The growth pattern and nucleation rate of carbon dioxide hydrate critically depend on the precise value of the hydrate–water interfacial free energy. There exist in the literature only two independent experimental measurements of this thermodynamic magnitude: one obtained by Uchida et al. [J. Phys. Chem. B 106, 8202 (2002)], 28(6) mJ/m2, and the other by Anderson and co-workers [J. Phys. Chem. B 107, 3507 (2003)], 30(3) mJ/m2. Recently, Algaba et al. [J. Colloid Interface Sci. 623, 354 (2022)] have extended the mold integration method proposed by Espinosa and co-workers [J. Chem. Phys. 141, 134709 (2014)] to deal with the CO2 hydrate–water interfacial free energy (mold integration–guest or MI-H). Computer simulations predict a value of 29(2) mJ/m2, in excellent agreement with experimental data. The method is based on the use of a mold of attractive wells located at the crystallographic positions of the oxygen atoms of water molecules in equilibrium hydrate structures to induce the formation of a thin hydrate slab in the liquid phase at coexistence conditions. We propose here a new implementation of the mold integration technique using a mold of attractive wells located now at the crystallographic positions of the carbon atoms of the CO2 molecules in the equilibrium hydrate structure. We find that the new mold integration–guest methodology, which does not introduce positional or orientational information of the water molecules in the hydrate phase, is able to induce the formation of CO2 hydrates in an efficient way. More importantly, this new version of the method predicts a CO2 hydrate–water interfacial energy value of 30(2) mJ/m2, in excellent agreement with experimental data, which is also fully consistent with the results obtained using the previous methodology.
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7 October 2022
Research Article|
October 07 2022
Simulation of the CO2 hydrate–water interfacial energy: The mold integration–guest methodology
Special Collection:
Fluids Meet Solids
Iván M. Zerón
;
Iván M. Zerón
(Conceptualization, Formal analysis, Funding acquisition, Visualization, Writing – original draft, Writing – review & editing)
1
Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Ciencias Integradas, Universidad de Huelva
, 21006 Huelva, Spain
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José Manuel Míguez
;
José Manuel Míguez
(Conceptualization, Validation)
1
Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Ciencias Integradas, Universidad de Huelva
, 21006 Huelva, Spain
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Bruno Mendiboure;
Bruno Mendiboure
(Formal analysis, Methodology)
2
Laboratoire des Fluides Complexes et Leurs Réserviors, UMR5150, Université de Pau et des Pays de l’Adour
, B.P. 1155, Pau Cdex 64014, France
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Jesús Algaba
;
Jesús Algaba
(Formal analysis, Investigation, Methodology, Visualization, Writing – original draft)
1
Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Ciencias Integradas, Universidad de Huelva
, 21006 Huelva, Spain
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Felipe J. Blas
Felipe J. Blas
a)
(Conceptualization, Funding acquisition, Investigation, Methodology, Writing – review & editing)
1
Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Ciencias Integradas, Universidad de Huelva
, 21006 Huelva, Spain
a)Author to whom correspondence should be addressed: felipe@uhu.es
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a)Author to whom correspondence should be addressed: felipe@uhu.es
Note: This paper is part of the JCP Special Topic on Fluids Meets Solids.
J. Chem. Phys. 157, 134709 (2022)
Article history
Received:
June 03 2022
Accepted:
September 13 2022
Citation
Iván M. Zerón, José Manuel Míguez, Bruno Mendiboure, Jesús Algaba, Felipe J. Blas; Simulation of the CO2 hydrate–water interfacial energy: The mold integration–guest methodology. J. Chem. Phys. 7 October 2022; 157 (13): 134709. https://doi.org/10.1063/5.0101746
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