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Salt-in-ionic liquid electrolytes have attracted significant attention aspotential electrolytes for next generation batteries largely due to theirsafety enhancements over typical organic electrolytes. However, recentexperimental and computational studies have shown that under certain conditionsalkali cations can migrate in electric fields as if they carried a net negativeeffective charge. In particular, alkali cations were observed to have negativetransference numbers at small mole fractions of alkali metal salt that revertto the expected net positive transference numbers at large mole fractions.Simulations have provided some insights into these observations, where theformation of asymmetric ionic clusters, as well as a percolating ion networkcould largely explain the anomalous transport of alkali cations. However, athermodynamic theory that captures such phenomena has not been developed, asionic associations were typically treated via the formation of ion pairs. Thetheory presented herein, based on the classical polymer theories, describesthermoreversible associations between alkali cations and anions, where theformation of large, asymmetric ionic clusters and a percolating ionic networkare a natural result of the theory. Furthermore, we present several generalmethods to calculate the effective charge of alkali cations in ionic liquids.We note that the negative effective charge is a robust prediction with respectto the parameters of the theory, and that the formation of a percolating ionicnetwork leads to the restoration of net positive charges of the cations atlarge mole fractions of alkali metal salt. Overall, we find excellentqualitative agreement between our theory and molecular simulations in terms ofionic cluster statistics and the effective charges of the alkali cations.

Salt-in-Ionic-Liquid Electrolytes: Ion Network Formation and Negative Effective Charges of Alkali Metal Cations