Dual Electron Uptake by Simultaneous Iron and Ligand Reduction in an N-Heterocyclic Carbene Substituted [FeFe] Hydrogenase Model Compound
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- 作者：Jesse W. Tye ; Jonghyuk Lee ; Hsiao-Wan Wang ; Rosario Mejia-Rodriguez ; Joseph H. Reibenspies ; Michael B. Hall ; and Marcetta Y. Darensbourg
- 刊名：Inorganic Chemistry
- 出版年：2005
- 出版时间：August 8, 2005
- 年：2005
- 卷：44
- 期：16
- 页码：5550 - 5552
- 全文大小：82K
- 年卷期：v.44,no.16(August 8, 2005)
- ISSN：1520-510X
文摘
An N-heterocyclic carbene containing [FeFe]H2ase model complex,whose X-ray structure displays an apical carbene, shows anunexpected two-electron reduction to be involved in its electrocatalytic dihydrogen production. Density functional calculationsshow, in addition to a one-electron Fe-Fe reduction, that the aryl-substituted N-heterocyclic carbene can accept a second electronmore readily than the Fe-Fe manifold. The juxtaposition of thesetwo one-electron reductions resembles the [FeFe]H2ase active sitewith an FeFe di-iron unit joined to the electroactive 4Fe4S cluster.