Li-stuffed garnet solid electrolytes: Current status, challenges, and perspectives for practical Li-metal batteries
Solid-state Li-metal batteries have gained considerable attention for next-generation energy storage because of their potential high energy densities and improved safety. Solid electrolytes are critical to the development of solid-state Li-metal batteries. While various solid electrolytes exhibit fast-ion conductivity, garnet-type oxides are among the few that show good chemical stability against Li metal. In addition, their high oxidation stability allows the use of high-voltage cathodes. However, the practical application of garnet solid electrolytes faces severe challenges: 1) difficulty in sintering thin and large-area garnet solid electrolytes, 2) large interfacial resistance between garnet electrolytes and electrode materials, and 3) Li dendrite growth. This review summarizes recent advances in garnet-type solid electrolytes and emphasizes the key challenges hindering their practical application in Li-metal batteries. Based on a comprehensive literature survey and our studies, the optimization of crystal structure and ionic conductivity in Li 7 La 3 Zr 2 O 12 (LLZO) is nearly complete. The focus of the field is shifting from high-temperature sintered thick pellets to low-temperature processed thin and flexible LLZO-based organic/inorganic sheet electrolytes, which are more promising for commercialization. Additional research is needed to fully understand the mechanics, interface behavior, Li-ion pathway, and manufacturability of castable LLZO-based sheet electrolytes. In terms of cell energy density, the gravimetric energy density of polycrystalline LLZO-based all-solid-state Li-metal pouch cells is estimated to reach only 272 Wh kg -1 under ideal conditions.
Authors
- Bo Gao (ORCID: https://orcid.org/0000-0003-1183-656X)
- Takeshi Abe (ORCID: https://orcid.org/0000-0002-1515-8340)
- Kohei Miyazaki (ORCID: https://orcid.org/0000-0001-5177-3570)
- Ryoji Inada (ORCID: https://orcid.org/0000-0002-6357-092X)
- Saneyuki Ohno (ORCID: https://orcid.org/0000-0001-8192-996X)
- Kiyoshi Kanamura (ORCID: https://orcid.org/0000-0002-0939-6748)
- Hidemi Kato (ORCID: https://orcid.org/0000-0002-9934-7922)
- Shin‐ichi Orimo (ORCID: https://orcid.org/0000-0002-4216-0446)
- Venkataraman Thangadurai (ORCID: https://orcid.org/0000-0001-6256-6307)
- Eric Kazyak (ORCID: https://orcid.org/0000-0001-5099-3985)
- Michael J. Wang (ORCID: https://orcid.org/0000-0002-9980-3828)
- Huanan Duan (ORCID: https://orcid.org/0000-0003-3052-3905)
- Hirokazu Munakata (ORCID: https://orcid.org/0000-0002-3824-0857)
- Eric Jianfeng Cheng (ORCID: https://orcid.org/0000-0003-0904-802X)
- Regina García-Méndez (ORCID: https://orcid.org/0000-0002-0980-3673)
- Hanyu Huo (ORCID: https://orcid.org/0000-0003-3006-4892)
- Tao Zhang (ORCID: https://orcid.org/0000-0001-9032-9982)
- Fei Chen (ORCID: https://orcid.org/0000-0001-9643-7191)
Institutions
- University of Science and Technology of China (CN)
- University of Wisconsin–Madison (US)
- Toyohashi University of Technology (JP)
- Johns Hopkins University (US)
- University of St Andrews (GB)
- Shanghai Jiao Tong University (CN)
- Jilin University (CN)
- Wuhan University of Technology (CN)
- Tohoku University (JP)
- Kyoto University (JP)
- University of Oxford (GB)
- Advanced Institute of Materials Science (JP)
- Shanghai Institute of Ceramics (CN)
- University of Chinese Academy of Sciences (CN)
- Massachusetts Institute of Technology (US)
- Tokyo Metropolitan University (JP)
Publication Details
- Journal
- Energy storage materials
- Published
- 2024-12-20
- DOI
- https://doi.org/10.1016/j.ensm.2024.103970
- Citations
- 18
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 3.76
Funders
- TEPCO Memorial Foundation
- Japan Science and Technology Agency
- Institute for Materials Research, Tohoku University
- Advanced Low Carbon Technology Research and Development Program