Advection and diffusion induced transport in chemical systems

Dr. Istvan Kiss

The travelling wave equations and the electric field effects on travelling waves in the Oregonator model for the Belousov-Zhabotinsky (BZ) reaction are studied. Numerical solutions of the travelling wave equations are computed when an electric field is applied and in field free conditions. The main result in the field free case is the saddle-node bifurcation in the solutions, giving upper bounds for the existence of the waves and indicating the change from excitable to subexcitable regimes observed experimentally. In the presence of electric fields conditions for the existence of single pulses are determined. The electric field decelerates or annihilates waves propagating towards the negative electrode and accelerates those propagating towards the positive electrode, again being in line with experiments. Wave reversal is observed in our model, however in a qualitatively different way to that seen in experiments. Where single pulses do not exist, wave trains consisting of equally distributed similar pulses can form. The phenomenon termed wave splitting observed experimentally is not supported by our model. The second class of problems considered are chaotic advection and diffusion induced effects in chemical systems. We consider the evolution of a 2D flame in an open chaotic flow and the corresponding 1D Lagrangian filament slice model. If the stirring is fast (slow reaction), localised heat inputs decay, the flame is quenched. When the stirring is slow (fast reaction), localised ignitions evolve into a permanent flame with complex filamentary structure. A chaotic closed flow is considered as a model for 2D mixing within a homogeneous and inhomogeneous oscillatory medium modelled by the CDIMA reaction. If the media is homogeneous, an initial perturbation decays, at a rate relatively insensitive to chemical effects and is entrained into oscillations. When both steady and oscillatory states are stable, the final state of the system can be tuned to be either of the two depending on the initial configuration of the two stable states and on the ratio of the chemical and advective time scales. In an inhomogeneous oscillatory medium (frequency mismatch) chaotic advection acts as coupling, and by varying the stirring rate we can control the macroscopic behaviour of the system producing collective oscillations (synchronisation) or oscillator death.
Above: Colour coded time evolution of the temperature (different shades of red correspond to higher temperatures) in a combustion reaction coupled with an open chaotic flow. The time evolution of the consecutive plots is from left to right and top to bottom. Results obtained by numerical integration of PDEs.
Above: Colour coded time evolution of a concentration of a chemical substance in the CDIMA reaction coupled with a closed chaotic flow obtained from numerical integration of a set of PDEs. The time evolution of the consecutive plots is from left to right and top to bottom.

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