基于梳型聚己内酯固态电解质的研究

聚己内酯是一种环境友好的酯类聚合物，拥有良好的链段柔顺性和高的介电常数。基于该类聚合物的固态电解质具有宽的电化学稳定窗口以及高的锂离子迁移数。与线性聚己内酯相比，梳型的聚己内酯由于其更好的链段运动能力和更高的介电常数，因此理论上具有更好的传输锂离子能力。本课题设计、合成与表征了一种梳型结构的聚己内酯，并将其与双氟磺酰亚胺锂复合制备出一种高浓盐聚合物固态电解质。将该电解质与静电纺丝法制备得到的聚酰亚胺膜进行复合后，制备出力学性能良好的聚合物固态电解质膜。该聚合物固态电解质在室温下离子电导率可达4´10⁻⁴ S·cm^-1，电化学窗口为4.8 V，锂离子迁移数可达0.61，离子迁移活化能为0.19 eV。将该聚合物固态电解质用于组装磷酸铁锂全固态锂电池并在室温下进行测试，其容量发挥特性十分优异。在0.1 C、0.2 C、0.5 C、0.7 C和1.0 C倍率下进行循环充放电，放电比容量分别为147 mAh·g⁻¹、140 mAh·g⁻¹、130 mAh·g⁻¹、120 mAh·g⁻¹和115 mAh·g⁻¹。该电池在0.2 C倍率下循环160圈后，平均库伦效率大于99.5%，在0.5 C倍率下循环300圈后容量保持率为92%，库伦效率接近100%。对充电循环后的锂金属负极表面进行扫描电镜与X射线光电子能谱分析，发现该SEI界面层有高含量的LiF，有助于稳定负极界面和抑制锂枝晶。

本课题通过制备梳型结构聚己内酯以提高锂盐溶解度，从而大幅提高聚合物固态电解质的离子电导率，利用过量锂盐在锂金属负极表面分解生成富含LiF的稳定致密SEI，为今后研发设计聚合物固态电解质提供了很好的思路。

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