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Spectroscopic Detection of Key Intermediates and Turnover Process in Catalytic H2 Formation by a Biomimetic Diiron Catalyst
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.ORCID iD: 0000-0001-7919-2444
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
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Abstract [en]

FeFe(Cl2-bdt)(CO)2 (1) (Cl2-bdt = dichlorobenzene-1,2-dthiolate), inspired by the active site of FeFe-hydrogenase, shows achemically reversible 2e- reduction at -1.20 V VS. Fc+/Fc. From thiscompound, the rigid and unsaturated bdt-bridging ligand lowers thereduction potential and stabilizes the reduced forms, allowing us tocharacterize the overall catalytic process. Herein, we provide theexact structural information on the key catalytic intermediates such as1H- that is not identified experimentally. In addition, we first report thespectroscopic evidence of turnover process of H2 formation catalysedby complex 1, and provide the straightforward determination ofturnover frequency (TOF).

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Physical Chemistry
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Physical Chemistry
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URN: urn:nbn:se:uu:diva-364111OAI: oai:DiVA.org:uu-364111DiVA, id: diva2:1258110
Available from: 2018-10-24 Created: 2018-10-24 Last updated: 2018-11-07Bibliographically approved
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Wang, ShihuaiLiu, TianfeiOtt, SaschaLomoth, ReinerHammarström, Leif

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