Poly(ethylene oxide) (PEO)-based solid-state polymer electrolyte (SPE) is a promising candidate for the next generation of safer lithium-metal batteries. However, the serious side reaction between PEO and lithium metal and the uneven deposition of lithium ions lead to the growth of lithium dendrites and the rapid decline of battery cycle life. Building a LiF-rich solid electrolyte interface (SEI) layer is considered to be an effective means to solve the above problems. Here, porous organic polymers (POPs) with aromatic structures and non-aromatic structures were synthesized and introduced into the PEO-based SPE as fillers to explore the effect of aromatic structures on LiF-rich SEI formation. The results show that the POPs containing aromatic groups could catalyze the decomposition of LiTFSI to form a stable LiF-rich SEI layer and inhibit the growth of lithium dendrites. The discharge capacity of the LFP/Li battery is 103 mA h g-1 after 500 cycles at 1C (100 °C). It provides a promising way to improve the stability of the solid electrolyte matrix and SEI layer.
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