Tetrahedral Lithium Stuffing in Disordered Rocksalt Cathodes for High-Power-Density and Energy-Density Batteries
Li-rich cation-disordered rocksalt (DRX) materials introduce new paradigms in the design of high-capacity Li-ion battery cathode materials. However, DRX materials show strikingly sluggish kinetics due to random Li percolation with poor rate performance. Here, we demonstrate that Li stuffing into the tetrahedral sites of the Mn-based rocksalt skeleton injects a novel tetrahedron-octahedron-tetrahedron diffusion path, which acts as a low-energy-barrier hub to facilitate high-speed Li transport. Moreover, the enhanced stability of lattice oxygen and the suppression of transition metal migration preserve the efficacy of the Li percolation network during cycling. Overall, the tetrahedral Li stuffing DRX material exhibits high energy density (311 mAh g<sup>-1</sup>, 923 Wh kg<sup>-1</sup>) and high power density (251 mAh g<sup>-1</sup>, 697 Wh kg<sup>-1</sup> at 1000 mA g<sup>-1</sup>). Our results highlight the potential to develop high-performance and earth-abundant cathode materials within the extensive range of rocksalt compounds.
Authors
- Craig E. Banks (ORCID: https://orcid.org/0000-0002-0756-9764)
- Chaoping Liang (ORCID: https://orcid.org/0000-0002-2910-2938)
- Baishan Chen (ORCID: https://orcid.org/0009-0002-0649-5043)
- Yu Mei (ORCID: https://orcid.org/0000-0001-7378-9880)
- Lianshan Ni (ORCID: https://orcid.org/0000-0003-1746-7590)
- Xiaobo Ji (ORCID: https://orcid.org/0000-0002-5405-7913)
- Debbie S. Silvester (ORCID: https://orcid.org/0000-0002-7678-7482)
- Khalil Amine (ORCID: https://orcid.org/0000-0001-9206-3719)
- Hongshuai Hou (ORCID: https://orcid.org/0000-0001-8201-4614)
- Guoqiang Zou (ORCID: https://orcid.org/0000-0001-7115-6190)
- Haoji Wang (ORCID: https://orcid.org/0000-0002-7707-0088)
- Jinqiang Gao
- Tongchao Liu (ORCID: https://orcid.org/0000-0002-6010-3891)
- Yujin Li
- Wentao Deng (ORCID: https://orcid.org/0000-0002-2064-2970)
Institutions
- Manchester Metropolitan University (GB)
- Argonne National Laboratory (US)
- Central South University (CN)
- Curtin University (AU)
- Powder Metallurgy Institute (BY)
- State Key Laboratory of Powder Metallurgy
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-01-22
- DOI
- https://doi.org/10.1021/jacs.4c15631
- Citations
- 10
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 7.30
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Fundamental Research Funds for Central Universities of the Central South University
- Vehicle Technologies Office