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Amide-mediated solvation remodeling enables cryogenic high-voltage lithium metal batteries
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DOI：10.1016/j.ensm.2026.105021.png)
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Abstract
En 中文
Extreme cryogenic conditions (< −30°C) severely limit lithium metal batteries due to sluggish ion transport and unstable interphases. This challenge is addressed by a strong–weak solvent synergy electrolyte, which incorporates the amide derivative (N,N-dimethyltrifluoroacetamide (DTA)) into a sulfone-based system. While sulfone ensures thermal and electrochemical stability, DTA restructures the solvation sheath via bipolar coordination through its C=O and –NH₂ groups, thereby enhancing interfacial kinetics. Strategic fluorination of DTA lowers the LUMO energy, which facilitates the formation of a LiF-rich solid-electrolyte interphase (SEI) and improves separator wettability. Simultaneously, methylation raises the HOMO level, promoting a Li₃N-containing cathode-electrolyte interphase (CEI) and increasing ionic conductivity. Furthermore, the π-conjugation within the amide structure enhances anion coordination and ion aggregates. As a result, the 4.4 V Li/LiCoO₂ cells retain 99.4% capacity after 100 cycles (0.02C) at −40°C. More notably, it delivers 116.16 mAh g−1 discharge capacity even at −60°C with 80% capacity retention over 80 cycles (0.02C). Besides, this electrolyte also exhibits excellent compatibility and enhanced safety features at 60°C, underscoring its promise for operation over an extensive temperature spectrum. This amide-mediated solvation remodeling strategy paves the way for designing advanced electrolyte systems capable of simultaneous low-temperature operation and high-voltage stability.
Keywords:
lithium metal batteries
cryogenic conditions
solvation remodeling
high-voltage stability
electrolyte design
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