Journal
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
Volume 168, Issue 3, Pages -Publisher
ELECTROCHEMICAL SOC INC
DOI: 10.1149/1945-7111/abec66
Keywords
Silicon; anode; Interface modification; electrolyte additive; carbon dioxide
Funding
- U.S. Department of Energy's Vehicle Technologies Office under the Silicon Electrolyte Interface Stabilization (SEISta) Consortium
- U.S. Department of Energy (DOE) [DE-AC05-00OR22725]
- U.S. DOE [DE-AC36-08GO28308]
- Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]
- DOE Public Access Plan
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The addition of CO2 in the electrolyte results in a thinner SEI layer dominated by LiF, leading to improved cycling performance by reducing irreversible side reactions. CO2 plays a similar role to additives like fluorinated ethylene carbonate and vinylene carbonate in terms of enhancing the polymeric components in the SEI.
We demonstrate that the addition of CO2 to a standard 1.0 M LiPF6 3:7 wt% ethylene carbonate:ethyl methyl carbonate electrolyte results in the formation of a thinner insoluble solid electrolyte interphase (SEI) that is dominated by the presence of LiF. In contrast, cells without CO2 result in a thicker insoluble SEI layer containing more organic constituents. The CO2 is incorporated in the dimethyl carbonate soluble part of the SEI composed primarily of polymeric poly(ethylene oxide) (PEO) on the surface of a thin inorganic layer. This combination of properties from CO2 addition provides an improved cycling performance through the reduction of irreversible side reactions, leading to higher coulombic efficiency. The results indicate that CO2 incorporates into the SEI and plays a role similar to additives like fluorinated ethylene carbonate and vinylene carbonate with respect to polymeric components.
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