Study On The Briggs-Rauscher Chemical Oscillating Reaction Catalyzed By A Macrocyclic Nickel Complex

Chemical oscillator is an open system which is a typical example of nonlinear and nonequilibrium reaction. It can spontaneously organize to an ordered structure in time and space and shows some characteristics those are similar to self-organize of life. In recently years, a novel chemical oscillating reaction catalyzed by tetraazamacrocyclic complexes have attracted the attention of chemical and biology researchers. In this paper we have studied three chemical oscillators catalyzed by two kinds of macrocyclic nickel(Ⅱ) complex [NiL](ClO4)2 and [Ni(TIM)](ClO4)2, where L=5,7,7,12,14,14-hexemethy-1,4,8,11-tetraazacyclotetradeca -4,11-diene and TIM=2,3,9,10-tetramethyl-1,4,8,11-tetraazacyclotetradeca-1,3,8,10-tetraene.The first chapter introduces the history of the oscillating reaction, the basic conditions of it takes place and several kinds of oscillating systems. We have also described the current situation and the research respect of the Briggs-Rauscher Oscillator.In the second chapter, the catalyst [NiL](C104)2, was synthesized according to the literature and identified by its IR spectra and elemental analyses. In the ice bath, we have founded two oscillating systems:KIO3-2,4-Petanedione-H2O2-H2SO4-[NiL](ClO4)2 and KIO3-EAA-H2O2-H2SO4-[NiL](ClO4)2. To these two oscillators we have studied some factors, such as the concentration of the component, the temperature and the foreign species. It was found that oscillation period (tp) is dependent on the initial concentrations of NiL2+ and H2O2. The concentration of I- can act as an on-off switch in the process while free radicals may be involved in.In the following chapter, [Ni(TIM)] (ClO4)2 was synthesized according to the literature and identified by its IR spectra and elemental analyses. At 15±0.5℃, the system of KIO3-EAA-H2O2-H2SO4-[Ni(TIM)](ClO4)2 was set up. To this oscillator, the contents of study were following to the former two in the second chapter. The conclusion was also similar to except that oscillation period (tp) is dependent on the initial concentrations of [Ni(TIM)]2+, H2O2 and KIO3(in a certain range of the concentration). In the last chapter, according to NF mechanism(Noyes-Furrow model), the conclusion of the experiment and the redox potential of NiL3+/NiL2+, [Ni(TIM)]3+/ [Ni(TIM)]2+, we have proposed a skeleton mechanism for the B-R chemical system catalyzed by a macrocyclic nickel(Ⅱ) complex.