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Title: Performance of density functionals for modeling vapor liquid equilibria of CO2 and SO2

Journal Article · · Journal of Computational Chemistry
DOI:https://doi.org/10.1002/jcc.25123· OSTI ID:1461662
 [1];  [1];  [1]; ORCiD logo [1]
  1. Mississippi State Univ., Mississippi State, MS (United States). Dave C. Swalm School of Chemical Engineering, and Center for Advanced Vehicular Systems
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Vapor liquid equilibria (VLE) and condensed phase properties of carbon dioxide and sulfur dioxide are calculated using first principles Monte Carlo (FPMC) simulations to assess the performance of several density functionals, notably PBE-D3, BLYP-D3,PBE0-D3, M062X-D3, and rVV10. GGA functionals were used to compute complete vapor liquid coexistence curves (VLCCs) to estimate critical properties, while the hybrid and nonlocal vander Waals functionals were used only for computing density at a single state point due to the high computational cost. Our results show that the BLYP-D3 functional performs well in predicting VLE properties for both molecules when compared with other functionals. In the liquid phase, pair correlation functions reveal that there is not a significant difference in the location of the peak for the first solvation shell while the peak heights are different for different functionals. Altogether, theBLYP-D3 functional is a good choice for modeling VLE of acidic gases with significant environmental implications such as CO2 and SO2.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1461662
Journal Information:
Journal of Computational Chemistry, Vol. 39, Issue 8; ISSN 0192-8651
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

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Cited By (1)

Solvent selection for extractive distillation using molecular simulation journal May 2019

Figures / Tables (20)

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Table 1(p. 31)table Table 1
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Table S1(p. 67)table Table S1
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Table S4(p. 69)table Table S4
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Figure S1(p. 70)figure Figure S1
Figure S2(p. 70)figure Figure S2

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
first principles Monte Carlo
dispersion
vapor liquid equilibria
CO2
SO2
density functional theory