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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Mitigating Li-Rich Layered Cathode Capacity Loss by Using a Siloxane Electrolyte Additive.

Yongwei Chen1,2, Xiangzhen Zheng1, Ying Pan1

  • 1Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, P. R. China.

ACS Applied Materials & Interfaces
|December 9, 2024
PubMed
Summary
This summary is machine-generated.

1,3-diphenyl-1,1,3,3-tetramethyldisiloxane (DTS) additive stabilizes high-voltage lithium-ion batteries. It forms a protective cathode electrolyte interface, improving cycling stability and capacity retention for Li-rich layered oxide cathodes.

Keywords:
1,3-diphenyl-1,1,3,3-tetramethyldisiloxanecathode electrolyte interfaceelectrolyte additivehigh-energy-density lithium-ion batterieslithium-rich layered oxides

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Electrode-electrolyte interface instability limits high-energy lithium-ion battery (LIB) development.
  • High-voltage cathode materials require robust interfacial protection for stable operation.

Purpose of the Study:

  • To investigate the efficacy of 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane (DTS) as an electrolyte additive.
  • To enhance the cycling stability and capacity retention of Li||Li-rich layered oxide (LLO) batteries operating at 4.8 V.

Main Methods:

  • Theoretical calculations to predict DTS oxidation behavior.
  • Electrochemical testing of Li||LLO batteries with and without DTS additive.
  • Analysis of cathode electrolyte interface (CEI) formation and stability.

Main Results:

  • DTS preferentially oxidizes on the LLO cathode surface, forming a stable CEI.
  • The DTS-modified CEI mitigates cathode cracking, regeneration, and phase transitions.
  • Li||LLO batteries with DTS showed 85.4% capacity retention after 100 cycles at 4.8 V (vs. 45.2% for baseline).
  • DTS-enhanced stability was observed even with 1000 ppm H2O contamination.

Conclusions:

  • DTS is an effective electrolyte additive for stabilizing high-voltage LLO cathodes.
  • The robust CEI formed by DTS significantly improves battery performance and durability.
  • DTS offers a promising strategy for advancing high-energy-density LIBs.