles for High Efficiency Generation of Hydrogen Fuels Using Nuclear Power

    International Nuclear Information System (INIS)

    OAK B188 Initial Screening of Thermochemical Water-Splitting Cycles for High Efficiency Generation of Hydrogen Fuels Using Nuclear Power There is currently no large scale, cost-effective, environmentally attractive hydrogen production process, nor is such a process available for commercialization. Hydrogen is a promising energy carrier, which potentially could replace the fossil fuels used in the transportation sector of our economy. Fossil fuels are polluting and carbon dioxide emissions from their combustion are thought to be responsible for global warming. The purpose of this work is to determine the potential for efficient, cost-effective, large-scale production of hydrogen utilizing high temperature heat from an advanced nuclear power station. Almost 800 literature references were located which pertain to thermochemical production of hydrogen from water and over 100 thermochemical watersplitting cycles were examined. Using defined criteria and quantifiable metrics, 25 cycles have been selected for more detailed study

  8. Initial Screening of Thermochemical Water-Splitting Cycles for High Efficiency Generation of Hydrogen Fuels Using Nuclear Power

    Energy Technology Data Exchange (ETDEWEB)

    Brown, L.C.; Funk, J.F.; Showalter, S.K.

    1999-12-15

    OAK B188 Initial Screening of Thermochemical Water-Splitting Cycles for High Efficiency Generation of Hydrogen Fuels Using Nuclear Power There is currently no large scale, cost-effective, environmentally attractive hydrogen production process, nor is such a process available for commercialization. Hydrogen is a promising energy carrier, which potentially could replace the fossil fuels used in the transportation sector of our economy. Fossil fuels are polluting and carbon dioxide emissions from their combustion are thought to be responsible for global warming. The purpose of this work is to determine the potential for efficient, cost-effective, large-scale production of hydrogen utilizing high temperature heat from an advanced nuclear power station. Almost 800 literature references were located which pertain to thermochemical production of hydrogen from water and over 100 thermochemical watersplitting cycles were examined. Using defined criteria and quantifiable metrics, 25 cycles have been selected for more detailed study.

  9. Inhibition of hydrogen sulfide generation from disposed gypsum drywall using chemical inhibitors

    International Nuclear Information System (INIS)

    Disposal of gypsum drywall in landfills has been demonstrated to elevate hydrogen sulfide (H2S) concentrations in landfill gas, a problem with respect to odor, worker safety, and deleterious effect on gas-to-energy systems. Since H2S production in landfills results from biological activity, the concept of inhibiting H2S production through the application of chemical agents to drywall during disposal was studied. Three possible inhibition agents - sodium molybdate (Na2MoO4), ferric chloride (FeCl3), and hydrated lime (Ca(OH)2) - were evaluated using flask and column experiments. All three agents inhibited H2S generation, with Na2MoO4 reducing H2S generation by interrupting the biological sulfate reduction process and Ca(OH)2 providing an unfavorable pH for biological growth. Although FeCl3 was intended to provide an electron acceptor for a competing group of bacteria, the mechanism found responsible for inhibiting H2S production in the column experiment was a reduction in pH. Application of both Na2MoO4 and FeCl3 inhibited H2S generation over a long period (over 180 days), but the impact of Ca(OH)2 decreased with time as the alkalinity it contributed was neutralized by the generated H2S. Practical application and potential environmental implications need additional exploration.

  10. Inhibition of hydrogen sulfide generation from disposed gypsum drywall using chemical inhibitors.

    Science.gov (United States)

