Abstract
Amorphous silica–water interfaces are found ubiquitously in nanoscale devices, including devices fabricated from silica as well as from silicon that acquire a surface oxide layer. The surface silanol groups serve as hydrogen-bonding sites for a variety of chemical species, and their reactivity enables convenient chemical modification, making silica surfaces strategic in bio-sensing applications. We have extended the popular BKS and SPC/E models for bulk silica and water to describe the hydrated, hydroxylated amorphous silica surface. The parameters of our model were determined using ab initio quantum chemical studies on small fragments. Our model will be useful in empirical potential studies, and as a starting point for ab initio molecular dynamics calculations. At this stage, we present a model for the undissociated surface. Our calculated value for the heat of immersion, 0.6Jm−2, falls within the range of reported experimental values of 0.2–0.8Jm−2. We also study the perturbation of water properties near the silica–water interface. The disordered surface is characterized by regions that are hydrophilic and hydrophobic, depending on the statistical variations in silanol group density. We report non-equilibrium molecular dynamics simulations of Poiseuille flow of water near an amorphous silica surface.
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van Beest B.W.H., Kramer G.J., van Santen R.A. (1990) Force fields for silicas and aluminophosphates based on ab initio calculations. Phys. Rev. Lett. 64(16): 1955–1958
Berendsen H.J.C., Grigera J.R., Straatsma T.P. (1987) The missing term in effective pair Potentials. J. Phys. Chem. 91(24): 6269–6271
Vessal B. (1994) Simulation studies of silicates and phosphates. J. Non-Crystalline Solids 177(1): 103–124
Smith W., Greaves G.N., Gillan M.J. (1995) Computer simulation of sodium disilicate glass. J. Chem. Phys. 103(8): 3091–3097
Møller C., Plesset M. (1934) Note on an approximation treatment for many-electron systems. Phys. Rev. 46(7): 618–622
Bartlett R.J., Silver D.M. (1974) Correlation energy in lithium hydride, boron monohydride, and hydrogen fluoride with many-body perturbation theory using slater-type atomic orbitals. Int. J. Quantum Chem. Symp. 8: 271–276
Binkley J.S., Pople J.A. (1975) Moeller-Plesset theory for atomic ground state energies. Int. J. Quantum Chem. 9(2): 229–236
Bartlett R.J., Silver D.M. (1975) Diagrammatic perturbation theory. Int. J. Quantum Chem. Symp. 9: 183–198
Pople, J.A., Binkley, J.S., Seeger, R.: Theoretical models incorporating electron correlation. Int. J. Quantum Chem. Symp. 10(1) (1976)
Hassanali, A.A., Singer, S.J.: A model for the water/amorphous silica interface: The undissociated surface. J. Phys. Chem. B (accepted for publication pending revisions) (2006)
Saengsawang O., Remsungnen T., Frizsche S., Haberlandt R., Hannongbua S. (2005) Structure and energetics of water-silanol binding on the surface of silicalite-1: Quantum chemical calculations. J. Phys.Chem. B 109(12): 5684–5690
Smith W., Forester T.R. (1996) DL POLY 2.0: A general-purpose parallel molecular dynamics simulation package J. Mol. Graph. 14(3): 136–141
Ryckaert J.-P., Ciccotti G., Berendsen H.J.C. (1977) Numerical integration of the Cartesian equations of motion of a system with constraints; molecular dynamics of n-alkanes. J. Comp. Phys. 23(3): 327–341
Darden T., York D., Pedersen L. (1993) Particle mesh Ewald: An n ln (n) method for Ewald sums in large systems. J. Chem. Phys. 98(12): 10089–10092
Perera U.E.L., Berkowitz M.L., Darden T., Lee H., Pedersen L.G. (1995) A smooth particle mesh Ewald method. J. Chem. Phys. 103(19): 8577–8593
Roder A., Kob W., Binder K. (2001) Structure and dynamics of amorphous silica surfaces. J. Chem. Phys. 114(17): 7602–7614
