Vacancy-Mediated Increases in Brine–Salt Surface Energies

Rimsza, Jessica M.; Kuhlman, Kristopher L.

doi:10.1021/acs.langmuir.4c04199

Vacancy-Mediated Increases in Brine–Salt Surface Energies

Journal Article · Mon Dec 30 00:00:00 EST 2024 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.4c04199· OSTI ID:2530824

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Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Salt formations have been explored for the permanent isolation of spent nuclear fuel based on their high thermal conductivity, self-healing nature, and low hydraulic permeability to brine flow. Vacancy defect concentrations in salt complicate fracture mechanics not driven by dislocation dynamics and can influence the resulting surface structure. Classical molecular dynamic simulations were used to simulate tensile testing of salt crystals (halite) with vacancy defect concentrations of up to 0.5 defects/nm³. Increasing defect concentrations resulted in a decrease in ultimate tensile strength and fracture surface energies, driven by increased surface roughness rather than changes in the amount of surface area. Brine–salt surface energies of the fractured surfaces were 0.22 to 0.26 J/m², significantly higher than values reported for atomically flat (100) surfaces at the same brine composition. This change in surface energy increased the brine–salt dihedral angle by ~27°. The dihedral angle threshold for percolation in salt is 60°, and a 27° increase due to rough fracture surfaces identifies a reduction in porosity percolation and a decrease in salt permeability. Therefore, bedded salt and salt domes may be even more stable than those previously predicted from dihedral angle calculations.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Office of Spent Fuel and Waste Disposition

