First principles models of the interactions of methane and carbon dioxide

Mark T. Oakley; Hainam Do; Richard J. Wheatley

doi:10.1016/j.fluid.2009.11.011

First principles models of the interactions of methane and carbon dioxide

Mark T. Oakley, Hainam Do, Richard J. Wheatley

Research output: Journal Publication › Article › peer-review

17 Citations (Scopus)

Abstract

We present ab initio calculations on the CH₄-CH₄ and CH₄-CO₂ dimer potential energy surfaces. We show that the fit to these surfaces is improved over the Lennard-Jones potential by changing the form of the repulsive wall. Ab initio calculations are also performed on trimers to evaluate the strength of nonadditive interactions. The experimental CH₄ phase properties are reproduced in simulations that include correction for nonadditive dispersion. The phase-coexistence curve of mixtures of CH₄ and CO₂ is also improved by including this nonadditive dispersion term.

Original language	English
Pages (from-to)	48-54
Number of pages	7
Journal	Fluid Phase Equilibria
Volume	290
Issue number	1-2
DOIs	https://doi.org/10.1016/j.fluid.2009.11.011
Publication status	Published - 25 Mar 2010
Externally published	Yes

Keywords

Ab initio calculations
Gibbs ensemble
Potential energy surface
Vapor-liquid equilibrium

ASJC Scopus subject areas

General Chemical Engineering
General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/j.fluid.2009.11.011

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title = "First principles models of the interactions of methane and carbon dioxide",

abstract = "We present ab initio calculations on the CH4-CH4 and CH4-CO2 dimer potential energy surfaces. We show that the fit to these surfaces is improved over the Lennard-Jones potential by changing the form of the repulsive wall. Ab initio calculations are also performed on trimers to evaluate the strength of nonadditive interactions. The experimental CH4 phase properties are reproduced in simulations that include correction for nonadditive dispersion. The phase-coexistence curve of mixtures of CH4 and CO2 is also improved by including this nonadditive dispersion term.",

keywords = "Ab initio calculations, Gibbs ensemble, Potential energy surface, Vapor-liquid equilibrium",

author = "Oakley, {Mark T.} and Hainam Do and Wheatley, {Richard J.}",

note = "Funding Information: We thank Professor Jonathan Hirst for helpful discussions. We thank the University of Nottingham High-Performance Computing facility for providing the computer resources used in this study and the Engineering and Physical Sciences Research Council for funding (grant number EP/E06082X/1 ). ",

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T1 - First principles models of the interactions of methane and carbon dioxide

AU - Oakley, Mark T.

AU - Do, Hainam

AU - Wheatley, Richard J.

N1 - Funding Information: We thank Professor Jonathan Hirst for helpful discussions. We thank the University of Nottingham High-Performance Computing facility for providing the computer resources used in this study and the Engineering and Physical Sciences Research Council for funding (grant number EP/E06082X/1 ).

PY - 2010/3/25

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N2 - We present ab initio calculations on the CH4-CH4 and CH4-CO2 dimer potential energy surfaces. We show that the fit to these surfaces is improved over the Lennard-Jones potential by changing the form of the repulsive wall. Ab initio calculations are also performed on trimers to evaluate the strength of nonadditive interactions. The experimental CH4 phase properties are reproduced in simulations that include correction for nonadditive dispersion. The phase-coexistence curve of mixtures of CH4 and CO2 is also improved by including this nonadditive dispersion term.

AB - We present ab initio calculations on the CH4-CH4 and CH4-CO2 dimer potential energy surfaces. We show that the fit to these surfaces is improved over the Lennard-Jones potential by changing the form of the repulsive wall. Ab initio calculations are also performed on trimers to evaluate the strength of nonadditive interactions. The experimental CH4 phase properties are reproduced in simulations that include correction for nonadditive dispersion. The phase-coexistence curve of mixtures of CH4 and CO2 is also improved by including this nonadditive dispersion term.

KW - Ab initio calculations

KW - Gibbs ensemble

KW - Potential energy surface

KW - Vapor-liquid equilibrium

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DO - 10.1016/j.fluid.2009.11.011

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JO - Fluid Phase Equilibria

JF - Fluid Phase Equilibria

IS - 1-2

ER -

First principles models of the interactions of methane and carbon dioxide

Abstract

Keywords

ASJC Scopus subject areas

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