This paper reports the influence of reaction temperature on the occurrence and characteristics of pH oscillations that are observed during the palladium-catalysed phenylacetylene oxidative carbonylation reaction in a catalytic system (PdI2, KI, air, NaOAc) in methanol. Isothermal experiments were performed over the temperature range 10-50 degrees C. The experiments demonstrate that oscillations occur in the range 10-40 degrees C and that a decrease in reaction temperature results in an increase in the period and amplitude of the pH oscillations. Furthermore, it is observed that during oscillations at any specific temperature, the time taken for pH to increase from a minimum to a maximum value varies with respect to reaction time. However, the time required for the pH to fall from maximum to new minimum is approximately constant with respect to the reaction time and is a function of the reaction temperature.
Complex responses have been observed in a wide range of chemical and engineering systems: In well-stirred and unstirred solution-phase, in gels, in heterogeneous catalysis and dissolution reactions, in gas-and solid-phase combustion, widely in biological systems, accompanying phase transitions, in atmospheric kinetics and even in interstellar dust clouds. Complex behaviour does not, however, imply a necessarily complex underlying chemical mechanism. The appropriate feedback mechanisms, built on chainbranching, autocatalysis or self-heating, arise quite commonly in Nature. In many instances, it is appropriate "rst to attempt to "nd reduced mechanisms giving a semi-quantitative "t to observed responses. An example of such an approach applied to a model for complex oscillations of species concentrations in the mesosphere is presented, and the reduced model used to investigate the e!ects of longitudinal mixing in this system. Once a general understanding of a particular reaction system has been obtained, more detailed questions can be addressed. This is exempli"ed by a study of the development of three-dimensional scroll waves in the Belousov}Zhabotinsky reaction. Such detailed information for a speci"c reaction also informs the general understanding of the class of &excitable media'.
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