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

Lam, Steven; Verma, Ankit; Schulze, Maxwell C.; Sacci, Robert L.; Meyer III, Harry M.; Lance, Michael J.; Araño, Khryslyn G.; Musgrove, Amanda L.; Fonseca Rodrigues, Marco-Tulio; Trask, Stephen E.; Colclasure, Andrew; Veith, Gabriel M.

doi:10.1021/acsami.5c07869

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

Journal Article · Thu Jul 17 00:00:00 EDT 2025 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.5c07869· OSTI ID:2586849

^[1]; ^[2]; ^[2]; ^[3]; ^[3]; ^[3]; Araño, Khryslyn G. ^[3]; ^[3]; ^[4]; ^[4]; ^[2]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

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, in this work, 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (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)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; AC36-08GO28308

OSTI ID:: 2586849

Alternate ID(s):: OSTI ID: 2586398
OSTI ID: 2587382

Journal Information:: ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 30 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

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

Journal Article · Thu Jul 17 00:00:00 EDT 2025 · ACS Applied Materials & Interfaces · OSTI ID:2586398

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calendar aging
localized high concentration electrolytes
parasitic reactions
solid electrolyte interphase

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

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