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Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation
- Zhao, Yanyan;
- Yang, Ke R;
- Wang, Zechao;
- Yan, Xingxu;
- Cao, Sufeng;
- Ye, Yifan;
- Dong, Qi;
- Zhang, Xizi;
- Thorne, James E;
- Jin, Lei;
- Materna, Kelly L;
- Trimpalis, Antonios;
- Bai, Hongye;
- Fakra, Sirine C;
- Zhong, Xiaoyan;
- Wang, Peng;
- Pan, Xiaoqing;
- Guo, Jinghua;
- Flytzani-Stephanopoulos, Maria;
- Brudvig, Gary W;
- Batista, Victor S;
- Wang, Dunwei
- et al.
Published Web Location
https://doi.org/10.1073/pnas.1722137115Abstract
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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