Artículo

Estamos trabajando para conseguir la versión final de este artículo
Consulte el artículo en la página del editor
Consulte la política de Acceso Abierto del editor

Abstract:

Nonlinear interactions between chemical reactions and buoyancy-driven Rayleigh-Taylor instability of reaction-diffusion acidity fronts of the chlorite-tetrathionate (CT) reaction are studied theoretically in a vertical Hele-Shaw cell or a porous medium. To do so, we perform a numerical integration of a two-variable reaction-diffusion model of the CT system coupled through an advection term to Darcy's law ruling the evolution of the velocity field of the fluid. The fingering dynamics of these chemical fronts is characterized by the appearance of several fingers at onset. These fingers then undergo coarsening and eventually merge to form one single symmetric finger. We study this asymptotic dynamics as a function of the three dimensionless parameters of the problem, i.e., the Damköhler number Da, the diffusivity ratio δ of the two chemical species, and the Rayleigh number Ra constructed here on the basis of the width Ly of the system. For moderate values of Ra, the asymptotic single finger is shown to have self-similar scaling properties while above a given value of Ra, which depends on the other values of the parameters, tip splitting comes into play. Increasing the difference of diffusivities of the two chemical species (i.e., increasing δ) leads to more efficient coarsening and smaller asymptotic fingers. Experimental procedures to verify our predictions are proposed. © 2006 American Institute of Physics.

Registro:

Documento: Artículo
Título:Nonlinear fingering dynamics of reaction-diffusion acidity fronts: Self-similar scaling and influence of differential diffusion
Autor:Lima, D.; D'Onofrio, A.; De Wit, A.
Filiación:Service de Chimie Physique, Centre for Nonlinear Phenomena and Complex Systems, Campus Plaine, CP231, 1050 Brussels, Belgium
Grupo de Medios Porosos, Departamento de Física, Universidad de Buenos Aires, Paseo Colon 850, (1063) Buenos Aires, Argentina
Palabras clave:Acidity; Dynamics; Fluid dynamics; Optimization; Porosity; Reaction kinetics; Asymptotic dynamics; Chlorite-tetrathionate (CT) reaction; Reaction-diffusion model; Diffusion
Año:2006
Volumen:124
Número:1
DOI: http://dx.doi.org/10.1063/1.2145746
Título revista:Journal of Chemical Physics
Título revista abreviado:J Chem Phys
ISSN:00219606
CODEN:JCPSA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00219606_v124_n1_p_Lima

Referencias:

