Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 21, Pages 11919-11927Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016716
Keywords
batteries; ionic liquids; lithium; lithium transport; polymer electrolytes
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Funding
- Projekt DEAL
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The study demonstrates that incorporating a pyrrolidinium cation with an oligo(ethylene oxide) substituent in SPEs can enhance lithium-ion transport speed. This not only accelerates the conduction modes of PEO, but also enables new conduction modes associated with the solvation of lithium by a single IL cation, leading to improved performance on lithium-metal polymer batteries.
N-alkyl-N-alkyl pyrrolidinium-based ionic liquids (ILs) are promising candidates as non-flammable plasticizers for lowering the operation temperature of poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs), but they present limitations in terms of lithium-ion transport, such as a much lower lithium transference number. Thus, a pyrrolidinium cation was prepared with an oligo(ethylene oxide) substituent with seven repeating units. We show, by a combination of experimental characterizations and simulations, that the cation's solvating properties allow faster lithium-ion transport than alkyl-substituted analogues when incorporated in SPEs. This proceeds not only by accelerating the conduction modes of PEO, but also by enabling new conduction modes linked to the solvation of lithium by a single IL cation. This, combined with favorable interfacial properties versus lithium metal, leads to significantly improved performance on lithium-metal polymer batteries.
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