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Decoding polarity gradient enabled ultra-high lithium ion conduction.

Yuqing Chen1,2, Aiping Wang3, Yun Zhao4

  • 1College of Materials Science and Engineering, Hunan Joint International Laboratory of Advanced Materials and Technology of Clean Energy, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha 410082, China.

National Science Review
|February 12, 2026
PubMed
Summary
This summary is machine-generated.

This study introduces polarity-gradient engineering (PGE) for lithium-ion batteries, enhancing cryogenic stability by reducing electrolyte heterogeneity. This breakthrough enables stable operation at extremely low temperatures, paving the way for advanced energy storage solutions.

Keywords:
dielectric heterogeneityelectrolytehomogenization solvation structurelithium-ion batterieslow-temperature performance

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Conventional lithium-ion battery electrolytes face operational instability at cryogenic temperatures due to solvation structure heterogeneity.
  • Imbalanced solvent polarity in electrolytes leads to high desolvation barriers and increased interfacial ion transport resistance.
  • This limits the performance and stability of batteries in extreme cold environments.

Purpose of the Study:

  • To introduce a polarity-gradient engineering (PGE) paradigm to address solvent polarity disparity in electrolytes.
  • To systematically resolve heterogeneity at the atomic scale through electronic modulation.
  • To enable stable lithium-ion battery operation at extreme cryogenic conditions.

Main Methods:

  • Substitution of carbon with sulfur in carbonate skeletons to reduce dielectric heterogeneity.
  • Atomic-scale electronic modulation to achieve balanced Li+ coordination.
  • Characterization of electrolyte properties, including dielectric heterogeneity, activation energy for desolvation, and ionic conductivity at low temperatures.

Main Results:

  • An 83% reduction in dielectric heterogeneity was achieved by replacing carbon with sulfur in electrolytes (Δε = 17.1).
  • Homogenized solvation accelerated desolvation kinetics (34.97 kJ·mol⁻¹ activation energy) and promoted LiF-rich interphase formation.
  • Optimized electrolytes enabled liquid operation down to -110°C, with 1 mS·cm⁻¹ conductivity at -80°C, and stable cycling of LiCoO₂/Li pouch cells at -20°C (81% retention over 400 cycles).

Conclusions:

  • The polarity-gradient engineering (PGE) paradigm effectively homogenizes solvation structures in electrolytes.
  • This leads to intrinsically coupled thermodynamic stability and accelerated interfacial kinetics for extreme-condition energy storage.
  • The study provides a universal design framework and an atomic-scale blueprint for developing high-performance cryogenic batteries.