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Glass formation and reorientational motions are widespread, butoften-neglected features of deep eutectic solvents, although both can berelevant for the technically important ionic conductivity at room temperature.Here we investigate these properties for two mixtures of ethylene glycol andZnCl2, which were recently considered as superior electrolyte materials forapplication in zinc-ion batteries. For this purpose, we employed dielectricspectroscopy performed in a broad temperature range, extending from thesupercooled state at low temperatures up to the liquid phase around roomtemperature and beyond. We find evidence for a relaxation process arising fromdipolar reorientation dynamics, which reveals the clear signatures of glassyfreezing. This freezing also governs the temperature dependence of the ionic dcconductivity. We compare the obtained results with those for deep eutecticsolvents that are formed by the same hydrogen-bond donor, ethylene glycol, butby two different salts, choline chloride and lithium triflate. The fourmaterials reveal significantly different ionic and reorientational dynamics.Moreover, we find varying degrees of decoupling of rotational dipolar andtranslational ionic motions, which partly can be described by a fractionalDebye-Stokes-Einstein relation. The typical glass-forming properties of thesesolvents strongly affect their room-temperature conductivity.

Rotational dynamics, ionic conductivity, and glass formation in a ZnCl2-based deep eutectic solvent