Decoding the Entropy‐Performance Relationship in Aqueous Electrolytes for Lithium‐Ion Batteries DOI

Yanxin Shang,

Nan Chen,

Yuejiao Li

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 17, 2025

Abstract Developing aqueous low‐temperature electrolytes aligns with the societal demand for lithium batteries in extreme climates and environments. However, main challenges include high thermodynamic freezing points, slow ion diffusion, instability at interface under low temperatures, resulting energy density poor cycle performance. Here, role of mixing entropy ΔS mix , hydrogen bonding, electrostatic interactions achieving an optimal electrolyte composition is explored. By systematically varying ethyl acetate (EA)/H 2 O ratio, a critical “mixing point” molar ratio 3.91, where exhibits best balance between molecular disorder interfacial stability identified. At this point, EA molecules polar ester group (‐COO‐) effectively break hydrogen‐bond network water, enhancing lowering point to −106.95 °C. Furthermore, stable chemistry derived from entropy‐driven solvation structure suppress evolution expand electrochemical window 6.2 V. Full Li‐ion LiMn 4 ‐Li Ti 5 12 full cell delivered initial discharge specific capacity 135.1 mAh g −1 1000 cycles rapid 10 C rate. The results provide promising foundation designing high‐performance electrolytes, implications next‐generation lithium‐ion batteries.

Language: Английский

Decoding the Entropy‐Performance Relationship in Aqueous Electrolytes for Lithium‐Ion Batteries DOI

Yanxin Shang,

Nan Chen,

Yuejiao Li

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 17, 2025

Abstract Developing aqueous low‐temperature electrolytes aligns with the societal demand for lithium batteries in extreme climates and environments. However, main challenges include high thermodynamic freezing points, slow ion diffusion, instability at interface under low temperatures, resulting energy density poor cycle performance. Here, role of mixing entropy ΔS mix , hydrogen bonding, electrostatic interactions achieving an optimal electrolyte composition is explored. By systematically varying ethyl acetate (EA)/H 2 O ratio, a critical “mixing point” molar ratio 3.91, where exhibits best balance between molecular disorder interfacial stability identified. At this point, EA molecules polar ester group (‐COO‐) effectively break hydrogen‐bond network water, enhancing lowering point to −106.95 °C. Furthermore, stable chemistry derived from entropy‐driven solvation structure suppress evolution expand electrochemical window 6.2 V. Full Li‐ion LiMn 4 ‐Li Ti 5 12 full cell delivered initial discharge specific capacity 135.1 mAh g −1 1000 cycles rapid 10 C rate. The results provide promising foundation designing high‐performance electrolytes, implications next‐generation lithium‐ion batteries.

Language: Английский

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