Advancing Thermodynamic Group-Contribution Methods by Machine Learning: UNIFAC 2.0
This work improves thermodynamic property prediction for chemical engineering, offering a more accurate and broadly applicable tool, though it is incremental as it builds on the existing UNIFAC method.
The paper tackled the problem of inaccurate and incomplete parameterizations in thermodynamic group-contribution methods by combining them with machine learning matrix completion, resulting in UNIFAC 2.0, which nearly halved the mean squared error and was validated on over 224,000 data points.
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.