Unraveling the Nature and Role of Layered Cation Ordering in Cation-Disordered Rock-Salt Cathodes

You Wang, Shengchi Huang, Basirat Raji-Adefila, Alexandra Outka, Jeng Han Wang*, Dongchang Chen*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

14 Citations (Scopus)

Abstract

Cation-disordered rock salts (DRXs), a new class of cathode materials for Li-ion batteries, have attracted a great amount of attention in recent years due to their fascinatingly simple cubic structure, highly diverse composition, and great electrochemical performance. As cations in DRXs are randomly distributed in a long range, how the cations are spatially arranged is an intriguing question for the community of solid-state materials chemistry. In this work, we report the vibrational structure of a series of Mn- and Fe-based DRXs with well-controlled compositions and reveal significant layered-like cation ordering in the DRXs. A scheme is proposed to describe how the layered-like anisotropy could exist in rock salt structures with an overall cubic diffraction pattern. Furthermore, we raise a model of Li-ion transport based on the proposed scheme, which complements the theory of Li percolation in DRXs. The electrochemical behavior of the DRX cathodes used in the study supports the scheme and clearly demonstrates the role of layered anisotropy in the battery performance of DRXs.

Original languageEnglish
Pages (from-to)19838-19848
Number of pages11
JournalJournal of the American Chemical Society
Volume144
Issue number43
DOIs
Publication statusPublished - 2022 Nov 2

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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