    Xu, Qiyong; Townsend, Timothy; Bitton, Gabriel

    2011-07-15

    Disposal of gypsum drywall in landfills has been demonstrated to elevate hydrogen sulfide (H(2)S) concentrations in landfill gas, a problem with respect to odor, worker safety, and deleterious effect on gas-to-energy systems. Since H(2)S production in landfills results from biological activity, the concept of inhibiting H(2)S production through the application of chemical agents to drywall during disposal was studied. Three possible inhibition agents - sodium molybdate (Na(2)MoO(4)), ferric chloride (FeCl(3)), and hydrated lime (Ca(OH)(2)) - were evaluated using flask and column experiments. All three agents inhibited H(2)S generation, with Na(2)MoO(4) reducing H(2)S generation by interrupting the biological sulfate reduction process and Ca(OH)(2) providing an unfavorable pH for biological growth. Although FeCl(3) was intended to provide an electron acceptor for a competing group of bacteria, the mechanism found responsible for inhibiting H(2)S production in the column experiment was a reduction in pH. Application of both Na(2)MoO(4) and FeCl(3) inhibited H(2)S generation over a long period (over 180 days), but the impact of Ca(OH)(2) decreased with time as the alkalinity it contributed was neutralized by the generated H(2)S. Practical application and potential environmental implications need additional exploration. PMID:21592650

  11. STANDALONE &LDQUO;GREEN&RDQUO; COMMUNITY-CENTER BUILDINGS: HYDROGEN GENERATION/STORAGE/DELIVERY SYSTEM FOR WHEN PRIMARY ENERGY STORAGE IS AT CAPACITY

    Science.gov (United States)

    Overall, the implementation of a computer-controlled hydrogen generation system and subsequent conversion of small engine equipment for hydrogen use has been surprisingly straightforward from an engineering and technology standpoint. More testing is required to get a better gr...

  12. Monopropellant engine investigation for space shuttle reaction control. Volume 2: Design, fabrication, and demonstration test of a catalytic gas generator for the space shuttle APU

    Science.gov (United States)

    1975-01-01

    The capability of a catalytic gas generator to meet the requirement specified for the space shuttle APU is established. A full-scale gas generator, designed to operate at a chamber pressure of 750 psia and a flow rate of 0.36 lbm/sec, was fabricated and subjected to three separate life test series. The nickel foam metal used for catalyst retention was investigated. Inspection of the foam metal following the first life test revealed significant degradation. Consequently an investigation was conducted to determine the mechanism of degradation and to provide an improved foam metal.

  13. Catalytic Conversion of Biofuels

    DEFF Research Database (Denmark)

    Jørgensen, Betina

    This thesis describes the catalytic conversion of bioethanol into higher value chemicals. The motivation has been the unavoidable coming depletion of the fossil resources. The thesis is focused on two ways of utilising ethanol; the steam reforming of ethanol to form hydrogen and the partial oxida...

  14. Hydrogen generation from polyvinyl alcohol-contaminated wastewater by a process of supercritical water gasification

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    Gasification of polyvinyl alcohol (PVA)-contaminated wastewater in supercritical water (SCW) was investigated in a continuous flow reactor at 723-873 K, 20-36 MPa and residence time of 20-60 s. The gas and liquid products were analyzed by GC/TCD, TOC analyzer and GC/MS. The main gas products were H2, CH4, CO and CO2. Pressure change had no significant influence on gasification efficiency. Higher temperature and longer residence time enhanced gasification efficiency, and lower temperature favored the production of H2. The effects of KOH catalyst on gas product composition were studied, and gasification efficiency were analyzed. The TOC removal efficiency (TOCR), carbon gasification ratio (CGR) and hydrogen gasification ratio (HGR) were up to 96.00%, 95.92% and 126.40% at 873 K and 60 s, respectively, which suggests PVA can be completely gasified in SCW. The results indicate supercritical water gasification for hydrogen generation is a promising process for the treatment of PVA wastewater.

  15. Efficiency Evaluation of a Photovoltaic System Simultaneously Generating Solar Electricity and Hydrogen for Energy Storage

    Directory of Open Access Journals (Sweden)

    Abermann S.

