Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species

	Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species
	Wang, Ning 1,2; Wang, Mei 1; Wang, Ying 3; Zheng, Dehua 1; Han, Hongxian 4; Ahlquist, Marten S. G.3; Sun, Licheng 1,5
刊名	journal of the american chemical society
	2013-09-18
卷号	135 期号:37 页码:13688-13691
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.
WOS标题词	science & technology ; physical sciences
类目[WOS]	chemistry, multidisciplinary
研究领域[WOS]	chemistry
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
收录类别	SCI
语种	英语
WOS记录号	WOS:000330163000020
公开日期	2015-11-10
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/137882]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
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
推荐引用方式 GB/T 7714	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.
APA	Wang, Ning.,Wang, Mei.,Wang, Ying.,Zheng, Dehua.,Han, Hongxian.,...&Sun, Licheng.(2013).Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species.journal of the american chemical society,135(37),13688-13691.
MLA	Wang, Ning,et al."Catalytic Activation of H-2 under Mild Conditions by an [FeFe]-Hydrogenase Model via an Active mu-Hydride Species".journal of the american chemical society 135.37(2013):13688-13691.