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用于水相介质中高效水氧化的铁配合物基催化体系。

Iron-complex-based catalytic system for high-performance water oxidation in aqueous media.

作者信息

Matsuzaki Takumi, Kosugi Kento, Iwami Hikaru, Kambe Tetsuya, Kiuchi Hisao, Harada Yoshihisa, Asakura Daisuke, Uematsu Taro, Kuwabata Susumu, Saga Yutaka, Kondo Mio, Masaoka Shigeyuki

机构信息

Division of Applied Chemistry, Graduate School of Engineering, Osaka University, Suita, Osaka, Japan.

Department of Chemistry, School of Science, Institute of Science Tokyo, Tokyo, Japan.

出版信息

Nat Commun. 2025 Mar 5;16(1):2145. doi: 10.1038/s41467-025-57169-y.

Abstract

Water oxidation is the key reaction in natural and artificial photosyntheses but is kinetically and thermodynamically sluggish. Extensive efforts have been made to develop artificial systems comparable to the natural system. However, constructing a molecular system based on ubiquitous metal ions with high performance in aqueous media similar to a natural system, remains challenging. In this study, inspired by nature, we successfully achieve highly efficient water oxidation in aqueous media. By electrochemical polymerisation of a pentanuclear iron complex bearing carbazole moieties, we successfully integrate two essential features of the natural system: catalytic centre composed of ubiquitous metal ions and charge transporting site. The resulting material catalyses water oxidation with a Faradaic efficiency of up to 99% in aqueous media. Our results provide a strategy to develop catalytic systems for water oxidation.

摘要

水氧化是自然光合作用和人工光合作用中的关键反应,但在动力学和热力学上都较为缓慢。人们已经做出了广泛的努力来开发与自然系统相当的人工系统。然而,构建一个基于普遍存在的金属离子、在水性介质中具有与自然系统相似的高性能的分子系统仍然具有挑战性。在本研究中,受自然启发,我们在水性介质中成功实现了高效水氧化。通过对带有咔唑基团的五核铁配合物进行电化学聚合,我们成功整合了自然系统的两个基本特征:由普遍存在的金属离子组成的催化中心和电荷传输位点。所得材料在水性介质中催化水氧化的法拉第效率高达99%。我们的结果为开发水氧化催化系统提供了一种策略。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/98e6/11882805/ecc61dce780b/41467_2025_57169_Fig1_HTML.jpg

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