碳酸二甲酯
酯交换
锂(药物)
材料科学
硝酸锂
电化学
无机化学
溶解
磷酸三甲酯
轨道能级差
电池(电)
阴极
阳极
溶剂化
化学工程
分解
溶剂
化学
磷酸盐
分子
离子
有机化学
催化作用
电极
工程类
电解质
离子键合
内分泌学
物理化学
医学
功率(物理)
物理
量子力学
作者
Yuanhang Gao,Gang Wu,Wenqiang Fang,Zuosu Qin,Tao Zhang,Jiaxing Yan,Yu Zhong,Ning Zhang,Gen Chen
标识
DOI:10.1002/anie.202403668
摘要
The electrolyte chemistry is crucially important for promoting the practical application of lithium metal batteries (LMBs). Here, we demonstrate for the first time that 1,3‐dimethylimidazolium dimethyl phosphate (DIDP) and trimethylsilyl trifluoroacetate (TMSF) can undergo in situ transesterification in carbonate electrolyte to generate dimethyl trimethylsilyl phosphate (DTMSP) and 1,3‐dimethylimidazolium trifluoroacetate (DITFA) as multifunctional additives for LMBs. H2O and HF can be removed by the Si−O group in DTMSP to improve the moisture resistance of electrolyte and the stability of cathode. Furthermore, the dissolution of lithium nitrate (LiNO3) in carbonate electrolyte can be promoted by the trifluoroacetate anion (TFA−) in DITFA, thereby optimizing the solvation structure and transport kinetics of Li+. More importantly, both DTMSP and DITFA tend to preferential redox decomposition due to the low lowest unoccupied molecular orbital (LUMO) and high highest occupied molecular orbital (HOMO). Consequently, a thin and robust layer rich in P/N/Si on the cathode and an inorganic‐rich layer (e.g. Li3N/Li3P) on the anode can be constructed and superior electrochemical performances are achieved. This artificial transesterification strategy to introduce favorable additives paves an efficient and ingenious route to high‐performance electrolyte for LMBs.
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