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用于水氧化的仿生三核铜催化剂
作者:小柯机器人 发布时间:2021/11/20 21:50:26

清华大学章名田团队开发了用于水氧化的仿生三核铜催化剂,周转频率高达20000s–1相关研究成果发表在2021年11月18日出版的《美国化学会杂志》。

太阳能分解水是一种理想的反应,可以构建一个人工光合系统来生产太阳能燃料。自然光系统II是研究人工太阳能转换的原型模板,它将水氧化成分子氧,并为燃料提供四个电子。尽管已经开发了一系列合成分子水氧化催化剂,但对该多电子多质子催化过程中O–O键形成的理解有限,因此水氧化仍然是一个巨大的挑战。

该文中,研究人员报告了一个三核铜簇,它在催化水氧化方面表现出优异的反应性,这是由多铜氧化酶(MCO)激发的,它能有效地催化O2的四电子还原为水。该合成模拟物在碳酸氢钠溶液中的周转频率为20000 s–1,分别比单核铜催化剂(F–N2O2Cu,131.6 s–1)和双核铜配合物(HappCu2,1375 s–1)高150倍和15倍。

研究工作表明,多种金属之间的协同作用是调节水氧化催化中O–O键形成的有效策略。

附:英文原文

Title: Bioinspired Trinuclear Copper Catalyst for Water Oxidation with a Turnover Frequency up to 20000 s–1

Author: Qi-Fa Chen, Ze-Yu Cheng, Rong-Zhen Liao, Ming-Tian Zhang

Issue&Volume: November 18, 2021

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.

DOI: 10.1021/jacs.1c08078

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期刊信息

JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000