Over the past few decades, ionic liquids (ILs) have gained attention as electrolytes, although concerns about their environmental persistence and toxicity challenge their status as green solvents. In this framework, choline chloride (ChCl) offers a more sustainable alternative due to its low toxicity, biodegradability, and cost-effectiveness. Although ChCl has a high melting point, its combination with hydrogen bond donor compounds (HBDs) can result in liquid mixtures at much lower temperatures, known as deep eutectic solvents (DESs). This study presents a comparative evaluation of three ChCl-based DESs, glyceline, ethaline, and reline (obtained from mixtures of ChCl and glycerol, ethylene glycol, and urea), with a focus specifically on their potential as electrolyte candidates for supercapacitors. Using differential scanning calorimetry (DSC), cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and nuclear magnetic resonance (NMR), we assess their thermal, electrochemical, and structural properties. All DESs displayed amorphous behavior and a strong tendency to remain liquid even at very low temperatures. Among them, ethaline showed the most promising electrochemical performance, exhibiting the lowest resistivity and the highest capacity.

The development of safer and more sustainable polymer electrolytes is essential for next-generation energy storage technologies. In this work, PVDF-based ionogels containing 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide were synthesized as potential semi-solid electrolytes. As a solvent for ionogel preparation, DMSO was employed as a safer and more environmentally favorable alternative to DMF. The resulting materials were characterized by electrochemical impedance spectroscopy, rheological measurements, and scanning electron microscopy to evaluate ionic conductivity, mechanical behavior, and morphology. The ionogels exhibited high ionic conductivity, predominantly elastic behavior, and homogeneous microstructures. These results demonstrate the feasibility of replacing DMF with DMSO while maintaining the functional properties required for electrochemical energy storage applications.