科研之友
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摘要
An infrared camera was used for the first time to monitor the progress of traveling fronts in oscillatory chemical reactions, taking the Belousov-Zhabotinsky (BZ) reaction as the test system. The experiments involved comparative visual imaging and infrared thermography measurements for the thin-layer of the BZ solution in the Petri dish, including both aqueous and gel media, the latter one hindering the convection. Infrared thermography experiments that supply information on the temperature distribution at the solution surface were compared with the bulk temperature variations of the stirred solution with BZ reaction, measured simultaneously with the oscillatory variations of the Pt electrode potential. The experimentally observed correlation between the ferroin catalyst concentration and the temperature distribution was compared with the results of numerical modeling of these distributions in 2-D reactor space, based on the classical Oregonator. Analogous experiments were performed for the oscillatory oxidation of thiocyanates with hydrogen peroxide, catalyzed with Cu(2+) ions, in search of factors causing the development of traveling fronts, previously reported. The inhomogeneous distribution of the free surface temperature that could contribute to surface instabilities was found. Also, periodical increase and decrease in temperature of solution surface was reported. This was interpreted as periodically predominating cooling of the surface in contact with the surroundings because for the bulk, thermally isolated stirred solution, the temperature monotonically increases. In terms of our nine-variable kinetic model of this system, it was possible to identify the reaction steps responsible for the experimentally observed temperature dynamics and ascribe the appropriate heat effects to them. Our results constitute the first contribution to the thermochemical characteristics of the H(2)O(2)-SCN(-)-OH -Cu(2+) oscillator.
- 出版日期2010-8-5
