All-solid-state lithium metal batteries (ASSLMBs) have
garnered
significant interest as a result of their enhanced safety features
and higher energy density compared to traditional lithium-ion batteries
with liquid electrolytes. Nonetheless, a substantial challenge within
ASSLMBs lies in the constrained lithium-ion flux encountered in solid-state
polymer electrolytes, resulting in subpar performance during high-current
charging and discharging scenarios. This limitation detrimentally
affects the electrochemical performance of ASSLMBs. In this present
work, we introduce a novel composite solid polymer electrolyte (CSPE)
comprising metal–organic frameworks, namely, UiO-66, poly(vinylidene
fluoride-co-hexafluoropropylene) (PVDF-HFP), and
lithium bis(trifluoromethane)-sulfonimide (LiTFSI) (referred to as
UPH-SPE). UPH-SPE containing 5 wt % UiO-66 demonstrates exceptional
characteristics, including a high ionic conductivity of 4.7 ×
10–4 S cm–1, an electrochemical
stability window of 4.9 V, and a remarkable lithium-ion transference
number of 0.58 at 25 °C. Full cell tests unequivocally showcase
that these newly developed composite electrolytes exhibit significantly
improved performance in terms of the rate capability and cycling stability
at room temperature. Specifically, the discharge capacity of ASSLMBs
with UPH-SPE remains at 140 mAh g–1 when operated
at a current density of 0.5 C over 100 cycles. Even after 200 cycles,
the capacity is sustained at 94 mAh g–1. This study
underscores the potential of our CSPE film to advance the practical
application of ASSLMBs, offering promising prospects for future developments
in this field.