Study On A Briggs-Rauscher(B-R) Chemical Oscillating Reaction Which Is Catalyzed By A Macrocyclic Nickel (Ⅱ) Complex

Chemical oscillating system could exhibit spatiotemporal phenomena which is similar to self-organization phenomenon in life system. It's nonlinear non-equilibrium phenomenon which attracted many scientists to focus on, especially in a novel chemical oscillating reaction which is catalyzed by a macrocyclic nickel(Ⅱ) complex, where L= 5,7,7,12,14,14-hexemethyl-1,4,8,11-tetraazacyclotetradeca-4,11-diene. This catalyst is important to simulation of biological oscillations because it has a similar structure to some enzymes of life system. In this paper, we had an investigation on a novel Briggs-Rauscher (B-R) system (KIO3-[NiL](ClO4)2-CH2(COOH)2-H2O2-H2SO4). At the same time, we studied the perturbations effects on this B-R chemical oscillating system by addition of rifampicin, m-dihydroxybenzene or m-trihydroxybenzene to this oscillating system.The 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 in details, which are based on the classical NF model.The catalyst([NiL](ClO4)2) was synthesized according to literature, then was identified. A novel Briggs-Rauscher(B-R) oscillation with [NiL] (ClO4)2 as catalyst and malonic acid as substrates was studied. This novel BR oscillating system includes KIO3-H2SO4-H2O2-CH2(COOH)2-[NiL](ClO4)2. Influencing factors were analyzed to investigate the mechanism of the system.Then we discussed the applications of B-R system. The Inhibitory effects of rifampicin on it are studied. The experimental results indicate that, injection of rifampicin in the concentration range of 2.6 to 22.5μM caused temporal ceasing of oscillations, and then the oscillator resumed oscillations with obvious changes both in oscillation period and oscillating cycles. Time pause and average cycle are second-order polynomial proportional to the concentration of [rifampicin]. A mechanism on the effects of rifampicin is proposed.The result showed that effects of injecting m-dihydroxybenzene and m-trihydroxybenzene were distinct.①Their concentration range which can affect the B-R system are similar. m-dihydroxybenzene:5×10-6-1.5×10-4M; m-trihydroxybenzene:4.0×10-6 2.5×10-4M.②They have different effects on B-R oscillating reactions. The m-dihydroxybenzene restrained oscillating reaction. And time pause the is linearly proportional to the m-dihydroxybenzene concentration in the range 5×10-6-1.5×10-4M(n=10, r=0.99507). But the effect brought by m-trihydroxybenzene is different. The amplitude changed, and the change of amplitude is linearly proportional to the m-trihydroxybenzene concentration.③In structure, the m-dihydroxybenzene has one less Ar-OH than the m-trihydroxybenzene. So we concluded that the different effects were related with this structure peculiarity.④Because of high sensitivity and easy operation, we can measure this two materials by the B-R oscillating reaction.