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Sulfur Coordination Effects on the Stability and Activity of a Ruthenium-Based Water Oxidation Catalyst
Southern Univ Sci & Technol SUSTech, Dept Chem, Shenzhen 518055, Peoples R China;Southern Univ Sci & Technol SUSTech, Shenzhen Grubbs Inst, Shenzhen 518055, Peoples R China.
Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
Guangzhou Univ, Dept Chem & Chem Engn, Guangzhou 510006, Guangdong, Peoples R China.
Southern Univ Sci & Technol SUSTech, Dept Chem, Shenzhen 518055, Peoples R China;Southern Univ Sci & Technol SUSTech, Shenzhen Grubbs Inst, Shenzhen 518055, Peoples R China.
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2019 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 58, no 5, p. 3137-3144Article in journal (Refereed) Published
Abstract [en]

Water oxidation is regarded as the bottleneck of the water splitting and the development of water oxidation catalysts is of importance in the view of reducing reaction barriers and promoting water oxidation efficiency. Recently, the Sun group has disclosed a family of highly active water oxidation catalysts, [Ru(bda)(L)(2)] (bda(2) = 2,2'-bipyridine-6,6'-dicarboxylate; L = N-containing ligands). Herein, we replaced the bda(2) ligand with a 2,2'-bipyridine-6,6'-dicarbothioate (bct(2)) ligand and prepared a mononuclear ruthenium complex [Ru(bct)(pic)(2)] (Ru-bct, pic = 4-picoline). Less equatorial ligand distortion is observed for Ru-II-bct which displays improved stability than Ru-II-bda. The Ru-bct complex undergoes chemicalstructural evolution during electrochemical and chemical oxidation, generating Ru-bda as the intrinsic active species to afford water oxidation. This study provides an example to understand structurestabilityreactivity relationship of molecular water oxidation catalysts.

Place, publisher, year, edition, pages
2019. Vol. 58, no 5, p. 3137-3144
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Inorganic Chemistry
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URN: urn:nbn:se:uu:diva-380466DOI: 10.1021/acs.inorgchem.8b03199ISI: 000460600300027PubMedID: 30785733OAI: oai:DiVA.org:uu-380466DiVA, id: diva2:1299697
Available from: 2019-03-28 Created: 2019-03-28 Last updated: 2019-03-28Bibliographically approved

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