Synergistic Anion and Solvent-Derived Interphases Enable Lithium-Ion Batteries under Extreme Conditions

Tan, Sha; Borodin, Oleg; Wang, Nan; Yen, Dean; Weiland, Conan; Hu, Enyuan

doi:10.1021/jacs.4c07806

Synergistic Anion and Solvent-Derived Interphases Enable Lithium-Ion Batteries under Extreme Conditions

Journal Article · Fri Oct 25 00:00:00 EDT 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.4c07806· OSTI ID:2477946

^[1]; Borodin, Oleg ^[2]; ^[1]; Yen, Dean ^[1]; Weiland, Conan ^[3]; ^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
DEVCOM Army Research Lab., Adelphi, MD (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)

Lithium-ion batteries (LIBs) face increasingly stringent demands as their application expands into new areas, including extreme temperatures and fast charging. To meet these demands, the electrolyte should enable fast lithium-ion transport and form stable interphases on electrodes simultaneously. In practice, however, improving one aspect often compromises another. For instance, the trend toward electrolytes forming anion-derived interphases typically reduces transport efficiency due to weak-solvating solvents. Here, we propose that instead of relying on anions to form the interphase, leveraging both solvents and anions to form interphases can potentially lead to a balancing point between robust interphase formation and effective ion transport. Guided by this design principle, 2,2-difluoroethyl ethyl carbonate (DFDEC) was identified as the promising solvent. With the new electrolyte using DFDEC as the major solvent and lithium bis(fluorosulfonyl) imide (LiFSI) as the salt, graphite||LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) full cells are capable of fast charging and demonstrate long-term cycling stability with a cutoff voltage of 4.5 V. Notably, the battery shows a capacity retention of 84.3% after 500 cycles with an average Coulombic efficiency (CE) as high as 99.93%. This new electrolyte also enables stable battery cycling across a wide temperature range (-20 to 60 °C), with excellent capacity retention.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: 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)

Grant/Contract Number:: SC0012704; 89243319SEE000004

OSTI ID:: 2477946

Report Number(s):: BNL--226346-2024-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 44 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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