Poly(ethylene oxide) (PEO)-based
composite solid electrolytes (CSEs)
are considered as one of the most promising candidates for all-solid-state
lithium batteries (ASSLBs). However, a key challenge for their further
development is to solve the main issues of low ionic conductivity
and poor mechanical strength, which can lead to insufficient capacity
and stability. Herein, β-cyclodextrin (β-CD) is first
demonstrated as a multifunctional filler that can form a continuous
hydrogen bond network with the ether oxygen unit from the PEO matrix,
thus improving the comprehensive performances of the PEO-based CSE.
By relevant characterizations, it is demonstrated that β-CD
is uniformly dispersed into the PEO substrate, inducing adequate dissociation
of lithium salt and enhancing mechanical strength through hydrogen
bond interactions. In a Li/Li symmetric battery, the β-CD-integrated
PEO-based (PEO-LiTFSI-15% β-CD) CSE works well at a critical
current density up to 1.0 mA cm–2 and retains stable
lithium plating/stripping for more than 1000 h. Such reliable properties
also enable its superior performance in LiFePO4-based ASSLBs,
with specific capacities of 123.6 and 114.0 mA h g–1 as well as about 100 and 81.8% capacity retention over 300 and 700
cycles at 1 and 2 C (1 C = 170 mA g–1), respectively.