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

Xu, Xiaomin and Pan, Yangli and Zhong, Yijun and Shi, Chenliang and Guan, Daqin and Ge, Lei ORCID: https://orcid.org/0000-0003-2989-0329 and Hu, Zhiwei and Chin, Yi‐Ying and Lin, Hong‐Ji and Chen, Chien‐Te and Wang, Hao and Jiang, San Ping and Shao, Zongping (2022) New Undisputed Evidence and Strategy for Enhanced Lattice‐Oxygen Participation of Perovskite Electrocatalyst through Cation Deficiency Manipulation. Advanced Science:2200530. pp. 1-10.

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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.


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Item Type: Article (Commonwealth Reporting Category C)
Refereed: Yes
Item Status: Live Archive
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Faculty/School / Institute/Centre: Current - Institute for Advanced Engineering and Space Sciences - Centre for Future Materials (1 Jan 2017 -)
Date Deposited: 10 May 2022 00:06
Last Modified: 10 May 2022 00:06
Uncontrolled Keywords: cation deficiency; lattice-oxygen participation; oxygen evolution reaction; perovskites; water splitting; Zn–air batteries
Fields of Research (2020): 34 CHEMICAL SCIENCES > 3403 Macromolecular and materials chemistry > 340301 Inorganic materials (incl. nanomaterials)
40 ENGINEERING > 4004 Chemical engineering > 400404 Electrochemical energy storage and conversion
Identification Number or DOI: https://doi.org/10.1002/advs.202200530
URI: http://eprints.usq.edu.au/id/eprint/48190

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