Improved Electrocatalytic Activity and Stability by Single Iridium Atoms on Iron-based Layered Double Hydroxides for Oxygen Evolution

Jing Cao; Tong Mou; Bingbao Mei; Pengfei Yao; Ce Han; Xue Gong; Ping Song; Zheng Jiang; Thomas Frauenheim; Jianping Xiao; Weilin Xu

doi:10.1002/anie.202310973

Improved Electrocatalytic Activity and Stability by Single Iridium Atoms on Iron-based Layered Double Hydroxides for Oxygen Evolution

Angew Chem Int Ed Engl. 2023 Oct 23;62(43):e202310973. doi: 10.1002/anie.202310973. Epub 2023 Sep 15.

Authors

Jing Cao^{1

2}, Tong Mou^{3

4}, Bingbao Mei⁵, Pengfei Yao^{1

2}, Ce Han^{1

2}, Xue Gong^{1

2}, Ping Song^{1

2}, Zheng Jiang⁶, Thomas Frauenheim^{7

8

4}, Jianping Xiao^{3

4}, Weilin Xu^{1

2}

Affiliations

¹ State Key Laboratory of Electroanalytical Chemistry and Jilin Province Key Laboratory of Low Carbon Chemical Power, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, P. R. China.
² University of Science and Technology of China, Anhui, 230026, China.
³ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, Dalian, 116023, P. R. China.
⁴ Beijing Computational Science Research Center, Beijing, 100193, P. R. China.
⁵ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201800, P. R. China.
⁶ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China.
⁷ Shenzhen JL Computational and Applied Research Institute, Shenzhen, 518131, P. R. China.
⁸ Bremen Center for Computational Materials Science, University of Bremen, 28359, Bremen, Germany.

PMID: 37667678
DOI: 10.1002/anie.202310973

Abstract

Full understanding to the origin of the catalytic performance of a supported nanocatalyst from the points of view of both the active component and support is significant for the achievement of high performance. Herein, based on a model electrocatalyst of single-iridium-atom-doped iron (Fe)-based layered double hydroxides (LDH) for oxygen evolution reaction (OER), we reveal the first completed origin of the catalytic performance of such supported nanocatalysts. Specially, besides the activity enhancement of Ir sites by LDH support, the stability of surface Fe sites is enhanced by doped Ir sites: DFT calculation shows that the Ir sites can reduce the activity and enhance the stability of the nearby Fe sites; while further finite element simulations indicate, the stability enhancement of distant Fe sites could be attributed to the much low concentration of OER reactant (hydroxyl ions, OH^- ) around them induced by the much fast consumption of OH^- on highly active Ir sites. These new findings about the interaction between the main active components and supports are applicable in principle to other heterogeneous nanocatalysts and provide a completed understanding to the catalytic performance of heterogeneous nanocatalysts.

Keywords: Activity; Fe Based on LDH; OER; Single Atom Iridium Catalysts; Stability.

Abstract

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