Mixing weak acids and bases can produce highly complicated binary mixtures, called pseudo-protic ionic liquids, in which a complex network of effects determines the physicochemical properties that are currently impossible to predict. In this joint computational-experimental study, we investigated 1-methylimidazole-acetic acid mixtures through the whole concentration range. Effects of the varying ionization and excess of either components on the properties, such as density, diffusion coefficients, and overall hydrogen bonding structure were uncovered. A special emphasis was put on understanding the multiple factors that govern the conductivity of the system. In the presence of an excess of acetic acid, the 1-methylimidazolium acetate ion pairs dissociate more efficiently, resulting in a higher concentration of independently moving, conducting ions. However, the conductivity measurements showed that higher concentrations of acetic acid improve the conductivity beyond this effect, suggesting in addition to standard dilution effects the occurrence of Grotthuss diffusion in high acid-to-base ratios. The results here will potentially help designing novel electrolytes and proton conducting systems, which can be exploited in a variety of applications.
Keywords: Grotthuss diffusion; autocorrelation functions; binary electrolytes; ionic liquids; polarizable molecular dynamics.
© 2023 The Authors. ChemSusChem published by Wiley-VCH GmbH.