Structure and Reactivity of an Asymmetric Synthetic Mimic of Nitrogenase Cofactor |
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| Authors: | Dr. Kazuki Tanifuji Dr. Nathaniel Sickerman Dr. Chi Chung Lee Dr. Takayuki Nagasawa Dr. Kosuke Miyazaki Prof. Dr. Yasuhiro Ohki Prof. Dr. Kazuyuki Tatsumi Prof. Dr. Yilin Hu Prof. Dr. Markus W. Ribbe |
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| Affiliation: | 1. Department of Molecular Biology and Biochemistry, University of California, Irvine, Irvine, CA, USA;2. Department of Chemistry, Graduate School of Science and Research Center for Materials Science, Nagoya University, Nagoya, Japan;3. Department of Chemistry, University of California, Irvine, Irvine, CA, USA |
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| Abstract: | The Mo nitrogenase catalyzes the ambient reduction of N2 to NH3 at its M‐cluster site. A complex metallocofactor with a core composition of [MoFe7S9C], the M‐cluster, can be extracted from the protein scaffold and used to facilitate the catalytic reduction of CN?, CO, and CO2 into hydrocarbons in the isolated state. Herein, we report the synthesis, structure, and reactivity of an asymmetric M‐cluster analogue with a core composition of [MoFe5S9]. This analogue, referred to as the Mo‐cluster, is the first synthetic example of an M‐cluster mimic with Fe and Mo positioned at opposite ends of the cluster. Moreover, the ability of the Mo‐cluster to reduce C1 substrates to hydrocarbons suggests the feasibility of developing nitrogenase‐based biomimetic approaches to recycle C1 waste into fuel products. |
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| Keywords: | CO/CO2 reduction cofactors hydrocarbons molybdenum nitrogenases |
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