Relation between shape of liquid-gas interface and evolution of buoyantly unstable three-dimensional chemical fronts.

Buoyantly unstable 3D chemical fronts were seen traveling through an iodate-arsenous acid reaction solution. The experiments were performed in channel reactors with rectangular cross sections, where the top of the reaction solution was in contact with air. A concave or convex meniscus was pinned to reactor lateral walls. Influence of the meniscus shape on front development was investigated. For the concave meniscus, an asymptotic shape of fronts holding negative curvature was observed. On the other hand, fronts propagating in the solution with the convex meniscus kept only positive curvature. Those fronts were also a bit faster than fronts propagating in the solution with the concave meniscus. A relation between the meniscus shape, flow distribution, velocity, and shape is discussed.

Buoyancy-driven convection may switch between reactive states in three-dimensional chemical waves.

Traveling waves in an extended reactor, whose width cannot be neglected, represent a three-dimensional (3D) reaction-diffusion-convection system. We investigate the effects of buoyancy-driven convection in such a setting. The 3D waves traveled through horizontal layers of the iodate-arsenous acid (IAA) reaction solution containing excess of arsenous acid. The depth of the reaction solution was the examined parameter. An increase in the intensity of buoyancy-driven flow caused an increase of the traveling wave velocities. Convection distorted the front of the chemical waves. For layers deeper than h>13 mm, heat release became smaller than heat production causing the emergence of Rayleigh-Bénard convection cells. At the interface, a dependency of wave shape on solution depth was observed. For h<7 mm, the waves adopted a stable V-like shape, while for h>13 mm a parabolic shape dominated. For 7

Flow-field development during finger splitting at an exothermic chemical reaction front.

Fingertip splitting may be observed at chemical reaction fronts subject to buoyancy-induced Rayleigh-Taylor fingering, as investigated in ascending fronts of the iodate-arsenous acid reaction in vertical Hele-Shaw cells. We study the properties of the flow-field evolution during a tip-splitting event both experimentally and theoretically. Experimental particle-image velocimetry techniques show that the flow field associated to a finger displays a quadrupole of vortices. The evolution of the flow field and the reorganization of the vortices after a tip-splitting event are followed experimentally in detail. Numerical integration of a model reaction-diffusion-convection system for an exothermic reaction taking into account possible heat losses through the walls of the reactor shows that the nonlinear properties of the flow field are different whether the walls are insulating or conducting. In insulating systems, the flow field inside one finger features only one pair of vortices. A quadrupole of flow vortices arranged around a saddle-node structure similar to the one observed experimentally is obtained in the presence of heat losses suggesting that heat effects, even if of very small amplitude, are important in understanding the nonlinear properties of fingering of exothermic chemical fronts.