Gaussian-Charge Polarizable and Nonpolarizable Models for CO2

Hao Jiang, Othonas A. Moultos, Ioannis Economou, Athanassios Z. Panagiotopoulos

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

A polarizable intermolecular potential model using three classical Drude oscillators on the atomic sites has been developed for CO2. The model is rigid with bond lengths and molecular geometries set to their experimental values. Electrostatic interactions are represented by three Gaussian charges connected to the molecular frame by harmonic springs. Nonelectrostatic interactions are represented by the Buckingham exponential-6 potential, with potential parameters optimized to vapor-liquid equilibria (VLE) data. A nonpolarizable CO2 model that shares the other ingredients of the polarizable model was also developed and optimized to VLE data. Gibbs ensemble Monte Carlo and molecular dynamics simulations were used to evaluate the two models with respect to a variety of thermodynamic and transport properties, including the enthalpy of vaporization, second virial coefficient, density in the one-phase fluid region, isobaric and isochoric heat capacities, radial distribution functions, self-diffusion coefficient, and shear viscosity. Excellent agreement between model predictions and experimental data was found for all properties studied. The polarizable and nonpolarizable models provide a similar representation of CO2 properties, which indicates that the properties of pure CO2 fluid are not strongly affected by polarization. The polarizable model, which has an order of magnitude higher computational cost than the nonpolarizable model, will likely be useful for the study of a mixture of CO2 and polar components for which polarization is important.

Original languageEnglish
Pages (from-to)984-994
Number of pages11
JournalJournal of Physical Chemistry B
Volume120
Issue number5
DOIs
Publication statusPublished - 18 Feb 2016

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Volatilization
Molecular Dynamics Simulation
Static Electricity
Thermodynamics
Viscosity
Theoretical Models
Hot Temperature
Costs and Cost Analysis
liquid-vapor equilibrium
Phase equilibria
Polarization
Fluids
Shear viscosity
fluids
virial coefficients
Bond length
polarization
Coulomb interactions
Vaporization
radial distribution

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Surfaces, Coatings and Films

Cite this

Gaussian-Charge Polarizable and Nonpolarizable Models for CO2 . / Jiang, Hao; Moultos, Othonas A.; Economou, Ioannis; Panagiotopoulos, Athanassios Z.

In: Journal of Physical Chemistry B, Vol. 120, No. 5, 18.02.2016, p. 984-994.

Research output: Contribution to journalArticle

Jiang, Hao ; Moultos, Othonas A. ; Economou, Ioannis ; Panagiotopoulos, Athanassios Z. / Gaussian-Charge Polarizable and Nonpolarizable Models for CO2 In: Journal of Physical Chemistry B. 2016 ; Vol. 120, No. 5. pp. 984-994.
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