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首页> 外文期刊>Chemical Society Reviews >O-O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O-O radical coupling
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O-O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O-O radical coupling

机译:钌催化水氧化中的O-O键形成:单点亲核攻击与O-O激进耦合

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摘要

In this review we discuss at the mechanistic level the different steps involved in water oxidation catalysis with ruthenium-based molecular catalysts. We have chosen to focus on ruthenium-based catalysts to provide a more coherent discussion and because of the availability of detailed mechanistic studies for these systems but many of the aspects presented in this review are applicable to other systems as well. The water oxidation cycle has been divided in four major steps: water oxidative activation, O-O bond formation, oxidative activation of peroxide intermediates, and O-2 evolution. A significant portion of the review is dedicated to the O-O bond formation step as the key step in water oxidation catalysis. The two main pathways to accomplish this step, single-site water nucleophilic attack and O-O radical coupling, are discussed in detail and compared in terms of their potential use in photoelectrochemical cells for solar fuels generation.
机译:在本次综述中,我们在机械水平上讨论了与钌的分子催化剂的水氧化催化剂中所涉及的不同步骤。 我们选择专注于基于钌的催化剂,以提供更加连贯的讨论,并且由于这种系统的详细机制研究的可用性,但本综述中提供的许多方面也适用于其他系统。 水氧化循环已分为四个主要步骤:水氧化活化,O-O键形成,过氧化物中间体的氧化活化和O-2进化。 作为水氧化催化的关键步骤,审查的一部分综述是专用于O-O键形成步骤。 为了实现该步骤,单站点水亲核攻击和O-O激进耦合的两个主要途径,并在其在光电化学电池中用于太阳能燃料产生的潜在使用比较。

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