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Homogeneous Photocatalytic Water Oxidation with a Dinuclear CoIII-Pyridylmethylamine Complex

Title
Homogeneous Photocatalytic Water Oxidation with a Dinuclear CoIII-Pyridylmethylamine Complex
Authors
Ishizuka T.Watanabe A.Kotani H.Hong D.Satonaka K.Wada T.Shiota Y.Yoshizawa K.Ohara K.Yamaguchi K.Kato S.Fukuzumi S.Kojima T.
Ewha Authors
Shunichi Fukuzumi
SCOPUS Author ID
Shunichi Fukuzumiscopus
Issue Date
2016
Journal Title
Inorganic Chemistry
ISSN
0020-1669JCR Link
Citation
vol. 55, no. 3, pp. 1154 - 1164
Publisher
American Chemical Society
Indexed
SCI; SCIE; SCOPUS WOS scopus
Abstract
A bis-hydroxo-bridged dinuclear CoIII-pyridylmethylamine complex (1) was synthesized and the crystal structure was determined by X-ray crystallography. Complex 1 acts as a homogeneous catalyst for visible-light-driven water oxidation by persulfate (S2O82-) as an oxidant with [RuII(bpy)3]2+ (bpy = 2,2′-bipyridine) as a photosensitizer affording a high quantum yield (44%) with a large turnover number (TON = 742) for O2 formation without forming catalytically active Co-oxide (CoOx) nanoparticles. In the water-oxidation process, complex 1 undergoes proton-coupled electron-transfer (PCET) oxidation as a rate-determining step to form a putative dinuclear bis-μ-oxyl CoIII complex (2), which has been suggested by DFT calculations. Catalytic water oxidation by 1 using [RuIII(bpy)3]3+ as an oxidant in a H216O and H218O mixture was examined to reveal an intramolecular O-O bond formation in the two-electron-oxidized bis-μ-oxyl intermediate, prior to the O2 evolution. © 2016 American Chemical Society.
DOI
10.1021/acs.inorgchem.5b02336
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자연과학대학 > 화학·나노과학전공 > Journal papers
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