Catalytic Water Oxidation by Ruthenium(II) Quaterpyridine (qpy) Complexes: Evidence for Ruthenium(III) qpy‐N,N′′′‐dioxide as the Real Catalysts |
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| Authors: | Yingying Liu Dr Siu‐Mui Ng Dr Shek‐Man Yiu Dr William W Y Lam Xi‐Guang Wei Dr Kai‐Chung Lau Prof Tai‐Chu Lau |
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| Institution: | 1. Department of Biology and Chemistry;2. Institute of Molecular Functional Materials, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong (China) |
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| Abstract: | Polypyridyl and related ligands have been widely used for the development of water oxidation catalysts. Supposedly these ligands are oxidation‐resistant and can stabilize high‐oxidation‐state intermediates. In this work a series of ruthenium(II) complexes Ru(qpy)(L)2]2+ (qpy=2,2′:6′,2′′:6′′,2′′′‐quaterpyridine; L=substituted pyridine) have been synthesized and found to catalyze CeIV‐driven water oxidation, with turnover numbers of up to 2100. However, these ruthenium complexes are found to function only as precatalysts; first, they have to be oxidized to the qpy‐N,N′′′‐dioxide (ONNO) complexes Ru(ONNO)(L)2]3+ which are the real catalysts for water oxidation. |
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| Keywords: | density functional calculations homogeneous catalysis polypyridyl ligands ruthenium complexes water oxidation |
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