Assessing Electrolyte Fluorination Impact on Calendar Aging of Blended Silicon-Graphite Lithium-Ion Cells Using Potentiostatic Holds

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

doi:10.1149/1945-7111/ace65d

Assessing Electrolyte Fluorination Impact on Calendar Aging of Blended Silicon-Graphite Lithium-Ion Cells Using Potentiostatic Holds

Journal Article · Wed Jul 19 00:00:00 EDT 2023 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ace65d· OSTI ID:1995187

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National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Silicon-based lithium-ion batteries have started to meet cycle life metrics, but they exhibit poor calendar life. Here, electrolyte fluorination impact on calendar fade of blended silicon-graphite anodes is explored using a LiPF₆ in EC:EMC:FEC electrolyte vs LiBOB in EC:EMC electrolyte. We utilize a combined experimental-modeling approach applying potentiostatic voltage holds (V-hold) to evaluate electrolyte suitability for calendar life in a shortened testing timeframe (~2 months). Our theoretical framework deconvolutes the irreversible parasitic capacity losses (lithium lost to the solid electrolyte interphase) from the V-hold electrochemical data. Unfluorinated electrolyte (dominant LiBOB reduction) exhibits higher cell resistance as compared to fluorinated electrolyte (dominant FEC reduction). Both systems have similar irreversible capacities during the voltage hold duration with slower rate of parasitic capacity loss for the LiBOB system. Extrapolation of the parasitic losses to end of life capacity fade of 20% shows LiBOB electrolyte outperforming LiPF₆ electrolyte in calendar life. The results demonstrate the applicability of the V-hold protocol as a rapid material screening tool providing semi-quantitative calendar lifetime estimates.

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); USDOE Office of Science (SC)

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

OSTI ID:: 1995187

Alternate ID(s):: OSTI ID: 2367272

Report Number(s):: NREL/JA-5700-86203; MainId:86976; UUID:8040650b-282b-453c-a0a9-59f741f18b14; MainAdminID:70197

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 7 Vol. 170; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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An Extended Formulation of Butler-Volmer Electrochemical Reaction Kinetics Including the Influence of Mechanics Ganser, Markus; Hildebrand, Felix E.; Klinsmann, Markus Journal of The Electrochemical Society, Vol. 166, Issue 4 https://doi.org/10.1149/2.1111904jes	journal	January 2019
Galvanostatic Intermittent Titration and Performance Based Analysis of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ Cathode Verma, Ankit; Smith, Kandler; Santhanagopalan, Shriram Journal of The Electrochemical Society, Vol. 164, Issue 13 https://doi.org/10.1149/2.1701713jes	journal	January 2017

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