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- Title
Redox‐Active Ligand Assisted Catalytic Water Oxidation by a Ru<sup>IV</sup>=O Intermediate.
- Authors
Shi, Jing; Guo, Yu‐Hua; Xie, Fei; Chen, Qi‐Fa; Zhang, Ming‐Tian
- Abstract
Water splitting is one of the most promising solutions for storing solar energy in a chemical bond. Water oxidation is still the bottleneck step because of its inherent difficulty and the limited understanding of the O−O bond formation mechanism. Molecular catalysts provide a platform for understanding this process in depth and have received wide attention since the first Ru‐based catalyst was reported in 1982. RuV=O is considered a key intermediate to initiate the O−O bond formation through either a water nucleophilic attack (WNA) pathway or a bimolecular coupling (I2M) pathway. Herein, we report a Ru‐based catalyst that displays water oxidation reactivity with RuIV=(O) with the help of a redox‐active ligand at pH 7.0. The results of electrochemical studies and DFT calculations disclose that ligand oxidation could significantly improve the reactivity of RuIV=O toward water oxidation. Under these conditions, sustained water oxidation catalysis occurs at reasonable rates with low overpotential (ca. 183 mV).
- Subjects
OXIDATION of water; CATALYTIC oxidation; BOND formation mechanism; RUTHENIUM catalysts; CHEMICAL bonds; CHEMICAL energy; SOLAR energy
- Publication
Angewandte Chemie, 2020, Vol 132, Issue 10, p4029
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201910614