Poly­(ethylene oxide) (PEO)-based polymer electrolytes have shown extraordinary promise for all-solid-state lithium batteries; however, the practical application was severely restricted by their low ionic conductivity. In this work, the robust pores of HKUST-1­(Cu) were first filled by a lithium-containing ionic liquid (Li-IL) to form ion-conductive Li-IL@HKUST-1. Subsequently, flexible composite polymer electrolytes (CPEs) were constructed via a solution-casting approach upon the incorporation of Li-IL@HKUST-1 with PEO. The as-synthesized CPE membrane showed a high ionic conductivity of 1.20 × 10–4 S cm–1 at 30 °C compared to 9.76 × 10–6 S cm–1 for the PEO-only electrolyte. Furthermore, the assembled LiFePO4/Li solid-state batteries delivered a stable reversible capacity of 136.2 mAh g–1 with a capacity retention of 92% after 100 cycles at a high current density of 1 C (60 °C). The excellent electrochemical performance was mainly attributed to the combination of Li-IL@HKUST-1 and the PEO matrix, which effectively reinforced the polymer matrix and facilitated the fast transport of lithium ions. The present research provides an effective strategy for building high-performance all-solid-state lithium batteries.

Electrode design strategies that aim to increase the electrochemical performance of Li‐ion batteries (LIBs) play a key role in tapping into the power of the energy transformations involved. Metal‐organic frameworks (MOFs) have attracted scientific interest as electrode materials for LIBs, while the utilization of pristine MOFs is hindered by limited conductivity and stability, partly due to their lack of hierarchically structured pores. Herein a hydrothermal‐mechanical synthesis is reported by combining the one‐pot chemical fabrication of Ni3(2,3,6,7,10,11‐hexaiminotriphenylene)2 sheets and particles, and the mechanical assembly of these building blocks to improve electrical conductivity is also described. The as‐prepared ensemble (denoted as NHM) exhibits a Tostadas‐shaped structure with enriched ultramicropores and micropores. The charge‐discharge profile of NHM gives a superior reversible capacity of 1280 mA h g−1 after 100 cycles at the rate of 0.1 A g−1, surpassing the state‐of‐art pristine MOFs‐based anodes. Moreover, NHM is capable of maintaining 392 mA h g−1 at 1 A g−1 after 1000 cycles, the completion of a stability test in coin cell‐powered light emitting diodes further visualizes the remitted capacity fading of NHM. This work breaks through the limitation of capacity for pristine MOFs, providing a new pathway for achieving better energy conversion and storage.

As a superconductive metal-organic framework (MOF) material, Cu-BHT (BHT: benzenehexathiol) can demonstrate outstanding electrochemical properties owing to the potential redox reactions of the cuprous ions, sulfur species and benzene rings...

Abstract3D‐skeleton‐reinforced hybrid polymer electrolytes (HPEs) are conducive to improving the electrochemical performance and mechanical strength, but their preparation methods are usually tedious and inappropriate for practical application. The simplification of the preparation process and the further optimization of 3D skeletons are urgent to develop high‐performance solid‐state batteries. In this work, glass fiber (GF) decorated with ZIF‐67 (GF@ZIF‐67) was originally selected as 3D skeleton to construct an anion‐immobilized and fiber‐reinforced polyethylene oxide (PEO)‐based HPE (GF@ZIF@PEO). The presence of GF@ZIF‐67 3D skeleton can enhance the mechanical strength, whereas Lewis‐acidic metal sites of ZIF‐67 can immobilize free anions of the polymer matrix, accelerating ion migration and facilitating long‐term cycling stability. Consequently, the assembled LiFePO4/Li solid‐state batteries delivered a reversible capacity of 132 mAh g−1 with the capacity retention of 92 % at 1 C after 200 cycles. Our universal approach paves the way for advanced solid‐state electrolytes.

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