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Abstract:

Using molecular dynamics techniques, we investigate surface states of the surfactant N-dodecylimidazole (DIm) in its basic and acid forms adsorbed at the water/air interface. Two different surface coverages were examined: an infinitely diluted detergent and a saturated monolayer. Spatial and orientational correlations of the surfactants and the aqueous substrate are presented. At large surface coverages, Dim presents two solvation states with well differentiated structural and dynamical characteristics. Solvation of the protonated surfactant becomes unstable at large concentrations, while the relative stability of the surface states of N-dodecylimidazolium (DImH +) with respect to bulk states increases at infinite dilution. The surface acidic behavior of DImH+ was investigated using a multistate empirical valence bond Hamiltonian model. Our simulation results suggest that the acidic characteristics of Dim are enhanced at the surface. The differences are rationalized in terms of the distinctive features in the overall solvation structure of the reactive complex. © 2007 American Chemical Society.

Registro:

Documento: Artículo
Título:Surface behavior of N-dodecylimidazole at air/water interfaces
Autor:Rodriguez, J.; Laria, D.
Filiación:Departamento de Quimica Inorganica, Analitica y Quimica-Fisica e INQUIMAE, Facultad de Ciencias Exactas y Naturales, Ciudad Universitaria, Pabellón II, 1428, Buenos Aires, Argentina
Unidad Actividad Química, Comisión Nacional de Energía Atómica, Avenida Libertador 8250, 1429, Buenos Aires, Argentina
Palabras clave:Computer simulation; Hamiltonians; Interfaces (materials); Mathematical models; Molecular dynamics; Monolayers; Surface properties; Acidic behavior; Hamiltonian model; Nitrogen compounds
Año:2007
Volumen:111
Número:2
Página de inicio:908
Página de fin:915
DOI: http://dx.doi.org/10.1021/jp0650883
Título revista:Journal of Physical Chemistry C
Título revista abreviado:J. Phys. Chem. C
ISSN:19327447
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_19327447_v111_n2_p908_Rodriguez

Referencias:

