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

Author:

Jia Hao1ORCID,Kim Ju‐Myung1ORCID,Gao Peiyuan2ORCID,Xu Yaobin3ORCID,Engelhard Mark H.3ORCID,Matthews Bethany E.1,Wang Chongmin3ORCID,Xu Wu1ORCID

Affiliation:

1. Energy and Environment Directorate Pacific Northwest National Laboratory Richland WA 99354 USA

2. Physical & Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99354 USA

3. Environmental and Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99354 USA

Abstract

AbstractLocalized 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.

Funder

Vehicle Technologies Office

Publisher

Wiley

Subject

General Chemistry,Catalysis

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