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Title: First-Principles-Based Machine Learning Models for Phase Behavior and Transport Properties of CO2

Journal Article · · Journal of Physical Chemistry. B
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Princeton Univ., NJ (United States)
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In this work, we construct distinct first-principles-based machine-learning models of CO2, reproducing the potential energy surface of the PBE-D3, BLYP-D3, SCAN and SCAN-rvv10 approximations of density functional theory. Here we employ the Deep Potential methodology to develop the models and consequently achieve a significant computational efficiency over ab initio molecular dynamics (AIMD) that allows for larger system sizes and time scales to be explored. Although our models are trained only with liquid phase configurations, they are able to simulate a stable interfacial system and predict vapor-liquid equilibrium properties, in good agreement with results from the literature. Because of the computational efficiency of the models, we are also able to obtain transport properties, such as viscosity and diffusion coefficients. We find that the SCAN-based model presents a temperature shift in the position of the critical point, while the SCAN-rvv10-based model shows improvement but still exhibits a temperature shift that remains approximately constant for all properties investigated in this work. We find that the BLYP-D3-based model generally performs better for liquid phase and vapor-liquid equilibrium properties, but the PBE-D3-based model is better suited for predicting transport properties.

Research Organization:
Princeton Univ., NJ (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0002128; SC001934; SC0019394
OSTI ID:
1992041
Alternate ID(s):
OSTI ID: 1994512
Journal Information:
Journal of Physical Chemistry. B, Vol. 127, Issue 20; ISSN 1520-6106
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ab initio molecular dynamics
density functional theory
equilibrium
liquids
potential energy