Graph Neural Networks embedded into Margules model for vapor-liquid equilibria prediction

Graph Neural Networks embedded into Margules model for vapor-liquid equilibria prediction Edgar Ivan Sanchez Medina a,, Kai Sundmacher a,b a Process Systems Engineering, Max Planck Institute for Dynamics of Complex Technical Systems, Sandtorstraße 1, Magdeburg, 39106, Saxony-Anhalt, Germany b Chair for Process Systems Engineering, Otto-von-Guericke University, Universit atsplatz 2, Magdeburg, 39106, Saxony-Anhalt, GermanyAbstract Predictive thermodynamic models are crucial for the early stages of product and process design. In this paper the performance of Graph Neural Networks (GNNs) embedded into a relatively simple excess Gibbs energy model, the extended Margules model, for predicting vapor-liquid equilibrium is analyzed. By comparing its performance against the established UNIFAC-Dortmund model it has been shown that GNNs embedded in Margules achieves an overall lower accuracy. However, higher accuracy is observed in the case of various types of binary mixtures. Moreover, since group contribution methods, like UNIFAC, are limited due to feasibility of molecular fragmentation or availability of parameters, the GNN in Margules model offers an alternative for VLE estimation. The findings establish a baseline for the predictive accuracy that simple excess Gibbs energy models combined with GNNs trained solely on infinite dilution data can achieve. Keywords: graph neural networks, vapor-liquid equilibria, Margules, activity coefficients 1. Introduction Modeling vapor-liquid equilibria is essential for the development of most chemical processes. This is because many chemical processes operate under conditions where vapor and liquid phases interact. Although vapor-liquid Corresponding author Email address: sanchez@mpi-magdeburg.mpg.de