A Theoretical Model for Computing Freezing Point Depression of Lithium-Ion Battery Electrolytes

Reliable prediction of freezing point depression in liquid electrolytes will accelerate the development improved Li-ion batteries which can operate low temperature environments. In this work we establish a computational methodology to calculate activity coefficients and liquidus lines for battery-relevant electrolytes. Electronic structure methods are used conjuction with classical molecular dynamics simulations theoretical expressions Born solvation energy, ion-atmosphere effects from Debye-Hückel theory solvent entropic effects. The framework uses no priori knowledge beyond neat properties concentration salt. LiPF 6 propylene carbonate (PC), dimethyl (DMC) LiClO 4 DMC investigated up 1 molal accuracy better than 3 °C when compared experimental measurements. We find that difference between carbonate-based electrolyte originates dielectric constant.