    2012-10-01

    Full Text Available The direct combination of a photovoltaic system with an energy storage component appears desirable since it produces and stores electrical energy simultaneously, enabling it to compensate power generation fluctuations and supply sufficient energy during low- or non-irradiation periods. A novel concept based on hydrogenated amorphous silicon (a-Si:H triple-junction solar cells, as for example a-Si:H/a-SiGe:H/a-SiGe:H, and a solar water splitting system integrating a polymer electrolyte membrane (PEM electrolyser is presented. The thin film layer-by-layer concept allows large-area module fabrication applicable to buildings, and exhibits strong cost-reduction potential as compared to similar concepts. The evaluation shows that it is possible to achieve a sufficient voltage of greater than 1.5 V for effective water splitting with the a-Si based solar cell. Nevertheless, in the case of grid-connection, the actual energy production cost for hydrogen storage by the proposed system is currently too high.

  16. Catalytic Oxidation with a Non-Heme Iron Complex That Generates a Low-Spin FeIIIOOH Intermediate

    NARCIS (Netherlands)

    Roelfes, Gerard; Lubben, Marcel; Hage, Ronald; Que, Jr.; Feringa, Bernard

    2000-01-01

    The antitumor drug bleomycin (BLM) is proposed to act via a low-spin iron(III) hydroperoxide intermediate called “activated bleomycin”. To gain more insight into the mechanistic aspects of catalytic oxidation by these intermediates we have studied the reactivity of [(N4Py)Fe(CH3CN)](ClO4)2 (1) (N4Py

  17. Generation of hydrogen peroxide from San Joaquin Valley particles in a cell-free solution

    Science.gov (United States)

    Shen, H.; Barakat, A. I.; Anastasio, C.

    2011-01-01

    Epidemiological studies have shown a correlation between exposure to ambient particulate matter (PM) and adverse health effects. One proposed mechanism of PM-mediated health effects is the generation of reactive oxygen species (ROS) - e.g., superoxide (•O2-), hydrogen peroxide (HOOH), and hydroxyl radical (•OH) - followed by oxidative stress. There are very few quantitative, specific measures of individual ROS generated from PM, but this information would help to more quantitatively address the link between ROS and the health effects of PM. To address this gap, we quantified the generation of HOOH by PM collected at an urban (Fresno) and rural (Westside) site in the San Joaquin Valley (SJV) of California during summer and winter from 2006 to 2009. HOOH was quantified by HPLC after extracting the PM in a cell-free, phosphate-buffered saline (PBS) solution with or without 50 μM ascorbate (Asc). Our results show that the urban PM generally generates much more HOOH than the rural PM but that there is no apparent seasonal difference in HOOH generation. In nearly all of the samples the addition of a physiologically relevant concentration of Asc greatly enhances HOOH formation, but a few of the coarse PM samples were able to generate a considerable amount of HOOH in the absence of added Asc, indicating the presence of unknown reductants. Normalized by air volume, the fine PM (PM2.5) generally makes more HOOH than the corresponding coarse PM (PMcf, i.e., 2.5 to 10 μm), primarily because the mass concentration of PM2.5 is much higher than that of PMcf. However, normalized by PM mass, the coarse PM typically generates more HOOH than the fine PM. The amount of HOOH produced by SJV PM is reduced on average by (78 ± 15)% when the transition metal chelator desferoxamine (DSF) is added to the extraction solution, indicating that transition metals play a dominant role in HOOH generation. By measuring calibration curves of HOOH generation from copper, and quantifying copper

  18. Generation of hydrogen peroxide from San Joaquin Valley particles in a cell-free solution

    Directory of Open Access Journals (Sweden)

