Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 6, Issue 14, Pages 10892-10899Publisher
AMER CHEMICAL SOC
DOI: 10.1021/am5001163
Keywords
lithium-ion batteries; electrolyte; negative electrode; graphite; concentrated solution; surface film
Funding
- Advanced Low Carbon Technology Research and Development Program (ALCA) of Japan Science and Technology Agency (JST)
- JSPS KAKENHI [23750211]
- Grants-in-Aid for Scientific Research [23750211] Funding Source: KAKEN
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Lithium-ion batteries have exclusively employed an ethylene carbonate (EC)-based electrolyte to ensure the reversibility of the graphite negative electrode reaction. Because of the limitation of electrolyte compositions, there has been no remarkable progress in commercial lithium-ion batteries despite active research on positive electrode materials. Herein, we present a salt-superconcentrating strategy as a simple and effective method of universalizing a graphite negative electrode reaction in various organic solvents. A dilute electrolyte (e.g., 1 mol dm(-3)) of sulfoxide, ether, and sulfone results in solvent cointercalation and/or severe electrolyte decomposition at a graphite electrode, whereas their superconcentrated electrolyte (e.g., >3 mol dm(-3)) allows for highly reversible lithium intercalation into graphite. We have found a unique coordination structure in the superconcentrated solution and an anion-based inorganic SEI film on the cycled graphite electrode, which would be the origin of the reversible graphite negative electrode reaction without EC. Our salt-superconcentrating strategy, expanding the graphite negative electrode reaction in various organic solvents other than EC, will contribute to the development of advanced lithium-ion batteries with high-voltage and fast-charging characters based on new EC-free functional electrolytes.
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