Influence of Hydrogen Bond Donor Identity and Intentional Water Addition on the Properties of Gelatin-Supported Deep Eutectic Solvent Gels

Deep eutectic solvent (DES) gel electrolytes have recently emerged as promising alternatives to ionic liquid- or water-based gels for "ionic skin" sensor applications. Researchers have also been exploring the effects that varying amounts of water may have on the local hydrogen bonding environment within a few model DES systems. In this study, the physical properties and ionic conductivities of biopolymer (gelatin)-supported gels featuring two established DESs and three DES/water mixture formulations are investigated and compared. The DES/water mixtures are formed by combining choline chloride with one of three organic hydrogen bond donors (HBDs), ethylene glycol, glycerol, or 1,2-propanediol, in a 1:2 molar ratio, together with a controlled amount of water, 25 mol % (approximately 5-6 wt % water). For the same fixed gelatin content (20 wt %), DES/water mixture gel Young's modulus values are found to be tunable based on the organic HBD identity, increasing 6-fold from 7 (1,2-propanediol) to 42 (glycerol) kPa. Furthermore, large differences are observed in the resulting gel properties when water has been intentionally added to well-studied DESs. Coformulation with water is found to increase ethylene glycol-based DES gel toughness, measured via tensile testing, from 23 to 68 kJ/m³ while simultaneously boosting gel room temperature ionic conductivity from 3.3 to 5.2 mS/cm. These results highlight the multiple roles that controlled amounts of water in DES can play within gelatin-supported DES/mixture gel electrolytes, such as influencing gelatin self-assembly and reducing local viscosity to promote facile ion transport.