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hydrogenase as the basis for green hydrogen production and utilization

Journal of Energy Chemistry 2023年第10期85卷 348-362,I0011页

作者： Haishuo Ji Lei Wan Yanxin Gao Ping Du Wenjin Li Hang Luo Jiarui Ning Yingying Zhao Huangwei Wang Lixin Zhang Liyun Zhang State Key Laboratory of Medicinal Chemical Biology College of PharmacyNankai UniversityTianjin 300350China Max Planck Institute for Chemical Energy Conversion Stiftstrasse 34-3645470 Mülheim an der RuhrGermany State Key Laboratory of Medicinal Chemical Biology College of Life SciencesNankai UniversityTianjin 300350China State Key Laboratory of Bioreactor Engineering and School of BiotechnologyEast China University of Science and Technology(ECUST)Shanghai 200237China

hydrogenase is a paradigm of highly efficient biocatalyst for H_(2) production and utilization evolved in nature. A dilemma is that despite the high activity and efficiency expected for hydrogenases as promising catalysts for the hydrogen economy, the poor oxygen tolerance and low yield of hydrogenases largely hinder their practical application. In these years, the enigmas surrounding hydrogenases regarding their structures, oxygen tolerance, mechanisms for catalysis, redox intermediates, and proton-coupled electron transfer schemes have been gradually elucidated;the schemes, which can well couple hydrogenases with other highly efficient(in)organic and biological catalysts to build novel reactors and drive valuable reactions, make it possible for hydrogenases to find their niches. To see how scientists put efforts to tackle this issue and design novel reactors in the fields where hydrogenases play crucial roles, in this review,recent advances were summarized, including different strategies for protecting enzyme molecules from oxygen, enzyme-based assembling systems for H_(2) evolution in the photoelectronic catalysis, enzymatic biofuel cells for H_(2) utilization and storage and the efficient electricity-hydrogen-carbohydrate cycle for high-purity hydrogen and biofuel automobiles. Limitations and future perspectives of hydrogenasebased applications in H_(2) production and utilization with great impact are discussed. In addition, this review also provides a new perspective on the use of biohydrogen in healthcare beyond energy.

关键词： hydrogenase Biological H_(2)energy Oxygen tolerance Artificial photosynthesis Biofuel cells

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Immobilizing [FeFe]-hydrogenase mimics to metal–organic frameworks for enhanced hydrogen production

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Science Bulletin 2019年第20期64卷 1476-1477页

作者： Daofeng Sun School of Materials Science and Engineering College of Science China University of Petroleum (East China)

Production of hydrogen from water by solar-energy conversion has long been considered a promising way to solve the climate change and energy crisis(1)However,some critical issues at this stage,such as catalysts for hydrogen evolution with high efficiency and low cost,definitely hinder the practical application of photocatalytic hydrogen production from water.[Fe Fe]-hydrogenase,an excellent natural biological enzyme catalyst bearing unique organometallic clusters with noble-metal-free element,is most efficient in reducing protons to hydrogen and demonstrates remarkable turnover frequencies(TOF 6000–9000 s1 per active site)[2].

关键词： mimics Immobilizing hydrogenase mimics to metal organic frameworks for enhanced hydrogen production

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Photoinduced hydrogen evolution in an artificial system containing photosystem I, hydrogenase, methy1 viologen and mercaptoacetic acid

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Chinese Chemical Letters 2008年第5期19卷 607-610页

作者： Dong Jin Qian mi Rong Liu Chikashi Nakamura Stephan Olav Wenk Jun Miyake Department of Chemistry Fudan University 220 Handan Road Shanghai 200433 China Tissue Engineering Research Center National Institute of Advanced Industrial Science and Technology 3-11-46 Nakouji Amagasaki Hyogo 661-0974 Japan

Hydrogen evolution was detected in an artificial system composed of light-harvesting unit of purified photosystem I, catalyst of hydrogenase, methyl viologen and electron donor under radiation. Absorption spectral features confirmed that electron transfer from electron donors to proton was via a photoinduced reductive process of methyl viologen.

