Zhang Tao, Shen Zhengyuan, Pan Xinhui, Zhang Man, Lian Tong, Shi Keqing, Qian Ji, Li Li, Wu Feng, Chen Renjie
Shandong Key Laboratory of Advanced Chemical Energy Storage and Intelligent Safety, Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300, China.
Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
Angew Chem Int Ed Engl. 2025 Sep 4:e202510624. doi: 10.1002/anie.202510624.
Lithium-sulfur batteries have been regarded as a promising candidate for next-generation energy storage systems owing to their high energy density and low cost. Sulfurized polyacrylonitrile (SPAN) as a cathode material has received wide interest due to the solid-solid conversion mechanism, while the Li-SPAN cell performance has been limited by the notorious issue of lithium metal anode. Developing solid-state electrolytes for lithium-sulfur batteries with favorable electrode-electrolyte compatibility is urgently desired. Herein, we demonstrate a dual-interface optimization strategy through in-situ polymerization interface construction, which synergistically enhances interfacial compatibility between the solid polymer electrolyte (SPE) and both the lithium metal anode and SPAN cathode. The initiator pre-buried in the SPE triggers the in-situ polymerization of 1,3-dioxolane (DOL) at the interface, thereby greatly reducing the electrode/electrolyte interfacial impedance. Additionally, the released fluoroethylene carbonate (FEC) into the poly-DOL interface could further reduce the impedance and enhance the interface stability during cycling, simultaneously preventing the dissolution of polysulfides, owing to the inorganic-rich and dense cathode electrolyte interphase formed on SPAN. As a result, the Li-SPAN cell could operate more than 200 cycles at 0.5C with a capacity retention of 90%. We believe that this strategy provides prospects for the development of high-energy solid-state lithium-sulfur batteries.
锂硫电池因其高能量密度和低成本，被视为下一代储能系统的一个有前景的候选者。硫化聚丙烯腈（SPAN）作为一种阴极材料，由于其固-固转化机制而受到广泛关注，然而锂硫电池的性能一直受到锂金属阳极这一棘手问题的限制。迫切需要开发具有良好电极-电解质兼容性的锂硫电池固态电解质。在此，我们通过原位聚合界面构建展示了一种双界面优化策略，该策略协同增强了固体聚合物电解质（SPE）与锂金属阳极和SPAN阴极之间的界面兼容性。预先埋入SPE中的引发剂触发了界面处1,3-二氧戊环（DOL）的原位聚合，从而大大降低了电极/电解质界面阻抗。此外，释放到聚-DOL界面中的氟代碳酸乙烯酯（FEC）可以进一步降低阻抗并增强循环过程中的界面稳定性，同时由于在SPAN上形成了富含无机物且致密的阴极电解质界面层，防止了多硫化物的溶解。结果，锂硫电池在0.5C下可运行超过200次循环，容量保持率为90%。我们相信，这一策略为高能固态锂硫电池的发展提供了前景。
