Modulating Lithium‐Ion Transport in LiAlBr<sub>4</sub> via S‐Modified Anion Sublattice
Tailoring the structures or chemical compositions of the host lattice modulates cation-anion interactions, enhancing active cation transport. Herein, a Br-S mixed-anion sublattice in LiAlBr<sub>4</sub> lowers the migration energy barrier, facilitating lithium redistribution, and enhanced ionic conductivity in Li<sub>1.2</sub>AlBr<sub>3.8</sub>S<sub>0.2</sub>. Ab initio molecular dynamics simulations reveal restricted diffusion in LiAlBr<sub>4</sub>, whereas Li<sub>1.2</sub>AlBr<sub>3.8</sub>S<sub>0.2</sub> features a delocalized network indicative of improved macroscopic Li<sup>+</sup> transport. Li<sub>1.2</sub>AlBr<sub>3.8</sub>S<sub>0.2</sub> exhibits excellent cycling stability and rate capability in all-solid-state batteries, delivering a high specific capacity of 150.2 mAh g<sup>-1</sup> at 2C in a Li-In|Li<sub>6</sub>PS<sub>5</sub>Cl|2(Li<sub>1.2</sub>AlBr<sub>3.8</sub>S<sub>0.2</sub>): TiS<sub>2</sub> cell, outperforming the LiAlBr<sub>4</sub>-based system (45.2 mAh g<sup>-1</sup>) under the same conditions. These findings offer key insights into structure-ion transport relationships, enabling the design of high-performance solid electrolytes.
Authors
- Pawan Kumar Ojha (ORCID: https://orcid.org/0000-0002-1207-5187)
- Tej P. Poudel (ORCID: https://orcid.org/0000-0003-4787-5739)
- Md. Mahinur Islam (ORCID: https://orcid.org/0000-0002-3042-0204)
- Erica Truong (ORCID: https://orcid.org/0000-0001-6140-2853)
- Ifeoluwa Peter Oyekunle (ORCID: https://orcid.org/0000-0001-7623-4493)
- Islamiyat A. Ojelade (ORCID: https://orcid.org/0009-0009-6316-2473)
- Yudan Chen (ORCID: https://orcid.org/0000-0003-1495-4289)
- Yongkang Jin
Institutions
- Florida State University (US)
- National High Magnetic Field Laboratory (US)
Publication Details
- Journal
- ChemSusChem
- Published
- 2025-08-09
- DOI
- https://doi.org/10.1002/cssc.202501192
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Science Foundation
- National High Magnetic Field Laboratory
- Division of Materials Research
- High Magnetic Field Laboratory, Chinese Academy of Sciences