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자연과학대학
화학·나노과학전공
Journal papers
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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 Fukuzumi
Issue Date
2016
Journal Title
Inorganic Chemistry
ISSN
0020-1669
Citation
Inorganic Chemistry vol. 55, no. 3, pp. 1154 - 1164
Publisher
American Chemical Society
Indexed
SCIE; SCOPUS
Document Type
Article
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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