Gel polymer electrolytes (GPEs) with high ionic conductivity
and
good flexibility have emerged as promising alternatives to traditional
liquid electrolytes. Metal–organic frameworks (MOFs), with
a hierarchical pore structure and high porosity, have attracted widespread
attention as high-performance solid electrolytes. However, severe
agglomeration of MOF particles hampers Li+ transport, and
the flammability of organic liquid electrolytes in GPEs poses safety
risks. Herein, inspired by the bioadhesive properties of marine mussels,
we developed novel polydopamine (PDA)-modified zeolitic imidazole
framework-90 (ZIF-90) nanoparticles to act as a robust support layer.
Based on the nonflammability and environmental friendliness of ionic
liquids (ILs), through thiol–ene click chemistry, an IL-based
gel is fabricated. PDA exhibits exceptional interfacial bonding between
organic and inorganic components, thereby facilitating efficient Li+ transfer. The stable three-dimensional open framework of
ZIF-90 anchors bulky ions of IL and lithium salt while allowing unrestricted
movement of small Li+. The nanowetting interface formed
by ZIF-90 and IL, along with the polyether segments on the gel backbone,
further facilitates Li+ migration. The resulting ZIF-90@PDA
GPE exhibits a high ionic conductivity of 2.98 × 10–4 S cm–1 at 30 °C and a lithium-ion transference
number of 0.43. Moreover, enhanced suppression of lithium dendrite
growth, along with notable thermal stability and flame retardancy
is achieved. The assembled LiFePO4/Li cell demonstrates
remarkable cycling performance, exhibiting an initial discharge capacity
of 140 mAh g–1 at 30 °C and 0.5 C, with a capacity
retention of 90% after 300 cycles.