Organic dyes and molecular catalysts co-adsorbed on a metal oxide substrate are widely employed for water-splitting photoelectrodes. In this manuscript, we employ first-principles calculations to investigate interactions between a coumarin dye and a molecular catalyst on the nickel oxide substrate in an experimentally verified water-splitting photocathode. The nanoscopic interfacial structures and interfacial charge transfer properties of dye/catalyst/metal oxide hybrid systems in the water-splitting photocathode are elucidated. In particular, the intermolecular hydrogen bond and the substrate-to-catalyst electron transfer stabilize the interfacial structure. The present study helps the fundamental understanding of water-splitting photoelectrodes co-adsorbed with organic dyes and molecular catalysts.

中文翻译：

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水分解系统中染料-催化剂的相互作用：基于香豆素343/[FeFe](mcbdt)(CO)6/NiO的界面结构第一性原理研究

共吸附在金属氧化物基材上的有机染料和分子催化剂被广泛用于水分解光电极。在这份手稿中，我们采用第一性原理计算来研究香豆素染料与经过实验验证的水分解光电阴极中氧化镍基材上的分子催化剂之间的相互作用。阐明了水分解光电阴极中染料/催化剂/金属氧化物杂化体系的纳米级界面结构和界面电荷转移特性。特别是，分子间氢键和底物到催化剂的电子转移稳定了界面结构。本研究有助于对与有机染料和分子催化剂共吸附的水分解光电极的基本理解。