Issue 33, 2023

Ab initio study of short-range ordering in vanadium-based disordered rocksalt structures

Abstract

Disordered rocksalt Li-excess (DRX) compounds are attractive new cathode materials for Li-ion batteries as they contain resource-abundant metals and do not require the use of cobalt or nickel. Understanding the delithiation process and cation short-range ordering (SRO) in DRX compounds is essential to improve these promising cathode materials. Herein, we use first-principles calculations along with the cluster-expansion approach to model the disorder in DRX Li2−xVO3, 0 < x < 1. We discuss the SRO of Li in tetrahedral and octahedral sites, and the order in which Li delithiates and V oxidizes with respect to local environments. We reveal that the number of nearest-neighbor V dictates the order of delithiation from octahedral sites and that V is oxidized in a manner that minimizes the electrostatic interactions among V. Our results provide valuable insight for tailoring the performance of V-based DRX cathode materials in general by controlling the SRO features that reduce energy density.

Graphical abstract: Ab initio study of short-range ordering in vanadium-based disordered rocksalt structures

  • This article is part of the themed collection: #MyFirstJMCA

Supplementary files

Article information

Article type
Paper
Submitted
25 Apr 2023
Accepted
27 Jul 2023
First published
27 Jul 2023

J. Mater. Chem. A, 2023,11, 17728-17736

Author version available

Ab initio study of short-range ordering in vanadium-based disordered rocksalt structures

Z. Jadidi, J. H. Yang, T. Chen, L. Barroso-Luque and G. Ceder, J. Mater. Chem. A, 2023, 11, 17728 DOI: 10.1039/D3TA02475J

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