Lithium-Rich Porous Aromatic Framework Doped Quasi-Solid Polymer Electrolyte for Lithium Battery with High Cycling...

Lithium-ion batteries (LIBs) have revolutionized the energy storage landscape and are the preferred power source for various applications, ranging from portable electronics to electric vehicles. The constant drive and growth in battery research and development aim to enhance their performance, energy density, and safety. Advanced lithium batteries (LIBs) are considered to be the most promising electrochemical storage devices, which can provide high specific energy, volumetric energy density, and power density. However, the trade-off between ionic conductivity and cycling stability is still a major contradiction for SPEs. In this work, a novel hydroxylated PAF-1 was designed and synthesized through post-modification, and the lithium-rich single-ion porous aromatic framework PAF-1-OLi was thereafter prepared by lithiation, achieved with a specific surface area to be 155 m² g^-1 and a lithium content of 2.01 mmol g^-1. PAF-1-OLi, lithium bis(trifluoromethanesulfony)limine (LiTFSI), and poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) were compounded to obtain PAF-1-OLi/PVDF by solution casting, which had good mechanical, thermodynamic, and electrochemical properties. The ion conductivity of PAF-1-OLi/PVDF infiltrated with plasticizer was 2.93 × 10^-4 S cm^-1 at 25 °C. The t_Li was 0.77, which was much higher than that of the traditional dual-ion polymer electrolytes. The electrochemical window of PAF-1-OLi/PVDF can reach 4.9 V. The Li//PAF-1-OLi/PVDF//LiFePO₄ battery initial discharge specific capacity was 147 mAh g^-1 and reached 134.9 mAh g^-1 after 600 cycles with a capacity retention rate of 91.2%, demonstrating its good cycling stability. The anionic part of lithium salt was fixed on the framework of PAF-1 to increase the Li⁺ transfer number of PAF-1-OLi/PVDF. The lithium-rich PAF-1-OLi and the LiTFSI provided abundant Li⁺ sources to transfer, while PAF-1-OLi helped to form a continuous Li⁺ transport channel, effectively promoting the migration of Li⁺ in the PAF-1-OLi/PVDF and effectively improving the Li⁺ conductivity. This study afforded a novel polymer electrolyte based on lithium-rich PAF-1-OLi, which has excellent electrochemical performance, providing a new choice for the polymer electrolyte of lithium batteries.