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Hoffknecht, Jan-Philipp [Verfasser:in]; Wettstein, Alina [Verfasser:in]; Atik, Jaschar [Verfasser:in]; Krause, Christian [Verfasser:in]; Thienenkamp, Johannes [Verfasser:in]; Brunklaus, Gunther [Verfasser:in]; Winter, Martin [Verfasser:in]; Diddens, Diddo [Verfasser:in]; Heuer, Andreas [Verfasser:in]; Paillard, Elie [Verfasser:in]

Coordinating Anions “to the Rescue” of the Lithium Ion Mobility in Ternary Solid Polymer Electrolytes Plasticized With Ionic Liquids

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  • Medientyp: E-Artikel
  • Titel: Coordinating Anions “to the Rescue” of the Lithium Ion Mobility in Ternary Solid Polymer Electrolytes Plasticized With Ionic Liquids
  • Beteiligte: Hoffknecht, Jan-Philipp [Verfasser:in]; Wettstein, Alina [Verfasser:in]; Atik, Jaschar [Verfasser:in]; Krause, Christian [Verfasser:in]; Thienenkamp, Johannes [Verfasser:in]; Brunklaus, Gunther [Verfasser:in]; Winter, Martin [Verfasser:in]; Diddens, Diddo [Verfasser:in]; Heuer, Andreas [Verfasser:in]; Paillard, Elie [Verfasser:in]
  • Erschienen: Wiley-VCH, 2023
  • Erschienen in: Advanced energy materials 13(1), 2202789 - (2023). doi:10.1002/aenm.202202789
  • Sprache: Englisch
  • DOI: https://doi.org/10.1002/aenm.202202789; https://doi.org/10.34734/FZJ-2023-01300
  • ISSN: 1614-6832; 1614-6840
  • Entstehung:
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  • Beschreibung: Lithium salts with low coordinating anions such as bis(trifluoromethanesulfonyl)imide (TFSI) have been the state-of-the-art for polyethylene oxide (PEO)-based “dry” polymer electrolytes for 3 decades. Plasticizing PEO with TFSI-based ionic liquids (ILs) to form ternary solid polymer electrolytes (TSPEs) increases conductivity and Li+ diffusivity. However, the Li+ transport mechanism is unaffected compared to their “dry” counterparts and is essentially coupled to the dynamics of the polymer host matrix, which limits Li+ transport improvement. Thus, a paradigm shift is hereby suggested: the utilization of more coordinating anions such as trifluoromethanesulfonyl-N-cyanoamide (TFSAM), able to compete with PEO for Li+ solvation, to accelerate the Li+ transport and reach a higher Li+ transference number. The Li–TFSAM interaction in binary and ternary TFSAM-based electrolytes is probed by experimental methods and discussed in the context of recent computational results. In PEO-based TSPEs, TFSAM drastically accelerates the Li+ transport (increases Li+ transference number by a factor 6 and the Li+ conductivity by 2–3) and computer simulations reveal that lithium dynamics are effectively re-coupled from polymer to anion dynamics. Last, this concept of coordinating anions in TSPEs is successfully applied in LFP||Li metal cells leading to enhanced capacity retention (86% after 300 cycles) and an improved rate performance at 2C.
  • Zugangsstatus: Freier Zugang