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Title: Covalency competition dominates the water oxidation structure-activity relationship on spinel oxides
Authors: Sun, Yuanmiao
Liao, Hanbin
Wang, Jiarui
Chen, Bo
Sun, Shengnan
Ong, Samuel Jun Hoong
Xi, Shibo
Diao, Caozheng
Du, Yonghua
Wang, Jia-Ou
Breese, Mark B. H.
Li, Shuzhou
Zhang, Hua
Xu, Jason Zhichuan
Keywords: Engineering::Materials
Issue Date: 2020
Source: Sun, Y., Liao, H., Wang, J., Chen, B., Sun, S., Ong, S. J. H., Xi, S., Diao, C., Du, Y., Wang, J., Breese, M. B. H., Li, S., Zhang, H. & Xu, J. Z. (2020). Covalency competition dominates the water oxidation structure-activity relationship on spinel oxides. Nature Catalysis, 3, 554-563.
Project: MOE2018-T2-2-027 
Journal: Nature Catalysis 
Abstract: Spinel oxides have attracted growing interest over the years for catalysing the oxygen evolution reaction (OER) due to their efficiency and cost-effectiveness, but fundamental understanding of their structure–property relationships remains elusive. Here we demonstrate that the OER activity on spinel oxides is intrinsically dominated by the covalency competition between tetrahedral and octahedral sites. The competition fabricates an asymmetric MT−O−MO backbone where the bond with weaker metal–oxygen covalency determines the exposure of cation sites and therefore the activity. Driven by this finding, a dataset with more than 300 spinel oxides is computed and used to train a machine-learning model for screening the covalency competition in spinel oxides, with a mean absolute error of 0.05 eV. [Mn]T[Al0.5Mn1.5]OO4 is predicted to be a highly active OER catalyst and subsequent experimental results confirm its superior activity. This work sets mechanistic principles of spinel oxides for water oxidation, which may be extendable to other applications.
ISSN: 2520-1158
DOI: 10.1038/s41929-020-0465-6
Rights: © 2020 The Author(s), under exclusive licence to Springer Nature Limited. All rights reserved. This paper was published in Nature Catalysis and is made available with permission of The Author(s).
Fulltext Permission: open
Fulltext Availability: With Fulltext
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