Gan Huihui, Ying Siqi, Dong Jia, Zheng Shizheng, Hu Changyuan, Ai Jianping, Wang Jing, Zhou Binghua
Jiangxi Provincial Key Laboratory of Surface Engineering, College of Materials and Energy, Jiangxi Science and Technology Normal University, Nanchang, P. R. China.
College of Chemistry and Materials, Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Jiangxi Normal University, Nanchang, P. R. China.
Macromol Rapid Commun. 2025 Sep;46(18):e00306. doi: 10.1002/marc.202500306. Epub 2025 Jun 29.
Rechargeable lithium batteries, including lithium-ion batteries, lithium metal batteries, and lithium-sulfur batteries, face significant safety concerns such as electrolyte leakage, flammability, and explosion when using conventional organic liquid electrolytes. Therefore, developing high-safety polymer electrolytes (PEs) is an urgent necessity. From the perspective of the preparation process, PEs fabricated via the solution-casting method or blade-casting process often suffer from poor solid/solid interfacial contact between the PEs and electrodes. This issue leads to high interface impedance and degraded cell performance. Compared to other methods, the in situ polymerization strategy is particularly advantageous for achieving excellent interfacial contact between the PEs and electrodes. This approach significantly reduces the interfacial resistance and efficiently promote Li-ion transport. This review aims to provide a comprehensive summary of the in situ polymerization processes, including free-radical polymerization, ion-initiated polymerization, as well as the materials involved, such as backbone materials, monomers, lithium salts, and initiators. Through this analysis, the review highlights how these processes can be optimized to improve the safety performance and achieve good interface stability between the PEs and electrodes. Additionally, this review evaluates the challenges and development trends of in situ polymerized electrolytes for high safety lithium batteries in the future.
包括锂离子电池、锂金属电池和锂硫电池在内的可充电锂电池，在使用传统有机液体电解质时面临着诸如电解液泄漏、易燃性和爆炸等重大安全问题。因此，开发高安全性的聚合物电解质（PEs）迫在眉睫。从制备工艺的角度来看，通过溶液浇铸法或刮刀浇铸工艺制备的聚合物电解质，在聚合物电解质与电极之间常常存在不良的固/固界面接触。这个问题导致高界面阻抗和电池性能下降。与其他方法相比，原位聚合策略在实现聚合物电解质与电极之间的优异界面接触方面具有特别的优势。这种方法显著降低了界面电阻，并有效地促进了锂离子传输。本综述旨在全面总结原位聚合过程，包括自由基聚合、离子引发聚合，以及所涉及的材料，如主链材料、单体、锂盐和引发剂。通过这一分析，本综述强调了如何优化这些过程以提高安全性能，并在聚合物电解质与电极之间实现良好的界面稳定性。此外，本综述评估了未来高安全性锂电池原位聚合电解质面临的挑战和发展趋势。
