1. Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s–1
- Author
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Ming-Tian Zhang, Rong-Zhen Liao, Qi-Fa Chen, and Ze-Yu Cheng
- Subjects
Photosystem II ,Chemistry ,chemistry.chemical_element ,General Chemistry ,Photosynthesis ,Biochemistry ,Copper ,Catalysis ,Colloid and Surface Chemistry ,Chemical engineering ,Oxidizing agent ,Cluster (physics) ,Water splitting ,Reactivity (chemistry) - Abstract
Solar-powered water splitting is a dream reaction for constructing an artificial photosynthetic system for producing solar fuels. Natural photosystem II is a prototype template for research on artificial solar energy conversion by oxidizing water into molecular oxygen and supplying four electrons for fuel production. Although a range of synthetic molecular water oxidation catalysts have been developed, the understanding of O-O bond formation in this multielectron and multiproton catalytic process is limited, and thus water oxidation is still a big challenge. Herein, we report a trinuclear copper cluster that displays outstanding reactivity toward catalytic water oxidation inspired by multicopper oxidases (MCOs), which provides efficient catalytic four-electron reduction of O2 to water. This synthetic mimic exhibits a turnover frequency of 20000 s-1 in sodium bicarbonate solution, which is about 150 and 15 times higher than that of the mononuclear Cu catalyst (F-N2O2Cu, 131.6 s-1) and binuclear Cu2 complex (HappCu2, 1375 s-1), respectively. This work shows that the cooperation between multiple metals is an effective strategy to regulate the formation of O-O bond in water oxidation catalysis.
- Published
- 2021
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