关键词： Hydrogen evolution hydrogenase Photosystem I Artificial system

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An[Fe-Fe]-hydrogenase Mimic Immobilized on MCM-41 for the Photochemical Production of Hydrogen in Pure Water

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Chinese Journal of Chemistry 2014年第6期32卷 479-484页

作者： Wen Wang Tianjun Yu Yi Zeng Jinping Chen Yi Li Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China

A composite proton-reducing catalyst Hy@MCM-41 was created by using a hydrophobic[Fe-Fe]-hydrogenase mimic(Hy)incorporated into the K^(+)-exchanged molecular sieve *** acts as the active site to generate H_(2) by reducing H^(+),and MCM-41 provide a large surface area to maintain the dispersion of Hy and to prevent aggrega-tion and ***@MCM-41 was successfully applied to the light-induced hydrogen production in pure water with an iridium compound[Ir(ppy)_(2)bpy]Cl and triethylamine(TEA)as the photosensitizer and the sacrificial electron donor,respectively,exhibiting good stability and catalytic *** present study provides a general strategy for the application of water-insoluble catalysts in pure water by using mesoporous molecular sieves.

关键词： energy conversion hydrogen hydrogenase MCM-41 immobilization photochemistry

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Optimization of detecting hydrogenase activity for acidogenic fermentation of activated sludge

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Journal of Harbin Institute of Technology(New Series) 2010年第5期17卷 721-725页

作者：郑国臣赫俊国李建政阿杰张立国 State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology School of Municipal and Environmental Engineering Harbin Institute of Technology

In order to evaluate the hydrogen-producing efficiency of anaerobic activated sludge in Anaerobic Baffled Reactor(ABR)fermentation processes,the optimal conditions for hydrogen producing hydrogenase method on methyl viologen(MV)assay was used to detect the hydrogen production activity of the activated *** most favorable parameters such as 0.6 mL sodium acetate buffer(pH 5.0),100 μL lysozyme,0.2 mL sodium dibromoethane(9.0 mmol/L)and 0.7 mmol/L iron added into 1 mL activated sludge(2.66～26.64 gMLVSS/L)were ***,reaction temperature and culture time were detected as 40 ℃ and 30 min *** thiosulfate and sodium sulfides were taken as the reducing agent while trichloroacetic acid as *** the MV optimal conditions,micro-toxic Dimethyl sulfoxide(DMSO)get higher security and better *** sensitivity of the detection methods(DMSO as electron carrier)was increased by more than 30%.The results show that the optimal conditions can be applied to measure hydrogenase activity correlating with its specific hydrogen production rate in a hydrogen-producing anaerobic activated sludge system.

关键词： fermentation anaerobe activated sludge hydrogenase

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Comparative evaluation of different cell disruption methods for the release of hydrogenase from H2 -producing bacterium E. harbinenase YUAN-3T

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Journal of Harbin Institute of Technology(New Series) 2011年第6期18卷 103-106页

作者：杜明任南琪张璐张文龙 School of Municipal and Environmental Engineering Harbin Institute of Technology School of Food Science and Engineering Harbin Institute of Technology

A comparative evaluation of three different cell-disruption methods for the release of hydrogenase from H2 -producing bacterium E. harbinenase YUAN-3T was investigated. The cell disruption techniques evaluated in this study were uhrasonieation, high-speed homogenization and bead milling. Ultrasonication process was found to be the most effective method in terms of cell disruption. As for the specific activity of hydrogenase, there is no significant difference among the three kinds of methods. An orthogonal experiment L9 （34） was designed to optimize the procedures of ultrasonication for cell disruption. The optimized uhrasonication disruption conditions were the treatment at 250 W, 20 kHz, 30 s/15 s and 0. 30 g bacteria cell （dry weight） in 15 mL suspension buffer. As a result, the optimized conditions allow the hydrogenase to maintain the active form with the yield of 93.95 mg protein/g cell and the final activity of 0. 252 μmol/min/mg protein. In this work, we have developed and optimized an ultrasonication protocol for YUAN-3T cel]s, which is adapted to laboratory- scale release of hydrogenase proteins.

关键词： hydrogenase E. harbinenase high-speed homogenization batch-mode bead milling uhrasonicatinn

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ISOLATION, PURIFICATION AND CHARACTERIZATION OF THE HYDROGEN EVOLUTION PROMOTING FACTOR OF hydrogenase OF SPIRULINA PLATENSIS

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Chinese Journal of Oceanology and Limnology 1996年第1期14卷 27-30页

作者：顾天青张惠苗孙世华 Institute of Botany Chinese Academy of Sciences Beijing

A component （s-factor） with obvious promoting effect on hydrogen evolution of hydrogenase has beenisolated and extracted from a Cell=free preparation of Spirulina *** effect of the s-factor in the re-action system is similar to that of Na2S2O4, but is coupled with ligh. The s-factor has the maximumabsorption peak at 620 nm in the oxidized state, at 590 nm in the reduced state. The partially purifieds-factor showed two bands by SDS-PAGE and is distinctly different from phycocyanin,which has nochange of oxidized state and reduced state absorption spectra, and also has no promoting effect onhydrogenase of Spirulina platensis under the light.

