Self‐Assembled Gels Formed in Deep Eutectic Solvents: Supramolecular Eutectogels with High Ionic Conductivity

Abstract 1,3:2,4‐Dibenzylidene‐ d ‐sorbitol (DBS), a simple, commercially relevant compound, was found to self‐assemble as a result of intermolecular noncovalent interactions into supramolecular gels in deep eutectic solvents (DESs) based on choline chloride combined with alcohols/ureas. DBS formed gels at a loading of 5 % w/v. Rheology confirmed the gel‐like nature of the materials, electron microscopy and X‐ray diffraction indicated underpinning nanofibrillar DBS networks, and differential scanning calorimetry showed the DES nature of the liquid‐like phase was retained. The ionic conductivities of the gels were similar to those of the unmodified DESs, thus proving the deep eutectic nature of the ionic liquid‐like phase. Gelation was tolerant of ionic additives Li + , Mg 2+ , and Ca 2+ ; the resulting gels had similar conductivities to electrolyte dissolved in the native DES. The low‐molecular‐weight gelator DBS is thus a low‐cost additive that forms gels in DESs from readily available constituents, with conductivity levels suitable for practical applications.