Membrane-Assisted Crystallization: A Molecular View of NaCl Nucleation and Growth

Membrane-assisted crystallization, aiming to induce supersaturation in a solution, has been successfully tested in the crystallization of ionic salts, low molecular organic acids, and proteins. Membrane crystallization is an emerging membrane process with the capability to simultaneously extract fresh water and valuable components from various streams. Successful application of crystallization for produced water treatment, seawater desalination, and salt recovery has been demonstrated. Recently, membrane crystallization has been developed to recover valuable minerals from highly concentrated solutions, since the recovery of high-quality minerals is expected to impact agriculture, pharmaceuticals, and household activities. In this work, molecular dynamics simulations were used to study the crystal nucleation and growth of sodium chloride in bulk and with hydrophobic polymer surfaces of polyvinylidene fluoride (PVDF) and polypropylene (PP) at a supersaturated concentration of salt. In parallel, membrane crystallization experiments were performed utilizing the same polymeric membranes in order to compare the experimental results with the computational ones. Moreover, the comparison in terms of nucleation time between the crystallization of sodium chloride (NaCl) using the traditional evaporation process and the membrane-assisted crystallization process was performed. Here, with an integrated experimental–computational approach, we demonstrate that the PVDF and PP membranes assist the crystal growth for NaCl, speeding up crystal nucleation in comparison to the bulk solution and leading to smaller and regularly structured face-centered cubic lattice NaCl crystals. This results in a mutual validation between theoretical data and experimental findings and provides the stimuli to investigate other mono and bivalent crystals with a new class of materials in advanced membrane separations.

[1]  H. Berendsen,et al.  Molecular dynamics with coupling to an external bath , 1984 .

[2]  H. Sun,et al.  COMPASS: An ab Initio Force-Field Optimized for Condensed-Phase ApplicationsOverview with Details on Alkane and Benzene Compounds , 1998 .

[3]  G. Grest,et al.  Precursor film controlled wetting of Pb on Cu. , 2003, Physical review letters.

[4]  Enrico Drioli,et al.  Membrane crystallization of lysozyme: kinetic aspects , 2003 .

[5]  Enrico Drioli,et al.  Interactive functional poly(vinylidene fluoride) membranes with modulated lysozyme affinity: a promising class of new interfaces for contactor crystallizers , 2009 .

[6]  F. Roosen‐Runge,et al.  On the question of two-step nucleation in protein crystallization. , 2015, Faraday discussions.

[7]  William L. Jorgensen,et al.  Energy component analysis for dilute aqueous solutions of lithium(1+), sodium(1+), fluoride(1-), and chloride(1-) ions , 1984 .

[8]  S. Toxvaerd.  Molecular dynamics simulation of heterogeneous nucleation at a structureless solid surface , 2002 .

[9]  Phase field theory of heterogeneous crystal nucleation. , 2006, Physical review letters.

[10]  Li Duan,et al.  The mass transfer process and the growth rate of NaCl crystal growth by evaporation based on temporal phase evaluation , 2012 .

[11]  Katarzyna B. Koziara,et al.  Simulation of Crystallization of Biominerals , 2018, Annual Review of Materials Research.

[12]  Hugues Fauconnier,et al.  Editorial, special issue of NETYS 2015 , 2019, Computing.

[13]  A. Shimosaka,et al.  Molecular dynamics simulations of the formation for NaCl cluster at the interface between the supersaturated solution and the substrate , 2010 .

[14]  G. Patey,et al.  Evidence that crystal nucleation in aqueous NaCl solution Occurs by the two-step mechanism , 2013 .

[15]  G. Patey,et al.  How Crystals Nucleate and Grow in Aqueous NaCl Solution. , 2013, The journal of physical chemistry letters.

[16]  J. Åqvist,et al.  Ion-water interaction potentials derived from free energy perturbation simulations , 1990 .

[17]  H. Meirovitch.  Computer simulation of self-avoiding walks: Testing the scanning method , 1983 .

[18]  D. Frenkel,et al.  Onset of heterogeneous crystal nucleation in colloidal suspensions , 2004, Nature.

[19]  W. L. Jorgensen,et al.  Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids , 1996 .

[20]  R. Cygan,et al.  Molecular Dynamics Modeling of Ion Adsorption to the Basal Surfaces of Kaolinite , 2007 .

[21]  M. J. Ruiz-Montero,et al.  Numerical evidence for bcc ordering at the surface of a critical fcc nucleus. , 1995, Physical review letters.

[22]  Enrico Drioli,et al.  Hydrophobic membranes for salts recovery from desalination plants , 2010 .

[23]  Carsten Kutzner,et al.  GROMACS 4:  Algorithms for Highly Efficient, Load-Balanced, and Scalable Molecular Simulation. , 2008, Journal of chemical theory and computation.

[24]  W. L. Jorgensen,et al.  Energy component analysis for dilute aqueous solutions of lithium(1+), sodium(1+), fluoride(1-), and chloride(1-) ions , 1984 .

[25]  J. Banavar,et al.  Computer Simulation of Liquids , 1988 .

[26]  A. Michaelides,et al.  Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations , 2016, Chemical reviews.

[27]  Bai-xin Liu,et al.  Two-step crystal growth mechanism during crystallization of an undercooled Ni50Al50 alloy , 2016, Scientific Reports.

