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

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⁺ , Mg²⁺ , and Ca²⁺ ; 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.