A fluorinated cation introduces new interphasial chemistries to enable high-voltage lithium metal batteries

Qian Liu, Wei Jiang, Jiayi Xu, Yaobin Xu, Zhenzhen Yang, Dong-Joo Yoo, Krzysztof Z. Pupek, Chongmin Wang, Cong Liu, Kang Xu () and Zhengcheng Zhang ()
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Qian Liu: Argonne National Laboratory
Wei Jiang: Computational Science Division, Argonne National Laboratory
Jiayi Xu: Argonne National Laboratory
Yaobin Xu: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Zhenzhen Yang: Argonne National Laboratory
Dong-Joo Yoo: Argonne National Laboratory
Krzysztof Z. Pupek: Applied Materials Division, Argonne National Laboratory
Chongmin Wang: Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory
Cong Liu: Argonne National Laboratory
Kang Xu: Battery Science Branch, Energy Science Division, Sensor and Electron Devices Directorate, U.S. Army Research Laboratory
Zhengcheng Zhang: Argonne National Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Fluorides have been identified as a key ingredient in interphases supporting aggressive battery chemistries. While the precursor for these fluorides must be pre-stored in electrolyte components and only delivered at extreme potentials, the chemical source of fluorine so far has been confined to either negatively-charge anions or fluorinated molecules, whose presence in the inner-Helmholtz layer of electrodes, and consequently their contribution to the interphasial chemistry, is restricted. To pre-store fluorine source on positive-charged species, here we show a cation that carries fluorine in its structure is synthesized and its contribution to interphasial chemistry is explored for the very first time. An electrolyte carrying fluorine in both cation and anion brings unprecedented interphasial chemistries that translate into superior battery performance of a lithium-metal battery, including high Coulombic efficiency of up to 99.98%, and Li0-dendrite prevention for 900 hours. The significance of this fluorinated cation undoubtedly extends to other advanced battery systems beyond lithium, all of which universally require kinetic protection of highly fluorinated interphases.

Date: 2023
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DOI: 10.1038/s41467-023-38229-7

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