Grant/Contract Number:: NA0003525

OSTI ID:: 2530824

Report Number(s):: SAND--2025-02261J

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 1 Vol. 41; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Kinetics of Water-Rock Interaction Brantley, Susan L.; Kubicki, James D.; White, Art F. Springer New York, NY https://doi.org/10.1007/978-0-387-73563-4	book	January 2008
Vacancy pairs and correlation effects in kCl and NaCl single crystals Beniere, Michelle; Chemla, Marius; Beniere, François Journal of Physics and Chemistry of Solids, Vol. 37, Issue 5 https://doi.org/10.1016/0022-3697(76)90080-9	journal	January 1976
Water adsorption on the NaCl surface Fölsch, S.; Henzler, M. Surface Science, Vol. 247, Issue 2-3 https://doi.org/10.1016/0039-6028(91)90136-G	journal	May 1991
Effect of dislocation activities on crack extension in ionic crystals Higashida, K.; Narita, N.; Matsunaga, K. Materials Science and Engineering: A, Vol. 176, Issue 1-2 https://doi.org/10.1016/0921-5093(94)90969-5	journal	March 1994
Birefringence observations of dislocation emission at crack tips in NaCl single crystals Foecke, T.; Gerberich, W. W. Scripta Metallurgica et Materialia, Vol. 24, Issue 3 https://doi.org/10.1016/0956-716X(90)90200-Z	journal	March 1990
Hydrology and hydraulic properties of a bedded evaporite formation Beauheim, Richard L.; Roberts, Randall M. Journal of Hydrology, Vol. 259, Issue 1-4 https://doi.org/10.1016/S0022-1694(01)00586-8	journal	March 2002
Ring statistics analysis of topological networks: New approach and application to amorphous GeS2 and SiO2 systems Le Roux, Sébastien; Jund, Philippe Computational Materials Science, Vol. 49, Issue 1 https://doi.org/10.1016/j.commatsci.2010.04.023	journal	June 2010
Molecular Dynamics Simulation of Water/CO2-quartz Interfacial Properties: Application to Subsurface Gas Injection McCaughan, Jack; Iglauer, Stefan; Bresme, Fernando Energy Procedia, Vol. 37 https://doi.org/10.1016/j.egypro.2013.06.457	journal	January 2013
Effect of strain rate on the mechanical properties of salt rock Liang, W. G.; Zhao, Y. S.; Xu, S. G. International Journal of Rock Mechanics and Mining Sciences, Vol. 48, Issue 1 https://doi.org/10.1016/j.ijrmms.2010.06.012	journal	January 2011
Effects of loading rate and temperature on tensile strength and deformation of rock salt Wisetsaen, Sopon; Walsri, Chaowarin; Fuenkajorn, Kittitep International Journal of Rock Mechanics and Mining Sciences, Vol. 73 https://doi.org/10.1016/j.ijrmms.2014.10.005	journal	January 2015
Receding and advancing (CO 2 + brine + quartz) contact angles as a function of pressure, temperature, surface roughness, salt type and salinity Al-Yaseri, Ahmed Z.; Lebedev, Maxim; Barifcani, Ahmed The Journal of Chemical Thermodynamics, Vol. 93 https://doi.org/10.1016/j.jct.2015.07.031	journal	February 2016
Atomistic simulation of temperature and defects effects on mechanical properties of selected single and bicrystalline geomaterials Molaei, Fatemeh; Nojabaei, Bahareh Journal of Molecular Graphics and Modelling, Vol. 117 https://doi.org/10.1016/j.jmgm.2022.108320	journal	December 2022
Mechanism of void growth in irradiated NaCl based on exiton-induced formation of divacancies at dislocations Dubinko, V. I.; Vainshtein, D. I.; den Hartog, H. W. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 228, Issue 1-4 https://doi.org/10.1016/j.nimb.2004.10.061	journal	January 2005
Molecular Modeling of Thermodynamic and Transport Properties for CO ₂ and Aqueous Brines Jiang, Hao; Economou, Ioannis G.; Panagiotopoulos, Athanassios Z. Accounts of Chemical Research, Vol. 50, Issue 4 https://doi.org/10.1021/acs.accounts.6b00632	journal	February 2017
Birth of NaCl Crystals: Insights from Molecular Simulations Lanaro, G.; Patey, G. N. The Journal of Physical Chemistry B, Vol. 120, Issue 34 https://doi.org/10.1021/acs.jpcb.6b05291	journal	August 2016
Temperature and Pressure Dependence of Salt–Brine Dihedral Angles in the Subsurface Rimsza, Jessica M.; Kuhlman, Kristopher L. Langmuir, Vol. 37, Issue 45 https://doi.org/10.1021/acs.langmuir.1c01836	journal	November 2021
Surface Structure and Stability of Partially Hydroxylated Silica Surfaces Rimsza, J. M.; Jones, R. E.; Criscenti, L. J. Langmuir, Vol. 33, Issue 15 https://doi.org/10.1021/acs.langmuir.7b00041	journal	April 2017
Surface Energies and Structure of Salt–Brine Interfaces Rimsza, Jessica M.; Kuhlman, Kristopher L. Langmuir, Vol. 36, Issue 9 https://doi.org/10.1021/acs.langmuir.9b03172	journal	February 2020
Structures and Surface Energies of (100) and Octopolar (111) Faces of Halite (NaCl): an Ab initio Quantum-Mechanical and Thermodynamical Study Bruno, Marco; Aquilano, Dino; Pastero, Linda Crystal Growth & Design, Vol. 8, Issue 7 https://doi.org/10.1021/cg8000027	journal	July 2008
Surface Tensions in NaCl−Water−Air Systems from MD Simulations Bahadur, Ranjit; Russell, Lynn M.; Alavi, Saman The Journal of Physical Chemistry B, Vol. 111, Issue 41 https://doi.org/10.1021/jp075356c	journal	October 2007
Molecular Dynamics Simulations of CO ₂ and Brine Interfacial Tension at High Temperatures and Pressures Li, Xuesong; Ross, Daniel A.; Trusler, J. P. Martin The Journal of Physical Chemistry B, Vol. 117, Issue 18 https://doi.org/10.1021/jp309730m	journal	April 2013
Structure and Dynamics of Potassium Chloride in Aqueous Solution Sindt, Julien O.; Alexander, Andrew J.; Camp, Philip J. The Journal of Physical Chemistry B, Vol. 118, Issue 31 https://doi.org/10.1021/jp5049937	journal	July 2014
Determination of Alkali and Halide Monovalent Ion Parameters for Use in Explicitly Solvated Biomolecular Simulations Joung, In Suk; Cheatham, Thomas E. The Journal of Physical Chemistry B, Vol. 112, Issue 30 https://doi.org/10.1021/jp8001614	journal	July 2008
Adsorption of Water on NaCl (100) Surfaces: Role of Atomic Steps Dai, Q.; Hu, J.; Salmeron, M. The Journal of Physical Chemistry B, Vol. 101, Issue 11 https://doi.org/10.1021/jp9625772	journal	March 1997
Structure and Energetics of the Water/NaCl(100) Interface Taylor, David P.; Hess, Wayne P.; McCarthy, Maureen I. The Journal of Physical Chemistry B, Vol. 101, Issue 38 https://doi.org/10.1021/jp970567a	journal	September 1997
Water Dissociation on Defective Sites on the NaCl(100) Surface. A Quantum ab Initio Study Allouche, A. The Journal of Physical Chemistry B, Vol. 102, Issue 50 https://doi.org/10.1021/jp9814496	journal	November 1998
An unconventional bilayer ice structure on a NaCl(001) film Chen, Ji; Guo, Jing; Meng, Xiangzhi Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5056	journal	May 2014
Novel Unexpected Reconstructions of (100) and (111) Surfaces of NaCl: Theoretical Prediction Kvashnin, Alexander G.; Kvashnin, Dmitry G.; Oganov, Artem R. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-50548-8	journal	October 2019
Dissolution of NaCl nanocrystals: an ab initio molecular dynamics study Holmberg, Nico; Chen, Jian-Cheng; Foster, Adam S. Phys. Chem. Chem. Phys., Vol. 16, Issue 33 https://doi.org/10.1039/C4CP00635F	journal	January 2014
Ab initio Kinetic Monte Carlo simulations of dissolution at the NaCl–water interface Chen, Jian-Cheng; Reischl, Bernhard; Spijker, Peter Phys. Chem. Chem. Phys., Vol. 16, Issue 41 https://doi.org/10.1039/C4CP02375G	journal	January 2014
Molecular dynamics computer simulation of thin films of LiCl, NaCl, KCl and RbCl possessing (100) crystal–vacuum surfaces Heyes, David M.; Barber, Michael; Clarke, Julian H. R. J. Chem. Soc., Faraday Trans. 2, Vol. 75, Issue 0 https://doi.org/10.1039/F29797501469	journal	January 1979
Thermodynamic properties and self-diffusion of molten sodium chloride. A molecular dynamics study Lewis, John W. E.; Singer, Konrad Journal of the Chemical Society, Faraday Transactions 2, Vol. 71 https://doi.org/10.1039/f29757100041	journal	January 1975
Pair potential for alkali metal halides with rock salt crystal structure. Molecular Dynamics Calculations on NaCl and LiI Michielsen, J.; Woerlee, P.; Graaf, F. v. d. Journal of the Chemical Society, Faraday Transactions 2, Vol. 71 https://doi.org/10.1039/f29757101730	journal	January 1975
