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Here we present a theory of ion aggregation and gelation of room temperatureionic liquids (RTILs). Based on it, we investigate the effect of ionaggregation on correlated ion transport - ionic conductivity and transferencenumbers - obtaining closed-form expressions for these quantities.The theorydepends on the maximum number of associations a cation and anion can form, andthe strength of their association. To validate the presented theory, we performmolecular dynamics simulations on several RTILs, and a range of temperaturesfor one RTIL. The simulations indicate the formation of large clusters, evenpercolating through the system under certain circumstances, thus forming a gel,with the theory accurately describing the obtained cluster distributions in allcases. We discuss the possibility of observing a gel phase in neat RTILs, whichhas hitherto not been discussed in any detail.

Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids