基于激光织构化界面设计的全固态锂金属电池性能研究

高能量密度和高安全性能的全固态锂金属电池是未来锂电池重点发展方向之一，对我国的能源转型至关重要。部分固态电解质的室温离子导电率已经能够满足实用化需求，但固态电解质与电极材料间较大的界面阻抗是限制全固态电池真正实现商业化应用的最大瓶颈。针对全固态电池界面问题，本文采用皮秒加工技术构建三维固态电解质/电极界面结构，为锂离子提供更多反应位点及交换通道，降低全固态电池界面阻抗，提高电池循环稳定性以及倍率性能。具体研究内容及结论如下：

（1）根据电化学模型结合有限元仿真技术，分析不同电解质/电极界面结构下电流密度及应力分布情况。仿真结果表明V字型界面结构能够有效降低电流集中效应。

（2）在仿真分析基础上，利用皮秒加工技术制备了具有周期性锥孔结构的3D-LAGP（Li_1.5Al_0.5Ge_1.5（PO₄）₃）固态电解质。以3D-LAGP构建的Li/3D-LAGP/Li对称电池的界面阻抗降低了54%，并且在0.05 mA cm^-2电流密度下可以稳定循环超过700 h。以LiFePO₄为正极的全电池的界面阻抗也下降了52%，同时循环与倍率性能也得到了显著的提升。

（3）通过球磨法制备了金属锂化学相容性更好的LAGP-PEO复合固态电解质，当LAGP质量分数为40%时，复合电解质室温离子导电率达到7.4×10^-6 S cm^-1。结合皮秒激光加工技术构建具有三维界面结构的Li/40%LAGP-PEO/3D-LFP全固态锂金属电池体系。该体系的界面阻抗从350 Ω cm^-2降低至162 Ω cm^-2，并且在0.1 C电流密度下循环充放电100次后容量保持率高达81.5%，同时也表现出了更好的倍率性能。

本文基于无机陶瓷与复合固态电解质体系构建的具有三维界面结构的锂金属电池在界面阻抗、循环稳定性以及倍率性能等方面都有显著的提升。不同于常见的无规则三维界面结构，本文基于有限元仿真分析以及精密加工技术构建的规则界面结构能够减轻电流集中效应以及提高界面结构稳定性，为三维界面结构的研究提供了一种全新的思路。

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