Dual Electron Uptake by Simultaneous Iron and Ligand Reduction in an N-Heterocyclic Carbene Substituted [FeFe] Hydrogenase Model Compound
- 2 July 2005
- journal article
- Published by American Chemical Society (ACS) in Inorganic Chemistry
- Vol. 44 (16), 5550-5552
- https://doi.org/10.1021/ic050402d
Abstract
An N-heterocyclic carbene containing [FeFe]H(2)ase model complex, whose X-ray structure displays an apical carbene, shows an unexpected two-electron reduction to be involved in its electrocatalytic dihydrogen production. Density functional calculations show, in addition to a one-electron Fe-Fe reduction, that the aryl-substituted N-heterocyclic carbene can accept a second electron more readily than the Fe-Fe manifold. The juxtaposition of these two one-electron reductions resembles the [FeFe]H(2)ase active site with an FeFe di-iron unit joined to the electroactive 4Fe4S cluster.Keywords
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