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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Increasing the upper cutoff voltage of lithium cobalt oxide (LCO) cathodes enhances reversible capacity but leads to structural instability, interfacial issues, and safety concerns.
  • Developing stable cathode/electrolyte interfaces is crucial for high-voltage LCO (HV-LCO) performance, yet interfacial chemistry remains poorly understood, complicating electrolyte design.

Purpose of the Study:

  • To propose a novel electrolyte design strategy for HV-LCO batteries.
  • To identify optimal solvents based on highest occupied molecular orbital energy level and LCO absorption energy.
  • To enhance the performance and safety of HV-LCO cathodes through electrolyte engineering.

Main Methods:

  • Screened potential electrolyte solvents using computational parameters: highest occupied molecular orbital energy level and LCO absorption energy.
  • Synthesized and tested electrolytes with Tris (2, 2, 2-trifluoroethyl) phosphate as the optimal solvent.
  • Fabricated and evaluated graphite||HV-LCO pouch cells using the developed electrolyte.

Main Results:

  • Tris (2, 2, 2-trifluoroethyl) phosphate promotes a LiF-rich cathode/electrolyte interface layer on LCO due to its low defluorination energy barrier.
  • The engineered interface suppresses phase transitions and improves Li+ diffusion kinetics.
  • Graphite||HV-LCO pouch cells demonstrated 85.3% capacity retention after 700 cycles, wide-temperature adaptability (-60-80 °C), and passed nail penetration safety tests.

Conclusions:

  • The novel electrolyte design strategy effectively enhances the stability and performance of HV-LCO cathodes.
  • Tris (2, 2, 2-trifluoroethyl) phosphate is identified as a promising solvent for constructing stable interfaces in high-energy lithium-ion batteries.
  • This work offers insights for rational electrolyte design to improve the cycle life, temperature range, and safety of advanced lithium-ion batteries.