非对称超薄电解质膜在固液混合电池中的应用及其界面机理研究

作为电池的重要组成部分，隔膜起着分隔正、负极并为锂离子提供自由传输通道的作用，其物理和化学性能对电池的性能有着显著影响。通过改性隔膜，可以有效提高隔膜的热稳定性、电化学稳定性、电解液润湿性，增强隔膜中锂离子的迁移动力学，实现隔膜更优异的电化学性能。但是基于固态电解质的隔膜改性工作研究还不够深入完善，特别是固态电解质涂层的界面作用机制及其对电极界面的影响机理亟需深入研究。

本文基于锂镧锆钽氧（LLZTO）和磷酸钛铝锂（LATP）固态电解质的优点， 设计了一种适用于固液混合锂电池的超薄非对称固态电解质膜（SWS@PE），主要通过简单的刮刀涂覆法在超薄9 μm PE 隔膜的两侧分别均匀涂覆2 μm 的LLZTO 层和1 μm 的LATP 层，最终制备出厚度约12 μm 的超薄固态电解质膜。SWS@PE 不仅具有出色的物理性能，还具有优异的电化学性能。涂覆的固态电解质涂层可以参与锂离子的传输，增强锂离子的迁移动力学，最终SWS@PE  Li||NCM811 全电池中实现了更好的倍率性能和更优异的长循环性能。通过对电解质涂层的作用机理研究发现，LLZTO 涂层可以有效吸附FSI−，在负极侧实现阴离子的富集，LATP 涂层则可以有效吸附溶出的过渡金属离子，从而减少其在锂负极上的沉积。得益于电解质涂层的界面作用，在负极上形成了更富含LiF 的固体电解质界面相（SEI），正极上形成了薄且均匀的CEI。

本文设计的SWS@PE，制备方法简单，兼具优异的物理和电化学性能，具有投入实际应用的潜力。此外，对LATP 和LLZTO 电解质涂层的界面作用和对电极界面的影响进行了深入研究，为后续使用固态电解质材料进行隔膜改性以定制功能化隔膜提供了一定的理论基础和方法指导。

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