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Progress Towards Extended Cycle Life Si-based Anodes: Investigation of Fluorinated Local High Concentration Electrolytes

Journal Article · · Journal of the Electrochemical Society

Silicon (Si) anodes are promising candidates for Li-ion batteries due to their high specific capacity and low operating potential. Implementation has been challenged by the significant Si volume changes during (de)lithiation and associated growth/regrowth of the solid electrolyte interphase (SEI). In this report, fluorinated local high concentration electrolytes (FLHCEs) were designed such that each component of the electrolyte (solvent, salt, diluent) is fluorinated to modify the chemistry and stabilize the SEI of high (30%) silicon content anodes. FLHCEs were formulated to probe the electrolyte salt concentration and ratio of the fluorinated carbonate solvents to a hydrofluoroether diluent. Higher salt concentrations led to higher viscosities, conductivities, and contact angles on polyethylene separators. Electrochemical cycling of Si-graphite/NMC622 pouch cells using the FLHCEs delivered up to 67% capacity retention after 100 cycles at a C/3 rate. Post-cycling X-ray photoelectron spectroscopy (XPS) analyses of the Si-graphite anodes indicated the FLHCEs formed a LiF rich solid electrolyte interphase (SEI). The findings show that the fluorinated local high concentration electrolytes contribute to stabilizing the Si-graphite electrode over extended cycling.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); New York State Department of Economic Development (DED); New York State Energy Research and Development Authority (NYSERDA); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
EE0009184; SC0012704
OSTI ID:
1885490
Alternate ID(s):
OSTI ID: 1881560
OSTI ID: 1889182
Report Number(s):
BNL-223445-2022-JAAM
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 9 Vol. 169; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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