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Title: Contact angles from Young’s equation in molecular dynamics simulations

Abstract

In this work, we propose a method to calculate the equilibrium contact angle of heterogeneous 3-phase solid/fluid/fluid systems using molecular dynamics simulations. The proposed method, which combines the phantom-wall method [F. Leroy and F. Müller-Plathe, J. Chem. Phys. 133, 044110 (2010)] and Bennett’s acceptance ratio approach [C. H. Bennett, J. Comput. Phys. 22, 245 (1976)], is able to calculate the solid/fluid surface tension relative to the solid surface energy. The calculated relative surface tensions can then be used in Young’s equation to estimate the equilibrium contact angle. A fluid droplet is not needed for the proposed method, in contrast to the situation for direct simulations of contact angles. In addition, while prior free-energy based methods for contact angles mainly focused on the wetting of fluids in coexistence with their vapor on solid surfaces, the proposed approach was designed to study the contact angles of fluid mixtures on solid surfaces above the fluid saturation pressures. Using the proposed approach, the contact angles of binary Lennard-Jones fluid mixtures on a non-polar solid substrate were calculated at various interaction parameters and the contact angle of water in equilibrium with CO 2 on a hydrophilic polar silica surface was obtained. For both non-polar andmore » polar systems, the calculated contact angles from the proposed method were in agreement with those obtained from the geometry of a cylindrical droplet. The computational cost of the proposed method was found to be comparable to that of simulations that use fluid droplets, but the new method provides a way to calculate the contact angle directly from Young’s equation without ambiguity.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering
  2. Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering; Technical Univ. of Darmstadt (Germany). Eduard Zintl Inst. of Inorganic and Physical Chemistry
Publication Date:
Research Org.:
Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States); German Research Foundation (DFG)
OSTI Identifier:
1474037
Alternate Identifier(s):
OSTI ID: 1377981
Grant/Contract Number:  
SC0002128; AWD 1004131
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 8; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS; Lennard-Jones fluid; chemical compounds and components; surface energy; fluid flows; chemical elements; liquid solid interfaces; fluid systems; molecular dynamics; free energy; electrostatics

Citation Formats

Jiang, Hao, Müller-Plathe, Florian, and Panagiotopoulos, Athanassios Z. Contact angles from Young’s equation in molecular dynamics simulations. United States: N. p., 2017. Web. doi:10.1063/1.4994088.
Jiang, Hao, Müller-Plathe, Florian, & Panagiotopoulos, Athanassios Z. Contact angles from Young’s equation in molecular dynamics simulations. United States. doi:10.1063/1.4994088.
Jiang, Hao, Müller-Plathe, Florian, and Panagiotopoulos, Athanassios Z. Thu . "Contact angles from Young’s equation in molecular dynamics simulations". United States. doi:10.1063/1.4994088. https://www.osti.gov/servlets/purl/1474037.
@article{osti_1474037,
title = {Contact angles from Young’s equation in molecular dynamics simulations},
author = {Jiang, Hao and Müller-Plathe, Florian and Panagiotopoulos, Athanassios Z.},
abstractNote = {In this work, we propose a method to calculate the equilibrium contact angle of heterogeneous 3-phase solid/fluid/fluid systems using molecular dynamics simulations. The proposed method, which combines the phantom-wall method [F. Leroy and F. Müller-Plathe, J. Chem. Phys. 133, 044110 (2010)] and Bennett’s acceptance ratio approach [C. H. Bennett, J. Comput. Phys. 22, 245 (1976)], is able to calculate the solid/fluid surface tension relative to the solid surface energy. The calculated relative surface tensions can then be used in Young’s equation to estimate the equilibrium contact angle. A fluid droplet is not needed for the proposed method, in contrast to the situation for direct simulations of contact angles. In addition, while prior free-energy based methods for contact angles mainly focused on the wetting of fluids in coexistence with their vapor on solid surfaces, the proposed approach was designed to study the contact angles of fluid mixtures on solid surfaces above the fluid saturation pressures. Using the proposed approach, the contact angles of binary Lennard-Jones fluid mixtures on a non-polar solid substrate were calculated at various interaction parameters and the contact angle of water in equilibrium with CO2 on a hydrophilic polar silica surface was obtained. For both non-polar and polar systems, the calculated contact angles from the proposed method were in agreement with those obtained from the geometry of a cylindrical droplet. The computational cost of the proposed method was found to be comparable to that of simulations that use fluid droplets, but the new method provides a way to calculate the contact angle directly from Young’s equation without ambiguity.},
doi = {10.1063/1.4994088},
journal = {Journal of Chemical Physics},
number = 8,
volume = 147,
place = {United States},
year = {2017},
month = {8}
}

