Abstract

Benefiting from employing solid composite electrolytes (SCEs), all‐solid‐state lithium‐ion batteries (ASSLBs) are recognized to occupy with high energy density and safety. Herein, a polymer‐based SCE membrane (SCE‐66@67) with core–shell structured metal–organic frameworks (MOFs) (UiO‐66‐NH2@67) as the fillers is presented. The SCE has combined the advantages of the two kinds of MOFs and shows a satisfying ionic conductivity (2.09 × 10−4 S cm−1 at 60 °C) and a wide electrochemical stability window of ≈5.0 V. The full cell (Li/SCE‐66@67/LiFePO4) also maintains a high capacity of 120.9 mAh g−1 at 3 C. This research might help to promote the development of future SCEs for ASSLBs.

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