Iwami Hikaru, Okamura Masaya, Kondo Mio, Masaoka Shigeyuki
Division of Applied Chemistry, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka, 565-0871, Japan.
Department of Life and Coordination-Complex Molecular Science, Institute for Molecular Science (IMS), 5-1 Higashiyama, Myodaiji, Okazaki, Aichi, 444-8787, Japan.
Angew Chem Int Ed Engl. 2021 Mar 8;60(11):5965-5969. doi: 10.1002/anie.202015174. Epub 2021 Feb 1.
Water oxidation is a key reaction in natural and artificial photosynthesis. In nature, the reaction is efficiently catalyzed by a metal-complex-based catalyst surrounded by hole-transporting amino acid residues. However, in artificial systems, there is no example of a water oxidation system that has a catalytic center surrounded by hole transporters. Herein, we present a facile strategy to integrate catalytic centers and hole transporters in one system. Electrochemical polymerization of a metal-complex-based precursor afforded a polymer-based material (Poly-1). Poly-1 exhibited excellent hole-transporting ability and catalyzed water oxidation with high performance. It was also revealed that the catalytic activity was almost completely suppressed in the absence of the hole-transporting moieties. The present study provides a novel strategy for constructing efficient molecule-based systems for water oxidation.
水氧化是自然光合作用和人工光合作用中的关键反应。在自然界中,该反应由被空穴传输氨基酸残基包围的金属络合物基催化剂有效催化。然而,在人工体系中,尚无催化中心被空穴传输体包围的水氧化体系的实例。在此,我们提出了一种在一个体系中整合催化中心和空穴传输体的简便策略。基于金属络合物的前体的电化学聚合得到了一种聚合物基材料(Poly-1)。Poly-1表现出优异的空穴传输能力,并能高效催化水氧化。研究还表明,在没有空穴传输部分的情况下,催化活性几乎完全被抑制。本研究为构建高效的基于分子的水氧化体系提供了一种新策略。