Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Yu, Zhiao; Rudnicki, Paul E.; Zhang, Zewen; Huang, Zhuojun; Celik, Hasan; Oyakhire, Solomon T.; Chen, Yuelang; Kong, Xian; Kim, Sang Cheol; Xiao, Xin; Wang, Hansen; Zheng, Yu; Kamat, Gaurav A.; Kim, Mun Sek; Bent, Stacey F.; Qin, Jian; Cui, Yi; Bao, Zhenan

doi:10.1038/s41560-021-00962-y

Title: Rational solvent molecule tuning for high-performance lithium metal battery electrolytes

Journal Article · 12 January 2022 · Nature Energy

DOI: https://doi.org/10.1038/s41560-021-00962-y · OSTI ID:1863763

^[1]; Rudnicki, Paul E. ^[1];

^[1]; Huang, Zhuojun ^[1]; Celik, Hasan ^[2]; Oyakhire, Solomon T. ^[1];

^[1]; Kong, Xian ^[1]; Kim, Sang Cheol ^[1];

^[1]; Wang, Hansen ^[1]; Zheng, Yu ^[1];

^[1];

^[1]; Bent, Stacey F. ^[1];

^[1];

^[3];

^[1]

Stanford Univ., CA (United States)
Univ. of California, Berkeley, CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Electrolyte engineering improved cycling of Li metal batteries and anode-free cells at low current densities; however, high-rate capability and tuning of ionic conduction in electrolytes are desirable yet less-studied. In this study, we design and synthesize a family of fluorinated-1,2-diethoxyethanes as electrolyte solvents. The position and amount of F atoms functionalized on 1,2-diethoxyethane were found to greatly affect electrolyte performance. Partially fluorinated, locally polar –CHF₂ is identified as the optimal group rather than fully fluorinated –CF₃ in common designs. Paired with 1.2 M lithium bis(fluorosulfonyl)imide, these developed single-salt-single-solvent electrolytes simultaneously enable high conductivity, low and stable overpotential, >99.5% Li||Cu half-cell efficiency (up to 99.9%, ±0.1% fluctuation) and fast activation (Li efficiency >99.3% within two cycles). Combined with high-voltage stability, these electrolytes achieve roughly 270 cycles in 50-μm-thin Li||high-loading-NMC811 full batteries and >140 cycles in fast-cycling Cu||microparticle-LiFePO₄ industrial pouch cells under realistic testing conditions. The correlation of Li⁺–solvent coordination, solvation environments and battery performance is investigated to understand structure–property relationships.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF); Stanford University

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1863763

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 1 Vol. 7; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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