Overall, we found that the SMx (x= 12, 8, or D) predicted values of ln γ ∞ i,j did not change substantially when ∆G self i,i was predicted compared to when it was computed using reference vapor pressure data, except in the case when water is the solute. Therefore, moving forward the selected method for calculating ln γ ∞ i,j will be to compute ∆G solv i,j and ∆G self i,i consistently; put differently, both ∆G solv i,j and ∆G self i,i will be predicted. To provide further insight into the potential utility of electronic structure calculations with SMx universal solvent models to predict ln γ ∞ i,j , the top performing SM12 was compared to two well-known methods, the Universal Quasichemical Functional-group Activity Coefficients (UNIFAC) method and the Modified Separation of Cohesive Energy Density (MOSCED) model . UNIFAC was selected as a comparative method because it is perhaps the most common predictive excess Gibbs free energy method . Additionally, it is widely used and integrated into most process simulators. Brouwer and Schuur recently conducted a comparative study of eight predictive methods to compute ln γ ∞ i,j at 298.15 K. Of the methods evaluated, the solubility parameter method MOSCED was the top performer. This strong performance of MOSCED is consistent with the findings of the 2005 re-parameterization and our recent work . MOSCED was therefore selected as an additional comparison alongside UNIFAC. Note that for water, we adopted the revised MOSCED parameters from ref. The Minnesota Solvation Database, DECHEMA, and Yaws' reference databases were constrained to match the compound availability provided by the two models, UNIFAC and MOSCED. In comparison to the Minnesota Solvation Database, UNIFAC was able to make predictions for 1065 (of 1140) systems with 99 unique solutes and 68 unique solvents. MOSCED was able to make predictions for 732 (of 1140) systems from the Minnesota Solvation Database with 58 unique solutes and 54 unique solvents. In regards to DECHEMA, UNIFAC was able to model 1988 (of 2163) systems with 112 unique solutes and 70 unique solvents. MOSCED was able to model 1818 (of 2163) systems with 71 unique solutes and 59 unique solvents. We again note that the DECHEMA data set includes repeated systems. All of the UNIFAC calculations were performed with . A simple GNU Octave/MATLAB M-file to predict limiting activity coefficients using MOSCED, a screen cast tutorial and additional references are available on the YouTube Channel of Andrew Paluch .