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.

中文翻译：

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用于水氧化的仿生三核铜催化剂，周转频率高达 20000 s–1

太阳能水分解是构建用于生产太阳能燃料的人工光合系统的理想反应。自然光系统 II 是通过将水氧化成分子氧并提供四个电子用于燃料生产的人工太阳能转换研究的原型模板。尽管已经开发了一系列合成分子水氧化催化剂，但对这种多电子和多质子催化过程中 O-O 键形成的理解有限，因此水氧化仍然是一个很大的挑战。_{在此，我们报告了一种受多铜氧化酶 (MCO) 启发而对催化水氧化表现出出色反应性的三核铜簇，它提供了有效的 O 2}催化四电子还原浇水。该合成模拟物在碳酸氢钠溶液中的周转频率为 20000 s ^{–1 ，比单核 Cu 催化剂（F–N} ₂ O ₂ Cu，131.6 s ^–1）和双核 Cu ₂高约 150 和 15 倍络合物（HappCu ₂ , 1375 s ^–1）。这项工作表明，多种金属之间的合作是调节水氧化催化中O-O键形成的有效策略。