期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 117, 期 1, 页码 73-79出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1911017116
关键词
Li metal anode; Li battery; solid electrolyte interface
资金
- National Science Foundation [DMR-14-19807, 1804247]
- Massachusetts Institute of Technology (MIT) Bose Fellowship research grant
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1804247] Funding Source: National Science Foundation
Lithium is the most attractive anode material for high-energy density rechargeable batteries, but its cycling is plagued by morphological irreversibility and dendrite growth that arise in part from its heterogeneous native solid electrolyte interphase (SEI). Enriching the SEI with lithium fluoride (LiF) has recently gained popularity to improve Li cyclability. However, the intrinsic function of LiF-whether chemical, mechanical, or kinetic in nature-remains unknown. Herein, we investigated the stability of LiF in model LiF-enriched SEls that are either artificially preformed or derived from fluorinated electrolytes, and thus, the effect of the LiF source on Li electrode behavior. We discovered that the mechanical integrity of LiF is easily compromised during plating, making it intrinsically unable to protect Li. The ensuing in situ repair of the interface by electrolyte, either regenerating LiF or forming an extra elastomeric outer layer, is identified as the more critical determinant of Li electrode performance. Our findings present an updated and dynamic picture of the LiF-enriched SEI and demonstrate the need to carefully consider the combined role of ionic and electrolyte-derived layers in future design strategies.
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