Spatio-temporal oscillations can be induced under batch conditions with ubiquitous bimolecular reactions in the absence of any nonlinear chemical feedback, thanks to an active interplay between the chemical process and chemically driven hydrodynamic flows. When two reactants A and B, initially separated in space, react upon diffusive contact, they can power convective flows by inducing a localized variation of surface tension and density at the mixing interface. These flows feedback with the reaction-diffusion dynamics, bearing damped or sustained spatio-temporal oscillations of the concentrations and flow field. By means of numerical simulations, we detail the mechanism underlying these chemohydrodynamic oscillations and classify the main dynamical scenarios in the relevant space drawn by parameters ΔM and ΔR, which rule the surface tension- and buoyancy-driven contributions to convection, respectively. The reactor height is found to play a critical role in the control of the dynamics. The analysis reveals the intimate nature of these oscillatory phenomena and the hierarchy among the different phenomena at play: oscillations are essentially hydrodynamic and the chemical process features the localized trigger for Marangoni flows unstable toward oscillatory instabilities. The characteristic size of Marangoni convective rolls mainly determines the critical conditions and properties of the oscillations, which can be further tuned or suppressed by the buoyancy competition. We finally discuss the possible experimental implementation of such a class of chemo-hydrodynamic oscillator and its implications in fundamental and applied terms.
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21 March 2021
Research Article|
March 15 2021
Chemo-hydrodynamic pulsations in simple batch A + B C systems
Special Collection:
2021 JCP Emerging Investigators Special Collection
Marcello A. Budroni
;
Marcello A. Budroni
a)
1
Department of Chemistry and Pharmacy, University of Sassari
, Via Vienna 2, 07100 Sassari, Italy
a)Author to whom correspondence should be addressed: mabudroni@uniss.it
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Alessandro Polo;
Alessandro Polo
1
Department of Chemistry and Pharmacy, University of Sassari
, Via Vienna 2, 07100 Sassari, Italy
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Virat Upadhyay;
Virat Upadhyay
2
Nonlinear Physical Chemistry Unit, Service de Chimie Physique et Biologie Théorique, Université Libre de Bruxelles
, CP 231 - Campus Plaine, 1050 Brussels, Belgium
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Adam Bigaj;
Adam Bigaj
2
Nonlinear Physical Chemistry Unit, Service de Chimie Physique et Biologie Théorique, Université Libre de Bruxelles
, CP 231 - Campus Plaine, 1050 Brussels, Belgium
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Laurence Rongy
Laurence Rongy
2
Nonlinear Physical Chemistry Unit, Service de Chimie Physique et Biologie Théorique, Université Libre de Bruxelles
, CP 231 - Campus Plaine, 1050 Brussels, Belgium
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a)Author to whom correspondence should be addressed: mabudroni@uniss.it
Note: This paper is part of the 2021 JCP Emerging Investigators Special Collection.
J. Chem. Phys. 154, 114501 (2021)
Article history
Received:
December 31 2020
Accepted:
February 24 2021
Citation
Marcello A. Budroni, Alessandro Polo, Virat Upadhyay, Adam Bigaj, Laurence Rongy; Chemo-hydrodynamic pulsations in simple batch A + B C systems. J. Chem. Phys. 21 March 2021; 154 (11): 114501. https://doi.org/10.1063/5.0042560
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