Comparison of the capillary wave method and pressure tensor route for calculation of interfacial tension in molecular dynamics simulations

Nickerson, Stella D.; Frost, Denzil S.; Phelan, Harrison; Dai, Lenore L.

doi:10.1002/jcc.23443

Cited by 6 publications

(9 citation statements)

References 71 publications

(110 reference statements)

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“…Figure 6 (left) shows a very good linear fit with a slope close to 1 and an intercept close to 0. It shows that the values predicted using our method are in overall very good agreement with experimentally determined values for binary systems, including low IFT values, where Molecular dynamics methods struggle (Nickerson et al, 2013). In Figure 6 (right) a comparison of our predicted IFT and experimental data for the ternary system water/dioxane/benzene as a function of dioxane concentration in the water and organic phase is shown.…”

Section: The Andersson Et Al Model For Ift Predictionsupporting

confidence: 76%

Predicting Interfacial Tension Of Multiphase Systems Based On Computational Single-Molecule Quantum Mechanics And Thermodynamics Applying Four Different Physical Models And COSMO-Theory

2014

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Reduction of interfacial tension is of key importance for mobilising residual oil trapped by capillary forces during a secondary waterflood. The Conductor-like Screening Model (COSMO) and its extension COSMO-RS, developed over the last decades, enables prediction of thermodynamic properties of mixtures. Molecular charge distributions and associated charge distribution properties, so-called sigma moments, can be calculated and used as input parameters for various physical models to predict IFT of fluid mixtures. In this paper we present and compare four different and complementary approaches to predict IFT based on single-molecule properties derived from COSMO-RS theory. The first method is based on predicted liquid-liquid extraction (LLE) phasespecific mole fractions using a formalism suggested by Apostoluk and Szymanowski (1996). The second method relies on a Taylor-like approximation of chemical potentials of mixtures using a realisation of Method of Moments (MoM) as described by Klamt and co-workers. The third method, recently described by Andersson et al., relies on LLE calculations as well as free energies for molecules present at the interfaces in multiphase immiscible systems. The fourth method, the so-called GSMmodel recently described by the authors of this paper, relies on non-linear statistical relations between COSMO-derived energy descriptors and IFT. By conducting a comprehensive comparative analysis we show that each of the four models estimates IFT with significant accuracy, that these models are complementary and that the models should be chosen based on the specific system of interest as well as the present available system information. Moreover, we demonstrate that COSMO-RS theory, when used in combination with physical models, provides a powerful tool for EOR research enabling fast, accurate computational prediction of IFT of multiphase fluid mixtures. Hence the models presented here may be used for systematic laboratory testing of e.g. surfactants and co-solvents for EOR processes as well as for predicting properties of multiphase fluid systems.

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Section: The Andersson Et Al Model For Ift Predictionsupporting

confidence: 76%

Predicting Interfacial Tension Of Multiphase Systems Based On Computational Single-Molecule Quantum Mechanics And Thermodynamics Applying Four Different Physical Models And COSMO-Theory

2014

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“…There is no loss of accuracy in absolute terms for low IFT values, which is an improvement over MD methods. 16 In particular, the TZVPD-fine performs well for the low IFT values (Figure 2). The results for binary systems are also compiled in Table 1 and show that the TZVPD-fine parametrization performs slightly better than TZVP.…”

Section: ■ Resultsmentioning

confidence: 91%

“…The MD approach is also less straightforward for very low IFT values, 1−5 mN/m. 16 In this paper, we present a method for predicting the IFT between two liquid phases of arbitrary composition using density functional theory (DFT) calculations combined with the COSMO-RS implicit solvent model. This means that no experimental input is required other than what has already been used for parametrizing COSMO-RS.…”

Section: ■ Introductionmentioning

confidence: 99%

First-Principles Prediction of Liquid/Liquid Interfacial Tension

Andersson

Bennetzen

Klamt

et al. 2014

J. Chem. Theory Comput.

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The interfacial tension between two liquids is the free energy per unit surface area required to create that interface. Interfacial tension is a determining factor for two-phase liquid behavior in a wide variety of systems ranging from water flooding in oil recovery processes and remediation of groundwater aquifers contaminated by chlorinated solvents to drug delivery and a host of industrial processes. Here, we present a model for predicting interfacial tension from first principles using density functional theory calculations. Our model requires no experimental input and is applicable to liquid/liquid systems of arbitrary compositions. The consistency of the predictions with experimental data is significant for binary, ternary, and multicomponent water/organic compound systems, which offers confidence in using the model to predict behavior where no data exists. The method is fast and can be used as a screening technique as well as to extend experimental data into conditions where measurements are technically too difficult, time consuming, or impossible.

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“…The CG simulations of the n -alkane–water using the MARTINI description reproduce the interfacial tension with a deviation of 20%, which is no so poor compared to simulations with atomistic models , that show some limitations in the production of well-equilibrated liquid–liquid complex interfacial systems. We have added in Figure the interfacial tensions of the benzene–water and cyclohexane–water systems calculated from CG models used with the DPD method.…”

Section: Resultsmentioning

confidence: 95%

Coarse-Graining the Liquid–Liquid Interfaces with the MARTINI Force Field: How Is the Interfacial Tension Reproduced?

Ndao

Devémy

Ghoufi

et al. 2015

J. Chem. Theory Comput.

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We report two-phase coarse-grained (CG) simulations of organic-water liquid-liquid interfaces with the MARTINI force field. We discuss the ability of the CG force field to predict quantitatively the interfacial tension of alkanes-water, benzene-water, chloroform-water, and alcohol-water systems. The performance of the prediction of the interfacial tension is evaluated through its dependence on temperature and alkane length. This study contributes to the challenging discussion about the robustness and the transferability of the MARTINI force field to interfacial properties. We have also used the distributions of the molecules along the direction normal to the interface to investigate the composition of the interfacial region and to compare the simulated densities of the coexisting phases with experiments.

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Comparison of the capillary wave method and pressure tensor route for calculation of interfacial tension in molecular dynamics simulations

Cited by 6 publications

References 71 publications

Predicting Interfacial Tension Of Multiphase Systems Based On Computational Single-Molecule Quantum Mechanics And Thermodynamics Applying Four Different Physical Models And COSMO-Theory

Predicting Interfacial Tension Of Multiphase Systems Based On Computational Single-Molecule Quantum Mechanics And Thermodynamics Applying Four Different Physical Models And COSMO-Theory

First-Principles Prediction of Liquid/Liquid Interfacial Tension

Coarse-Graining the Liquid–Liquid Interfaces with the MARTINI Force Field: How Is the Interfacial Tension Reproduced?

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