A simple anaerobic biodegradation process using wastewater treatment plant (WWTP) effluent, shredded paper, and a purge of nitrogen gas was used to produce hydrogen and simultaneously capture nitrogen and phosphorus. Two reactor configurations a sequencing batch reactor (SBR) and a classic batch reactor (CBR) were tested as simultaneous saccharification and fermentation reactors (enzymatic hydrolysis and fermentation in one tank). The CBR demonstrated greater stability of hydrogen production and simplicity of operation, while the SBR provided better nitrogen and phosphorus removal efficiencies. Nuclear magnetic resonance analyses showed acetic acid to be the main product from both reactors. Optimal CBR conditions were found to be pH 5, 4 g/L loading 0.45 ml/g Accellerase 1500, and 38 C. Experiments with an argon purge in place of nitrogen and with ammonium chloride spiking suggested that hydrogenase and nitrogenase enzymes contributed similarly to hydrogen production in the cultures. Analysis of a single fermentation showed that hydrogen production occurred relatively early in the course of TOC removal, and that follow-on treatments might extract more energy from the products.

关键词：制氢；铵化合物；冰醋酸；生物降解

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Develop and demonstrate reversible nanostructured activated carbon hydrogen storage material which has at least a 5.5 wtmaterial-based gravimetric capacity and a 40 gH2/L material-based volumetric capacity at-38-85C, and the potential to meet DOE 2017 system-level targets. Prepare and characterize nanostructured polymer derivatives as carbon precursors. Initiate the production of nanostructured activated carbon for hydrogen storage. Develop methods for sorbent-based doped polymer/carbon.

关键词：储氢;活性炭;纳米结构聚合物;吸附剂

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Thermochemical water splitting cycles, using the heat of nuclear power plants, offer an alternate highly efficient route for the production of hydrogen. Among the many possible thermochemical cycles for the hydrogen production, the sulfur-based cycles lead the competition in overall energy efficiency. A variant on sulfur-based thermochemical cycles is the Hybrid Sulfur (HyS) Process, which uses a sulfur dioxide depolarized electrolyzer (SDE) to produce hydrogen. The Savannah River National Laboratory (SRNL) selected the fuel cell MEA design concept for the SDE in the HyS process since the MEA concept provides a much smaller cell footprint than conventional parallel plate technology. The electrolyzer oxidizes sulfur dioxide to form sulfuric acid at the anode and reduces protons to form hydrogen at the cathode. The overall electrochemical cell reaction consists of the production of H(sub 2)SO(sub 4) and H(sub 2). There is a significant need to provide the membrane materials that exhibit reduced sulfur dioxide transport characteristics without sacrificing other important properties such as high ionic conductivity and excellent chemical stability in highly concentrated sulfuric acid solutions saturated with sulfur dioxide. As an alternative membrane, sulfonated Perfluorocyclobutyl aromatic ether polymer (sPFCB) were expected to posses low SO2 permeability due to their stiff backbones as well as high proton conductivity, improved mechanical properties. The major accomplishments of this project were the synthesis, characterizations, and optimizations of suitable electrolyzers for good SDE performance and higher chemical stability against sulfuric acid. SDE performance results of developed sPFCB polyelectrolytes have shown that these membranes exhibit good chemical stability against H(sub 2)SO(sub 4).

关键词：氟代电解质；高导电性；制氢；热化学循环

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Idaho National Laboratory (INL), GE Global Research (GEGR), and Western Research Institute (WRI) have successfully produced hydrogenselective membranes for water-gas-shift (WGS) modules that enable high-pressure hydrogen product streams. Several high performance (HP) polymer membranes were investigated for their gas separation performance under simulated (mixed gas) and actual syngas conditions. To enable optimal module performance, membranes with high hydrogen (H2) selectivity, permeance, and stability under WGS conditions are required. The team determined that the VTEC PI 80-051 and VTEC PI 1388 (polyimide from Richard Blaine International, Inc.) are prime candidates for the H2 gas separations at operating temperatures (approx. 200DGC). VTEC PI 80-051 was thoroughly analyzed for its H2 separations under syngas processing conditions using more-complex membrane configurations, such as tube modules and hollow fibers. These membrane formats have demonstrated that the selected VTEC membrane is capable of providing highly selective H2/CO2 separation (a = 79) and H2/CO separation (a = 4080) in humidified syngas streams. In addition, the VTEC polymer membranes are resilient within the syngas environment (WRI coal gasification) at 200DGC for over 1000 hours. The information within this report conveys current developments of VTEC PI 80-051 as an effective H2 gas separations membrane for high-temperature syngas streams.

关键词：制氢；化学反应器；供水供气过程；移位过程

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Air Products and Chemicals, Inc., is developing the sour pressure swing adsorption (PSA) technology which can be used to reject acid gas components (hydrogen sulfide (H(sub 2)S) and carbon dioxide (CO(sub 2))) from sour syngas streams such as coal gasification syngas. In the current work, tests were conducted to investigate the impact of continuous exposure of real sour syngas and dilute levels of hydrochloric acid (HCl) and ammonia (NH(sub 3)) on the preferred adsorbent of that process. The results show a modest (approximately 10-15) decrease in CO(sub 2) adsorption capacity after sour syngas exposure, as well as deposition of metals from carbonyl decomposition. Continuous exposure to HCl and NH3 yield a higher degree of CO2 capacity degradation (up to 25). These tests represent worst-case approaches since the exposure is continuous and the HCl and NH3 levels are relatively high compare to an industrial sour syngas stream. Long-term PSA tests are needed to unequivocally evaluate the impact of cyclic exposure to these types of streams.

