Homogeneous Photocatalytic Water Oxidation with a Dinuclear CoIII-Pyridylmethylamine Complex

Tomoya Ishizuka, Atsuko Watanabe, Hiroaki Kotani, Dachao Hong, Kenta Satonaka, Tohru Wada, Yoshihito Shiota, Kazunari Yoshizawa, Kazuaki Ohara, Kentaro Yamaguchi, Satoshi Kato, Shunichi Fukuzumi, Takahiko Kojima

研究成果: Contribution to journalArticle

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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.

ジャーナルInorganic chemistry
出版物ステータス出版済み - 2 1 2016

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

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    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. (2016). Homogeneous Photocatalytic Water Oxidation with a Dinuclear CoIII-Pyridylmethylamine Complex. Inorganic chemistry, 55(3), 1154-1164. https://doi.org/10.1021/acs.inorgchem.5b02336