Covalency competition dominates the water oxidation structure–activity relationship on spinel oxides

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Author(s)

  • Yuanmiao Sun
  • Hanbin Liao
  • Jiarui Wang
  • Bo Chen
  • Shengnan Sun
  • Samuel Jun Hoong Ong
  • Shibo Xi
  • Caozheng Diao
  • Yonghua Du
  • Jia-Ou Wang
  • Mark B. H. Breese
  • Shuzhou Li
  • Zhichuan J. Xu

Detail(s)

Original languageEnglish
Pages (from-to)554-563
Journal / PublicationNature Catalysis
Volume3
Issue number7
Online published15 Jun 2020
Publication statusPublished - Jul 2020

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. [Figure not available: see fulltext.]

Research Area(s)

  • EVOLUTION ACTIVITIES, REACTION-MECHANISM, OXYGEN REDUCTION, RATIONAL DESIGN, LATTICE OXYGEN, METAL-OXIDES, ENERGY, ELECTROCATALYSTS, PERFORMANCE, TRANSITION

Citation Format(s)

Covalency competition dominates the water oxidation structure–activity relationship on spinel oxides. / Sun, Yuanmiao; Liao, Hanbin; Wang, Jiarui et al.
In: Nature Catalysis, Vol. 3, No. 7, 07.2020, p. 554-563.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review