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Methylation enables the use of fluorine-free ether electrolytes in high-voltage lithium metal batteries.
Li, Ai-Min; Borodin, Oleg; Pollard, Travis P; Zhang, Weiran; Zhang, Nan; Tan, Sha; Chen, Fu; Jayawardana, Chamithri; Lucht, Brett L; Hu, Enyuan; Yang, Xiao-Qing; Wang, Chunsheng.
Afiliación
  • Li AM; Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA.
  • Borodin O; Battery Science Branch, DEVCOM Army Research Laboratory, Adelphi, MD, USA.
  • Pollard TP; Battery Science Branch, DEVCOM Army Research Laboratory, Adelphi, MD, USA.
  • Zhang W; Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA.
  • Zhang N; Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA.
  • Tan S; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA.
  • Chen F; Department of Chemistry and Biochemistry, University of Maryland, College Park, MD, USA.
  • Jayawardana C; Department of Chemistry, University of Rhode Island, Kingston, RI, USA.
  • Lucht BL; Department of Chemistry, University of Rhode Island, Kingston, RI, USA.
  • Hu E; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA.
  • Yang XQ; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA.
  • Wang C; Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, USA. cswang@umd.edu.
Nat Chem ; 16(6): 922-929, 2024 Jun.
Article en En | MEDLINE | ID: mdl-38570729
ABSTRACT
Lithium metal batteries represent a promising technology for next-generation energy storage, but they still suffer from poor cycle life due to lithium dendrite formation and cathode cracking. Fluorinated solvents can improve battery longevity by improving LiF content in the solid-electrolyte interphase; however, the high cost and environmental concerns of fluorinated solvents limit battery viability. Here we designed a series of fluorine-free solvents through the methylation of 1,2-dimethoxyethane, which promotes inorganic LiF-rich interphase formation through anion reduction and achieves high oxidation stability. The anion-derived LiF interphases suppress lithium dendrite growth on the lithium anode and minimize cathode cracking under high-voltage operation. The Li+-solvent structure is investigated through in situ techniques and simulations to draw correlations between the interphase compositions and electrochemical performances. The methylation strategy provides an alternative pathway for electrolyte engineering towards high-voltage electrolytes while reducing dependence on expensive fluorinated solvents.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido