Wetting Properties of the CO2-Water-Calcite System via Molecular Simulations: Shape and Size Effects.

Assessment of the risks and environmental impacts of carbon geosequestration requires knowledge about the wetting behavior of mineral surfaces in the presence of CO2 and the pore fluids. In this context, the interfacial tension (IFT) between CO2 and the aqueous fluid and the contact angle, θ, with the pore mineral surfaces are the two key parameters that control the capillary pressure in the pores of the candidate host rock. Knowledge of these two parameters and their dependence on the local conditions of pressure, temperature and salinity is essential for the correct prediction of structural and residual trapping. We have performed classical molecular dynamics simulations to predict the CO2-water IFT and the CO2-water-calcite contact angle. The IFT results are consistent with previous simulations, where simple point charge water models have been shown to underestimate the water surface tension, thus affecting the simulated IFT values. When combined with the EPM2 CO2 model, the SPC/Fw water model indeed underestimates the IFT in the low pressure region at all temperatures studied. On the other hand, at high pressure and low temperature, the IFT is overestimated by ~5 mN/m. Literature data regarding the water contact angle on calcite are contradictory. Using our new set of force field parameters, we performed NVT simulations at 323 K and 20 MPa to calculate the contact angle of a water droplet on the calcite {10.4} surface in a CO2 atmosphere. We performed simulations for both spherical and cylindrical droplet configurations for different initial radii, to study the size dependence of the water contact angle on calcite in the presence of CO2. Our results suggest that the contact angle of a cylindrical water droplet on calcite {10.4}, in the presence of CO2, is independent of droplet size, for droplets with a radius of 50 Å or more. On the contrary, spherical droplets make a contact angle that is strongly influenced by their size. At the largest size explored in this study, both spherical and cylindrical droplets converge to the same contact angle, 38˚, indicating that calcite is strongly wetted by water.

[1]  Sidqi A. Abu-Khamsin,et al.  Wettability of rock/CO2/brine and rock/oil/CO2-enriched-brine systems:Critical parametric analysis and future outlook. , 2019, Advances in colloid and interface science.

[2]  C. Böhm,et al.  Wettability of calcite under carbon storage conditions , 2019, International Journal of Greenhouse Gas Control.

[3]  J. Gale,et al.  Where is the Most Hydrophobic Region? Benzopurpurine Self-Assembly at the Calcite-Water Interface , 2017 .

[4]  Julian D. Gale,et al.  A Quantum Mechanically Derived Force Field To Predict CO2 Adsorption on Calcite {10.4} in an Aqueous Environment , 2017 .

[5]  Yongchen Song,et al.  Wettability of Supercritical CO2–Brine–Mineral: The Effects of Ion Type and Salinity , 2017 .

[6]  S. Iglauer,et al.  CO2 storage in carbonates: Wettability of calcite , 2017 .

[7]  T. Matsuoka,et al.  Modeling CO2-Water-Mineral Wettability and Mineralization for Carbon Geosequestration. , 2017, Accounts of chemical research.

[8]  Lingling Zhao,et al.  Molecular Gibbs Surface Excess and CO2-Hydrate Density Determine the Strong Temperature- and Pressure-Dependent Supercritical CO2-Brine Interfacial Tension. , 2017, The journal of physical chemistry. B.

[9]  Govind Paneru,et al.  Line tension and its influence on droplets and particles at surfaces , 2017 .

[10]  N. Bovet,et al.  Adsorbed Organic Material and Its Control on Wettability , 2017 .

[11]  M. Andersson,et al.  Calcite Wettability in the Presence of Dissolved Mg2+ and SO42- , 2017 .

[12]  M. Andersson,et al.  Predicting CO2-H2O Interfacial Tension Using COSMO-RS. , 2017, Journal of chemical theory and computation.

[13]  Lingling Zhao,et al.  Ionic Effects on Supercritical CO2-Brine Interfacial Tensions: Molecular Dynamics Simulations and a Universal Correlation with Ionic Strength, Temperature, and Pressure. , 2016, Langmuir : the ACS journal of surfaces and colloids.

[14]  Yongchen Song,et al.  Pressure and Temperature Dependence of Contact Angles for CO2/Water/Silica Systems Predicted by Molecular Dynamics Simulations , 2016 .

[15]  Yongchen Song,et al.  Water Contact Angle Dependence with Hydroxyl Functional Groups on Silica Surfaces under CO2 Sequestration Conditions. , 2015, Environmental science & technology.

[16]  Yongchen Song,et al.  Water contact angles on quartz surfaces under supercritical CO 2 sequestration conditions: Experimental and molecular dynamics simulation studies , 2015 .

[17]  J. Gale,et al.  Thermodynamically Consistent Force Field for Molecular Dynamics Simulations of Alkaline-Earth Carbonates and Their Aqueous Speciation , 2015 .

[18]  D. DePaolo,et al.  The Nanoscale Basis of CO2 Trapping for Geologic Storage. , 2015, Environmental science & technology.

