Ab initio Study of Substitutional Defects in Li3OCl Solid Electrolyte for Li-ion Batteries
Abstract
Improving ion transport in solid electrolytes and cathode coatings remains a key challenge for all-solid-state Li-ion batteries because their room-temperature ionic conductivity is still substantially lower than that of liquid electrolytes. In our previous combined experimental and theoretical study, we showed that thermal neutron irradiation enables defect engineering in LiBO2 through the transmutation of 6Li and 10B, generating lattice vacancies that enhance ionic conductivity. Here, we examine whether this approach can be extended to Li3OCl, a representative antiperovskite solid electrolyte. Using density functional theory, we investigate substitutional defects at Li sites involving B, He, and H, associated with B doping and the neutron-capture reactions 6Li+n→ 3H+α and 10B+n→ 7Li+α+γ. We evaluate defect formation energetics, the resulting structural distortions, and compare these substitutional defects with other mono-, di-, and trication substitutions at Li sites. Our results show that substitutional defects associated with neutron irradiation provide a feasible route to tune the defect chemistry of antiperovskite solid electrolytes and support neutron-driven defect engineering as a strategy for developing advanced materials for high-performance all-solid-state Li-ion batteries.
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BibTeX
@misc{ziemke2026initio,
title = {{$Ab$ $initio$ Study of Substitutional Defects in Li$_3$OCl Solid Electrolyte for Li-ion Batteries}},
author = {Carson D. Ziemke and Naveed Naemi and Ha M. Nguyen and Anthony Dorhauer and Carlos Garcia and Narendirakumar Narayanan and Yangchuan Xin and John Gahl and Thomas W. Heitmann and Carlos Wexler},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.12300},
eprint = {2609.12300},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.12300},
}
RIS
TY - UNPB
TI - Ab initio Study of Substitutional Defects in Li_3OCl Solid Electrolyte for Li-ion Batteries
AU - Carson D. Ziemke
AU - Naveed Naemi
AU - Ha M. Nguyen
AU - Anthony Dorhauer
AU - Carlos Garcia
AU - Narendirakumar Narayanan
AU - Yangchuan Xin
AU - John Gahl
AU - Thomas W. Heitmann
AU - Carlos Wexler
PY - 2026
DA - 2026/09/11
PB - arXiv
DO - 10.48550/arxiv.2609.12300
UR - https://arxiv.org/abs/2609.12300
AB - Improving ion transport in solid electrolytes and cathode coatings remains a key challenge for all-solid-state Li-ion batteries because their room-temperature ionic conductivity is still substantially lower than that of liquid electrolytes. In our previous combined experimental and theoretical study, we showed that thermal neutron irradiation enables defect engineering in LiBO_2 through the transmutation of ^6Li and ^10B, generating lattice vacancies that enhance ionic conductivity. Here, we examine whether this approach can be extended to Li_3OCl, a representative antiperovskite solid electrolyte. Using density functional theory, we investigate substitutional defects at Li sites involving B, He, and H, associated with B doping and the neutron-capture reactions ^6Li+n→ ^3H+α and ^10B+n→ ^7Li+α+γ. We evaluate defect formation energetics, the resulting structural distortions, and compare these substitutional defects with other mono-, di-, and trication substitutions at Li sites. Our results show that substitutional defects associated with neutron irradiation provide a feasible route to tune the defect chemistry of antiperovskite solid electrolytes and support neutron-driven defect engineering as a strategy for developing advanced materials for high-performance all-solid-state Li-ion batteries.
ER -