[28]  U. Suter,et al.  Detailed molecular structure of a vinyl polymer glass , 1985 .

[29]  S. Whitelam.  Control of pathways and yields of protein crystallization through the interplay of nonspecific and specific attractions. , 2010, Physical review letters.

[30]  Daan Frenkel,et al.  Homogeneous nucleation and the Ostwald step rule , 1999 .

[31]  E. Drioli,et al.  Study of the surface character as responsible for controlling interfacial forces at membrane-feed interface. , 2006, Journal of colloid and interface science.

[32]  Neal T. Skipper,et al.  X-ray and neutron diffraction studies on concentrated aqueous solutions of sodium nitrate and silver nitrate , 1989 .

[33]  T. Straatsma,et al.  THE MISSING TERM IN EFFECTIVE PAIR POTENTIALS , 1987 .

[34]  Elodie Chabanon,et al.  Membranes and crystallization processes: State of the art and prospects , 2016 .

[35]  E. Drioli,et al.  Membrane Crystallization Technology , 2010 .

[36]  K. Tsukamoto,et al.  Two types of amorphous protein particles facilitate crystal nucleation , 2017, Proceedings of the National Academy of Sciences.

[37]  D. Maes,et al.  Observing classical nucleation theory at work by monitoring phase transitions with molecular precision , 2014, Nature Communications.

[38]  K Schulten,et al.  VMD: visual molecular dynamics. , 1996, Journal of molecular graphics.

[39]  D. Gil-Carton,et al.  Molecular nucleation mechanisms and control strategies for crystal polymorph selection , 2018, Nature.

[40]  Enrico Drioli,et al.  Membrane distillation-crystallization of seawater reverse osmosis brines , 2010 .

[41]  E. Drioli,et al.  Bi2Se3-assisted membrane crystallization , 2018 .

[42]  V. Lachet,et al.  Classical force field for hydrofluorocarbon molecular simulations. Application to the study of gas solubility in poly(vinylidene fluoride). , 2015, The journal of physical chemistry. A.

[43]  Ingmar Persson,et al.  A Study of the Hydration of the Alkali Metal Ions in Aqueous Solution , 2011, Inorganic chemistry.

[44]  M. Sahimi,et al.  Nucleation of Salt Crystals in Clay Minerals: Molecular Dynamics Simulation. , 2017, The journal of physical chemistry letters.

[45]  B. Roux,et al.  The Solvation Structure of Na(+) and K(+) in Liquid Water Determined from High Level ab Initio Molecular Dynamics Simulations. , 2012, Journal of chemical theory and computation.

[46]  Atherton Seidell,et al.  Solubilities of inorganic and organic compounds , 1919 .

[47]  G. Lu,et al.  Molecular dynamics simulations of the local structures and transport coefficients of molten alkali chlorides. , 2014, The journal of physical chemistry. B.

[48]  Francesca Macedonio,et al.  Integrated membrane desalination systems with membrane crystallization units for resource recovery: A new approach for mining from the sea , 2016 .

[49]  P. Vekilov,et al.  The two-step mechanism of nucleation of crystals in solution. , 2010, Nanoscale.

[50]  Enrico Drioli,et al.  Influence of the structural properties of poly(vinylidene fluoride) membranes on the heterogeneous nucleation rate of protein crystals. , 2006, The journal of physical chemistry. B.

[51]  K. Bolton,et al.  Simulation of α- and β-PVDF melting mechanisms , 2012 .

[52]  E. Drioli,et al.  Testing of three different PVDF membranes in membrane assisted-crystallization process: Influence of membrane structural-properties on process performance , 2017, Desalination.

[53]  M. Parrinello,et al.  Canonical sampling through velocity rescaling. , 2007, The Journal of chemical physics.

[54]  Lachlan M. D. Cranswick,et al.  Halite-sylvite thermoelasticity , 2004 .

[55]  S. Meng,et al.  Atomistic nature of NaCl nucleation at the solid-liquid interface. , 2007, The Journal of chemical physics.

[56]  C. Bertozzi,et al.  Self-catalyzed growth of S layers via an amorphous-to-crystalline transition limited by folding kinetics , 2010, Proceedings of the National Academy of Sciences.

[57]  T. Matsuoka,et al.  Molecular dynamics study of salt-solution interface: solubility and surface charge of salt in water. , 2014, The Journal of chemical physics.

[58]  T. Darden,et al.  A smooth particle mesh Ewald method , 1995 .

[59]  F. Tezcan,et al.  Observations of the birth of crystals , 2018, Nature.

[60]  B. Peters,et al.  Pre-ordering of interfacial water in the pathway of heterogeneous ice nucleation does not lead to a two-step crystallization mechanism. , 2016, The Journal of chemical physics.

[61]  J. Anwar,et al.  Uncovering molecular processes in crystal nucleation and growth by using molecular simulation. , 2011, Angewandte Chemie.

[62]  Chiwoo Park,et al.  Directly Observing Micelle Fusion and Growth in Solution by Liquid-Cell Transmission Electron Microscopy. , 2017, Journal of the American Chemical Society.

[63]  Grant D. Smith,et al.  Quantum Chemistry Based Force Field for Simulations of Poly(vinylidene fluoride) , 2000 .

[64]  G. Patey,et al.  Molecular dynamics simulation of NaCl dissolution. , 2015, The journal of physical chemistry. B.