Operando resonant soft X-ray emission spectroscopy of the LiMn2O4 cathode using an aqueous electrolyte solution

Daisuke Asakura*, Yusuke Nanba, Hideharu Niwa, Hisao Kiuchi, Jun Miyawaki, Masashi Okubo, Hirofumi Matsuda, Yoshihisa Harada, Eiji Hosono

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The Mn 3d electronic-structure change of the LiMn2O4 cathode during Li-ion extraction/insertion in an aqueous electrolyte solution was studied by operando resonant soft X-ray emission spectroscopy (RXES). The Mn L3 RXES spectra for the charged state revealed the Mn4+ state with strong charge-transfer from the O 2p to Mn 3d orbitals dominates, while for the open-circuit-voltage and discharged states it is ascribed to the mixture of sites with Mn3+ and Mn4+ states. The degree of charge transfer is significantly different between the Mn3+ and Mn4+ states, indicating that the redox reaction takes place on the strongly-hybridized Mn 3d-O 2p orbital rather than the localized Mn 3d orbital.

Original languageEnglish
Pages (from-to)19177-19183
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume24
Issue number32
DOIs
Publication statusPublished - 2022 Jun 8
Externally publishedYes

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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