Ex Situ Reconstruction-Shaped Ir/CoO/Perovskite Heterojunction for Boosted Water Oxidation Reaction

Hongquan Guo; Yanling Yang; Guangming Yang; Xiaojuan Cao; Ning Yan; Zhishan Li; Emily Chen; Lina Tang; Meilan Peng; Lei Shi; Shunji Xie; Huabing Tao; Chao Xu; Yinlong Zhu; Xianzhu Fu; Yuanming Pan; Ning Chen; Jinru Lin; Xin Tu; Zongping Shao; Yifei Sun

doi:10.1021/acscatal.2c05684

Ex Situ Reconstruction-Shaped Ir/CoO/Perovskite Heterojunction for Boosted Water Oxidation Reaction

ACS Catal. 2023 Mar 29;13(7):5007-5019. doi: 10.1021/acscatal.2c05684. eCollection 2023 Apr 7.

Authors

Hongquan Guo¹, Yanling Yang¹, Guangming Yang², Xiaojuan Cao³, Ning Yan³, Zhishan Li¹, Emily Chen⁴, Lina Tang⁵, Meilan Peng¹, Lei Shi⁶, Shunji Xie^{7

8}, Huabing Tao^{7

8}, Chao Xu⁹, Yinlong Zhu¹⁰, Xianzhu Fu¹¹, Yuanming Pan¹², Ning Chen¹³, Jinru Lin¹⁴, Xin Tu⁹, Zongping Shao², Yifei Sun^{1

7

15}

Affiliations

¹ College of Energy, Xiamen University, Xiamen 361005, China.
² State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China.
³ School of Physics and Technology, Wuhan University, Wuhan 430072, China.
⁴ Monash Centre for Electron Microscopy, Monash University, Victoria 3800, Australia.
⁵ Key Laboratory of Low-grade Energy Utilization Technologies and Systems, MOE, Chongqing University, Chongqing 40030, China.
⁶ School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
⁷ State Key Laboratory of Physical Chemistry of Solid Surface, Xiamen University, Xiamen 361005, China.
⁸ College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
⁹ Department of Electrical Engineering and Electronics, University of Liverpool, Liverpool L69 3GJ, U.K.
¹⁰ Institute for Frontier Science, Nanjing University of Aeronautics and Astronautics, Nanjing 210001, China.
¹¹ Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China.
¹² Department of Geological Sciences, University of Saskatchewan, Saskatoon SK S7N 5E2, Canada.
¹³ Canadian Light Source, University of Saskatchewan, Saskatoon SK S7N 0X4, Canada.
¹⁴ Key Laboratory of Pollution Ecology and Environmental Engineering, Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang, Liaoning 110016, China.
¹⁵ Shenzhen Research Institute of Xiamen University, Shenzhen 518057, China.

Abstract

The oxygen evolution reaction (OER) is the performance-limiting step in the process of water splitting. In situ electrochemical conditioning could induce surface reconstruction of various OER electrocatalysts, forming reactive sites dynamically but at the expense of fast cation leaching. Therefore, achieving simultaneous improvement in catalytic activity and stability remains a significant challenge. Herein, we used a scalable cation deficiency-driven exsolution approach to ex situ reconstruct a homogeneous-doped cobaltate precursor into an Ir/CoO/perovskite heterojunction (SCI-350), which served as an active and stable OER electrode. The SCI-350 catalyst exhibited a low overpotential of 240 mV at 10 mA cm^-2 in 1 M KOH and superior durability in practical electrolysis for over 150 h. The outstanding activity is preliminarily attributed to the exponentially enlarged electrochemical surface area for charge accumulation, increasing from 3.3 to 175.5 mF cm^-2. Moreover, density functional theory calculations combined with advanced spectroscopy and ¹⁸O isotope-labeling experiments evidenced the tripled oxygen exchange kinetics, strengthened metal-oxygen hybridization, and engaged lattice oxygen oxidation for O-O coupling on SCI-350. This work presents a promising and feasible strategy for constructing highly active oxide OER electrocatalysts without sacrificing durability.