Interplay of Lattice Distortion and Cation Disorder Governs Li-Ion Transport in Cation-Disordered Rocksalt Cathodes.
6 affiliations
- 1School of Materials Science and Engineering, Peking University, Beijing100871, China.
- 2Zhejiang Key Laboratory of All-Solid-State Battery, Eastern Institute of Technology, Ningbo315200, China.
- 3High Energy Photon Source, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing100049, China.
- 4Multi-disciplinary Research Division, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
- 5Department of Materials Science and Engineering, University of Wisconsin─Madison, Madison, Wisconsin53706, United States.
- 6Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, Peking University, Beijing100871, China.
Abstract
Cation-disordered solids provide a chemically complex landscape in which local environments, lattice responses, and configurational disorder collectively influence ion transport. In cation-disordered rocksalt cathodes, Li+ diffusion has traditionally been interpreted using the static 0-transition-metal (0-TM) percolation rule, which assumes an ideal lattice and often underestimates experimentally accessible capacities. Here, we show that lattice distortion constitutes an essential and previously overlooked chemical degree of freedom that actively reshapes the Li+ percolation networks in disordered oxides. By combining Monte Carlo sampling of cation configurations with molecular dynamics simulations accelerated by machine learning interatomic potentials, we develop a lattice-responsive framework that quantitatively predicts Li+ percolation and electrochemical capacities with deviations from experiment below 5%. Our results reveal a causal coupling between lattice distortion and cation short-range order: enhanced local distortions suppress ordering and activate Li+ migration through nominally inaccessible 1-transition-metal (1-TM) diffusion channels, thereby extending the percolation network beyond the conventional 0-TM paradigm. Guided by this insight, we design and synthesize a multication cation-disordered rocksalt cathode, Li1.2Mn0.2Ti0.2V0.2Mo0.2O2, which exhibits increased lattice distortion, an expanded Li+ percolation network, and a high reversible capacity consistent with theoretical predictions. These findings establish lattice distortion as an active chemical parameter governing ion transport in disordered solids and provide a general design principle for ion-conducting materials.
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BibTeX
@article{zhang2026interplay,
title = {{Interplay of Lattice Distortion and Cation Disorder Governs Li-Ion Transport in Cation-Disordered Rocksalt Cathodes.}},
author = {Zichang Zhang and Lihua Feng and Jiewei Cheng and Peng-Hu Du and Chu-Liang Fu and Xintao Long and Anchun Tang and Longlong Fan and Kang Dong and Haoyu Wu and Weihan Li and Jian Peng and Shuo Wang and Dingguo Xia and Xueliang Sun and Qiang Sun},
journal = {Journal of the American Chemical Society},
year = {2026},
month = sep,
doi = {10.1021/jacs.6c05378},
url = {https://europepmc.org/article/MED/42937883},
note = {CC BY-NC-ND},
}
RIS
TY - JOUR
TI - Interplay of Lattice Distortion and Cation Disorder Governs Li-Ion Transport in Cation-Disordered Rocksalt Cathodes.
AU - Zichang Zhang
AU - Lihua Feng
AU - Jiewei Cheng
AU - Peng-Hu Du
AU - Chu-Liang Fu
AU - Xintao Long
AU - Anchun Tang
AU - Longlong Fan
AU - Kang Dong
AU - Haoyu Wu
AU - Weihan Li
AU - Jian Peng
AU - Shuo Wang
AU - Dingguo Xia
AU - Xueliang Sun
AU - Qiang Sun
PY - 2026
DA - 2026/09/01
JO - Journal of the American Chemical Society
DO - 10.1021/jacs.6c05378
UR - https://europepmc.org/article/MED/42937883
AB - Cation-disordered solids provide a chemically complex landscape in which local environments, lattice responses, and configurational disorder collectively influence ion transport. In cation-disordered rocksalt cathodes, Li+ diffusion has traditionally been interpreted using the static 0-transition-metal (0-TM) percolation rule, which assumes an ideal lattice and often underestimates experimentally accessible capacities. Here, we show that lattice distortion constitutes an essential and previously overlooked chemical degree of freedom that actively reshapes the Li+ percolation networks in disordered oxides. By combining Monte Carlo sampling of cation configurations with molecular dynamics simulations accelerated by machine learning interatomic potentials, we develop a lattice-responsive framework that quantitatively predicts Li+ percolation and electrochemical capacities with deviations from experiment below 5%. Our results reveal a causal coupling between lattice distortion and cation short-range order: enhanced local distortions suppress ordering and activate Li+ migration through nominally inaccessible 1-transition-metal (1-TM) diffusion channels, thereby extending the percolation network beyond the conventional 0-TM paradigm. Guided by this insight, we design and synthesize a multication cation-disordered rocksalt cathode, Li1.2Mn0.2Ti0.2V0.2Mo0.2O2, which exhibits increased lattice distortion, an expanded Li+ percolation network, and a high reversible capacity consistent with theoretical predictions. These findings establish lattice distortion as an active chemical parameter governing ion transport in disordered solids and provide a general design principle for ion-conducting materials.
SN - 0002-7863
SN - 1520-5126
ER -