Peroxo Species Formed in the Bulk of Silicate Cathodes

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

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Author(s)

  • Zhenlian Chen
  • Bjoern Schwarz
  • Xianhui Zhang
  • Wenqiang Du
  • Lirong Zheng
  • Ailing Tian
  • Ying Zhang
  • Zhiyong Zhang
  • Zhifeng Zhang
  • Liyuan Huai
  • Jinlei Wu
  • Helmut Ehrenberg
  • Deyu Wang
  • Jun Li

Detail(s)

Original languageEnglish
Pages (from-to)10056-10063
Journal / PublicationAngewandte Chemie - International Edition
Volume60
Issue number18
Online published23 Feb 2021
Publication statusPublished - 26 Apr 2021
Externally publishedYes

Link(s)

Abstract

Oxygen redox in Li-rich oxides may boost the energy density of lithium-ion batteries by incorporating oxygen chemistry in solid cathodes. However, oxygen redox in the bulk usually entangles with voltage hysteresis and oxygen release, resulting in a prolonged controversy in literature on oxygen transformation. Here, we report spectroscopic evidence of peroxo species formed and confined in silicate cathodes amid oxygen redox at high voltage, accompanied by Co2+/Co3+ redox dominant at low voltage. First-principles calculations reveal that localized electrons on dangling oxygen drive the O-O dimerization. The covalence between the binding cation and the O-O dimer determines the degree of electron transfer in oxygen transformation. Dimerization induces irreversible structural distortion and slow kinetics. But peroxo formation can minimize the voltage drop and volume expansion in cumulative cationic and anionic redox. These findings offer insights into oxygen redox in the bulk for the rational design of high-energy-density cathodes.

Research Area(s)

  • ab initio calculations, lithium-ion batteries, oxygen redox, peroxo formation, X-ray spectroscopy

Citation Format(s)

Peroxo Species Formed in the Bulk of Silicate Cathodes. / Chen, Zhenlian; Schwarz, Bjoern; Zhang, Xianhui et al.
In: Angewandte Chemie - International Edition, Vol. 60, No. 18, 26.04.2021, p. 10056-10063.

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

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