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Works referenced in this record:

Carbon Dioxide's Liquid-Vapor Coexistence Curve And Critical Properties as Predicted by a Simple Molecular Model
journal, August 1995

  • Harris, Jonathan G.; Yung, Kwong H.
  • The Journal of Physical Chemistry, Vol. 99, Issue 31
  • DOI: 10.1021/j100031a034

Test-area simulation method for the direct determination of the interfacial tension of systems with continuous or discontinuous potentials
journal, October 2005

  • Gloor, Guy J.; Jackson, George; Blas, Felipe J.
  • The Journal of Chemical Physics, Vol. 123, Issue 13
  • DOI: 10.1063/1.2038827

Molecular Modeling of Thermodynamic and Transport Properties for CO 2 and Aqueous Brines
journal, February 2017

  • Jiang, Hao; Economou, Ioannis G.; Panagiotopoulos, Athanassios Z.
  • Accounts of Chemical Research, Vol. 50, Issue 4
  • DOI: 10.1021/acs.accounts.6b00632

Computer simulation of the liquid–solid–vapour contact angle
journal, January 1977


Conceptual aspects of line tensions
journal, October 2007

  • Schimmele, L.; Napiórkowski, M.; Dietrich, S.
  • The Journal of Chemical Physics, Vol. 127, Issue 16
  • DOI: 10.1063/1.2799990

The Nanoscale Basis of CO 2 Trapping for Geologic Storage
journal, August 2015

  • Bourg, Ian C.; Beckingham, Lauren E.; DePaolo, Donald J.
  • Environmental Science & Technology, Vol. 49, Issue 17
  • DOI: 10.1021/acs.est.5b03003

From hydration repulsion to dry adhesion between asymmetric hydrophilic and hydrophobic surfaces
journal, September 2015

  • Kanduč, Matej; Netz, Roland R.
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 40
  • DOI: 10.1073/pnas.1504919112

Efficient estimation of free energy differences from Monte Carlo data
journal, October 1976


Direct calculation of the crystal–melt interfacial free energies for continuous potentials: Application to the Lennard-Jones system
journal, January 2003

  • Davidchack, Ruslan L.; Laird, Brian B.
  • The Journal of Chemical Physics, Vol. 118, Issue 16
  • DOI: 10.1063/1.1563248

Wetting and contact-line effects for spherical and cylindrical droplets on graphene layers: A comparative molecular-dynamics investigation
journal, December 2011


Can Dynamic Contact Angle Be Measured Using Molecular Modeling?
journal, October 2012


The mold integration method for the calculation of the crystal-fluid interfacial free energy from simulations
journal, October 2014

  • Espinosa, J. R.; Vega, C.; Sanz, E.
  • The Journal of Chemical Physics, Vol. 141, Issue 13
  • DOI: 10.1063/1.4896621

Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes
journal, March 1977

  • Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C.
  • Journal of Computational Physics, Vol. 23, Issue 3
  • DOI: 10.1016/0021-9991(77)90098-5

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Ewald summation for systems with slab geometry
journal, August 1999

  • Yeh, In-Chul; Berkowitz, Max L.
  • The Journal of Chemical Physics, Vol. 111, Issue 7
  • DOI: 10.1063/1.479595

On the cohesion of fluids and their adhesion to solids: Young's equation at the atomic scale
journal, July 2017

  • Fernandez-Toledano, J. -C.; Blake, T. D.; Lambert, P.
  • Advances in Colloid and Interface Science, Vol. 245
  • DOI: 10.1016/j.cis.2017.03.006

