The safety issue of lithium batteries
based on liquid electrolytes
has become the focus of attention, especially when the batteries are
exposed to mechanical, thermal, or electrical abuse conditions. To
address this issue, gel polymer electrolytes (GPEs) have attracted
widespread interest due to the property of solid–liquid coexistence
with higher ionic conductivity, flexibility, and safety. In this work,
a poly(vinylidene-fluoride-co-hexafluoropropylene)
(PVDF-HFP)/poly(methyl methacrylate) (PMMA) matrix GPE, containing
bis(trifluoromethane)sulfonimide lithium salt (LiTFSI) and spherical
zirconium dioxide (ZrO2) nanoparticles, is successfully
designed and synthesized by a simple one-step solution-casting route.
It has been found that the obtained PVDF-HFP/PMMA-ZrO2-6%
(PPZ-6%) electrolyte film possesses an excellent tensile strength
of 37.7 MPa. Moreover, the PPZ-6% GPE not only has a high ionic conductivity
of 1.46 × 10–3 S cm–1 at
25 °C but also presents excellent interface compatibility in
an Li||Li symmetrical battery. The LiFePO4||Li cell assembled
with the PPZ-6% GPE exhibits good cyclic stability at room temperature,
e.g., a high discharge specific capacity of 153.0 mAh g–1, and a high Coulombic efficiency of 99% after 200 cycles at 0.5
C. Therefore, this organic–inorganic hybrid GPE modified with
spherical ZrO2 nanoparticles reveals a good application
prospect for high-performance lithium metal batteries (LMBs).