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Multifunctional Additive for Electrolyte Stabilization and Electrode/Electrolyte Interphase Regulation in

Heyuan Sun1,2,3, Yue Dong2,4, Kai Zhang1,2,3

  • 1State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metal, Lanzhou University of Technology, Lanzhou 730050, China.

ACS Applied Materials & Interfaces
|April 17, 2025
PubMed
Summary

Azidotrimethylsilane (ATMS) additive stabilizes interfaces in lithium-metal batteries. This improves cycle life and energy density by preventing dendrite growth and enhancing cathode stability.

Keywords:
HF eliminationNCM811additiveazidotrimethylsilaneelectrode−electrolyte interphaseslithium metal batteries

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Lithium-metal batteries (LMBs) offer high energy density but face challenges with electrolyte-electrode interphases (EEIs).
  • Nickel-rich cathodes in LMBs require stable interfaces for practical application.
  • Existing electrolytes struggle to maintain performance due to interphase instability.

Purpose of the Study:

  • To investigate azidotrimethylsilane (ATMS) as a multifunctional additive for carbonate-based electrolytes in LMBs.
  • To understand the dual role of the azido group in ATMS for stabilizing cathode and anode interfaces.
  • To evaluate the impact of ATMS on the electrochemical performance and cycle life of LMBs.

Main Methods:

  • Introduction of ATMS as an additive in traditional carbonate electrolytes.
  • Electrochemical characterization of Li||NCM811, Li||Li symmetric, and Li||Cu cells with ATMS.
  • Analysis of interphase formation and stability using electrochemical performance metrics.

Main Results:

  • ATMS forms a stable cathode electrolyte interphase and inhibits lithium dendrite growth at the anode.
  • The Si-N bond in ATMS neutralizes HF, preventing recurrent interphase issues.
  • Capacity retention in Li||NCM811 cells improved from 34.7% to 82.6% after 600 cycles.
  • Li||Li symmetric cell lifespan extended over 800 h, and Li||Cu cell Coulombic efficiency increased from 81.6% to 91.6%.

Conclusions:

  • ATMS effectively stabilizes electrolyte-electrode interphases in LMBs.
  • The additive significantly enhances long-cycle performance, Coulombic efficiency, and high-voltage stability.
  • ATMS presents a promising solution for advancing the practical application of high-energy-density lithium-metal batteries.