Rarivomanantsoa M., Jund P., Jullien R. (2001) Classical molecular dynamics simulations of amorphous silica surfaces. J. Phys. Condens. Matter, 13(31): 6707–6718
Ceresoli D., Bernasconi M., Iarlori S., Parrinello M., Tosatti E. (2000) Two-membered silicon rings on the dehydroxylated surface of silica. Phys. Rev. Lett. 84(17): 3887–3890
Bakos, T., Rashkeev, S.N., Pantiledes, S.T.: Reactions and diffusion of water and oxygen molecules in amorphous SiO2. Phys. Rev. Lett. 88(5): 55508-1–55508-4 (2002)
Masini P., Bernasconi M. (2002) J. Phys.: Ab initio simulations of hydroxylation and dehydroxylation reactions at surfaces: amorphous silica and brucite. Condens. Matter, 14(16): 4133–4144
Du M.-H., Kolchin A., Cheng H.-P. (2003) Water-silica surface interactions: A combined quantum classical molecular dynamic study of energetics and reaction pathways. J. Chem. Phys. 119(13): 6418–6422
Mischler C., Horbach J., Kob W., Binder K. (2005) Water adsorption on amorphous silica surfaces: a Car-Parrinello simulation study. J. Phys. Condens. Matter, 17(26): 4005–4013
Rignanese G.-M., Charlier J.-C., Gonze X. (2004) First-principles molecular dynamics investigation of the hydration mechanisms of the (0001) α-quartz surface. Phys. Chem. Chem. Phys. 6(8): 1920–1925
Walsh T.R., Wilson M., Sutton A.P. (2000) Hydrolysis of the amorphous silica surface. II. Calculation of activation barriers and mechanisms. J. Chem. Phys. 113(20): 9191–9201
Iler R.K. (1979) The Chemistry of Silica. Wiley, New York
Zhuravlev L.T. (1989) Structurally bound water and surface characterization of amorphous silica. Pure Appl. Chem. 61(11): 1969–1976
Ong S., Zhao X., Eisenthal K.B. (1992) Polarization of water molecules at a charged interface: second harmonic studies of the silica/water interface. Chem. Phys. Lett. 191(3–4): 327–335
Fisk J.D., Batten R., Jones G., O’Reilly J.P., M.Shaw A. (2005) pH dependence of the crystal violet adsorption isotherm at the silica-water interface. J. Phys. Chem. B109(30): 14475–14480
Chuang I.-S., Kinney D.R., Maciel G.E. (1993) Interior hydroxyls of the silica gel system as studied by 29Si CP-MAS NMR spectroscopy. J. Am. Chem. Soc. 115(19): 8695–8705
Chuang I.-S., Maciel G.E. (1996) Probing hydrogen bonding and the local environment of silanols on silica surfaces via nuclear spin cross polarization dynamics. J. Am. Chem. Soc. 118(2): 401–406
Chuang I.-S., Maciel G.E. (1997) A detailed model of local structure and silanol hydrogen bonding of silica gel surfaces. J. Phys. Chem. B101(16): 3052–3064
Taylor J.A.G., Hockey J.A. (1966) Heats of immersion in water of characterized silicas of varying specific area. J. Phys. Chem. 70(7): 2169–2172
Taylor J.A.G., Hockey J.A., Pethica B.A. (1965) The silica-water interface. Proc. Br. Ceramic Soc. 5: 133–141
Makrides A.C., Hackerman N. (1958) Heat of immersion. I. The system silica-water. J. Phys. Chem. 63(4): 594–598
Takei T., Chikazawa M. (1998) Origin of differences in heats of immersion of silicas in water. J. Colloid Interface Sci. 208(2): 570–574
Takei T., Eriguchi E., Fuji M., Watanabe T., Chikazawa M. (1998) Heat of immersion of amorphous and crystalline silicas in water: effect of crystallinity. Themochimia. Acta, 308(1–2): 139–145
Berendsen H.J.C., Postma J.P.M., van Gunsteren W.F., DiNola A., Haak J.R. (1984) Molecular dynamics with coupling to an external bath. J. Chem. Phys. 81(8): 3684–3690
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Hassanali, A.A., Singer, S.J. Static and dynamic properties of the water/amorphous silica interface: a model for the undissociated surface. J Computer-Aided Mater Des 14, 53–63 (2007). https://doi.org/10.1007/s10820-006-9038-5
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DOI: https://doi.org/10.1007/s10820-006-9038-5