关键词：制氢；曝光；氢硫化物；金属

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Hydrogenation of CO and CO2 to methanol on a stepped Copper surface has been calculated using the BEEF-vdW functional and is compared to values derived with RPBE. It is found that the inclusion of vdW forces in the BEEF-vdW functional yields a better description of CO2 hydrogenation as compared to RPBE. These differences are significant for a qualitative description of the overall methanol synthesis kinetics and it is suggested that the selectivity with respect to CO and CO2 is only described correctly with BEEF-vdW.

关键词：加氢；铜；二氧化碳；功能；动力学；甲醇

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This work is directed towards the preparation of chemoselective ruthenium catalyst.The catalyst is a new type of ruthenium(Ⅱ) complexes supported on γ-Al2O3,which have ruthenium(Ⅱ) centers coordinated to the ligands triphenylphosphine and (1 S,2S)-1,2-Diphenyl-1,2-ethanediamine.The catalyst for the selective hydrogenation of ketones in the mild conditions is investigated.The results show that the performance of the catalystis greatly influenced by the ratio of Ru and PPh3 and reduction time,respectively.

关键词：加氢；化学选择性；钌；酮类

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Conventional storage of large amounts of hydrogen in its molecular form is difficult and expensive because it requires employing either extremely high pressure gas or very low temperature liquid. Because of the importance of hydrogen as a fuel, the DOE has set system targets for hydrogen storage of gravimetric (5.5 wt) and volumetric (40 g L-1) densities to be achieved by 2015. Given that these are system goals, a practical material will need to have higher capacity when the weight of the tank and associated cooling or regeneration system is considered. The size and weight of these components will vary substantially depending on whether the material operates by a chemisorption or physisorption mechanism. In the latter case, metal-organic frameworks (MOFs) have recently been identified as promising adsorbents for hydrogen storage, although little data is available for their sorption behavior. This grant was focused on the study of MOFs with these specific objectives. (1) To examine the effects of functionalization, catenation, and variation of the metal oxide and organic linkers on the low-pressure hydrogen adsorption properties of MOFs. (2) To develop a strategy for producing MOFs with high surface area and porosity to reduce the dead space and increase the hydrogen storage capacity per unit volume. (3) To functionalize MOFs by post synthetic functionalization with metals to improve the adsorption enthalpy of hydrogen for the room temperature hydrogen storage. This effort demonstrated the importance of open metal sites to improve the adsorption enthalpy by the systematic study, and this is also the origin of the new strategy, which termed isoreticular functionalization and metalation. However, a large pore volume is still a prerequisite feature. Based on our principle to design highly porous MOFs, guest-free MOFs with ultrahigh porosity have been experimentally synthesized. MOF-210, whose BET surface area is 6240 m2 g-1 (the highest among porous solids), takes up 15 wtof total H2 uptake at 80 bar and 77 K. More importantly, the total H2 uptake by MOF-210 was 2.7 wtat 80 bar and 298 K, which is the highest number reported for physisorptive materials.

关键词：储氢；吸附剂；化学吸附；孔隙度；焓

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Hydrogen fuel cells can potentially reduce greenhouse gas emissions and the United States dependence on foreign oil, but issues with hydrogen storage are impeding their widespread use. To help overcome these challenges, this study analyzes opportunities for their near-term deployment in five categories of non-motive equipment: portable power, construction equipment, airport ground support equipment, telecom backup power, and man-portable power and personal electronics. To this end, researchers engaged end users, equipment manufacturers, and technical experts via workshops, interviews, and electronic means, and then compiled these data into meaningful and realistic requirements for hydrogen storage in specific target applications. In addition to developing these requirements, end-user benefits (e.g., low noise and emissions, high efficiency, potentially lower maintenance costs) and concerns (e.g., capital cost, hydrogen availability) of hydrogen fuel cells in these applications were identified. Market data show potential deployments vary with application from hundreds to hundreds of thousands of units.

关键词：储氢；燃料电池；能源效率；温室气体

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Effective storage of hydrogen presents one of the most significant technical gaps to successful implementation of the hydrogen economy, particularly for transportation applications. Amine boranes, such as ammonia borane H3NBH3 and ammonia triborane H3NB3H7, have been identified as promising, high-capacity chemical hydrogen storage media containing potentially readily released protic (N-H) and hydridic (B-H) hydrogens. At the outset of our studies, dehydrogenation of ammonia borane had been studied primarily in the solid state, but our DOE sponsored work clearly demonstrated that ionic liquids, base-initiators and/or metal-catalysts can each significantly increase both the rate and extent of hydrogen release from amine boranes under moderate conditions. Our studies also showed that depending upon the activation method, hydrogen release from amine boranes can occur by very different mechanistic steps and yield different types of spent-fuel materials. The fundamental understanding that was developed during this grant of the pathways and controlling factors for each of these hydrogen-release mechanisms is now enabling continuing discovery and optimization of new chemical-hydride based hydrogen storage systems.

关键词：储氢；胺硼烷脱氢催化剂；氢化物

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