A molecular dynamics study of the lattice vibrations of sodium chloride Jacucci, G.; Klein, M. L.; McDonald, I. R. Journal de Physique Lettres, Vol. 36, Issue 4 https://doi.org/10.1051/jphyslet:0197500360409700	journal	January 1975
Thickness-dependent ordering of water layers at the NaCl(100) surface Arsic, J.; Kaminski, D. M.; Radenovic, N. The Journal of Chemical Physics, Vol. 120, Issue 20 https://doi.org/10.1063/1.1712971	journal	May 2004
Cleavage Surface Energy of NaCl and MgO in Vacuum Gutshall, Paul L.; Gross, Gordon E. Journal of Applied Physics, Vol. 36, Issue 8 https://doi.org/10.1063/1.1714511	journal	August 1965
Calculation of the Surface Energies of Alkali Halide Crystals van Zeggeren, F.; Benson, G. C. The Journal of Chemical Physics, Vol. 26, Issue 5 https://doi.org/10.1063/1.1743473	journal	May 1957
Rate of homogeneous crystal nucleation in molten NaCl Valeriani, C.; Sanz, E.; Frenkel, D. The Journal of Chemical Physics, Vol. 122, Issue 19 https://doi.org/10.1063/1.1896348	journal	May 2005
Initial stages of water adsorption on NaCl (100) studied by scanning polarization force microscopy Verdaguer, Albert; Sacha, G. M.; Luna, M. The Journal of Chemical Physics, Vol. 123, Issue 12 https://doi.org/10.1063/1.1996568	journal	September 2005
Understanding the role of ions and water molecules in the NaCl dissolution process Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos The Journal of Chemical Physics, Vol. 139, Issue 23 https://doi.org/10.1063/1.4840675	journal	December 2013
Application of the molecular dynamics method to a liquid system with long range forces (Molten NaCl) Lantelme, Frédéric; Turq, Pierre; Quentrec, Bernard Molecular Physics, Vol. 28, Issue 6 https://doi.org/10.1080/00268977400102791	journal	December 1974
On the core structures of edge dislocations in NaCl and MgO. Consequences for the core configurations of dislocation dipoles Rabier, Jacques; Puls, Manfred P. Philosophical Magazine A, Vol. 59, Issue 4 https://doi.org/10.1080/01418618908209822	journal	April 1989
The structure of molten sodium chloride Edwards, F. G.; Enderby, J. E.; Howe, R. A. Journal of Physics C: Solid State Physics, Vol. 8, Issue 21 https://doi.org/10.1088/0022-3719/8/21/018	journal	November 1975
Morphological method for surface metrology and dimensional metrology based on the alpha shape Jiang, Xiangqian; Lou, Shan; Scott, Paul J. Measurement Science and Technology, Vol. 23, Issue 1 https://doi.org/10.1088/0957-0233/23/1/015003	journal	December 2011
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
Association Energy of Vacancies and Impurities with Edge Dislocations in NaCl Bassani, Franco; Thomson, Robb Physical Review, Vol. 102, Issue 5 https://doi.org/10.1103/PhysRev.102.1264	journal	June 1956
Density functional theory study of flat and stepped NaCl(001) Li, Bo; Michaelides, Angelos; Scheffler, Matthias Physical Review B, Vol. 76, Issue 7 https://doi.org/10.1103/PhysRevB.76.075401	journal	August 2007
Color centers in NaCl by hybrid functionals Chen, Wei; Tegenkamp, Christoph; Pfnür, Herbert Physical Review B, Vol. 82, Issue 10 https://doi.org/10.1103/PhysRevB.82.104106	journal	September 2010
Irreducible Finite-Size Effects in the Surface Free Energy of NaCl Crystals from Crystal-Nucleation Data Zykova-Timan, T.; Valeriani, C.; Sanz, E. Physical Review Letters, Vol. 100, Issue 3 https://doi.org/10.1103/PhysRevLett.100.036103	journal	January 2008
Equilibrium halite-H2O dihedral angles: High rock-salt permeability in the shallow crust? Lewis, Stephanie; Holness, Marian Geology, Vol. 24, Issue 5 https://doi.org/10.1130/0091-7613(1996)024<0431:EHHODA>2.3.CO;2	journal	January 1996
Crack Tip Plasticity in Ionic Crystals with the NaCl-Type Structure Higashida, Kenji; Narita, Nobutaka MATERIALS TRANSACTIONS, Vol. 42, Issue 1 https://doi.org/10.2320/matertrans.42.33	journal	January 2001
Structure of Cross-Slip Bands and Brittle-to-Ductile Transition in Ionic Crystals Narita, Nobutaka; Yoshimura, Takuya; Takahara, Yoshihiro MATERIALS TRANSACTIONS, Vol. 42, Issue 1 https://doi.org/10.2320/matertrans.42.41	journal	January 2001

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