Solid polymer electrolytes (SPEs) with high ionic conductivity
and strong mechanical properties are preconditions for the stable
cycling of high-performance Li metal batteries. However, single-polymer
SPEs often have low ionic conductivity, which greatly limits their
further application. Herein, a SPE composed of polyvinyl alcohol (PVA),
reactive aramid nanofibers (RANFs), and lithium bistrifluoromethanesulfonimide
(LiTFSI) is prepared using a simple solution-casting method. After
introducing the RANFs, the SPE of RANFs/PVA-containing LiTFSI not
only exhibits high mechanical properties but also has good thermal
stability. The RANFs/PVA SPE constructed from the strong hydrogen
bond interaction between rigid RANFs and flexible PVA shows high migration
efficiency of lithium ions. When the loading amount of RANFs is 2
wt %, the ionic conductivity of RANFs/PVA reaches ∼7.7 ×
10 –4 S·cm–1, and the lithium-ion
migration number is ∼0.54 at 60 °C. Toward the Li|RANFs/PVA-2
wt %|LiFePO4 full cell, the discharge specific capacity
could reach 162.5 mA h·g–1 at 60 °C and
0.1 C. Meanwhile, the Li|RANFs/PVA-2 wt %|LiFePO4 battery
also shows outstanding long-term cycling performance and could maintain
81% of the initial capacity after 1200 cycles at 1 C. The solid-state
Li|RANFs/PVA|LiFePO4 cell also exhibits excellent resilience
in destructive tests such as cell bending, piercing, and cutting.