LATP-Enhanced Polymer Electrolyte for an Integrated Solid-State Battery.

Traditional liquid electrolyte batteries face safety concerns such as leakage and flammability, while further optimization has reached a bottleneck. Solid electrolytes are therefore considered a promising solution. Here, a PEO-LiTFSI-LATP (PELT) composite electrolyte was developed by incorporating nanosized Li1.3Al0.3Ti1.7(PO4)3 fillers into a polyethylene oxide matrix, effectively reducing crystallinity, enhancing mechanical robustness, and providing additional Li+ transport channels. The PELT electrolyte exhibited an electrochemical stability window of 4.9 V, an ionic conductivity of 1.2 × 10-4 S·cm-1 at 60 °C, and a Li+ transference number (tLi+) of 0.46, supporting stable Li plating/stripping for over 600 h in symmetric batteries. More importantly, to address poor electrode-electrolyte contact in conventional layered cells, we proposed an integrated electrode-electrolyte architecture by in situ coating the PELT precursor directly onto LiFePO4 cathodes. This design minimized interfacial impedance, improved ion transport, and enhanced electrochemical stability. The integrated PELT/LFP battery retained 74% of its capacity after 200 cycles at 1 A·g-1 and showed superior rate capability compared with sandwich-type batteries. These results highlight that coupling LATP-enhanced polymer electrolytes with an integrated architecture is a promising pathway toward high-safety, high-performance solid-state lithium-ion batteries.