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Transesterification Induced Multifunctional Additives Enable High-Performance Lithium Metal Batteries.

Yuanhang Gao1, Gang Wu1, Wenqiang Fang1

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Summary

This study introduces a novel artificial transesterification strategy for lithium metal batteries (LMBs). New additives, dimethyl trimethylsilyl phosphate (DTMSP) and 1,3-dimethylimidazolium trifluoroacetate (DITFA), enhance electrolyte stability and battery performance.

Keywords:
Lithium metal batteryMoisture resistanceMultifunctional additivesSolvation structureTransesterification

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Battery Technology

Background:

  • Electrolyte chemistry is critical for the advancement of lithium metal batteries (LMBs).
  • Existing electrolytes face challenges with stability and performance in LMBs.

Purpose of the Study:

  • To develop a novel strategy for creating multifunctional electrolyte additives for LMBs.
  • To enhance the stability and electrochemical performance of LMBs through in situ generated additives.

Main Methods:

  • In situ transesterification of 1,3-dimethylimidazolium dimethyl phosphate (DIDP) and trimethylsilyl trifluoroacetate (TMSF) in carbonate electrolyte.
  • Generation of dimethyl trimethylsilyl phosphate (DTMSP) and 1,3-dimethylimidazolium trifluoroacetate (DITFA) as additives.
  • Electrochemical performance testing of LMBs with the novel electrolyte formulation.

Main Results:

  • DTMSP effectively removes H2O and HF, improving electrolyte moisture resistance and cathode stability.
  • DITFA enhances lithium nitrate dissolution, optimizing Li+ solvation and transport.
  • Preferential redox decomposition of DTMSP and DITFA forms protective P/N/Si-rich cathode layers and inorganic-rich anode layers (Li3N/Li3P).
  • Superior electrochemical performances were achieved in the modified LMBs.

Conclusions:

  • Artificial transesterification is an efficient strategy for creating advanced electrolyte additives for high-performance LMBs.
  • The generated DTMSP and DITFA additives significantly improve electrolyte stability and battery performance by forming protective interfacial layers.