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Transference numbers play an important role for understanding the dynamics ofelectrolytes and assessing their performance in batteries. Unfortunately, thesetransport parameters are difficult to measure in highly concentrated, liquidelectrolytes such as ionic liquids. Also, the interpretation of their sign andmagnitude has provoked an ongoing debate in the literature further complicatedby the use of different language. In this work, we highlight the role of thereference frame for the interpretation of transport parameters using our novelthermodynamically consistent theory for highly correlated electrolytes. Weargue that local volume conservation is a key principle in incompressibleliquid electrolytes and use the volume-based drift velocity as reference. Weapply our general framework to electrophoretic NMR experiments. For ionicliquid based electrolytes, we find that the results of the eNMR measurementscan be best described using this volume-based description. This highlights thelimitations of the widely used center-of-mass reference frame which for exampleforms the basis for molecular dynamics simulations - a standard tool for thetheoretical calculation of transport parameters. It shows that the assumptionof local momentum conservation is incorrect in those systems on the macroscopicscale.

A Volume-based Description of Transport in Incompressible Liquid Electrolytes and its Application to Ionic Liquids