Advancing Thermodynamic Group-Contribution Methods by Machine Learning: UNIFAC 2.0

Abstract

Accurate prediction of thermodynamic properties is pivotal in chemical engineering for optimizing process efficiency and sustainability. Physical group-contribution (GC) methods are widely employed for this purpose but suffer from historically grown, incomplete parameterizations, limiting their applicability and accuracy. In this work, we overcome these limitations by combining GC with matrix completion methods (MCM) from machine learning. We use the novel approach to predict a complete set of pair-interaction parameters for the most successful GC method: UNIFAC, the workhorse for predicting activity coefficients in liquid mixtures. The resulting new method, UNIFAC 2.0, is trained and validated on more than 224,000 experimental data points, showcasing significantly enhanced prediction accuracy (e.g., nearly halving the mean squared error) and increased scope by eliminating gaps in the original model's parameter table. Moreover, the generic nature of the approach facilitates updating the method with new data or tailoring it to specific applications.

References in corpus (4)

• Variational Inference: A Review for Statisticians
• Pyro: Deep Universal Probabilistic Programming
• Machine Learning in Thermodynamics: Prediction of Activity Coefficients by Matrix Completion
• HANNA: Hard-constraint Neural Network for Consistent Activity Coefficient Prediction

Cited by in corpus (6)

• Modified UNIFAC 2.0 -- A Group-Contribution Method Completed with Machine Learning
• GRAPPA -- A Hybrid Graph Neural Network for Predicting Pure Component Vapor Pressures
• Prediction of Activity Coefficients by Similarity-Based Imputation using Quantum-Chemical Descriptors
• MLPROP -- an open interactive web interface for thermophysical property prediction with machine learning
• Prediction of Diffusion Coefficients in Mixtures with Tensor Completion
• Batch Distillation Data for Developing Machine Learning Anomaly Detection Methods