Ionogel‐Based Electrodes for Non‐Flammable High‐Temperature Operating Electrochemical Double Layer Capacitors

: The design of interfaces between nanostructured electrodes and advanced electrolytes is critical for realizing advanced electrochemical double-layer capacitors (EDLCs) that combine high charge-storage capacity, high-rate capability, and enhanced safety. Toward this goal, this work presents a novel and sustainable approach for fabricating ionogel-based electrodes using a renewed slurry casting method, in which the solvent is replaced by the ionic liquid (IL), namely 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIFSI). This method avoids time-consuming and costly electrolyte-filling steps by integrating the IL directly into the electrode during slurry preparation, while improving the rate capability of EDLCs based on non-flammable ILs. The resulting ionogel electrodes demonstrate exceptional electrolyte accessibility and enable the production of symmetric EDLCs with high energy density (over 30Wh/kg based on electrode material weight) and high-rate performance. These EDLCs could operate at temperatures up to 180°C, far exceeding the limitations of traditional EDLCs based on organic electrolytes (1M TEABF4 in acetonitrile, up to 65°C). Ionogel-type EDLCs exhibit remarkable stability, retaining 88% specific capacity after 10000 galvanostatic charge/discharge cycles at 10Ag-1 and demonstrating superior retention compared to conventional EDLCs (50%), while also maintaining 92.4% energy density during 100h floating tests at 2.7V. These electrochemical properties highlight their potential for robust performance under demanding conditions.