Graph Neural Networks for Temperature-Dependent Activity Coefficient Prediction of Solutes in Ionic Liquids

RWTH Publications (RWTH Aachen)

Abstract

Ionic liquids (ILs) are important solvents for sustainable processes and predicting activity coefficients (ACs) of solutes in ILs is needed. Recently, matrix completion methods (MCMs), transformers, and graph neural networks (GNNs) have shown high accuracy in predicting ACs of binary mixtures, superior to well-established models, e.g., COSMO-RS and UNIFAC. GNNs are particularly promising here as they learn a molecular graph-to-property relationship without pretraining, typically required for transformers, and are, unlike MCMs, applicable to molecules not included in training. For ILs, however, GNN applications are currently missing. Herein, we present a GNN to predict temperature-dependent infinite dilution ACs of solutes in ILs. We train the GNN on a database including more than 40,000 AC values and compare it to a state-of-the-art MCM. The GNN and MCM achieve similar high prediction performance, with the GNN additionally enabling high-quality predictions for ACs of solutions that contain ILs and solutes not considered during training.

Authors 5

1. Jan G. Rittig Aachen

   RWTH Aachen University

   Affiliation as printed

   RWTH Aachen University , Process Systems Engineering (AVT.SVT) , Aachen 52074 , Germany

2. Karim Ben Hicham Aachen

   RWTH Aachen University

   Affiliation as printed

   RWTH Aachen University , Process Systems Engineering (AVT.SVT) , Aachen 52074 , Germany

3. Artur M. Schweidtmann

   Delft University of Technology

   Affiliation as printed

   Delft University of Technology , Department of Chemical Engineering , Delft 2629 HZ , The Netherlands

4. Manuel Dahmen

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH , Institute for Energy and Climate Research IEK-10: Energy Systems Engineering , Jülich 52425 , Germany

5. Alexander Mitsos