Developing a poly(ethylene oxide) (PEO)-based polymer
electrolyte
with high ionic conductivity and robust mechanical property is beneficial
for real applications of all-solid-state lithium metal batteries (ASSLMBs).
Herein, an excellent organic/inorganic interface compatibility of
all-solid-state composite polymer electrolytes (CPEs) is achieved
using a novel imidazolium-type poly(ionic liquid) with strong electrostatic
interactions, providing insights into the achievement of highly stable
CPEs. The key properties such as micromorphologies, thermal behavior,
crystallinity, t
Li
+, mechanical property, lithium anode surficial
morphology, and electrochemical performance are systematically investigated.
The combined experimental and density functional theory (DFT) simulation
results exhibit that the strong electrostatic interaction and ion–dipole
interaction cooperated to improve the compatibility of the CPE, with
a high ionic conductivity of 1.46 × 10–4 S
cm–1 at 40 °C and an incredible mechanical
strain of 2000% for dendrite-free and highly stable all-solid-state
LMBs. This work affords a promising strategy to accelerate the development
of PEO-based polymer electrolytes for real applications in ASSLMBs.