Development of thermodynamically consistent machine-learning equations of state: Application to the Mie fluid
File(s)Supporting_Information_FE_ANN_EoS.pdf (539.83 KB) 184505_1_5.0146634.pdf (6.25 MB)
Supporting information
Published version
Author(s)
Chaparro Maldonado, Gustavo
Muller, Erich
Type
Journal Article
Abstract
A procedure for deriving thermodynamically consistent data-driven equations of state (EoS) for fluids is presented. The method is based on fitting the Helmholtz free energy using artificial neural networks to obtain a closed-form relationship between the thermophysical properties of fluids (FE-ANN EoS). As a proof-of-concept, an FE-ANN EoS is developed for the Mie fluids, starting from a database obtained by classical molecular dynamics simulations. The FE-ANN EoS is trained using first- (pressure and internal energy) and second-order (e.g., heat capacities, Joule–Thomson coefficients) derivative data. Additional constraints ensure that the data-driven model fulfills thermodynamically consistent limits and behavior. The results for the FE-ANN EoS are shown to be as accurate as the best available analytical model while being developed in a fraction of the time. The robustness of the “digital” equation of state is exemplified by computing physical behavior it has not been trained on, for example, fluid phase equilibria. Furthermore, the model’s internal consistency is successfully assessed using Brown’s characteristic curves.
Date Issued
2023-05-14
Date Acceptance
2023-04-24
Citation
Journal of Chemical Physics, 2023, 158 (18)
ISSN
0021-9606
Publisher
American Institute of Physics
Journal / Book Title
Journal of Chemical Physics
Volume
158
Issue
18
Copyright Statement
© 2023 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).
License URL
Publication Status
Published
Article Number
ARTN 184505
Date Publish Online
2023-05-10