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Identification of the Active-Layer Structures for Acidic Oxygen Evolution from 9R-BaIrO3 Electrocatalyst with Enhanced Iridium Mass Activity.
Li, Na; Cai, Liang; Wang, Chao; Lin, Yue; Huang, Jinzhen; Sheng, Hongyuan; Pan, Haibin; Zhang, Wei; Ji, Qianqian; Duan, Hengli; Hu, Wei; Zhang, Wenhua; Hu, Fengchun; Tan, Hao; Sun, Zhihu; Song, Bo; Jin, Song; Yan, Wensheng.
  • Li N; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Cai L; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Wang C; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Lin Y; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Huang J; Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Sheng H; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Pan H; Center for Composite Materials and Structures, Harbin Institute of Technology, Harbin 150001, P.R. China.
  • Zhang W; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Ji Q; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Duan H; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Hu W; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Zhang W; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Hu F; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Tan H; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Sun Z; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Song B; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Jin S; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, P.R. China.
  • Yan W; Center for Composite Materials and Structures, Harbin Institute of Technology, Harbin 150001, P.R. China.
J Am Chem Soc ; 143(43): 18001-18009, 2021 11 03.
Article en En | MEDLINE | ID: mdl-34694127
ABSTRACT
Iridium-based perovskites show promising catalytic activity for oxygen evolution reaction (OER) in acid media, but the iridium mass activity remains low and the active-layer structures have not been identified. Here, we report highly active 1 nm IrOx particles anchored on 9R-BaIrO3 (IrOx/9R-BaIrO3) that are directly synthesized by solution calcination followed by strong acid treatment for the first time. The developed IrOx/9R-BaIrO3 catalyst delivers a high iridium mass activity (168 A gIr-1), about 16 times higher than that of the benchmark acidic OER electrocatalyst IrO2 (10 A gIr-1), and only requires a low overpotential of 230 mV to reach a catalytic current density of 10 mA cm-2geo. Careful scanning transmission electron microscopy, synchrotron radiation-based X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy analyses reveal that, during the electrocatalytic process, the initial 1 nm IrOx nanoparticles/9R-BaIrO3 evolve into amorphous Ir4+OxHy/IrO6 octahedrons and then to amorphous Ir5+Ox/IrO6 octahedrons on the surface. Such high relative content of amorphous Ir5+Ox species derived from trimers of face-sharing IrO6 octahedrons in 9R-BaIrO3 and the enhanced metallic conductivity of the Ir5+Ox/9R-BaIrO3 catalyst are responsible for the excellent acidic OER activity. Our results provide new insights into the surface active-layer structure evolution in perovskite electrocatalysts and demonstrate new approaches for engineering highly active acidic OER nanocatalysts.

Texto completo: 1 Banco de datos: MEDLINE Tipo de estudio: Diagnostic_studies Idioma: En Año: 2021 Tipo del documento: Article

Texto completo: 1 Banco de datos: MEDLINE Tipo de estudio: Diagnostic_studies Idioma: En Año: 2021 Tipo del documento: Article