Abstract
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. 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.
| Original language | English |
|---|---|
| Pages (from-to) | 10902-10911 |
| Number of pages | 10 |
| Journal | Chemistry of Materials |
| Volume | 36 |
| Issue number | 21 |
| DOIs | |
| State | Published - Nov 12 2024 |
Funding
This work was supported by the U.S. Department of Energy (DOE) Vehicle Technologies Office under the Silicon Anode Consortium program directed by Brian Cunningham and managed by Anthony Burrell. The manuscript has been authored by UT-Battelle LLC under Contract DE-AC05-00OR22725 with DOE. The electrodes in this article were fabricated at Argonne\u2019s Cell Analysis, Modeling and Prototyping (CAMP) Facility. The authors thank Drs. Andrew Jansen, Bryant Polzin, Yunya Zhang, and Fulya Dogan Key for experiment support. The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of the manuscript, or allow other to do so, for U.S. government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Acknowledgments
| Funders | Funder number |
|---|---|
| U.S. Department of Energy | |
| DOE Public Access Plan | |
| U.S. Government | |
| UT-Battelle | DE-AC05-00OR22725 |
