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

  • Author(s): 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.
Abstract

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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