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

Liu, Qian; Jiang, Wei; Xu, Jiayi; Xu, Yaobin; Yang, Zhenzhen; Yoo, Dong-Joo; Pupek, Krzysztof Z.; Wang, Chongmin; Liu, Cong; Xu, Kang; Zhang, Zhengcheng

doi:10.1038/s41467-023-38229-7

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

Journal Article · 20 June 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-38229-7 · OSTI ID:1986102

Liu, Qian; Jiang, Wei; Xu, Jiayi;

; Yang, Zhenzhen; Yoo, Dong-Joo; Pupek, Krzysztof Z.;

;

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 Li ⁰ -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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-06CH11357; AC05-76RL01830

OSTI ID:: 1986102

Report Number(s):: PNNL-SA-184275; 3678; PII: 38229

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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