Preparation of Nanocomposite Polymer Electrolyte via In Situ Synthesis of SiO₂ Nanoparticles in PEO

Composite polymer electrolytes provide an emerging solution for new battery development by replacing liquid electrolytes, which are commonly complexes of polyethylene oxide (PEO) with ceramic fillers. However, the agglomeration of fillers and weak interaction restrict their conductivities. By contrast with the prevailing methods of blending preformed ceramic fillers within the polymer matrix, here we proposed an in situ synthesis method of SiO₂ nanoparticles in the PEO matrix. In this case, robust chemical interactions between SiO₂ nanoparticles, lithium salt and PEO chains were induced by the in situ non-hydrolytic sol gel process. The in situ synthesized nanocomposite polymer electrolyte delivered an impressive ionic conductivity of ~1.1 × 10^-4 S cm^-1 at 30 °C, which is two orders of magnitude higher than that of the preformed synthesized composite polymer electrolyte. In addition, an extended electrochemical window of up to 5 V vs. Li/Li⁺ was achieved. The Li/nanocomposite polymer electrolyte/Li symmetric cell demonstrated a stable long-term cycling performance of over 700 h at 0.01-0.1 mA cm^-2 without short circuiting. The all-solid-state battery consisting of the nanocomposite polymer electrolyte, Li metal and LiFePO₄ provides a discharge capacity of 123.5 mAh g^-1, a Coulombic efficiency above 99% and a good capacity retention of 70% after 100 cycles.