Navigating surface reconstruction of spinel oxides for electrochemical water oxidation

Yuanmiao Sun, Jiarui Wang, Shibo Xi, Jingjing Shen, Songzhu Luo, Jingjie Ge, Shengnan Sun, Yubo Chen, John V. Hanna, Shuzhou Li, Xin Wang and Zhichuan J. Xu ()
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Yuanmiao Sun: Chinese Academy of Sciences
Jiarui Wang: Nanyang Technological University
Shibo Xi: Agency for Science Technology and Research (A*Star)
Jingjing Shen: Nanyang Technological University
Songzhu Luo: Nanyang Technological University
Jingjie Ge: The Hong Kong University of Science and Technology
Shengnan Sun: Agency for Science, Technology and Research (A*Star)
Yubo Chen: Nanyang Technological University
John V. Hanna: Nanyang Technological University
Shuzhou Li: Nanyang Technological University
Xin Wang: City University of Hong Kong
Zhichuan J. Xu: Nanyang Technological University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the MT–O–MO backbone. A stronger MO–O covalency relative to MT–O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.

Date: 2023
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DOI: 10.1038/s41467-023-38017-3

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