  • A comprehensive description of recent advances in reactivity at water/air interfaces is presented in Chem. Rev. 2006, 106, Issue 4; Benjamin, I., (1995) Acc. Chem. Res, 28, p. 233
  • (1996) Chem. Rev, 96, p. 1449
  • Annu, (1997) Rev. Phys. Chem, 48, p. 407
  • Richmond, G.L., (2002) Chem. Rev, 102, p. 2693
  • Mucha, M., Frigato, T., Levering, L.M., Allen, H.C., Tobias, D.J., Dang, L.X., Jungwirth, P., (2005) J. Phys. Chem. B, 109, p. 7617
  • Petersen, P.B., Saykally, R.J., Mucha, M., Jungwirth, P., (2005) J. Phys. Chem. B, 109, p. 10915
  • Gragson, D.E., Richmond, G.L., (1998) J. Am. Chem. Soc, 120, p. 366
  • Zimdars, D.J., Dadap, I., Eisenthal, K.B., Heinz, T.F., (1999) Chem. Phys. Lett, 301, p. 112
  • Zimdars, D., Eisenthal, K.B., (1999) J. Phys. Chem. A, 103, p. 10567
  • Zimdars, D., Eisenthal, K.B., (2001) J. Phys. Chem. B, 105, p. 3393
  • Pantano, D.A., Laria, D., (2003) J. Phys. Chem. B, 107, p. 297
  • Smart, J.L., McCammon, J.A., (1996) J. Am. Chem. Soc, 118, p. 2283
  • Wang, H., Zhao, X., Eisenthal, K.B., (2000) J. Phys. Chem. B, 104, p. 8855
  • Xiao, X., Vogel, V., Shen, Y.R., Marowsky, G., (1991) J. Chem. Phys, 94, p. 2315
  • Benjamin, I., Pohorille, A., (1993) J. Chem. Phys, 98, p. 236
  • Fitchett, B.D., Conboy, J.C., (2004) J. Phys. Chem. B, 108, p. 20255
  • Bowers, J., Butts, C.P., Martin, P.J., Vergara-Gutierrez, M.C., Heenan, R.K., (2004) Langmuir, 20, p. 2191
  • de Duve, C., de Barsy, T., Poole, B., Trouet, A., Tulkens, P., van Hoof, F., (1974) Biochem. Pharmacol, 23, p. 2495
  • Firestone, R.A., Pisano, J.M., (1979) J. Med. Chem, 22, p. 1130
  • Miller, D.K., Griggiths, E., Lenard, J., Firestone, R.A., (1983) J. Cell Biol, 97, p. 1841
  • Forster, S., Scarlett, L., Lloyd, J.B., (1987) Biochem. Biophys. Acta, 924, p. 452
  • Boyer, M.J., Horn, I., Firestone, R.A., Steele-Norwood, D., Tannock, I.F., (1993) Br. J. Cancer, 67, p. 81
  • Čuma, M., Schmitt, U.W., Voth, G.A., (2000) Chem. Phys, 258, p. 187
  • Čuma, M., Schmitt, U.W., Voth, G.A., (2001) J. Phys. Chem. A, 105, p. 2814
  • Petersen, P.B., Saykally, R.J., (2005) J. Phys. Chem. B, 109, p. 7976
  • Tarbuck, T.L., Ota, S.T., Richmond, G.L., (2006) J. Am. Chem. Soc, 128, p. 14519
  • Petersen, M.K., Iyengar, S.S., Day, T.J.F., Voth, G.A., J. Phys. Chem, 52004 (108), p. 14804
  • Wang, H., Second Harmonic Generation Studies, , http://digitalcommons. libraries.columbia.edu/dissertations/AAI9706914, at Liquid Interfaces. Ph.D. Thesis Defense Dissertation, Columbia University, New York, 1996; Chapter 3. An electronic version of this manuscript can be found at
  • Wang, H., Zhao, X., Eisenthal, K.B., (2000) J. Phys. Chem. B, 104, p. 8855
  • Dang, X.L., Pettitt, B.M., (1987) J. Phys. Chem, 91, p. 3349
  • Berendsen, H.J.C., van der Spoel, D., van Drunen, R., (1995) Comput. Phys. Commun, 91, p. 43
  • Lindahl, E., Hess, B., van der Spoel, D., (2001) J. Mol. Model, 7, p. 306
  • Schuettelkope, A.W., van Aalten, D.M.F., (2004) Acta Crystallogr, D60, p. 1355
  • Yeh, I.-C., Berkowitz, M.L., (1999) J. Chem. Phys, 111, p. 3155
  • Åqvist, J., Warshel, A., (1993) Chem. Rev, 93, p. 2523
  • Lobaugh, J., Voth, G.A., (1996) J. Chem. Phys, 104, p. 2056
  • Schmitt, U.W., Voth, G.A., (1998) J. Phys. Chem. B, 102, p. 5547
  • Schmitt, U.W., Voth, G.A., (1999) J. Chem. Phys, 111, p. 9361
  • Vuilleumier, R., Borgis, D., (1998) J. Phys. Chem. B, 102, p. 4261
  • Vuilleumier, R., Borgis, D., (1998) Chem. Phys. Lett, 284, p. 71
  • Vuilleumier, R., Borgis, D., (1999) J. Chem. Phys, 111, p. 4251
  • Laria, D., Martí, J., Guàrdia, E., (2004) J. Am. Chem. Soc, 126, p. 2125
  • Maupin, C.M., Wong, K.F., Soudackov, A.V., Kim, S., Voth, G.A., (2006) J. Phys. Chem. A, 110, p. 631. , A similar modification was operated in a recent study of proton transfer. See
  • Feynman, R.P., (1939) Phys. Rev, 56, p. 340
  • Lenarcik, B., Ojczenasz, P., (2002) J. Heterocycl. Chem, 39, p. 287
  • Geissler, P.L., Dellago, C., Chandler, D., (1999) J. Phys. Chem. B, 103, p. 3706. , For a detailed analysis of reaction coordinates for ion pair dissociation in solution, see
  • Tepper, H.L., Voth, G.A., (2005) Biophys. J, 88, p. 3095
  • Rodriguez, J., Laria, D., (2005) J. Phys. Chem. B, 109, p. 6473
  • Wilson, M.A., Pohorille, A., Pratt, L.R., (1989) Chem. Phys. Lett, 129, p. 209
  • Benjamin, I., (1991) J. Chem. Phys, 95, p. 3698
  • Pohorille, A., Benjamin, I., (1991) J. Chem. Phys, 94, p. 5599
  • Torrie, G.M., Valleau, J.P., (1974) Chem. Phys. Lett, 28, p. 578
  • Valleau, J.P., Torrie, G.M., A guide for Monte Carlo for statistical mechanics (1977) Statistical Mechanics, Part A, pp. 169-194. , Berne, B. J, Ed, Plenum Press: New York
  • Roux, B., (1995) Comput. Phys. Commun, 91, p. 275
  • Lapid, H., Agmon, N., Petersen, M.K., Voth, G.A., (2005) J. Chem. Phys, 122, p. 14506
  • In order to bring the two sets of curves to the same asymptotic behavior at large distances, the density of site γ at the surface, that is, ργ, was taken as half of the bulk value; For recent studies dealing for proton transfer in water in the close vicinity of a phospholipid membrane and in channels, see: Smondyrev, A. M, Voth, G. A. Biophys. J. 2003, 85, 864; Wu, Y., Voth, G.A., (2002) Biophys. J, 82, p. 1460
  • Xu, J., Voth, G.A., (2005) Proc. Natl. Acad. Sci. U.S.A, 102, p. 6795

Citas:

---------- APA ----------
Rodriguez, J. & Laria, D. (2007) . Surface behavior of N-dodecylimidazole at air/water interfaces. Journal of Physical Chemistry C, 111(2), 908-915.
http://dx.doi.org/10.1021/jp0650883
---------- CHICAGO ----------
Rodriguez, J., Laria, D. "Surface behavior of N-dodecylimidazole at air/water interfaces" . Journal of Physical Chemistry C 111, no. 2 (2007) : 908-915.
http://dx.doi.org/10.1021/jp0650883
---------- MLA ----------
Rodriguez, J., Laria, D. "Surface behavior of N-dodecylimidazole at air/water interfaces" . Journal of Physical Chemistry C, vol. 111, no. 2, 2007, pp. 908-915.
http://dx.doi.org/10.1021/jp0650883
---------- VANCOUVER ----------
Rodriguez, J., Laria, D. Surface behavior of N-dodecylimidazole at air/water interfaces. J. Phys. Chem. C. 2007;111(2):908-915.
http://dx.doi.org/10.1021/jp0650883