[19]  W. Welch,et al.  Molecular Dynamics Simulations of CO2/Water/Quartz Interfacial Properties: Impact of CO2 Dissolution in Water. , 2015, Langmuir : the ACS journal of surfaces and colloids.

[20]  M. Olsson,et al.  Adsorption of ethanol and water on calcite: dependence on surface geometry and effect on surface behavior. , 2015, Langmuir : the ACS journal of surfaces and colloids.

[21]  Andreas Busch,et al.  CO2 wettability of seal and reservoir rocks and the implications for carbon geo‐sequestration , 2015 .

[22]  H. Urbassek,et al.  Contact angle of sessile drops in Lennard-Jones systems. , 2014, Langmuir : the ACS journal of surfaces and colloids.

[23]  S. Gíslason,et al.  Carbon Storage in Basalt , 2014, Science.

[24]  E. A. Müller,et al.  Resolving Discrepancies in the Measurements of the Interfacial Tension for the CO2 + H2O Mixture by Computer Simulation. , 2014, The journal of physical chemistry letters.

[25]  R. Cygan,et al.  Molecular simulation of carbon dioxide, brine, and clay mineral interactions and determination of contact angles. , 2014, Environmental science & technology.

[26]  P. Debenedetti,et al.  Simulations of vapor–liquid phase equilibrium and interfacial tension in the CO2–H2O–NaCl system , 2013 .

[27]  M. Piri,et al.  Wettability of supercritical carbon dioxide/water/quartz systems: simultaneous measurement of contact angle and interfacial tension at reservoir conditions. , 2013, Langmuir : the ACS journal of surfaces and colloids.

[28]  E. Boek,et al.  Molecular dynamics simulations of CO2 and brine interfacial tension at high temperatures and pressures. , 2013, The journal of physical chemistry. B.

[29]  Shibo Wang,et al.  Wettability phenomena at the CO2-brine-mineral interface: implications for geologic carbon sequestration. , 2013, Environmental science & technology.

[30]  Danny Perez,et al.  Insights into Microscopic Diffusion Processes at a Solid/Fluid Interface under Supercritical Conditions: A Study of the Aqueous Calcite (101̅4) Surface , 2012 .

[31]  S. Iglauer,et al.  Molecular dynamics computations of brine-CO2 interfacial tensions and brine-CO2-quartz contact angles and their effects on structural and residual trapping mechanisms in carbon geo-sequestration. , 2012, Journal of colloid and interface science.

[32]  D. Broseta,et al.  Are rocks still water‐wet in the presence of dense CO2 or H2S? , 2012 .

[33]  C. Massard,et al.  Nanoporous surface wetting behavior: the line tension influence. , 2012, Langmuir : the ACS journal of surfaces and colloids.

[34]  R. Cygan,et al.  Molecular Simulation of Carbon Dioxide Capture by Montmorillonite Using an Accurate and Flexible Force Field , 2012 .

[35]  Ian C. Bourg,et al.  Predicting CO2-water interfacial tension under pressure and temperature conditions of geologic CO2 storage , 2012 .

[36]  E. Boek,et al.  Interfacial Tension of (Brines + CO2): (0.864 NaCl + 0.136 KCl) at Temperatures between (298 and 448) K, Pressures between (2 and 50) MPa, and Total Molalities of (1 to 5) mol·kg–1 , 2012 .

[37]  P. Bikkina.  Reply to the comments on “Contact angle measurements of CO2–water–quartz/calcite systems in the perspective of carbon sequestration” , 2012 .

[38]  A. Ortona,et al.  Wetting and contact-line effects for spherical and cylindrical droplets on graphene layers: a comparative molecular-dynamics investigation. , 2011, Physical review. E, Statistical, nonlinear, and soft matter physics.

[39]  A. V. van Duin,et al.  A reactive force field for aqueous-calcium carbonate systems. , 2011, Physical chemistry chemical physics : PCCP.

[40]  M. Riazi,et al.  WETTABILITY OF COMMON ROCK-FORMING MINERALS IN A CO 2 -BRINE SYSTEM AT RESERVOIR CONDITIONS , 2011 .

[41]  J. Bohr,et al.  Thickness and structure of the water film deposited from vapour on calcite surfaces , 2010 .

[42]  Daniel Blankschtein,et al.  Molecular dynamics simulation study of water surfaces: comparison of flexible water models. , 2010, The journal of physical chemistry. B.

[43]  D. Lohse,et al.  Origin of line tension for a Lennard-Jones nanodroplet , 2010, 1010.0517.

[44]  Shuyan Liu,et al.  Molecular dynamics simulation of wetting behavior at CO2/water/solid interfaces , 2010 .

[45]  J. Carlos Santamarina,et al.  Water‐CO2‐mineral systems: Interfacial tension, contact angle, and diffusion—Implications to CO2 geological storage , 2010 .

[46]  David Quigley,et al.  Derivation of an accurate force-field for simulating the growth of calcium carbonate from aqueous solution : a new model for the calcite-water interface , 2010 .

[47]  A. Nakajima,et al.  Evaporation behavior of microliter- and sub-nanoliter-scale water droplets on two different fluoroalkylsilane coatings. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[48]  A. Méndez-Vilas,et al.  Ultrasmall liquid droplets on solid surfaces: production, imaging, and relevance for current wetting research. , 2009, Small.

[49]  J. Alejandre,et al.  Effect of flexibility on surface tension and coexisting densities of water. , 2008, The Journal of chemical physics.

[50]  Søren Toxvaerd,et al.  Contact Angles of Lennard-Jones Liquids and Droplets on Planar Surfaces , 2007 .

[51]  D. Broseta,et al.  CO2/water interfacial tensions under pressure and temperature conditions of CO2 geological storage , 2007 .

[52]  G. Voth,et al.  Flexible simple point-charge water model with improved liquid-state properties. , 2006, The Journal of chemical physics.

[53]  A. Amirfazli,et al.  Status of the three-phase line tension: a review. , 2004, Advances in colloid and interface science.

[54]  Petros Koumoutsakos,et al.  On the Water−Carbon Interaction for Use in Molecular Dynamics Simulations of Graphite and Carbon Nanotubes , 2003 .

[55]  P. Rossky,et al.  Molecular Structure of the Water−Supercritical CO2 Interface , 2001 .

[56]  A. Amirfazli,et al.  Measurements of Line Tension for Solid−Liquid−Vapor Systems Using Drop Size Dependence of Contact Angles and Its Correlation with Solid−Liquid Interfacial Tension , 2000 .

[57]  S. Stipp.  Toward a conceptual model of the calcite surface: hydration, hydrolysis, and surface potential , 1999 .

[58]  T. D. Blake,et al.  DYNAMIC WETTING STUDIED BY MOLECULAR MODELING SIMULATIONS OF DROPLET SPREADING , 1999 .

[59]  Kwong H. Yung,et al.  Carbon Dioxide's Liquid-Vapor Coexistence Curve And Critical Properties as Predicted by a Simple Molecular Model , 1995 .

[60]  B. Widom.  LINE TENSION AND THE SHAPE OF A SESSILE DROP , 1995 .

[61]  Steve Plimpton,et al.  Fast parallel algorithms for short-range molecular dynamics , 1993 .

[62]  M. Hochella,et al.  Structure and bonding environments at the calcite surface as observed with X-ray photoelectron spectroscopy (XPS) and low energy electron diffraction (LEED) , 1991 .

[63]  Davenport,et al.  Analytic embedded-atom potentials for fcc metals: Application to liquid and solid copper. , 1991, Physical review. B, Condensed matter.

[64]  D. Platikanov,et al.  Line tension in three-phase equilibrium systems , 1988 .

[65]  M. Matsumoto,et al.  Study on liquid–vapor interface of water. I. Simulational results of thermodynamic properties and orientational structure , 1988 .

[66]  M. Parrinello,et al.  Polymorphic transitions in single crystals: A new molecular dynamics method , 1981 .

[67]  G. Scherillo,et al.  Interfacial tension , 2021, Supercritical Fluid Science and Technology.

[68]  Jia‐Jyun Dong,et al.  Numerical assessment of CO2 geological sequestration in sloping and layered heterogeneous formations: A case study from Taiwan , 2014 .

[69]  Ole Torsæter,et al.  Wettability behaviour of CO2 at storage conditions , 2013 .

[70]  David R. Cole,et al.  Geochemistry of Geologic Carbon Sequestration: An Overview , 2013 .

[71]  T. Matsuoka,et al.  Molecular Dynamics Simulations of the CO2-Water-silica Interfacial Systems , 2013 .

[72]  S. Iglauer,et al.  Molecular Dynamics Simulation of Water/CO2-quartz Interfacial Properties: Application to Subsurface Gas Injection , 2013 .

[73]  Laura M. Hamm,et al.  Molecular Simulation of CO2- and CO3-Brine-Mineral Systems , 2013 .

[74]  L. C. Nielsen.  Predicting CO 2 -water interfacial tension under pressure and temperature conditions of geologic CO 2 storage , 2012 .

[75]  J. Santamarina,et al.  Water ‐ CO 2 ‐ mineral systems : Interfacial tension , contact angle , and diffusion — Implications to CO 2 geological storage , 2010 .

[76]  Bjørn Kvamme,et al.  Measurements and modelling of interfacial tension for water + carbon dioxide systems at elevated pressures , 2007 .

[77]  M. Klein,et al.  Nos&Hoover chains: The canonical ensemble via continuous dynamics , 1999 .

[78]  R W Hockney,et al.  Computer Simulation Using Particles , 1966 .

[79]  Thomas Young,et al.  An Essay on the Cohesion of Fluids , 1800 .