New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation. Issue 14 (20th March 2022)

• Record Type: Journal Article
• Authors: Xu, Xiaomin; Pan, Yangli; Zhong, Yijun; Shi, Chenliang; Guan, Daqin; Ge, Lei; Hu, Zhiwei; Chin, Yi‐Ying; Lin, Hong‐Ji; Chen, Chien‐Te; Wang, Hao; Jiang, San Ping; Shao, Zongping
• Is Part Of: Advanced science. Volume 9:Issue 14(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-03-20
• Subjects: cation deficiency -- lattice‐oxygen participation -- oxygen evolution reaction -- perovskites -- water splitting -- Zn–air batteries; Science -- Periodicals; 505
• DOI: 10.1002/advs.202200530
• Languages: English
• ISSNs: 2198-3844

Abstract

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. Abstract : A dopant‐free, cation‐deficiency manipulation strategy is reported to regulate the bulk oxygen‐ion diffusion properties of perovskites without altering their surface properties, offering a perfect platform to understand the role of lattice‐oxygen participation in oxygen evolution reaction electrocatalysis. Optimizing the cation deficiency level identifies a perovskite candidate with excellent catalytic activity applicable in Zn–air batteries and water electrolyzers.