Machine Learning-Enabled Development of Accurate Force Fields for Refrigerants

• Published in: Journal of chemical theory and computation Vol. 19; no. 14; pp. 4546 - 4558
• Main Authors: Wang, Ning, Carlozo, Montana N., Marin-Rimoldi, Eliseo, Befort, Bridgette J., Dowling, Alexander W., Maginn, Edward J.
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 25.07.2023
• Subjects: Chlorofluorocarbons; Enthalpy; Gaussian process; Hydrofluorocarbons; Liquid-vapor equilibrium; Machine learning; Molecular dynamics; Molecular Mechanics; Optimization; Parameters; Refrigerants; Simulation; Support vector machines; Thermophysical properties; Vapor density; Vapor pressure; Vaporization; Workflow
• ISSN: 1549-9618; 1549-9626
• DOI: 10.1021/acs.jctc.3c00338

Hydrofluorocarbon (HFC) refrigerants with zero ozone-depleting potential have replaced chlorofluorocarbons and are now ubiquitous. However, some HFCs have high global warming potential, which has led to calls by governments to phase out these HFCs. Technologies to recycle and repurpose these HFCs need to be developed. Therefore, thermophysical properties of HFCs are needed over a wide range of conditions. Molecular simulations can help understand and predict the thermophysical properties of HFCs. The prediction capability of a molecular simulation is directly tied to the accuracy of the force field. In this work, we applied and refined a machine learning-based workflow to optimize the Lennard-Jones parameters of classical HFC force fields for HFC-143a (CF3CH3), HFC-134a (CH2FCF3), R-50 (CH4), R-170 (C2H6), and R-14 (CF4). Our workflow involves liquid density iterations with molecular dynamics simulations and vapor–liquid equilibrium (VLE) iterations with Gibbs ensemble Monte Carlo simulations. Support vector machine classifiers and Gaussian process surrogate models save months of simulation time and can efficiently select optimal parameters from half a million distinct parameter sets. Excellent agreement as evidenced by low mean absolute percent errors (MAPEs) of simulated liquid density (ranging from 0.3% to 3.4%), vapor density (ranging from 1.4% to 2.6%), vapor pressure (ranging from 1.3% to 2.8%), and enthalpy of vaporization (ranging from 0.5% to 2.7%) relative to experiments was obtained for the recommended parameter set of each refrigerant. The performance of each new parameter set was superior or similar to the best force field in the literature.