A Functional Model of [Fe]-Hydrogenase
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- 作者：Tao Xu ; Chih-Juo Madeline Yin ; Matthew D. Wodrich ; Simona Mazza ; Katherine M. Schultz ; Rosario Scopelliti ; Xile Hu
- 刊名：Journal of the American Chemical Society
- 出版年：2016
- 出版时间：March 16, 2016
- 年：2016
- 卷：138
- 期：10
- 页码：3270-3273
- 全文大小：362K
- ISSN：1520-5126
文摘
[Fe]-Hydrogenase catalyzes the hydrogenation of a biological substrate via the heterolytic splitting of molecular hydrogen. While many synthetic models of [Fe]-hydrogenase have been prepared, none yet are capable of activating H2 on their own. Here, we report the first Fe-based functional mimic of the active site of [Fe]-hydrogenase, which was developed based on a mechanistic understanding. The activity of this iron model complex is enabled by its unique ligand environment, consisting of biomimetic pyridinylacyl and carbonyl ligands, as well as a bioinspired diphosphine ligand with a pendant amine moiety. The model complex activates H2 and mediates hydrogenation of an aldehyde.