An inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries

Rahman, Muhammad Mominur; Tan, Sha; Yang, Yang; Zhong, Hui; Ghose, Sanjit; Waluyo, Iradwikanari; Hunt, Adrian; Ma, Lu; Yang, Xiao-Qing; Hu, Enyuan

doi:10.1038/s41467-023-44282-z

Title: An inorganic-rich but LiF-free interphase for fast charging and long cycle life lithium metal batteries

Journal Article · 18 December 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-44282-z · OSTI ID:2242554

Rahman, Muhammad Mominur ^[1];

^[1];

^[1]; Zhong, Hui ^[2]; Ghose, Sanjit ^[1];

^[1]; Hunt, Adrian ^[1]; Ma, Lu ^[1];

^[1];

^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stony Brook University, NY (United States)

Li metal batteries using Li metal as negative electrode and LiNi_1-x-yMnxCoyO₂ as positive electrode represent the next generation high-energy batteries. A major challenge facing these batteries is finding electrolytes capable of forming good interphases. Conventionally, electrolyte is fluorinated to generate anion-derived LiF-rich interphases. However, their low ionic conductivities forbid fast-charging. Here, we use CsNO₃ as a dual-functional additive to form stable interphases on both electrodes. Such strategy allows the use of 1,2-dimethoxyethane as the single solvent, promising superior ion transport and fast charging. LiNi_1-x-yMnxCoyO₂ is protected by the nitrate-derived species. On the Li metal side, large Cs⁺ has weak interactions with the solvent, leading to presence of anions in the solvation sheath and an anion-derived interphase. The interphase is surprisingly dominated by cesium bis(fluorosulfonyl)imide, a component not reported before. Its presence suggests that Cs⁺ is doing more than just electrostatic shielding as commonly believed. The interphase is free of LiF but still promises high performance as cells with high LiNi_0.8Mn_0.1Co_0.1O₂ loading (21 mg/cm²) and low N/P ratio (~2) can be cycled at 2C (~8 mA/cm²) with above 80% capacity retention after 200 cycles. These results suggest the role of LiF and Cs-containing additives need to be revisited.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 2242554

Alternate ID(s):: OSTI ID: 2283311

Report Number(s):: BNL-225246-2024-JAAM

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

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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