Combining Molecular Dynamics and Experimental Methods for the Parametrization of Binary Carbonate-Based Electrolytes

Modelling the ionic transport in battery cells requires precise parametrization of the involved electrolytes. For carbonate-based electrolytes, however, the evaluation of their parameters suffers from interphase effects between the bulk electrolyte and the Li metal electrode, commonly present in the usual electrochemical polarization experiments. In this work, we combine measurements on conductivity and concentration cells with molecular dynamics simulations, avoiding these difficulties and thus, allowing for a more accurate determination of the parameters. We determine the conductivity, the transference number, the thermodynamic factor and the salt diffusion coefficient for three different electrolytes, i.e. mixtures of ethylene carbonate (EC), ethyl methyl carbonate (EMC), methyl propionate (MP), dimethyl carbonate (DMC) and propylene carbonate (PC), containing LiPF6 at various concentrations and temperatures. In order to validate the simulated transference numbers, we employ electrophoretic Nuclear Magnetic Resonance spectroscopy (eNMR).