Boosting lithium batteries under harsh operating conditions by a resilient ionogel with liquid-like ionic conductivity

New chemistries are being developed to increase the capacity and power of rechargeable batteries. However, the risk of safety issues increases when high-energy batteries using highly active materials encounter harsh operating conditions. Here we report on the synthesis of a unique ionogel electrolyte for abuse-tolerant lithium batteries. A hierarchically architected silica/polymer scaffold is designed and fabricated through a facile soft chemistry route, which is competent to confine ionic liquids with superior uptake ability (92.4 wt%). The monolithic ionogel exhibits high conductivity and thermal/mechanical stability, featuring high-temperature elastic modulus and dendrite-free lithium cycling. The Li/LiFePO₄ pouch cells achieve outstanding cyclability at different temperatures up to 150 °C, and can sustain cutting, crumpling, and even coupled thermal–mechanical abuses. Moreover, the solid-state lithium batteries with LiNi_0.60Co_0.20Mn_0.20O₂, LiNi_0.80Co_0.15Al_0.05O₂, and Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ cathodes demonstrate excellent cycle performances at 60 °C. These results indicate that the resilient and high-conductivity ionogel electrolyte is promising to realize high-performance lithium batteries with high energy density and safety.