Mitigating Calendar Aging in Si-NMC Batteries with Advanced Dual-Salt Glyme Electrolytes

Yang, Guang; Browning, Katie; Meyer III, Harry M.; Li, Yuanshun; Neale, Nathan R.; Veith, Gabriel M.; Nanda, Jagjit

doi:10.1021/acs.chemmater.4c00971

Title: Mitigating Calendar Aging in Si-NMC Batteries with Advanced Dual-Salt Glyme Electrolytes

Journal Article · 29 October 2024 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.4c00971 · OSTI ID:2478822

^[1]; Browning, Katie ^[1];

^[1]; Li, Yuanshun ^[1];

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Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)

In addressing the critical challenge of calendar aging in silicon (Si)-based lithium-ion batteries, this study introduces a groundbreaking strategy utilizing glyme-type dual-salt electrolytes (lithium bis(trifluoromethanesulfonyl)imide [LiTFSI] and lithium difluoro(oxalato)borate [LiDFOB]). These electrolytes are demonstrated to significantly mitigate parasitic reactions and capacity loss in Si-NMC (lithium nickel manganese cobalt oxide) full cells, especially when compared with traditional carbonate-based electrolytes. Further, our exhaustive mechanistic analysis reveals that such electrolytes not only preserve the integrity of the Si anode but also improve the cathode/electrolyte interphases (CEI) through the formation of a conformal coating on the high-voltage cathode surface. This dual-salt approach, enhanced by the addition of a phosphate additive, effectively decelerates calendar aging, marking a substantial advance in the quest for durable and reliable Si-based energy storage technologies. The findings underscore the vital role of electrolyte composition in extending the calendar life of Si batteries, offering an alternative avenue toward maximizing the performance and longevity of next-generation Li-Si batteries.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

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

Contributing Organization:: National Renewable Energy Laboratory (NREL)

Grant/Contract Number:: AC02-76SF00515; AC05-00OR22725; AC36-08GO28308

OSTI ID:: 2478822

Report Number(s):: MainAdminId:74014; MainId:90491; NREL/JA--5900-89712; UUID:43d2416f-4e8c-4ab1-acad-6a72675b051d; MainAdminId:74014; MainId:90491; UUID:43d2416f-4e8c-4ab1-acad-6a72675b051d

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 21 Vol. 36; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Mitigating Calendar Aging in Si-NMC Batteries with Advanced Dual-Salt Glyme Electrolytes

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