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Extended classification of the buoyancy-driven flows induced by a neutralization reaction in miscible fluids. Part 1. Experimental study

Published online by Cambridge University Press:  12 April 2021

A.I. Mizev
Affiliation:
Institute of Continuous Media Mechanics, Russian Academy of Science, Perm614013, Russia Perm National Research Polytechnic University, Perm614990, Russia
E.A. Mosheva
Affiliation:
Institute of Continuous Media Mechanics, Russian Academy of Science, Perm614013, Russia Perm National Research Polytechnic University, Perm614990, Russia
D.A. Bratsun*
Affiliation:
Perm National Research Polytechnic University, Perm614990, Russia
*
Email address for correspondence: DABracun@pstu.ru

Abstract

The buoyancy-driven instabilities triggered by neutralization reaction were studied experimentally in a miscible two-layer system placed in a vertically oriented Hele-Shaw cell. The initial density stratification was always set to exclude the development of the Rayleigh–Taylor instability. The problem was examined for a few reactant pairs formed by a strong acid and a strong base. To classify the numerous experimental observations we introduced a dimensionless parameter, namely, a reaction-induced buoyancy number ${K}_{\rho }$, which defines the density of the reaction zone relative to that of the upper layer. We show that, depending on the value of this parameter, one of two global scenarios develops in the system right after the layers came into contact. If ${K}_{\rho }>1$, the process is governed mainly by diffusion, which results later on in the development of relatively weak convective motion caused by a differential-diffusion effect. Besides the irregular finger-type flow structures, reported earlier in numerous studies, we found a new type of instability, called the concentration-dependent diffusion instability, which is characterized by the formation of a regular cell-type convective pattern. In the case ${K}_{\rho }\le 1$, the unstable density stratification above the reaction front leads to the development of vigorous convection in the upper layer, forcing the reaction front to move downwards fast, so that it takes just a few minutes for reagents to burn out. We show that a new parameter can be used to plot the stability maps, which allows us to predict reaction–diffusion–convection processes in similar systems prior to experiment.

Type
JFM Papers
Copyright
© The Author(s), 2021. Published by Cambridge University Press

