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Polyphosphates-Based Cathode-Electrolyte Interphase for 4.65 V LiCoO2.

Hengyu Ren1, Xiaohu Wang1, Wenwei Cai1

  • 1School of Advanced Materials, Peking University Shenzhen Graduate School, Peking University, Shenzhen, China.

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Summary
This summary is machine-generated.

Functional phosphate derivatives (FPD) in electrolytes stabilize high-voltage lithium cobalt oxide (LCO) cathodes. This electrolyte engineering approach forms a robust cathode-electrolyte interphase (CEI), enhancing battery cycle life and performance.

Keywords:
CEIcovalent interactionhigh‐voltage LiCoO2polyphosphatestargeted construction

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Stable interfacial chemistry is crucial for high-voltage lithium cobalt oxide (LCO) operation.
  • Interfacial side reactions, including electrolyte oxidation and LCO degradation, limit battery performance.
  • Catalytic Co/O sites on LCO surfaces drive these detrimental interfacial reactions.

Purpose of the Study:

  • To develop a method for targeted regulation of the polyphosphates cathode-electrolyte interphase (CEI) on LCO.
  • To enhance the stability and performance of high-voltage LCO cathodes through electrolyte engineering.
  • To investigate the formation and function of functional phosphate derivatives (FPD) in the electrolyte.

Main Methods:

  • Synthesis of functional phosphate derivatives (FPD) via reaction of tris(trimethylsilyl) phosphate (TMSP) and PF6- anions.
  • In situ construction of a robust CEI on LCO through covalent interactions between FPD and surface Co/O sites.
  • Electrochemical testing of LCO//graphite pouch cells with optimized electrolyte formulations.

Main Results:

  • The optimized electrolyte (1.0 M LiPF6 in FEC with 2.0 wt.% TMSP) formed a uniform, polyphosphate-enriched CEI.
  • The CEI exhibited high thermodynamic stability and facilitated fast Li+ transport.
  • Exceptional cycling stability was achieved: 81.0% capacity retention after 3000 cycles (3.0-4.6 V) and 81.6% after 2000 cycles (3.0-4.65 V).

Conclusions:

  • Functional phosphate derivatives (FPD) effectively regulate CEI formation for high-voltage LCO cathodes.
  • This electrolyte engineering strategy significantly improves LCO battery cycle life and performance.
  • The study offers a novel approach for constructing uniform CEI layers in advanced battery systems.