Highly Conductive, Flexible, and Nonflammable Double-Network Poly(ionic liquid)-Based Ionogel Electrolyte for Flexible Lithium-Ion Batteries

The solid-state lithium-ion battery is proposed as the ultimate form of battery and has rapidly become an updated attentive research field due to its high safety and extreme temperature tolerance. However, current solid-state electrolytes hardly meet the requirement in practical applications due to its low ionic conductivity, weak mechanical properties, and poor interfacial contact between the electrolyte and the electrode. In this work, we developed a double-network-supported poly(ionic liquid)-based ionogel electrolyte (DN-Ionogel) via a one-step method. Due to its compact cross-linking structure, the leakage-free DN-Ionogel electrolyte exhibits outstanding flexibility and favorable mechanical properties. In this ionogel electrolyte, the double network favors dissociation of lithium bis(trifluoromethanesulfony)imide (LiTFSI), further resulting in remarkable ionic conductivity (1.8 × 10–3 S/cm, room temperature), wide electrochemical window (up to 5.0 V), and high lithium-ion transference number (0.33). Furthermore, the cell (LiFePO4||DN-Ionogel||Lithium) delivers a discharge capacity as high as 150.5 mAh/g, stable cyclic performance (over 200 cycles), and superior rate behavior.