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Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation.

Yanyan ZhaoKe R YangZechao WangXingxu YanSufeng CaoYifan YeQi DongXizi ZhangJames E ThorneLei JinKelly L MaternaAntonios TrimpalisHongye BaiSirine C FakraXiaoyan ZhongPeng WangXiaoqing PanJinghua GuoMaria Flytzani-StephanopoulosGary W BrudvigVictor S BatistaDunwei Wang
Published in: Proceedings of the National Academy of Sciences of the United States of America (2018)
Atomically dispersed catalysts refer to substrate-supported heterogeneous catalysts featuring one or a few active metal atoms that are separated from one another. They represent an important class of materials ranging from single-atom catalysts (SACs) and nanoparticles (NPs). While SACs and NPs have been extensively reported, catalysts featuring a few atoms with well-defined structures are poorly studied. The difficulty in synthesizing such structures has been a critical challenge. Here we report a facile photochemical method that produces catalytic centers consisting of two Ir metal cations, bridged by O and stably bound to a support. Direct evidence unambiguously supporting the dinuclear nature of the catalysts anchored on α-Fe2O3 is obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM). Experimental and computational results further reveal that the threefold hollow binding sites on the OH-terminated surface of α-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.
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