Significant Improvements to Si Calendar Lifetime Using Rapid Electrolyte Screening via Potentiostatic Holds

Verma, Ankit; Schulze, Maxwell C.; Colclasure, Andrew; Rodrigues, Marco-Tulio Fonseca; Trask, Stephen E.; Pupek, Krzysztof; Abraham, Daniel P.

doi:10.1149/1945-7111/ad6376

Significant Improvements to Si Calendar Lifetime Using Rapid Electrolyte Screening via Potentiostatic Holds

Journal Article · Thu Jul 25 00:00:00 EDT 2024 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ad6376· OSTI ID:2446844

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National Renewable Energy Laboratory (NREL), Golden, CO (United States). Energy Conversion and Storage Systems Center
Argonne National Laboratory (ANL), Argonne, IL (United States)

Silicon-based lithium-ion batteries exhibit severe time-based degradation resulting in poor calendar lives. This has been identified as the major impediment towards commercialization with cycle life considered a solved issue through nanosizing and protective coatings allowing over 1000 cycles of life to be achieved. In this work, rapid screening of sixteen electrolytes for calendar life extension of Si-rich systems (70 wt% Si) is performed using the voltage hold (V-hold) protocol. V-hold significantly shortens the testing duration over the traditional open circuit voltage reference performance test allowing us to screen electrolytes within a span of two months. We find a novel ethylene carbonate (EC) free electrolyte formulation containing lithium hexafluorophosphate (LiPF₆) salt, and binary solvent mix of fluoroethylene carbonate (FEC), ethyl methyl carbonate (EMC) that extends calendar life of Si cells as compared to conventional EC based electrolyte. Our coupled experimental-theoretical analysis framework provides a decoupling of the parasitic currents during V-hold, allowing us to extrapolate the capacity loss to predict semiquantitative calendar lifetimes. Subsequently, cycle aging and oxidative stability tests of the EC free system also show enhanced performance over baseline electrolyte.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

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

OSTI ID:: 2446844

Report Number(s):: NREL/JA--5700-89454; MainId:90233; UUID:9ce73e56-fdc3-4d44-b8d6-c20a26c38bb3; MainAdminId:73706

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 7 Vol. 171; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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Significant Improvements to Si Calendar Lifetime Using Rapid Electrolyte Screening via Potentiostatic Holds

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