    H. Shen

    2010-09-01

    Full Text Available Epidemiological studies have shown a correlation between exposure to ambient particulate matter (PM and adverse health effects. One proposed mechanism of PM-mediated health effects is the generation of reactive oxygen species (ROS – e.g., superoxide (•O2, hydrogen peroxide (HOOH, and hydroxyl radical (•OH – followed by oxidative stress. There are very few quantitative, specific measures of individual ROS generated from PM, but this information would help to more quantitatively address the link between ROS and the health effects of PM. To address this gap, we quantified the generation of HOOH by PM collected at an urban (Fresno and rural (Westside site in the San Joaquin Valley (SJV of California during summer and winter from 2006 to 2009. HOOH was quantified by HPLC after extracting the PM in a cell-free, phosphate-buffered saline (PBS solution with or without 50 μM ascorbate (Asc. Our results show that the urban PM generally generates much more HOOH than the rural PM but that there is no apparent seasonal difference in HOOH generation. In nearly all of the samples the addition of a physiologically relevant concentration of Asc greatly enhances HOOH formation, but a few of the coarse PM samples were able to generate a considerable amount of HOOH in the absence of added Asc, indicating the presence of unknown reductants. Normalized by air volume, the fine PM (PM2.5 generally makes more HOOH than the corresponding coarse PM (PMcf, i.e., 2.5 to 10 μm, primarily because the mass concentration of PM2.5 is much higher than that of PMcf. However, normalized by PM mass, the coarse PM typically generates more HOOH than the fine PM. The amount of HOOH produced by SJV PM is reduced on average by (78±15% when the transition metal chelator desferoxamine (DSF is added to the extraction solution, indicating that transition metals play a dominant role in HOOH generation. By

  19. Generation of hydrogen peroxide from San Joaquin Valley particles in a cell-free solution

    Directory of Open Access Journals (Sweden)

    H. Shen

    2011-01-01

    Full Text Available Epidemiological studies have shown a correlation between exposure to ambient particulate matter (PM and adverse health effects. One proposed mechanism of PM-mediated health effects is the generation of reactive oxygen species (ROS – e.g., superoxide (O2, hydrogen peroxide (HOOH, and hydroxyl radical (OH – followed by oxidative stress. There are very few quantitative, specific measures of individual ROS generated from PM, but this information would help to more quantitatively address the link between ROS and the health effects of PM. To address this gap, we quantified the generation of HOOH by PM collected at an urban (Fresno and rural (Westside site in the San Joaquin Valley (SJV of California during summer and winter from 2006 to 2009. HOOH was quantified by HPLC after extracting the PM in a cell-free, phosphate-buffered saline (PBS solution with or without 50 μM ascorbate (Asc. Our results show that the urban PM generally generates much more HOOH than the rural PM but that there is no apparent seasonal difference in HOOH generation. In nearly all of the samples the addition of a physiologically relevant concentration of Asc greatly enhances HOOH formation, but a few of the coarse PM samples were able to generate a considerable amount of HOOH in the absence of added Asc, indicating the presence of unknown reductants. Normalized by air volume, the fine PM (PM2.5 generally makes more HOOH than the corresponding coarse PM (PMcf, i.e., 2.5 to 10 μm, primarily because the mass concentration of PM2.5 is much higher than that of PMcf. However, normalized by PM mass, the coarse PM typically generates more HOOH than the fine PM. The amount of HOOH produced by SJV PM is reduced on average by (78 ± 15% when the transition metal chelator desferoxamine (DSF is added to the extraction solution, indicating that transition metals play a dominant role in HOOH

  20. Acoustically induced optical second harmonic generation in hydrogenated amorphous silicon films

    CERN Document Server

    Ebothe, J; Cabarrocas, P R I; Godet, C; Equer, B

    2003-01-01

    Acoustically induced second harmonic generation (AISHG) in hydrogenated amorphous silicon (a-Si : H) films of different morphology has been observed. We have found that with increasing acoustical power, the optical SHG of Gd : YAB laser light (lambda = 2.03 mu m) increases and reaches its maximum value at an acoustical power density of about 2.10 W cm sup - sup 2. With decreasing temperature, the AISHG signal strongly increases below 48 K and correlates well with the temperature behaviour of differential scanning calorimetry indicating near-surface temperature phase transition. The AISHG maxima were observed at acoustical frequencies of 10-11, 14-16, 20-22 and 23-26 kHz. The independently performed measurements of the acoustically induced IR spectra have shown that the origin of the observed phenomenon is the acoustically induced electron-phonon anharmonicity in samples of different morphology.