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Temperature-Responsive Evolution and Mechanism Exploration of Static and Dynamic Solvation Structures in Localized

Caiwei Zhang1, Xucheng Lv1, Yifan Gao1

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Temperature significantly impacts localized high-concentration electrolytes (LHCEs) solvation structures, affecting ion transport. This study reveals how temperature influences these structures and provides guidance for designing better electrolytes.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Solvation structures in localized high-concentration electrolytes (LHCEs) are crucial for ion transport and interfacial reactions.
  • The influence of temperature on these solvation structures is often overlooked, hindering mechanistic understanding of electrochemical performance.
  • Temperature is a key parameter affecting intermolecular interactions within electrolytes.

Purpose of the Study:

  • To systematically elucidate the temperature responsiveness of solvation structures in LHCEs with varying compositions.
  • To uncover the underlying mechanisms governing temperature-induced structural evolution in LHCEs.
  • To establish a comprehensive understanding of solvation structure changes across a wide temperature range.

Main Methods:

  • Integration of in situ variable-temperature small-angle X-ray scattering (SAXS) and Raman spectroscopy.
  • Complementary molecular dynamics (MD) simulations and density functional theory (DFT) calculations.
  • Development of a unified static-dynamic framework using conventional descriptors (CN, RDF, cluster population) and novel dynamic metrics (activity factor, cluster lifetime, ligand-exchange probability).

Main Results:

  • Elevated temperatures reduce solvation structure differences caused by compositional variations in LHCEs.
  • High-diluent electrolytes exhibit distinct temperature sensitivities in static versus dynamic structural parameters.
  • An ordered cluster transition process was identified: anion incorporation precedes solvent molecule dissociation.

Conclusions:

  • This work disentangles the coupled concentration-temperature effects on solvation structures in LHCEs.
  • A comprehensive understanding of structural evolution across wide temperature ranges was established.
  • Provides experimentally validated theoretical guidance for designing advanced electrolytes with improved interfacial stability and cycling performance.