Engineering 3D Interpenetrated ZIF-8 Network in Poly(ethylene oxide) Composite Electrolyte for Fast Lithium-Ion Conduction and Effective Lithium-Dendrite Inhibition

A novel 3D ZIF-8 network-reinforced polyethylene oxide (PEO) composite polymer electrolyte (Z-C-PAN-PEO) is successfully built, in which the network with an interpenetrated structure is tactfully developed by in situ assembling ZIF-8 nanoparticles on electrospinning carboxylated polyacrylonitrile (C-PAN) nanofiber surfaces. ZIF-8 with high porosity and unsaturated open metal sites will act as the bridge between C-PAN nanofibers and the PEO matrix. It is proven that the selected ZIF-8 can play a significant role in facilitating Li+ conduction and transference by effectively interacting with the oxygen atoms of C–O–C to promote the segmental movement of PEO and immobilizing TFSI– anions to release more free Li+. The 3D interpenetrating structure of Z-C-PAN further enables the conduction channels more consecutive and long-ranged, endowing the Z-C-PAN-PEO electrolyte with an optimum ionic conductivity of 4.39 × 10–4 S cm–1 and a boosted Li+ transference number of 0.42 at 60 °C. Other improvements occurring in the reinforced electrolytes are the broaden electrochemical stability window of ∼4.9 V and sufficient mechanical strength. Consequently, the stable Li-plating/stripping for 1000 cycles at 0.1 mA cm–1 witnesses the splendid compatibility against Li dendrite. The cycling performance of LiFePO4/Z-C-PAN-PEO/Li cells with a reversible capacity of 116.2 mAh g–1 after 600 cycles at 0.2 C guarantees the long-term running potential in lithium metal batteries. This study puts forward new insights in designing and exploiting the active role of MOFs for high-performance solid polymer electrolytes.