Molecular-dynamics study of a three-dimensional one-component model for distortive phase transitions
journal, February 1978


Application of the interface potential approach to calculate the wetting properties of a water model system
journal, December 2013


Surface Tensions in NaCl−Water−Air Systems from MD Simulations
journal, October 2007

  • Bahadur, Ranjit; Russell, Lynn M.; Alavi, Saman
  • The Journal of Physical Chemistry B, Vol. 111, Issue 41
  • DOI: 10.1021/jp075356c

Atomistic simulations of wetting properties and water films on hydrophilic surfaces
journal, April 2017

  • Kanduč, Matej; Netz, Roland R.
  • The Journal of Chemical Physics, Vol. 146, Issue 16
  • DOI: 10.1063/1.4979847

Contact Angles of Lennard-Jones Liquids and Droplets on Planar Surfaces
journal, June 2007

  • Ingebrigtsen, T.; Toxvaerd, S.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 24
  • DOI: 10.1021/jp0676235

Molecular Dynamics Simulations of the CO2-Water-silica Interfacial Systems
journal, January 2013


Dry-Surface Simulation Method for the Determination of the Work of Adhesion of Solid–Liquid Interfaces
journal, July 2015


Influence of Contact-Line Curvature on the Evaporation of Nanodroplets from Solid Substrates
journal, July 2014


Parametrizing Nonbonded Interactions from Wetting Experiments via the Work of Adhesion: Example of Water on Graphene Surfaces
journal, December 2015

  • Leroy, Frédéric; Liu, Shengyuan; Zhang, Jianguo
  • The Journal of Physical Chemistry C, Vol. 119, Issue 51
  • DOI: 10.1021/acs.jpcc.5b10267

Solid-liquid surface free energy of Lennard-Jones liquid on smooth and rough surfaces computed by molecular dynamics using the phantom-wall method
journal, July 2010

  • Leroy, Frédéric; Müller-Plathe, Florian
  • The Journal of Chemical Physics, Vol. 133, Issue 4
  • DOI: 10.1063/1.3458796

Does Young's equation hold on the nanoscale? A Monte Carlo test for the binary Lennard-Jones fluid
journal, October 2010


Young’s Equation for a Two-Liquid System on the Nanometer Scale
journal, March 2017


Molecular dynamics investigation of the crystal–fluid interface. VI. Excess surface free energies of crystal–liquid systems
journal, May 1986

  • Broughton, J. Q.; Gilmer, G. H.
  • The Journal of Chemical Physics, Vol. 84, Issue 10
  • DOI: 10.1063/1.449884

Force Field and a Surface Model Database for Silica to Simulate Interfacial Properties in Atomic Resolution
journal, April 2014

  • Emami, Fateme S.; Puddu, Valeria; Berry, Rajiv J.
  • Chemistry of Materials, Vol. 26, Issue 8
  • DOI: 10.1021/cm500365c

Molecular Simulation of Carbon Dioxide, Brine, and Clay Mineral Interactions and Determination of Contact Angles
journal, January 2014

  • Tenney, Craig M.; Cygan, Randall T.
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es404075k

Interfacial Excess Free Energies of Solid-Liquid Interfaces by Molecular Dynamics Simulation and Thermodynamic Integration
journal, May 2009

  • Leroy, Frédéric; dos Santos, Daniel J. V. A.; Müller-Plathe, Florian
  • Macromolecular Rapid Communications, Vol. 30, Issue 9-10
  • DOI: 10.1002/marc.200800746

Wetting of Graphene Oxide: A Molecular Dynamics Study
journal, March 2014

  • Wei, Ning; Lv, Cunjing; Xu, Zhiping
  • Langmuir, Vol. 30, Issue 12
  • DOI: 10.1021/la500513x

Calculation of interfacial properties via free-energy-based molecular simulation: The influence of system size
journal, June 2010

  • Grzelak, Eric M.; Errington, Jeffrey R.
  • The Journal of Chemical Physics, Vol. 132, Issue 22
  • DOI: 10.1063/1.3431525

