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A "Flexible" Solvent Molecule Enabling High-Performance Lithium Metal Batteries.

Lu Chen1,2, Qing Zhang1, Chunlei Song1,2

  • 1Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.

Angewandte Chemie (International Ed. in English)
|January 31, 2025
PubMed
Summary

New localized high-concentration electrolytes (LHCEs) use hydrogen bonding in solvents and diluents to improve lithium metal battery performance. This enhances ion solvation and electrode interfaces for high energy density and cycling stability.

Keywords:
Hydrogen bondLithium metal batteriesMolecular conformationSolvent-diluent interaction

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Chemical Engineering

Background:

  • Electrolyte chemistry is vital for high-performance lithium metal batteries (LMBs).
  • Localized high-concentration electrolytes (LHCEs) show promise for LMBs.
  • Limited understanding exists on how solvent-diluent interactions affect solvation and interfacial layers in LHCEs.

Purpose of the Study:

  • To investigate how intermolecular interactions in LHCEs regulate ion solvation and interfacial layer structures.
  • To develop a novel LHCE that enhances lithium metal battery performance through controlled molecular interactions.

Main Methods:

  • Utilized benzotrifluoride (BTF) as a diluent and 2,5-dimethyltetrahydrofuran (2,5-THF) as a solvent in a novel LHCE.
  • Investigated the formation of hydrogen bonds between the H-terminus of 2,5-THF and the F of BTF.
  • Analyzed changes in 2,5-THF conformation, polarity, and steric hindrance due to hydrogen bonding.
  • Examined the impact on Li+ ion solvation structure and anion content.

Main Results:

  • Strong hydrogen bonding between 2,5-THF and BTF expanded the 2,5-THF bond angle (119° to 123°), increasing steric hindrance and decreasing polarity.
  • This molecular modification promoted higher anion concentration in the Li+ solvation shell.
  • Achieved a high Coulombic efficiency (CE) of 99.4% for the lithium metal anode.
  • Demonstrated stable cycling of Li||SPAN batteries with an average CE of 99.8% over 700 cycles.
  • Attained a high energy density of 301.4 Wh kg-1 in Li||SPAN pouch cells.

Conclusions:

  • Molecular-level understanding of intermolecular interactions in LHCEs is key to designing advanced electrolytes.
  • The developed LHCE effectively regulates solvation structure and promotes robust interfaces for high-performance LMBs.
  • This work provides insights for future electrolyte design for high-energy-density lithium metal batteries.