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Surprising Relationship between Silicon Anode Calendar Aging and Electrolyte Components in a Localized High-Concentration Electrolyte System

Journal Article · · ACS Applied Materials & Interfaces
 [1];  [2];  [2];  [3];  [3];  [3];  [3];  [3];  [4];  [4];  [2];  [1]
  1. Oak Ridge National Laboratory; University of Tennessee at Knoxville
  2. National Renewable Energy Lab., Golden, CO (United States)
  3. Oak Ridge National Laboratory
  4. Argonne National Laboratory
+ Show Author Affiliations
Although localized high-concentration electrolytes (LHCEs) have been shown to improve the calendar lifetime of silicon anodes, the roles of the electrolyte constituents in calendar aging are not well understood. Here, we utilize a voltage hold protocol and an LHCE with varying molar ratios of lithium bis(fluorosulfonyl)imide (LiFSI), tetramethylene sulfone (TMS), and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) to probe the component roles during aging. Interestingly, the estimated calendar lifetime and irreversible lithium losses from the V-hold experiments are independent of the electrolyte formulations. Contrarily, the solid electrolyte interphase (SEI) composition depends on the electrolyte formulation. X-ray photoelectron spectroscopy shows that TMS-coordinated species decompose to form insoluble alkanes and lithium hydroxide (LiOH), while lithium fluoride (LiF) originates from the anion-coordination complex. The SEI composition does not appear to play a significant role in the silicon anode passivity, as measured by parasitic current, suggesting that the SEI-electrolyte interactions dictate the calendar aging mechanisms.
Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
DOE Contract Number:
AC36-08GO28308
OSTI ID:
2586398
Report Number(s):
NREL/JA-5700-94538
Journal Information:
ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 30 Vol. 17
Country of Publication:
United States
Language:
English

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Surprising Relationship between Silicon Anode Calendar Aging and Electrolyte Components in a Localized High-Concentration Electrolyte System
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Related Subjects

36 MATERIALS SCIENCE
Si anode
calendar aging
localized high concentration electrolyte
parasitic reactions
solid electrolyte interphase