醚基电解液中成膜添加剂稳定三元锂金属电池界面的研究

锂金属负极具有高比容量（3860 mAh g^-1）和低电化学电势（与标准氢电极相比为-3.040 V）的优势，有望取代石墨成为新一代负极材料。然而，商业化碳酸酯电解液还原稳定性较差，易与锂金属反应并生成过厚且脆弱的固体电解质界面，导致电池容量损失和锂枝晶生长。针对这些问题，本文以醚类溶剂（DME）为电解液主体，引入两种锂盐型添加剂（二氟草硼酸锂，LiDFOB与二氟磷酸锂，LiDFP）与溶剂型添加剂（氟代碳酸乙烯酯，FEC），通过调控溶剂化结构与设计固体电解质界面（SEI），制备耐高电压NCM811（LiNi_0.8Co_0.1Mn_0.1O₂）锂金属电池。本文引入两种锂盐型添加剂LiDFOB和LiDFP，成功提高醚基电解液在高镍三元-锂金属电池中的长循环性能。LiDFOB和LiDFP具备协同作用，两者能互相抑制对方在循环初期的剧烈分解，在长循环中发挥更稳定作用。基于该电解液的Li || NCM811电池（正极负载3.5 mAh cm^-2），在2.8-4.4 V电化学窗口下，以1 C倍率稳定循环150圈（容量保持率76%）。进一步提升醚基电解液在Li||NCM811电池的长循环表现，本文引入溶剂型添加剂氟代碳酸乙烯酯，借助不同种类添加剂的协同作用提升电池性能，基于该电解液的Li||NCM811电池（正极负载3.5 mAh cm^-2），在4.4 V高电压下以1 C倍率稳定循环300圈，容量保持率高达86.3%。由于锂盐型添加剂与溶剂型添加剂的协同作用，LiDFOB和LiDFP分解形成最初的表面膜基质，生成富含LiF、Li₂O等无机颗粒的SEI，该类SEI具有优良力学性能。此外，FEC在后续长循环中充当修补剂，在SEI界面破损后进行修复，且FEC分解形成有机聚合物能有效增强SEI界面的韧性。三种添加剂共同作用下的界面膜均匀且致密，对正负极均起到良好的保护效果。

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