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References

REFERENCES

Almarcha, C., Trevelyan, P.M.J., Riolfo, L.A., Zalts, A., El Hasi, C., D'Onofrio, A. & De Wit, A. 2010 Active role of a color indicator in buoyancy-driven instabilities of chemical fronts. J. Phys. Chem. Lett. 1 (4), 752757.CrossRefGoogle Scholar
Ash, R. & Espenhahn, S.E. 2000 Transport through a slab membrane governed by a concentration-dependent diffusion coefficient: III. Numerical solution of the diffusion equation: ‘early-time’ and ‘t’ procedures. J. Membr. Sci. 180, 133146.CrossRefGoogle Scholar
Belk, M., Kostarev, K., Volpert, V. & Yudina, T. 2003 Frontal photopolymerization with convection. J. Phys. Chem. B 107, 1029210298.CrossRefGoogle Scholar
Bhatia, R.N., Gubbins, K.E. & Walker, R.D. 1968 Mutual diffusion in concentrated aqueous potassium hydroxide solutions. Trans. Faraday Soc. 64, 20912099.CrossRefGoogle Scholar
Bowen, W.R. & Williams, P.M. 2001 Prediction of the rate of cross-flow ultrafiltration of colloids with concentration-dependent diffusion coefficient and viscosity-theory and experiment. Chem. Engng Sci. 56, 30833099.CrossRefGoogle Scholar
Bratsun, D.A. 2017 Internal density waves of shock type induced by chemoconvection in miscible reacting liquid. Tech. Phys. Lett. 43 (10), 944947.CrossRefGoogle Scholar
Bratsun, D., Kostarev, K., Mizev, A., Aland, S., Mokbel, M., Schwarzenberger, K. & Eckert, K. 2018 Adaptive micromixer based on the solutocapillary marangoni effect in a continuous-flow microreactor. Micromachines 9 (11), 600.CrossRefGoogle Scholar
Bratsun, D., Kostarev, K., Mizev, A. & Mosheva, E. 2015 Concentration-dependent diffusion instability in reactive miscible fluids. Phys. Rev. E 92 (1), 011003.CrossRefGoogle ScholarPubMed
Bratsun, D.A., Mizev, A.I. & Mosheva, E.A. 2021 Extended classification of the buoyancy-driven flows induced by a neutralization reaction in miscible fluids. Part 2. Theoretical study. J. Fluid Mech. 916, A23.Google Scholar
Bratsun, D., Mizev, A., Mosheva, E. & Kostarev, K. 2017 Shock-wave-like structures induced by an exothermic neutralization reaction in miscible fluids. Phys. Rev. E 96 (5), 053106.CrossRefGoogle ScholarPubMed
Bratsun, D. & Siraev, R. 2020 Controlling mass transfer in a continuous-flow microreactor with a variable wall relief. Intl Commun. Heat Mass Transfer 113, 104522.CrossRefGoogle Scholar
Bratsun, D.A., Stepkina, O.S., Kostarev, K.G., Mizev, A.I. & Mosheva, E.A. 2016 Development of concentration-dependent diffusion instability in reactive miscible fluids under influence of constant or variable inertia. Microgravity Sci. Technol. 28 (6), 575585.CrossRefGoogle Scholar
Carballido-Landeira, J., Trevelyan, P.M.J., Almarcha, C. & De Wit, A. 2013 Mixed-mode instability of a miscible interface due to coupling between Rayleigh–Taylor and double-diffusive convective modes. Phys. Fluids 25, 024107.CrossRefGoogle Scholar
Crank, J. 1975 The Mathematics of Diffusion. Oxford University Press.Google Scholar
De Wit, A. 2020 Chemo-hydrodynamic patterns and instabilities. Annu. Rev. Fluid Mech. 52 (1), 531555.CrossRefGoogle Scholar
Dupeyrat, M. & Nakache, E. 1978 Direct conversion of chemical energy into mechanical energy at an oil water interface. Bioelectrochem. Bioenergetics 5 (1), 134141.CrossRefGoogle Scholar
Eckert, K., Acker, M. & Shi, Y. 2004 Chemical pattern formation driven by a neutralization reaction. I. Mechanism and basic features. Phys. Fluids 16 (2), 385399.CrossRefGoogle Scholar
Epstein, I.R. & Pojman, J.A. 1998 An Introduction to Nonlinear Chemical Dynamics: Oscillations, Waves, Patterns, and Chaos. Oxford University Press.CrossRefGoogle Scholar
Evans, M. & Uri, N. 1949 Polymerization in aqueous solution. Nature 164, 404405.CrossRefGoogle ScholarPubMed
Fary, D.A 1966 The diffusional properties of sodium hydroxide. PhD thesis, The Institute of Paper Chemistry.Google Scholar
Fernandez, J., Kurowski, P., Petitjeans, P. & Meiburg, E. 2002 Density-driven unstable flows of miscible fluids in a Hele-Shaw cell. J. Fluid Mech. 451, 239260.CrossRefGoogle Scholar
Gálfi, L. & Rácz, Z. 1988 Properties of the reaction front in an $A+B\to C$ type reaction-diffusion process. Phys. Rev. A 38, 3151(R).CrossRefGoogle Scholar
Grindrod, P. 1996 The Theory and Applications of Reaction-Diffusion Equations: Patterns and Waves. Oxford University Press.Google Scholar
Hejazi, S. & Azaiez, J. 2012 Stability of reactive interfaces in saturated porous media under gravity in the presence of transverse flows. J. Fluid Mech. 695, 439466.CrossRefGoogle Scholar
Jakobsen, H.A. 2008 Chemical Reactor Modeling, Multiphase Reactive Flows. Springer-Verlag.Google Scholar
Jensen, K.F. 2001 Microreaction engineering – is small better? Chem. Engng Sci. 56, 293303.CrossRefGoogle Scholar
Karlov, S.P., Kazenin, D.A., Baranov, D.A., Volkov, A.V., Polyanin, D.A. & Vyazmin, A.V. 2007 Interphase effects and macrokinetics of chemisorption in the absorption of CO$_2$ by aqueous solutions of alkalis and amines. Russ. J. Phys. Chem. A 81 (5), 665679.CrossRefGoogle Scholar
Kim, M.C. 2014 Effect of the irreversible $A+B\to C$ reaction on the onset and the growth of the buoyancy-driven instability in a porous medium. Chem. Engng Sci. 112, 5671.CrossRefGoogle Scholar
