New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation

Advanced Science

Lei Ge¹  Yangli Pan¹  Hao Wang¹  Daqin Guan²  Yi‐Ying Chin³  Zhiwei Hu⁴  Chien‐Te Chen⁵  Hong‐Ji Lin⁵  Chenliang Shi⁶  Yijun Zhong⁷  San Ping Jiang⁷  Zongping Shao⁷  Xiaomin Xu⁷ 

[1] Centre for Future Materials University of Southern Queensland Springfield Central QLD 4300 Australia;Department of Building and Real Estate Research Institute for Sustainable Urban Development (RISUD) and Research Institute for Smart Energy (RISE) The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 China;Department of Physics National Chung Cheng University Min‐Hsiung Chiayi 62102 Taiwan;Max Planck Institute for Chemical Physics of Solids Nöthnitzer Str. 40 Dresden 01187 Germany;National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan;State Key Laboratory of Materials‐Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Nanjing 211800 China;WA School of Mines: Minerals, Energy and Chemical Engineering (WASM‐MECE) Curtin University Perth WA 6102 Australia;

关键词: cation deficiency;    lattice‐oxygen participation;    oxygen evolution reaction;    perovskites;    water splitting;    Zn–air batteries;   

DOI  :  10.1002/advs.202200530

来源: DOAJ

【 摘 要 】

Abstract Oxygen evolution reaction (OER) is a key half‐reaction in many electrochemical transformations, and efficient electrocatalysts are critical to improve its kinetics which is typically sluggish due to its multielectron‐transfer nature. Perovskite oxides are a popular category of OER catalysts, while their activity remains insufficient under the conventional adsorbate evolution reaction scheme where scaling relations limit activity enhancement. The lattice oxygen‐mediated mechanism (LOM) has been recently reported to overcome such scaling relations and boost the OER catalysis over several doped perovskite catalysts. However, direct evidence supporting the LOM participation is still very little because the doping strategy applied would introduce additional active sites that may mask the real reaction mechanism. Herein, a dopant‐free, cation deficiency manipulation strategy to tailor the bulk diffusion properties of perovskites without affecting their surface properties is reported, providing a perfect platform for studying the contribution of LOM to OER catalysis. Further optimizing the A‐site deficiency achieves a perovskite candidate with excellent intrinsic OER activity, which also demonstrates outstanding performance in rechargeable Zn–air batteries and water electrolyzers. These findings not only corroborate the key role of LOM in OER electrocatalysis, but also provide an effective way for the rational design of better catalyst materials for clean energy technologies.

【 授权许可】

Unknown