Chemoconvection of miscible solutions in an inclined layer
DOI:
https://doi.org/10.7242/1999-6691/2023.16.1.1Keywords:
chemoconvection, neutralization reaction, miscible liquids, density wave, numerical experimentsAbstract
This paper presents an experimental and numerical investigation of the chemoconvective flow of two miscible reacting solutions that generate a plain layer oriented at some angle to the gravity field. In the experiments, the aqueous solutions of nitric acid and sodium hydroxide were used. The system evolves from an initial state, in which each homogeneous solution occupies half of the layer, and the contact surface between the layers is flat. When the reacting solutions come into contact with each other, an acid-base neutralization reaction occurs, forming salt and water. The system configuration is chosen so that the acid solution of lower density rests on top of the denser base. This excludes the development of the Rayleigh–Taylor instability. The experiments were performed for such initial concentrations of the reagents at which a wave regime is realized in the system. The wave comprises a density jump rapidly advancing in the direction of gravity and separating the immobile alkali solution and the layer of acid and salt mixture, the convective motion of which feeds the frontal reaction with fresh acid. The visualization of the flow in the experiments was performed using a Fizeau interferometer. The numerical study of a complete three-dimensional problem was carried out using the ANSYS CFX hydrodynamic simulation program. We studied the flow evolution at a gradual increase in the angle of inclination from 0° to 70°. We found that the layer inclination leads to a significant change in the structure and intensity of the convective motion. Already at small inclination angles (up to 30°), the flow becomes three-dimensional, which makes the Hele-Shaw approximation inapplicable to this case. We show that there is a spontaneous stratification of salt and acid concentration fields in the cocurrent wave flow. With an increase in the angle of inclination, the wave velocity decreases, and chemoconvection in the cocurrent flow becomes less intense and acquires a certain vortex structure. At larger angles (from 50° to 70°), the wave front is strongly deformed or the wave breaks up. We demonstrate that an up-and-down fluid flow develops in the layer above the density jump. This flow eventually loses its stability with respect to the vertical rolls of solutal Rayleigh convection. There is a good agreement between the experimental measurements and the results of numerical simulation of the 3D problem.
Downloads
References
Levich V.G. Physicochemical hydrodynamics. New Jersey, Prentice-Hall Inc., 1962. 700 p.
Kutepov A.M., Polyanin A.D., Zapryanov A.D., Vyaz'min A.D., Kazenin D.A. Khimicheskaya gidrodinamika [Chemical fluid dynamics]. Moscow, Kvantum, 1996. 336 p.
Dupeyrat M., Nakache E. 205 – Direct conversion of chemical energy into mechanical energy at an oil water interface. Bioelectrochem. Bioenerg., 1978, vol. 5, pp. 134-141. http://dx.doi.org/10.1016/0302-4598(87)87013-7
Belk M., Kostarev K.G., Volpert V., Yudina T.M. Frontal photopolymerization with convection. J. Phys. Chem. B, 2003, vol. 107, pp. 10292-10298. http://dx.doi.org/10.1021/jp0276855
Reschetilowski W. Microreactors in preparative chemistry. Weinheim, Wiley-VCH, 2013. 352 p. http://dx.doi.org/10.1002/9783527652891
Baumann M., Baxendale I.R. The synthesis of active pharmaceutical ingredients (APIs) using continuous flow chemistry. Beilstein J. Org. Chem., 2015, vol. 11, pp. 1194-1219. https://doi.org/10.3762/bjoc.11.134
Karlov S.P., Kazenin D.A., Baranov D.A., Volkov A.V., Polyanin D.A., Vyaz'min A.V. Interphase effects and macrokinetics of chemisorption in the absorption of CO2 by aqueous solutions of alkalis and amines. Russ. J. Phys. Chem., 2007, vol. 81, pp. 665-679. http://dx.doi.org/10.1134/S0036024407050019
Wylock C., Rednikov A., Haut B., Colinet P. Nonmonotonic Rayleigh-Taylor instabilities driven by gas-liquid CO2 chemisorption. J. Phys. Chem. B, 2014, vol. 118, pp. 11323-11329. http://dx.doi.org/10.1021/jp5070038
Thomson P.J., Batey W., Watson R.J. Proc. of Extraction '84: Symposium on Liquid-Liquid Extraction Science. Scotland, Dounreay, November 27-29, 1984. Vol. 88, pp. 231-244.
Gershuni G.Z., Lyubimov D.V. Thermal vibrational convection. New York, Wiley & Sons, 1998. 372 p.
Gershuni G.Z. On the problem of stability of plane convective motion of liquids. Technical Physics, 1955, vol. 25, no. 2, pp. 351-357.
Birikh R.V., Gershuni G.Z., Zhukhovitskiy E.M., Rudakov R.N. Gidrodinamicheskaya i teplovaya neustoychivost’ statsionarnogo konvektivnogo dvizheniya [Hydbodynamic and thermal instability of a steady convective flow]. PMM – Journal of Applied Mathematics and Mechanics, 1968, vol. 32, no. 2, pp. 256-263.