Kim, M.C. 2019 Effect of the irreversible $A+B\to C$ reaction on the onset and the growth of the buoyancy-driven instability in a porous medium: asymptotic, linear, and nonlinear stability analyses. Phys. Rev. Fluids 4, 073901.CrossRefGoogle Scholar
Koza, Z. & Taitelbaum, H. 1996 Motion of the reaction front in the $A+B\to C$ reaction-diffusion system. Phys. Rev. E 54, 1040R.CrossRefGoogle ScholarPubMed
Krienke, H., Ahn-Ercan, G. & Maurer, A. 2013 On the influence of molecular structure on the conductivity of electrolyte solutions-sodium chloride in dioxane-water mixtures. Z. Phys. Chem. 227 (2–3), 285302.CrossRefGoogle Scholar
Kuster, S., Riolfo, L.A., Zalts, A., El Hasi, C., Almarcha, C., Trevelyan, P.M.J., De Wit, A. & D'Onofrio, A. 2011 Differential diffusion effects on buoyancy-driven instabilities of acid-base fronts: the case of a color indicator. Phys. Chem. Chem. Phys. 13 (38), 1729517303.CrossRefGoogle ScholarPubMed
Lambert, R.M. 1997 Chemisorption and Reactivity on Supported Clusters and Thin Films: Towards an Understanding of Microscopic Processes in Catalysis. Springer Science & Business Media.CrossRefGoogle Scholar
Lemaigre, L., Budroni, M.A., Riolfo, L.A., Grosfils, P. & De Wit, A. 2013 Asymmetric Rayleigh–Taylor double-diffusive fingers in reactive systems. Phys. Fluids 25, 385399.CrossRefGoogle Scholar
Levich, V.G. 1962 Physicochemical Hydrodynamics. Prentice-Hall Inc.Google Scholar
Levich, V.G., Brodskii, A.M. & Pismen, L.M. 1967 A contribution to theory of branching homogeneous chain reaction in a flow. Dokl. Akad. Nauk SSSR 176, 371373.Google Scholar
Mosheva, E.A. & Shmyrov, A.V. 2017 Effect of the universal acid-base indicator on the formation of the concentration-dependent diffusion instability. IOP Conf. Ser.: Mater. Sci. Engng 208 (1), 012029.CrossRefGoogle Scholar
Nikolsky, B.N. (Ed.) 1965 Spravochnik Khimika (Chemist's Handbook), Vol. 3, 2nd edn. Khimiya Publishing House.Google Scholar
Nisancioglu, K. & Newman, J. 1973 Diffusion in aqueous nitric acid solutions. AIChE J. 19 (4), 797801.CrossRefGoogle Scholar
Nishimura, T., Tanoue, K.-I., Watanabe, T., Itoh, Y. & Kunitsugu, K. 2006 Instabilized fluid flow at interface of chemical reaction in liquid phase. Trans. JSME B 18 (7), 17731780.CrossRefGoogle Scholar
Pismen, L.M. 2006 Patterns and Interfaces in Dissipative Dynamics. Springer Science & Business Media.Google Scholar
Prigogine, I. & Nicolis, G. 1977 Self-Organization in Non-Equilibrium Systems. Wiley-Interscience.Google Scholar
Pringle, S.E., Glass, R.J. & Cooper, C.A. 2002 Double-diffusive finger convection in a Hele-Shaw cell: an experiment exploring the evolution of concentration fields, length scales and mass transfer. Transp. Porous Med. 47 (2), 195214.CrossRefGoogle Scholar
Quincke, G. 1888 Ueber periodische ausbreitung an flussigkeitsoberflachen und dadurch hervorgerufene bewegungserscheinungen. Ann. Phys. 271 (12), 580642.CrossRefGoogle Scholar
Sorkin, A., Sorkin, V. & Leizerson, I. 2002 Salt fingers in double-diffusive systems. Phys. A 303 (1–2), 1326.CrossRefGoogle Scholar
Stern, M.E. & Turner, J.S. 1969 Salt fingers and convecting layers. In Deep Sea Research and Oceanographic Abstracts, vol. 16, pp. 497–511. Elsevier.Google Scholar
Stokes, R.H. 1950 The diffusion coefficients of eight uni-univalent electrolytes in aqueous solution at 25. J. Am. Chem. Soc. 72 (5), 22432247.CrossRefGoogle Scholar
Taylor, J.R. & Veronis, G. 1996 Experiments on double-diffusive sugar-salt fingers at high stability ratio. J. Fluid Mech. 321, 315333.CrossRefGoogle Scholar
Thomson, P.J., Batey, W. & Watson, R.J. 1984 Interfacial activity in the two phase systems UO$_2$(NO$_3$)$_2$/Pu(NO$_3$)$_4$/HNO$_3$-H$_2$O-TBP/OK. In Proceedings of the Extraction’84, Symposium on Liquid–Liquid Extraction Science, Dounreay, Scotland, November 27–29, 1984, vol. 88, pp. 231–244. Elsevier.CrossRefGoogle Scholar
Trevelyan, P.M.J., Almarcha, C. & De Wit, A. 2011 Buoyancy-driven instabilities of miscible two-layer stratifications in porous media and Hele-Shaw cells. J. Fluid Mech. 670, 3865.CrossRefGoogle Scholar
Trevelyan, P.M.J., Almarcha, C. & De Wit, A. 2015 Buoyancy-driven instabilities around miscible $A+B\to C$ reaction fronts: a general classification. Phys. Rev. E 91 (2), 023001.CrossRefGoogle Scholar
Tsuji, K. & Müller, S.C. 2012 Chemical reaction evolving on a droplet. J. Phys. Chem. Lett. 3, 977980.CrossRefGoogle Scholar
Wishaw, B.F. & Stokes, R.H. 1954 The diffusion coefficients and conductances of some concentrated electrolyte solutions at 25. J. Am. Chem. Soc. 76 (8), 20652071.CrossRefGoogle Scholar
Zaitsev, I.D. & Avseev, G.G. (Ed.) 1988 Fiziko-himicheskie svojstva binarnyh i mnogokomponentnyh rastvorov neorganicheskih veshchestv (Chemist's Handbook). Khimiya Publishing House.Google Scholar
Zalts, A., El Hasi, C., Rubio, D., Urena, A. & D'Onofrio, A. 2008 Pattern formation driven by an acid-base neutralization reaction in aqueous media in a gravitational field. Phys. Rev. E 77, 015304.CrossRefGoogle Scholar
Zeldovich, Y.B. & Kompaneets, A.S. 1960 Theory of Detonation. Academic Press.Google Scholar