关键词： Spirulina platensis cyanobacteria hydrogen evolution hydrogenase s-factor

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Proton production and transfer mechanism in [NiFe] hydrogenase

Proton production and transfer mechanism in [NiFe] hydrogena...

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第十一届全国化学生物学学术会议

作者： Hulin Tai Shun Hirota MOE Key Laboratory of Natural Resources of the Changbai Mountain and Functional Molecules Department of ChemistryYanbian University Division of Materials Science Graduate School of Science and TechnologyNara Institute of Science and Technology

Owing to its reversible H2 oxidation reaction, hydrogenase（H2 ase） is one of the most highly studied enzymes, with promising applications in future energy technologies. The most well-studied H2 ase is the [NiFe] H2 ase. Knowledge of the catalytic cycle of this enzyme has increased;however, its proton transfer pathway is still under debate.[1] This uncertainty is due to the lack of useful methods to monitor protons during the conversion between the intermediates（Ni-SIa, Ni-R, Ni-C, and Ni-L states）[2] during the catalytic H2-oxidation cycle of [NiFe] H2 ase. In this study,[3] we observed the protonation of Cys546-SH and Glu34-COOH near the Ni–Fe site with high-sensitive IR difference spectra by utilizing Ni-C-to-Ni-L and Ni-C-to-Ni-SIa photoconversions. Protonated Cys546-SH in the Ni-L state was verified by the observed SH stretching frequency（2505 cm-1）, whereas Cys546 was deprotonated in the Ni-C and Ni-SIa states. Glu34-COOH was double H-bonded in the Ni-L state, as determined by the COOH stretching frequency（1700 cm-1）, and single H-bonded in the Ni-C and Ni-SIa states. Additionally, a stretching mode of an ordered water molecule was observed in the Ni-L and Ni-C states. These results show that the Ni–Fe site of [NiFe] H2 ase behaves as an optimized proton transfer system, and the direction of the proton transfer is regulated by the realignment of the H-bond network around Cys546, Glu34, and an ordered water molecule. These findings provide novel insights into the mechanism of the catalytic cycle of [NiFe] H2 ase.

关键词： Biocatalysis hydrogen hydrogenase IR spectroscopy proton transfer

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浮动海上有机农场——hydrogenase

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建筑技艺 2011年第1期17卷 221-223页

作者：杨永悦李昭君 Vincent Callebaut Architect

浮动有机农场hydrogenase外形看起来如同丝网编织的精美花边,是一个真正的净化站.位于4个碳回收塔内的绿色海藻将回收船舶带来的碳废物,可以直接用于这座"飞艇"形的有机农场的生物制氢,相当于传统飞机跑道边的加油站.

关键词：有机农场 hydrogenase 生物制氢

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Synthesis, structure and electrocatalytic H2-evoluting activity of a dinickel model complex related to the active site of [NiFe]-hydrogenases

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Chinese Chemical Letters 2020年第9期31卷 2483-2486页

作者： Dengmeng Song Xuyun Gao Bo Li Jun Li Xuzhuo Sun Chengbo Li Jiale Zhao Lin Chen Ning Wang Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education College of Chemistry&Materials ScienceNorthwest UniversityXi'an 710069China College of Chemistry Chemical and Environmental EngineeringHenan University of TechnologyZhengzhou 450001China State Key Laboratory of Environment-Friendly Energy Material Southwest University of Science and TechnologyMianyang 621010China

Structural and functional biomimicking of the active site of [NiFe]-hydrogenases can provide helpful hints for designing bioinspired catalysts to replace the expensive noble metal catalysts for H2 generation and *** of dianion [Ni(phma)]2-[H4 phma=N,N’-1,2-phenylenebis(2-mercaptoacetamide)] with [NiCl2(dppp)](dppp=bis(diphenylphosphino)propane) yielded a dinickel product[Ni(phma)(μ-S,S’)Ni(dppp)](1) as the model complex relevant to the active site of [NiFe]-H2 *** structure of complex 1 has been characterized by single-crystal X-ray *** cyclic voltammetry and controlled potential electrolysis studies,complex 1 was found to be a moderate electrocatalyst for the H2-evoluting reaction using ClCH2COOH as the proton source.

关键词： hydrogenase Electrocatalysis Hydrogen evolution Nickel complex Metallothiolate ligand

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