Alleviating the decomposition of the electrolyte is of great significance to improving the cycle stability of cathodes, especially for LiCoO2 (LCO), its volumetric energy density can be effectively promoted by increasing the charge cutoff voltage to 4.6 V, thereby supporting the large‐scale application of clean energy. However, the rapid decomposition of the electrolyte under 4.6 V conditions not only loses the transport carrier for lithium ion, but also produces HF and insulators that destroy the interface of LCO and increase impedance. In this work, the decomposition of electrolyte is effectively suppressed by changing the adsorption force between LCO interface and EC. Density functional theory illustrates the LCO coated with lower electronegativity elements has a weaker adsorption force with the electrolyte, the adsorption energy between LCO@Mg and EC (0.49 eV) is weaker than that of LCO@Ti (0.73 eV). Meanwhile, based on the results of time of flight secondary ion mass spectrometry, conductivity‐atomic force microscopy, in situ differential electrochemical mass spectrometry, soft X‐ray absorption spectroscopy, and nuclear magnetic resonance, as the adsorption force increases, the electrolyte decomposes more seriously. This work provides a new perspective on the interaction between electrolyte and the interface of cathode and further improves the understanding of electrolyte decomposition.

中文翻译：

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通过界面吸附力的调节抑制电解质分解行为以提高 LiCoO2 在 4.6 V 下的循环性能

减轻电解液的分解对于提高正极的循环稳定性具有重要意义，特别是对于LiCoO2（LCO），通过将充电截止电压提高至4.6 V，可以有效提升其体积能量密度，从而支持清洁能源的大规模应用。然而，电解液在4.6 V条件下的快速分解不仅失去了锂离子的传输载体，而且产生了HF和绝缘体，破坏了LCO的界面并增加了阻抗。在这项工作中，通过改变LCO界面和EC之间的吸附力来有效抑制电解质的分解。密度泛函理论表明，涂覆较低电负性元素的LCO对电解质的吸附力较弱，LCO@Mg和EC之间的吸附能（0.49 eV）弱于LCO@Ti（0.73 eV）。同时，根据飞行时间二次离子质谱、电导原子力显微镜、原位微分电化学质谱、软X射线吸收光谱和核磁共振的结果，随着吸附力的增加，电解质分解得更多。严重地。这项工作为电解质与正极界面之间的相互作用提供了新的视角，并进一步提高了对电解质分解的理解。