期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 15, 期 11, 页码 4823-4835出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ee01489k
关键词
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资金
- University of Chicago
- Neubauer Family Assistant Professors program
- Sloan Scholars Mentoring Network seed grant
- 3M Nontenured Faculty Award
- NSF-CAREER Award [CBET-2144454]
- National Science Foundation [DMR-2011854]
- NIH [1S10RR025105-01]
- DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
- National Science Foundation - Earth Sciences [EAR-1634415]
- Samuel Gillard at the U.S. Department of Energy (DOE), Vehicle Technologies Office
- DOE Office of Science by UChicago Argonne, LLC [DE-AC02-06CH11357]
The research demonstrates that using fluoroethers as electrolyte solvents can support reversible lithium-ion intercalation into graphite without solvent co-intercalation, providing higher energy density and a wider working temperature window for next-generation lithium-ion batteries.
Carbonate-based electrolytes are widely used in Li-ion batteries but are limited by a small operating temperature window and poor cycling with silicon-containing graphitic anodes. The lack of non-carbonate electrolyte alternatives such as ether-based electrolytes is due to undesired solvent co-intercalation that occurs with graphitic anodes. Here, we show that fluoroethers are the first class of ether solvents to intrinsically support reversible lithium-ion intercalation into graphite without solvent co-intercalation at conventional salt concentrations. In full cells using a graphite anode, they enable 10-fold higher energy densities compared to conventional ethers, and better thermal stability over carbonate electrolytes (operation up to 60 degrees C) by producing a robust solvent-derived solid electrolyte interphase (SEI). As single-solvent-single-salt electrolytes, they remarkably outperform carbonate electrolytes with fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives when cycled with graphite-silicon composite anodes. Our molecular design strategy opens a new class of electrolytes that can enable next generation Li-ion batteries with higher energy density and a wider working temperature window.
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