Hart J.E. Stability of the flow in a differentially heated inclined box. J. Fluid Mech., 1971, vol. 47, pp. 547-576. http://dx.doi.org/10.1017/S002211207100123X
Korpela S.A. A study on the effect of Prandtl number on the stability of the conduction regime of natural convection in an inclined slot. Int. J. Heat Mass Tran., 1974, vol. 17, pp. 215-222. https://doi.org/10.1016/0017-9310(74)90083-0
Bratsun D.A., Krasnyakov I.V., Zyuzgin A.V. Active control of thermal convection in a rectangular loop by changing its spatial orientation. Microgravity Sci. Technol., 2018, vol. 30, pp. 43-52. http://doi.org/10.1007/s12217-017-9573-6
Wolf G.H. Dynamic stabilization of the Rayleigh–Taylor instability of miscible liquids and the related “frozen waves”. Phys. Fluids, 2018, vol. 30, 021701. https://doi.org/10.1063/1.5017846
Kozlov N. Numerical investigation of double-diffusive convection at vibrations. J. Phys.: Conf. Ser., 2021, vol. 1809, 012023. https://doi.org/10.1088/1742-6596/1809/1/012023
Demin V.A., Gershuni G.Z., Verkholantsev I.V. Mechanical quasi-equilibrium and thermovibrational convective instability in an inclined fluid layer. Int. J. Heat Mass Tran., 1996, vol. 39, pp. 1979-1991. https://doi.org/10.1016/0017-9310(95)00239-1
Demin V.А. Vibrational convection in an inclined fluid layer heated from below. Fluid Dyn., 2005, vol. 40, pp. 865-874. https://doi.org/10.1007/s10697-006-0003-5
Bratsun D.A., Mosheva E.A. Peculiar properties of density wave formation in a two-layer system of reacting miscible liquids. Vychisl. mekh. splosh. sred – Computational Continuum Mechanics, 2018, vol. 11, no. 3, pp. 302-322. http://doi.org/10.7242/1999-6691/2018.11.3.23
Mizev A.I., Mosheva E.A., Bratsun D.A. Extended classification of the buoyancy-driven flows induced by a neutralization reaction in miscible fluids. Part 1. Experimental study. J. Fluid Mech., 2021, vol. 916, A22. http://doi.org/10.1017/jfm.2021.201
Demin V.A., Popov E.A. The estimation of Damkohler number in chemiconvective problems. Vestnik Permskogo universiteta. Seriya Fizika – Bulletin of Perm University. Physics, 2015, no. 2 (30), pp. 44-50.
Bratsun D.A., Mizev A.I., Mosheva E.A. Extended classification of the buoyancy-driven flows induced by a neutralization reaction in miscible fluids. Part 2. Theoretical study. J. Fluid Mech., 2021, vol. 916, A23. http://doi.org/10.1017/jfm.2021.202
Loodts V., Thomas C., Rongy L., De Wit A. Control of convective dissolution by chemical reactions: General classification and application to CO2 dissolution in reactive aqueous solutions. Phys. Rev. Lett., 2014, vol. 113, 114501. https://doi.org/10.1103/PhysRevLett.113.114501
Bratsun D., Siraev R. Controlling mass transfer in a continuous-flow microreactor with a variable wall relief. Int. Comm. Heat Mass Tran., 2020, vol. 113, 104522. https://doi.org/10.1016/j.icheatmasstransfer.2020.104522
Eckert K., Rongy L., De Wit A. A+ B → C reaction fronts in Hele-Shaw cells under modulated gravitational acceleration. Phys. Chem. Chem. Phys., 2012, vol. 14, pp. 7337-7345. https://doi.org/10.1039/C2CP40132K
Mosheva E., Kozlov N. Study of chemoconvection by PIV at neutralization reaction under normal and modulated gravity. Exp. Fluids, 2021, vol. 62, 10. https://doi.org/10.1007/s00348-020-03097-0
Bratsun D.A., Stepkina O.S., Kostarev K.G., Mizev A.I., Mosheva E.A. Development of concentration-dependent diffusion instability in reactive miscible fluids under influence of constant or variable inertia. Microgravity Sci. Technol., 2016, vol. 28, pp. 575-585. http://doi.org/10.1007/s12217-016-9513-x
Utochkin V.Yu., Siraev R.R., Bratsun D.A. Pattern formation in miscible rotating Hele-Shaw flows induced by a neutralization reaction. Microgravity Sci. Technol., 2021, vol. 33, 67. http://doi.org/10.1007/s12217-021-09910-7
Spravochnik khimika. T. 3. Khimicheskoye ravnovesiye i kinetika. Svoystva rastvorov. Elektrodnyye protsessy [Chemist’s handbook. Vol. 3. Chemical equilibrium and kinetics. Properties of solutions. Electrode processes]. Moscow, Leningrad, Khimiya, 1965. 1008 p.
Schöpf W., Stiller O. Three-dimensional patterns in a transient, stratified intrusion flow. Phys. Rev. Lett., 1997, vol. 79, pp. 4373-4376. https://doi.org/10.1103/PhysRevLett.79.4373
Downloads
Published
Issue
Section
License
Copyright (c) 2023 Computational Continuum Mechanics
This work is licensed under a Creative Commons Attribution-NonCommercial 4.0 International License.