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Updated: Jun 14, 2025

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Gibbs Free Energy Regulation to Decrease Desolvation Barrier for Ultralow-Temperature Lithium Metal Batteries at

Ke-Feng Ren1, Yun-Fei Du2, Jia-Xin Guo2

  • 1Jiangsu Key Laboratory of New Energy Devices & Interface Science, School of Chemistry and Materials Science, Nanjing University of Information Science and Technology, Nanjing, Jiangsu, 210044, China.

Small (Weinheim an Der Bergstrasse, Germany)
|June 13, 2025
PubMed
Summary

Researchers developed a new electrolyte to improve lithium metal battery performance at low temperatures. This electrolyte enhances lithium-ion desolvation kinetics, leading to better stability and longer lifespan in cold conditions.

Keywords:
Gibbs free energydesolvationentropy‐enthalpylithium metal batterylow temperature

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Lithium metal batteries (LMBs) suffer from poor lifespan at ultralow temperatures due to sluggish lithium-ion (Li) desolvation kinetics.
  • Efficient Li-ion transport and uniform deposition are critical for stable LMB operation, especially under demanding thermal conditions.

Purpose of the Study:

  • To enhance the desolvation kinetics of Li ions at electrode-electrolyte interfaces for improved LMB performance at low temperatures.
  • To reduce the Gibbs free energy barrier for Li-ion desolvation by manipulating enthalpy and entropy changes.

Main Methods:

  • Designed a Gibbs free energy-driven electrolyte with multiple anions to create complex solvation structures.
  • Engineered weak ion-dipole interactions between Li ions and solvents to lower enthalpy change.
  • Investigated the formation of inorganic-rich solid electrolyte interphase (SEI) induced by anions.

Main Results:

  • Achieved rapid Li-ion desolvation by increasing entropy change (△S) and decreasing enthalpy change (△H).
  • Demonstrated anion-induced SEI formation, promoting uniform Li deposition and enhanced plating kinetics at low temperatures.
  • Maintained 95.5% capacity retention in Li||LiNi0.5Co0.2Mn0.3O2 cells after 210 cycles at -20°C with high cathode loading.
  • Achieved 87.7% capacity retention after 220 cycles at -40°C.

Conclusions:

  • The Gibbs free energy regulation strategy effectively lowers the desolvation barrier for Li ions.
  • The developed electrolyte enables rapid interfacial kinetics and uniform Li deposition, significantly improving LMB performance at ultralow temperatures.
  • This approach provides a novel perspective for designing advanced low-temperature electrolytes for energy storage applications.