The Study Of Briggs-Rauscher Chemical Oscillating Reaction Catalyzed By The MacrocyclicComplex Nickel Complexes [Ni（TIM）]（ClO₄）₂

Chemical oscillation reaction especially a novel chemical oscillating reaction which is catalyzed by a macrocyclic nickel(Ⅱ) complex have been aroused interests from the majority of scientists since it was discovered. The macrocyclic nickel(Ⅱ) has a similar structure to some enzymes of life system, so the study of it is important to simulation of biological oscillations. This article discusses the nature of the new BR chemical oscillation system which catalysted by tetraazamacrocyclic nickel complexes [Ni(TIM)](ClO4)2and with acetylacetone or malonic acid as the organic substrate, where TIM=2,3,9,10-tetramethyl-1,4,8,11-tetraazacyclotetradeca-1,3,8,10-tetraene. The specifics were showed in the following aspects:1. The summary of chemical oscillating reactionThe first chapter introduces some research of chemical oscillation, such as its history, development, the basic conditions, several usual oscillating systems and so on. We explained the mechanisms of Briggs-Rauscher oscillating systems catalysted by metal ion in details, which are based on the classical NF model. Finally, we discussed the important applications of the chemical oscillation in the various fields and significance of chemical oscillation.2. Chemical oscillation experimentsThe second chapter describes the new BR chemical oscillation system catalysted by [Ni(TIM)](ClO4)2and with the acetylacetone as organic substrates, the system is KIO3-acetylacetone-H2O2-H2SO4-[Ni(TIM)](ClO4)2. The catalyst [Ni(TIM)](ClO4)2was synthesized according to the literature and identified by its IR spectra and elemental analyses. Then we studied some factors which could affect the parameters of the chemical oscillation, such as the concentration of the component, the temperature and the foreign species. The results show that the concentration of the I-is the controlling factor of the chemical oscillation and when the temperature is higher than313.15K the oscillation systemcease to oscillate. It also shows the linear relationship between the oscillation period (tp) and the concentrations of the components such as [Ni(TIM)](CIC4)2and KIO3. Finally, the skeleton reaction mechanism of the system was proposed based on experimental results and NF mechanism.The third chapter describes the new BR chemical oscillating with the malonic acid as the organic substrate. The system of KIO3-malonate-H2O2-H2SO4-[Ni(TIM)](CI04)2was set up under the acidic conditions. We are also discussed the maximum range of temperature and reactants concentrations where the oscillations occur, as well as the effects of changes in reactants concentrations on the oscillation behavior. The results show that the oscillation period decreased with the increasing temperature. Finally, the skeleton reaction mechanism of the system was proposed based on experimental results and NF mechanism.The fourth chapter discusses the main content of the full text and the results of the mechanism.