All-Polymer Nanocomposite as Salt-Free Solid Electrolyte for Lithium Metal Batteries

Solid polymer electrolytes that combine both a high lithium-ion transference number and mechanical properties at high temperatures are searched for improving the performance of batteries. Here, we show a salt-free all-polymer nanocomposite solid electrolyte for lithium metal batteries that improves the mechanical properties and shows a high lithium-ion transference number. For this purpose, lithium sulfonamide-functionalized poly(methyl methacrylate) nanoparticles (LiNPs) of very small size (20–30 nm) were mixed with poly(ethylene oxide) (PEO). The morphology of all-polymer nanocomposites was first investigated by transmission electron microscopy (TEM), showing a good distribution of nanoparticles (NPs) even at high contents (50 LiNP wt %). The crystallinity of PEO was investigated in detail and decreased with the increasing concentration of LiNPs. The highest ionic conductivity value for the PEO 50 wt % LiNP nanocomposite at 80 °C is 1.1 × 10^–5 S cm^–1, showing a lithium-ion transference number of 0.68. Using dynamic mechanic thermal analysis (DMTA), it was shown that LiNPs strengthen PEO, and a modulus of ≈10⁸ Pa was obtained at 80 °C for the polymer nanocomposite. The nanocomposite solid electrolyte was stable with respect to lithium in a Li||Li symmetrical cell for 1000 h. In addition, in a full solid-state battery using LiFePO₄ as the cathode and lithium metal as the anode, a specific capacity of 150 mAhg^–1 with a current density of 0.05 mA cm^–2 was achieved.