Vapor–liquid equilibria of mixtures containing nitrogen, oxygen, carbon dioxide, and ethane

Stoll, Jürgen; Vrabec, Jadran; Hasse, Hans

doi:10.1002/aic.690490826

Cited by 96 publications

(117 citation statements)

References 57 publications

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“…7,30,[67][68][69] But as shown there, a significant improvement can be achieved by introducing one state independent binary parameter n to adjust the unlike energy parameters…”

Section: Molecular Mixture Modelsmentioning

confidence: 47%

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

et al. 2011

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Vapor-liquid equilibria (VLE) of nine binary mixtures containing hydrogen chloride or phosgene in the solvents benzene, chlorobenzene, ortho-dichlorobenzene, and toluene as well as the mixture hydrogen chloride þ phosgene are predicted by molecular modeling and simulation. The underlying force fields for the pure substances are developed on the basis of quantum chemical information on molecular geometry and electrostatics. These are individually optimized to experimental pure fluid data on the vapor pressure and saturated liquid density, where the deviations are typically less than 5 and 0.5 %, respectively. The unlike dispersive interaction is optimized for seven of the nine studied binaries. Previously unpublished experimental binary VLE data, measured by BASF in the vicinity of ambient temperature, are predominantly used for these fits. VLE data, including dew point composition, saturated densities and enthalpy of vaporization, are predicted for a wide range of temperatures and compositions.

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“…7,30,[67][68][69] But as shown there, a significant improvement can be achieved by introducing one state independent binary parameter n to adjust the unlike energy parameters…”

Section: Molecular Mixture Modelsmentioning

confidence: 47%

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

et al. 2011

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“…The Lennard-Jones cutoff radius was chosen to be the maximum value allowed by the box size, which was typically larger than 17Å. These simulation settings have previously been shown to be adequate for quantitative simulations of CO 2 mixtures with comparable diatomic molecules 23 .…”

Section: Simulations With Literature Force-fieldssupporting

confidence: 42%

“…Therefore they are generally unsuited to simulate mixtures at these higher temperatures. Some binary mixture simulations have been performed that optimise the mixing parameters but these are also for lower temperatures 23 . In this section we run molecular simulations for CO 2 mixtures at CCS-relevant temperatures, using literature force-fields.…”

Section: Simulations From Semi-empirical Molecular Interactionsmentioning

confidence: 39%

Molecular simulation of the thermophysical properties and phase behaviour of impure CO₂ relevant to CCS

2016

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Impurities from the CCS chain can greatly influence the physical properties of CO 2 . This has important design, safety and cost implications for the compression, transport and storage of CO 2 . There is an urgent need to understand and predict the properties of impure CO 2 to assist with CCS implementation. However, CCS presents demanding modelling requirements. A suitable model must both accurately and robustly predict CO 2 phase behaviour over a wide range of temperature and pressure, and maintain that predictive power for CO 2 mixtures with numerous, mutually interacting chemical species. A promising technique to address this task is molecular simulation. It offers a molecular approach, with foundations in firmly established physical principles, along with the potential to predict the wide range of physical properties required for CCS. The quality of predictions from molecular simulation depends on accurate force-fields to describe the interactions between CO 2 and other molecules. Unfortunately, there is currently no universally applicable method to obtain force-fields suitable for molecular simulation.In this paper we present two methods of obtaining force-fields: the first being semi-empirical and the second using ab initio quantum-chemical calculations. In the first approach we optimise the impurity force-field against measurements of the phase and pressure-volume behaviour of CO 2 binary mixtures with N 2 , O 2 , Ar and H 2 . A gradient-free optimiser allows us to use the simulation itself as the underlying model. This leads to accurate and robust predictions under conditions relevant to CCS. In the second approach we use quantum-chemical calculations to produce ab initio evaluations of the interactions between CO 2 and relevant impurities, taking N 2 as an exemplar. We use a modest number of these calculations to train a machine-learning algorithm, known as a Gaussian process, to describe these data. The resulting model is then able to accurately predict a much broader set of ab initio force-field calculations at comparatively low numerical cost. Although our method is not yet ready to be implemented in a molecular simulation, † Electronic Supplementary Information (ESI) available: [details of any supplementary information available should be included here]. See

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“…That potential allows to describe the thermodynamic properties of many real fluids, like carbon dioxide, ethyne, propyne, or carbon disulfide with good accuracy, as has been shown in a comprehensive study [18,19]. The present study is performed in the NpT ensemble at high densities.…”

Section: Introductionsupporting

confidence: 41%

Chemical potential of quadrupolar two-centre Lennard-Jones fluids by gradual insertion

Vrabec

Kettler

Hasse

2002

Chemical Physics Letters

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The gradual insertion method for direct calculation of the chemical potential by molecular simulation is applied in the NpT ensemble to different quadrupolar two-centre LennardJones fluids at high density state points. The results agree well with Widom's test particle insertion but show at very high densities significantly smaller statistical uncertainties.The gradual insertion method, which is coupled here with preferential sampling, extends the density range where reliable information on the chemical potential can be obtained.Application details are reported.

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Vapor–liquid equilibria of mixtures containing nitrogen, oxygen, carbon dioxide, and ethane

Cited by 96 publications

References 57 publications

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

Molecular simulation of the thermophysical properties and phase behaviour of impure CO₂ relevant to CCS

Chemical potential of quadrupolar two-centre Lennard-Jones fluids by gradual insertion

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Vapor–liquid equilibria of mixtures containing nitrogen, oxygen, carbon dioxide, and ethane

Cited by 96 publications

References 57 publications

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

Vapor–liquid equilibria of hydrogen chloride, phosgene, benzene, chlorobenzene, ortho‐dichlorobenzene, and toluene by molecular simulation

Molecular simulation of the thermophysical properties and phase behaviour of impure CO2 relevant to CCS

Chemical potential of quadrupolar two-centre Lennard-Jones fluids by gradual insertion

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Molecular simulation of the thermophysical properties and phase behaviour of impure CO₂ relevant to CCS