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High-Energy and Safe Lithium Metal Batteries Enabled by Interphase Optimization with Synergistic Electrolyte

Yongkang Han1,2, Yike Lei2, Cunman Zhang2

  • 1School of Chemistry and Chemical Engineering, Key Laboratory of Theoretical Organic Chemistry and Functional Molecule, Ministry of Education, Hunan University of Science and Technology, Xiangtan 411201, China.

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Summary

This study introduces a novel electrolyte for lithium metal batteries (LMBs) using flame-retardant hexafluorocyclotriphosphazene (HFPN) and other additives. The new electrolyte enhances energy density and safety by improving interphase layers for better performance.

Keywords:
Li-rich Mn-based cathodesfast kineticflame-retardant electrolytelithium metal batteriessynergistic electrolyte additives

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Lithium metal batteries (LMBs) with Li-rich Mn-based cathodes (LMLO) offer high energy densities (>500 W h kg⁻¹).
  • Practical application is hindered by sluggish kinetics, interfacial instability, and safety concerns.
  • Effective management of cathode and anode interphases is crucial for LMB performance.

Purpose of the Study:

  • To design a flame-retardant electrolyte for high-energy LMBs.
  • To enhance the stability and kinetics of cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI).
  • To improve the overall safety and cycle life of LMBs.

Main Methods:

  • Development of a carbonate-based electrolyte with hexafluorocyclotriphosphazene (HFPN), lithium difluoro(oxalato) borate (LiDFOB), and 1-butyl-2,3-dimethylimidazolium nitrate (BDIN) coadditives.
  • Investigation of interphase formation and composition using electrochemical and material characterization techniques.
  • Fabrication and testing of LMLO||Li full cells.

Main Results:

  • The designed electrolyte enables LMBs with an energy density of 528 W h kg⁻¹ and improved safety.
  • HFPN promotes a stable, P-, F-, and N-containing CEI, enhancing thermal stability and Li⁺ kinetics.
  • LiDFOB and BDIN contribute to a robust SEI on the lithium anode, achieving >95.9% Coulombic efficiency in Li||Cu cells.
  • The LMLO||Li full cell demonstrated a capacity of 272 mA h g⁻¹ with 94.7% retention after 50 cycles.

Conclusions:

  • Synergistic use of HFPN, LiDFOB, and BDIN effectively regulates CEI and SEI formation in LMBs.
  • This strategy significantly enhances the electrochemical performance and safety of high-energy LMBs.
  • The interphase regulation approach is potentially applicable to other high-energy lithium-ion battery systems.