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Oscillations in Belousov-Zhabotinskii (BZ) systems without metal catalysts have been studied in batch and continuously stirred tank reactors at different temperatures. It is observed that there is an upper temperature limit and a lower temperature limit between which oscillations are observed and beyond which no oscillations are observed. The upper limit is characterized by high Br~ and high Br2 concentration whereas the lower temperature limit is characterised by low Br~ and low Br2 concentration. Further, at the lower temperature limit, oscillations can be revived by addition of BrO J. The oscillations are essentially controlled by autocatalytic reaction subset. It is suggested that at the lower temperature limit the thermodynamic condition for stability is voilated while at the upper temperature limit, the autocatalytic reaction is not allowed to proceed in view of the high Br~ concentration. Introduction The thermodynamic theory of non-equilibrium steady states suggests that for stability [1, 2], the condition 6/^>0 (1) must hold in situations in which convection is absent or in other words, when the gradient of the barycentric velocity is negligible. The inequality (1) is only a necessary condition and not a sufficient one. denotes the perturbation in the thermodynamic force X while /denotes
Journal of Non-Equilibrium Thermodynamics – de Gruyter
Published: Jan 1, 1987
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