Bioinspired Artificial [FeFe]-Hydrogenase with a Synthetic H-Cluster 机翻标题: 暂无翻译,请尝试点击翻译按钮。

来源
ACS catalysis
年/卷/期
2019 / 9 / 5
页码
4495-4501
ISSN号
2155-5435
作者单位
Sorbonne Univ, CNRS, Coll France, Lab Chim Proc Biol,UMR 8229, 11 Pl Marcelin Berthelot, F-75231 Paris 05, France;Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany;Sorbonne Univ, CNRS, Coll France, Lab Chim Proc Biol,UMR 8229, 11 Pl Marcelin Berthelot, F-75231 Paris 05, France;Univ Grenoble Alpes, Lab Chim & Biol Metaux, CEA, CNRS,Fundamental Res Div, 17 Rue Martyrs, F-38054 Grenoble 9, France;Univ Grenoble Alpes, Lab Chim & Biol Metaux, CEA, CNRS,Fundamental Res Div, 17 Rue Martyrs, F-38054 Grenoble 9, France;Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany;Ruhr Univ Bochum, Inorgan Chem 1, Univ Str 150, D-44780 Bochum, Germany;Univ Grenoble Alpes, Lab Chim & Biol Metaux, CEA, CNRS,Fundamental Res Div, 17 Rue Martyrs, F-38054 Grenoble 9, France;Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany;Sorbonne Univ, CNRS, Coll France, Lab Chim Proc Biol,UMR 8229, 11 Pl Marcelin Berthelot, F-75231 Paris 05, France;
作者
Papini, Cecilia;Sommer, Constanze;Pecqueur, Ludovic;Pramanik, Debajyoti;Roy, Souvik;Reijerse, Edward J.;Wittkamp, Florian;Artero, Vincent;Lubitz, Wolfgang;Fontecave, Marc;
摘要
[FeFe]-hydrogenases are powerful hydrogen evolution biocatalysts because of the activity of their unique metallocofactor, the H-cluster, derived from the association of a [4Fe-4S] cluster and a [2Fe]-subcluster, containing 2 CO and 2 CN- ligands as well as an aza-propanedithiolate (adt(2-)) ligand bridging the two Fe atoms. Various analogues of the H-cluster have been assembled in the iron-sulfur protein HydF, containing a [4Fe-4S] cluster, by reaction with a series of synthetic di-iron complexes mimicking the [2Fe]-subcluster of hydrogenases. The mimics contain a mixture of CO and CN- ligands and various dichalcogenide (S or Se) bridging ligands. The resulting hybrid proteins have been characterized and shown to behave as active artificial hydrogenases. On the basis of the present structure-activity relationship study, we report that the most active and stable artificial hydrogenase was obtained with the mimic containing a propane diselenol bridging ligand. This opens the possibility to developing a class of hydrogen-evolving enzymes with a synthetic active site mimicking that of the natural hydrogenase.
机翻摘要
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关键词/主题词
hydrogenase;iron-sulfur cluster;selenium;artificial enzyme;hydrogen production;
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