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Electrochemistry, Oxidation, Electrolytic


Oxidation reactions of a series of organosulfur compounds by chlorite are excitable, autocatalytic, and exothermic and generate a lateral instability upon being triggered by the autocatalyst. This article reports on the convective instabilities derived from the reaction of chlorite and thiourea in a Hele-Shaw cell. Reagent concentrations used for the development of convective instabilities delivered a temperature jump at the wave front of 2.1 K. The reaction zone was 2 mm and due to normal cooling after the wave front, this induced a spike rather than the standard well-studied front propagation. Localized spatiotemporal patterns develop around the wave front. This exothermic autocatalytic reaction has solutal and thermal contributions to density changes that act in opposite directions due to the existence of a positive isothermal density change in the reaction. The competition between these effects generates thermal plumes. The fascinating feature of this system is the coexistence of plumes and fingering in the same solution as the front propagates through the Hele-Shaw cell. Wave velocities of descending and ascending fronts are oscillatory. Fingers and plumes are generated in alternating frequency as the front propagates. This generates hot and cold spots within the Hele-Shaw cell, and subsequently spatiotemporal inhomogeneities. The small ΔT at the wave front generated thermocapillary convection which competed effectively with thermogravitational forces at low Eötvös numbers. A simplified reaction-diffusion-convection model was derived for the system. Plume formation is heavily dependent on boundary effects from the cell dimensions. This article reports of self-organization derived from the dissipation of chemical energy. The unique aspect of this article is as follows: generally, addition of convection to reaction-diffusion mechanisms destroys most coherence and self-organization. It is not so, as reported in this article. The delicate balance between thermogravitational, thermocapillary diffusion effects can deliver remarkable self-organization in ungelled environments.


This is the publisher's final pdf. Article appears in AIP Chaos: An Interdisciplinary Journal of Nonlinear Science and is copyrighted (2019) by the American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.

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