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题名: Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species
作者: Wang, Ning1, 2;  Wang, Mei1;  Wang, Ying3;  Zheng, Dehua1;  Han, Hongxian4;  Ahlquist, Marten S. G.3;  Sun, Licheng1, 5
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2013-09-18
DOI: 10.1021/ja408376t
卷: 135, 期:37, 页:13688-13691
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: A [FeFe]-hydrogenase model (1) containing a chelating diphosphine ligand with a pendant amine was readily oxidized by Fc(+) (Fc = Cp2Fe) to a (FeFeI)-Fe-II complex ([1](+)), which was isolated at room temperature. The structure of [1](+) with a semibridging CO and a vacant apical site was determined by X-ray crystallography. Complex [1](+) catalytically activates H-2 at 1 atm at 25 C in the presence of excess Fc(+) and P(o-tol)(3). More interestingly, the catalytic activity of [1](+) for H-2 oxidation remains unchanged in the presence of ca. 2% CO. A computational study of the reaction mechanism showed that the most favorable activation free energy involves a rotation of the bridging CO to an apical position followed by activation of H-2 with the help of the internal amine to give a bridging hydride intermediate.
关键词[WOS]: FE-ONLY HYDROGENASE ;  H-OX STATE ;  DESULFOVIBRIO-DESULFURICANS ;  IRON HYDROGENASE ;  FUNCTIONAL MODELS ;  PROTON TRANSFERS ;  DIIRON COMPLEX ;  PENDANT AMINE ;  MIXED-VALENT ;  SITE
语种: 英语
WOS记录号: WOS:000330163000020
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/137882
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.DUT, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116024, Peoples R China
2.Henan Univ Technol, Sch Chem & Chem Engn, Zhengzhou 450001, Peoples R China
3.KTH Royal Inst Technol, Sch Biotechnol, SE-10691 Stockholm, Sweden
4.Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
5.KTH Royal Inst Technol, Dept Chem, SE-10044 Stockholm, Sweden

Recommended Citation:
Wang, Ning,Wang, Mei,Wang, Ying,et al. Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2013,135(37):13688-13691.
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