RESUMEN
Severe electrolyte decomposition under high voltage can easily lead to degradation of the performance of lithium-ion batteries, which has become a major obstacle to the practical application of high-energy-density batteries. To solve these problems, a dual-functional electrolyte additive comprising inorganic lithium difluorophosphate (LiDFP) and organic 1,3,6-hexanetrinitrile (HTN) was designed and employed to improve the performance of high-voltage Si@C/LiNi0.5Mn1.5O4 full batteries. LiDFP with a lower LUMO energy than the solvent in the electrolyte takes priority in reduction, facilitating the formation of a dense and stable film on the anode, effectively suppressing side reactions of the electrolyte and aiding tolerance to the volume expansion of the Si@C electrode. Additionally, the lower HOMO energy of HTN can improve the oxidation resistance of the electrolyte, with the C≡N functional group of HTN helping to remove the trace water and the byproduct HF from the electrolyte. The Si@C/LiNi0.5Mn1.5O4 full battery with 1 wt % LiDFP and 1 wt % HTN in 1.0 M LiPF6 traditional electrolyte delivers high capacity retention of 91.57% after 150 cycles at 0.2C, compared to 34.58% capacity retention without any additives. Moreover, the Coulombic efficiency of batteries with electrolyte additives can reach 99.75% on average, compared to their counterparts at â¼96.54%. The synergistic effect of LiDFP and HTN provides a promising strategy for enhancing the performance of high-voltage batteries for practical industrialization.
RESUMEN
The electrolyte of a lithium ion battery is unstable and is easily decomposed at high temperature, which can lead to the degradation of battery performance. To solve this problem, herein a novel electrolyte additive 1-(2-cyanoethyl)pyrrole (CP) has been proposed to improve the electrochemical performance of LiFePO4 batteries at high temperature. The capacity retention of the battery with 1 wt% CP is 76.7%, while that of the battery without the additive is 38.1% after 200 cycles at 60 °C. Theoretical calculation results reveal that the binding energy of CP and PF5/HF is much higher than that of the solvents in the electrolyte. Surface analysis of the electrodes demonstrates that CP can reduce the decomposition of the electrolyte, and restrain the dissolution of transition metals in the electrolyte at high temperature. TEM/XPS results indicate that CP can modify the protective film on the surface of the cathode material and promote the formation of more regular and thinner CEI films. The promotion of the CP additive is of great significance for improving the high temperature performance of lithium ion batteries and is expected to be applied on a large scale.