Mn−O Covalency Governs the Intrinsic Activity of Co-Mn Spinel Oxides for Boosted Peroxymonosulfate Activation

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Author(s)

  • Zhi-Yan Guo
  • Chen-Xuan Li
  • Miao Gao
  • Xiao Han
  • Ying-Jie Zhang
  • Wen-Wei Li

Detail(s)

Original languageEnglish
Pages (from-to)274-280
Number of pages7
Journal / PublicationAngewandte Chemie - International Edition
Volume60
Issue number1
Online published23 Sep 2020
Publication statusPublished - 4 Jan 2021

Abstract

Transition metal (TM)-based bimetallic spinel oxides can efficiently activate peroxymonosulfate (PMS) presumably attributed to enhanced electron transfer between TMs, but the existing model cannot fully explain the efficient TM redox cycling. Here, we discover a critical role of TM−O covalency in governing the intrinsic catalytic activity of Co3−xMnxO4 spinel oxides. Experimental and theoretical analysis reveals that the Co sites significantly raises the Mn valence and enlarges Mn−O covalency in octahedral configuration, thereby lowering the charge transfer energy to favor MnOh–PMS interaction. With appropriate MnIV/MnIII ratio to balance PMS adsorption and MnIV reduction, the Co1.1Mn1.9O4 exhibits remarkable catalytic activities for PMS activation and pollutant degradation, outperforming all the reported TM spinel oxides. The improved understandings on the origins of spinel oxides activity for PMS activation may inspire the development of more active and robust metal oxide catalysts.

Research Area(s)

  • bimetal, covalency, octahedron, peroxymonosulfate (PMS), spinel oxides

Citation Format(s)

Mn−O Covalency Governs the Intrinsic Activity of Co-Mn Spinel Oxides for Boosted Peroxymonosulfate Activation. / Guo, Zhi-Yan; Li, Chen-Xuan; Gao, Miao; Han, Xiao; Zhang, Ying-Jie; Zhang, Wen-Jun; Li, Wen-Wei.

In: Angewandte Chemie - International Edition, Vol. 60, No. 1, 04.01.2021, p. 274-280.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review