Contact Angle of Sessile Drops in Lennard-Jones Systems
journal, November 2014

  • Becker, Stefan; Urbassek, Herbert M.; Horsch, Martin
  • Langmuir, Vol. 30, Issue 45
  • DOI: 10.1021/la503974z

Wetting Behavior of Water near Nonpolar Surfaces
journal, October 2013

  • Kumar, Vaibhaw; Errington, Jeffrey R.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 44
  • DOI: 10.1021/jp4084647

Obtaining the solid-liquid interfacial free energy via multi-scheme thermodynamic integration: Ag-ethylene glycol interfaces
journal, November 2016

  • Qi, Xin; Zhou, Ya; Fichthorn, Kristen A.
  • The Journal of Chemical Physics, Vol. 145, Issue 19
  • DOI: 10.1063/1.4967521

What Is the Contact Angle of Water on Graphene?
journal, January 2013

  • Taherian, Fereshte; Marcon, Valentina; van der Vegt, Nico F. A.
  • Langmuir, Vol. 29, Issue 5
  • DOI: 10.1021/la304645w

The Statistical Mechanical Theory of Surface Tension
journal, March 1949

  • Kirkwood, John G.; Buff, Frank P.
  • The Journal of Chemical Physics, Vol. 17, Issue 3
  • DOI: 10.1063/1.1747248

Polymorphic transitions in single crystals: A new molecular dynamics method
journal, December 1981

  • Parrinello, M.; Rahman, A.
  • Journal of Applied Physics, Vol. 52, Issue 12
  • DOI: 10.1063/1.328693

CO 2 –Water–Rock Wettability: Variability, Influencing Factors, and Implications for CO 2 Geostorage
journal, April 2017


Molecular dynamics simulation of the contact angle of liquids on solid surfaces
journal, January 2009

  • Shi, Bo; Dhir, Vijay K.
  • The Journal of Chemical Physics, Vol. 130, Issue 3
  • DOI: 10.1063/1.3055600

Phase Equilibria of Water/CO 2 and Water/ n -Alkane Mixtures from Polarizable Models
journal, February 2017

  • Jiang, Hao; Economou, Ioannis G.; Panagiotopoulos, Athanassios Z.
  • The Journal of Physical Chemistry B, Vol. 121, Issue 6
  • DOI: 10.1021/acs.jpcb.6b12791

Young’s Equation at the Nanoscale
journal, August 2013


Computation of interfacial properties via grand canonical transition matrix Monte Carlo simulation
journal, January 2008

  • Grzelak, Eric M.; Errington, Jeffrey R.
  • The Journal of Chemical Physics, Vol. 128, Issue 1
  • DOI: 10.1063/1.2812285

A molecular dynamics study to determine the solid-liquid interfacial tension using test area simulation method (TASM)
journal, August 2012

  • Nair, Anjan R.; Sathian, Sarith P.
  • The Journal of Chemical Physics, Vol. 137, Issue 8
  • DOI: 10.1063/1.4746750

Contact Angle, Liquid Film, and Liquid–Liquid and Liquid–Solid Interfaces in Model Oil–Brine–Substrate Systems
journal, May 2016

  • Jiménez-Ángeles, Felipe; Firoozabadi, Abbas
  • The Journal of Physical Chemistry C, Vol. 120, Issue 22
  • DOI: 10.1021/acs.jpcc.6b01521

The missing term in effective pair potentials
journal, November 1987

  • Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P.
  • The Journal of Physical Chemistry, Vol. 91, Issue 24
  • DOI: 10.1021/j100308a038

Molecular Dynamics Simulation of Contact Angles of Water Droplets in Carbon Nanotubes
journal, December 2001

  • Werder, Thomas; Walther, Jens H.; Jaffe, Richard L.
  • Nano Letters, Vol. 1, Issue 12
  • DOI: 10.1021/nl015640u

Molecular Dynamics Simulations of CO 2 /Water/Quartz Interfacial Properties: Impact of CO 2 Dissolution in Water
journal, May 2015