Mechanism of high-concentration electrolyte inhibiting the destructive effect of Mn(II) on the performance of lithium-ion batteries

电解质 电化学 锂(药物) 溶剂化 阳极 溶解 离子 电池(电) 介电谱 化学 材料科学 密度泛函理论 化学工程 溶剂化壳 无机化学 计算化学 电极 医学 物理化学 有机化学 热力学 物理 工程类 功率(物理) 内分泌学
作者
Xiaoling Cui,Jinlong Sun,Dongni Zhao,Jingjing Zhang,Jie Wang,Hong Dong,Peng Wang,Junwei Zhang,Shumin Wu,Linhu Song,Ningshuang Zhang,Chunlei Li,Shiyou Li
出处
期刊:Journal of Energy Chemistry [Elsevier BV]
卷期号:78: 381-392 被引量:20
标识
DOI:10.1016/j.jechem.2022.12.008
摘要

By optimizing electrolyte formulation to inhibit the deposition of transition metal ions (TMIs) on the surface of the graphite anode is an effective way to improve the electrochemical performance of lithium-ion batteries. At present, it is generally believed the formation of an effective interfacial film on the surface of the anode electrode is the leading factor in reducing the dissolution of TMIs and prevent TMIs from being embedded in the electrode. It ignores the influence of the solvation structures in the electrolyte system with different composition, and is not conducive to the design of the electrolyte formulation from the perspective of changing the concentration and the preferred solvent to inhibit the degradation of battery performance caused by TMIs deposition. In this work, by analyzing the special solvation structures of the high-concentration electrolyte, we study the main reason why high-concentration electrolyte inhibits the destructive effect of Mn (II) on the electrochemical performance of LIBs. By combining the potential-resolved in-situ electrochemical impedance spectroscopy technology (PRIs-EIS) and density functional theory (DFT) calculation, we find that Mn (II) mainly exists in the form of contact ions pairs (CIPs) and aggregates (AGGs) in high-concentration electrolyte. These solvation structures can reduce the destructive effect of Mn (II) on battery performance from two aspects: on the one hand, it can rise the lowest unoccupied orbital (LUMO) value of the solvation structures of Mn (II), thereby reducing the chance of its reduction; on the other hand, the decrease of Mn2+ ions reduction can reduce the deposition of metallic manganese in the solid electrolyte interphase (SEI), thereby avoiding the continuous growth of the SEI. This study can be provided inspiration for the design of electrolytes to inhibit the destructive effect of TMIs on LIBs.
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