A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High‐Concentration Electrolytes over Electrochemical Performance of Lithium‐Ion Batteries

Jia, Hao; Kim, Ju‐Myung; Gao, Peiyuan; Xu, Yaobin; Engelhard, Mark H.; Matthews, Bethany E.; Wang, Chongmin; Xu, Wu

doi:10.1002/ange.202218005

Title: A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High‐Concentration Electrolytes over Electrochemical Performance of Lithium‐Ion Batteries

Journal Article · 19 March 2023 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202218005 · OSTI ID:1962712

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Energy and Environment Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
Physical &, Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
Environmental and Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99354 USA

Abstract Localized high‐concentration electrolytes (LHCEs) based on five different types of solvents were systematically studied and compared in lithium (Li)‐ion batteries (LIBs). The unique solvation structure of LHCEs promotes the participation of Li salt in forming solid electrolyte interphase (SEI) on graphite (Gr) anode, which enables solvents previously considered incompatible with Gr to achieve reversible lithiation/delithiation. However, the long cyclability of LIBs is still subject to the intrinsic properties of the solvent species in LHCEs. Such issue can be readily resolved by introducing a small amount of additive into LHCEs. The synergetic decompositions of Li salt, solvating solvent and additive yield effective SEIs and cathode electrolyte interphases (CEIs) in most of the studied LHCEs. This study reveals that both the structure and the composition of solvation sheaths in LHCEs have significant effect on SEI and CEI, and consequently, the cycle life of energetically dense LIBs.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; EE0008444; AC05-76RL01830

OSTI ID:: 1962712

Alternate ID(s):: OSTI ID: 1983550

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 17 Vol. 135; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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