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Decrypting the antisolvent-modulating mechanism in localized high-concentration electrolytes.

Ruilin Hou1,2, Linlin Zheng1,2, Tianze Shi1,2

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Antisolvents in localized high-concentration electrolytes (LHCEs) critically influence lithium metal battery performance by altering solvation structures and interface chemistry. Optimizing antisolvent polarity enhances ion conductivity and Li deposition efficiency.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Battery Technology

Background:

  • Localized high-concentration electrolytes (LHCEs) are crucial for lithium metal batteries (LMBs).
  • Antisolvents in LHCEs are traditionally viewed as diluents, with their role in microstructure and interface chemistry poorly understood.
  • Understanding antisolvent effects is key to advancing high-energy-density LMBs.

Purpose of the Study:

  • To investigate the impact of antisolvent polarity on solvation structure, interface chemistry, and lithium deposition in LHCEs.
  • To elucidate the mechanism by which antisolvents influence the solid electrolyte interphase (SEI) formation and ion transport.
  • To optimize LHCEs for improved lithium metal battery performance.

Main Methods:

  • Utilized LHCEs with trifluorobenzene isomers as antisolvents.
  • Investigated antisolvent polarity-dependent solvation structure and interface chemistry.
  • Evaluated lithium deposition/stripping efficiency and full cell performance (Li||LiFePO4).

Main Results:

  • Antisolvent 'dragging effect' alters solvation environment, challenging existing LHCE models.
  • Polar antisolvent adsorption negatively impacts SEI formation and ion transport dynamics.
  • Enhanced Li deposition/stripping efficiency (98.55%) achieved with low-polarity antisolvents in ester-based LHCEs.
  • Li||LiFePO4 full cell demonstrated 90% capacity retention over 250 cycles.
  • High-polarity antisolvents significantly enhance bulk electrolyte ion conductivity, especially at low temperatures.

Conclusions:

  • Antisolvents play a pivotal role in LHCEs, significantly influencing battery performance.
  • Antisolvent polarity is a critical design parameter for optimizing LHCEs for LMBs.
  • This study provides valuable insights for developing advanced electrolytes for high-energy-density lithium metal batteries.