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<p>Elevating the upper cutoff voltage to 4.6&#xa0;V could effectively increase the reversible capacity of LiCoO<sub>2</sub> (LCO) cathode, whereas the irreversible structural transition, unstable electrode/electrolyte interface and potentially induced safety hazards severely hinder its industrial application. Building a robust cathode/electrolyte interface film by electrolyte engineering is one of the efficient approaches to boost the performance of high-voltage LCO (HV-LCO); however, the elusive interfacial chemistry poses substantial challenges to the rational design of highly compatible electrolytes. Herein, we propose a novel electrolyte design strategy and screen proper solvents based on two factors: highest occupied molecular orbital energy level and LCO absorption energy. Tris (2, 2, 2-trifluoroethyl) phosphate is determined as the optimal solvent, whose low defluorination energy barrier significantly promotes the construction of LiF-rich cathode/electrolyte interface layer on the surface of LCO, thereby eventually suppresses the phase transition and enhances Li<sup>+</sup> diffusion kinetics. The rationally designed electrolyte endows graphite||HV-LCO pouch cells with long cycle life (85.3% capacity retention after 700 cycles), wide-temperature adaptability (− 60–80&#xa0;°C) and high safety (pass nail penetration). This work provides new insights into the electrolyte screening and rational design to constructing stable interface for high-energy lithium-ion batteries.</p>

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Manipulating Interfacial Stability via Preferential Absorption for Highly Stable and Safe 4.6 V LiCoO2 Cathode

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年3月12日

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  • Long Chen,
  • Xin He,
  • Yiqing Chen,
  • Youmin Hou,
  • Yujie Zhang,
  • Kangli Wang,
  • Xinping Ai,
  • Yuliang Cao,
  • Zhongxue Chen

摘要

Elevating the upper cutoff voltage to 4.6 V could effectively increase the reversible capacity of LiCoO2 (LCO) cathode, whereas the irreversible structural transition, unstable electrode/electrolyte interface and potentially induced safety hazards severely hinder its industrial application. Building a robust cathode/electrolyte interface film by electrolyte engineering is one of the efficient approaches to boost the performance of high-voltage LCO (HV-LCO); however, the elusive interfacial chemistry poses substantial challenges to the rational design of highly compatible electrolytes. Herein, we propose a novel electrolyte design strategy and screen proper solvents based on two factors: highest occupied molecular orbital energy level and LCO absorption energy. Tris (2, 2, 2-trifluoroethyl) phosphate is determined as the optimal solvent, whose low defluorination energy barrier significantly promotes the construction of LiF-rich cathode/electrolyte interface layer on the surface of LCO, thereby eventually suppresses the phase transition and enhances Li+ diffusion kinetics. The rationally designed electrolyte endows graphite||HV-LCO pouch cells with long cycle life (85.3% capacity retention after 700 cycles), wide-temperature adaptability (− 60–80 °C) and high safety (pass nail penetration). This work provides new insights into the electrolyte screening and rational design to constructing stable interface for high-energy lithium-ion batteries.