  • Van Saarloos, W., (2003) Phys. Rep., 386, p. 29
  • Epstein, I.R., Pojman, J.A., (1998) An Introduction to Nonlinear Dynamics: Oscillations, Waves, Patterns and Chaos, , Oxford University Press, New York
  • Nagypál, I., (1986) J. Am. Chem. Soc., 108, p. 3635
  • Nagypál, I., (1990) J. Phys. Chem., 94, p. 4966
  • Pojman, J.A., (1991) J. Phys. Chem., 95, p. 1299
  • Pojman, J.A., (1991) J. Phys. Chem., 95, p. 1299
  • Masere, J., (1994) J. Phys. Chem., 98, p. 6505
  • Edwards, B.F., (1991) Phys. Rev. A, 43, p. 749
  • Vasquez, D.A., (1993) J. Chem. Phys., 98, p. 2138
  • Vasquez, D.A., (1994) Phys. Rev. E, 50, p. 280
  • Pojman, J.A., (1991) J. Phys. Chem., 95, p. 1306
  • Huang, J., (1993) Phys. Rev. E, 48, p. 4378
  • Wu, Y., (1995) Phys. Rev. E, 52, p. 6175
  • Huang, J., (1996) Phys. Rev. E, 54, p. 2620
  • Vasquez, D.A., (1996) J. Chem. Phys., 104, p. 9926
  • Vasquez, D.A., (1998) Phys. Rev. E, 58, p. 6865
  • Carey, M.R., (1996) Phys. Rev. E, 53, p. 6012
  • Böckmann, M., (2000) Phys. Rev. Lett., 85, p. 2506
  • De Wit, A., (2001) Phys. Rev. Lett., 87, p. 054502
  • Martin, J., (2001) J. Phys. IV, 11, pp. 6-99
  • Martin, J., (2002) Phys. Rev. E, 65, p. 051605
  • Yang, J., (2002) J. Chem. Phys., 117, p. 9395
  • Horváth, D., (2002) J. Chem. Phys., 117, p. 4399
  • Bánsági Jr., T., Horváth, D., Tóth, Á., Yang, J., Kalliadasis, S., De Wit, A., (2003) Phys. Rev. E, 68, p. 055301
  • Bánsági Jr., T., Horváth, D., Tóth, Á., (2003) Phys. Rev. E, 68, p. 026303
  • Bánsági Jr., T., Horváth, D., Tóth, Á., (2004) Chem. Phys. Lett., 384, p. 153
  • Kalliadasis, S., (2004) Phys. Fluids, 16, p. 1395
  • Vasquez, D.A., (2004) J. Chem. Phys., 121, p. 935
  • Rica, T., (2005) Chem. Phys. Lett., 408, p. 422
  • Bánsági Jr., T., Horváth, D., Tóth, Á., (2004) J. Chem. Phys., 121, p. 11912
  • De Wit, A., (2004) Phys. Fluids, 16, p. 163
  • Böckmann, M., (2004) Phys. Rev. E, 70, p. 046302
  • Vasquez, D.A., (2002) Chaos, 12, p. 49
  • Coroian, D.I., (2003) J. Chem. Phys., 119, p. 3354
  • Nagypál, I., (1986) J. Phys. Chem., 90, p. 6285
  • Tóth, A., (1997) J. Chem. Soc., Faraday Trans., 93, p. 73
  • Horváth, D., (1998) J. Chem. Phys., 108, p. 1447
  • Kuramoto, Y., (1984) Chemical Oscillations, Waves and Turbulence, , Springer-Verlag, Berlin
  • Horváth, D., (1993) J. Chem. Phys., 98, p. 6322
  • Horváth, D., (1995) J. Chem. Phys., 102, p. 2471
  • Tóth, A., (1996) J. Phys. Chem., 100, p. 14837
  • Tan, C.T., (1988) Phys. Fluids, 31, p. 1330
  • De Wit, A., (1999) J. Chem. Phys., 110, p. 8663
  • Press, W.H., Teukolsky, S.A., Vetterling, W.T., Flannery, B.P., (1988) Numerical Recipes in C, , Cambridge University Press, Cambridge
  • Homsy, G.M., (1987) Annu. Rev. Fluid Mech., 19, p. 271
  • Fuentes, M., (2001) J. Phys. Chem. A, 105, p. 6769

Citas:

---------- APA ----------
Lima, D., D'Onofrio, A. & De Wit, A. (2006) . Nonlinear fingering dynamics of reaction-diffusion acidity fronts: Self-similar scaling and influence of differential diffusion. Journal of Chemical Physics, 124(1).
http://dx.doi.org/10.1063/1.2145746
---------- CHICAGO ----------
Lima, D., D'Onofrio, A., De Wit, A. "Nonlinear fingering dynamics of reaction-diffusion acidity fronts: Self-similar scaling and influence of differential diffusion" . Journal of Chemical Physics 124, no. 1 (2006).
http://dx.doi.org/10.1063/1.2145746
---------- MLA ----------
Lima, D., D'Onofrio, A., De Wit, A. "Nonlinear fingering dynamics of reaction-diffusion acidity fronts: Self-similar scaling and influence of differential diffusion" . Journal of Chemical Physics, vol. 124, no. 1, 2006.
http://dx.doi.org/10.1063/1.2145746
---------- VANCOUVER ----------
Lima, D., D'Onofrio, A., De Wit, A. Nonlinear fingering dynamics of reaction-diffusion acidity fronts: Self-similar scaling and influence of differential diffusion. J Chem Phys. 2006;124(1).
http://dx.doi.org/10.1063/1.2145746