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Research About Disturbance Of Phenolic Compounds And Surfactant On Tetraazamacrochclic Copper(Ⅱ)Complex-catalyzed B-Z Oscillating System

Posted on:2014-01-29Degree:MasterType:Thesis
Country:ChinaCandidate:Y Y ChenFull Text:PDF
GTID:2231330398478646Subject:Analytical Chemistry
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Chemical oscillating reaction as a typical phenomenon of nonlinear and non-equilibrium has more than one hundred years of history. Chemical oscillation belongs to a field of crossed subjects, so it has some high relevnce with physics, bioscience, etc. subjects. There is a bright prospect in the research of chemical oscillation reaction in many aspects, such as, promoting the communication of each discipline, establishing stability theoretical and practical foundation. At this stage, the study of chemical oscillation focused on as follows:designing the oscillator, discussing the reaction mechanism, furthering application of chemical oscillation, and enhancing the cooperation between oscillator and computer simulation, etc. Now, many significant research results have been accumulated. More and more catalysts besides transition metal ions could be found and one of these flashpoints is the finding of tetraazamacrocyclic complex [CuL](ClO4)2as chemical oscillator catalyst.(The unsaturated ligand L in the complex [CuL](clO4)2is5,7,7,12,14,14-hexemethyl-1,4,8,11-tetraazacyclotetradeca-4,11-diene.) The cyclical phenomena of oscillation reactions and the common cyclical phenomena in nature and our human societies are very similar. We have established a stable B-Z oscillating system not only concerning tetraazamacrocyclic complexes (enzyme-like catalyst) as catalyst but involving intermediates of Krebs cycle as substrate. So it is great significance for mimic studies of biochemical oscillations in vitro. In addition, this Belousov-Zhbaotinskii oscillator could be applied to the aspect of determination. This analytical method equipped with a simple instrument and provides a high selectivity for accurate determination of metal ions, vitamins, polyphenols and surfactants. In this thesis, there are three substances which are applied to research their disturbance on the B-Z oscillating system. These three substances are phenolic compounds, such as guaiacol, tannic and anionic surfactant sodium dodecyl benzene sulphonate (SDBS). We could observe some characteristic responses in the B-Z oscillation system which was perturbed by the chemicals, such as the change of oscillation amplitude (AA), the time of oscillating inhibition (At) or the change of oscillation period (AT). Some relationships which between the characteristic responses and the concentration of chemicals injected into oscillating system could be established, and the interference mechanisms were also discussed.This thesis mainly is divided into five parts:1. The summary of chemical oscillating reaction This chapter review provides a brief introduction to the nonlinear reaction, the history of chemical oscillating reaction, reaction conditions, and types of oscillating reaction. The B-Z oscillating system is set forth in detail, and there are analyses about the famous FKN mechanism and the mechanism of novel oscillator which contains the macrocyclic complexes as catalyst and malic acid as substrate. Meanwhile, we also give some introductions about related applications and the current state of chemical oscillation.2. Research about disturbance of guaiacol on teraazamacrochclic copper (Ⅱ) complex catalyzed B-Z oscillating system. According to literature, tetraazamacrocyclic copper (Ⅱ) complex [CuL](C104)2was synthesized. We used I.R spectrum and elemental analyses to identify the target product. The novel oscillating system could be established by sodium bromate, D-L malic acid,[CuL](ClO4)2and the sulfuric acid. We explored the interference of guaiacol on the stable oscillator and the influence of experimental variables on the system. There is a linear relationship between the change of the amplitude (AA) and the logarithm of concentration of guaiacol. When the different amount of guaiacol was injected to the oscillating system, the change of the oscillation period (△T) is linearly proportional. The probable mechanism involving the perturbation of guaiacol on the oscillating chemical system was also discussed.3. Research about disturbance of tannin on teraazamacrochclic copper (Ⅱ) complex catalyzed B-Z oscillating system.With macrocyclic complex [CuL](C104)2as catalyst and malic acid as the substrate, this B-Z system could be perturbed by tannin. The change of the amplitude (AA) and the time of oscillating inhibition (At) were more obvious with the increase of tannin injected to the oscillating system. There is a linear relationship between the change of the amplitude (△A) and the logarithm of concentration of tannin. There is other linear relationship between, the time of oscillating inhibition (△t) and the logarithm of concentration of tannin. We discussed the influence of experimental variables and the probable interference mechanism.4. Research about disturbance of anionic surfactant SDBS micelle on teraazamacrochclic copper (Ⅱ) complex catalyzed B-Z oscillating system. This chapter discusses the influence of anionic surfactant SDBS on B-Z oscillating reaction which was catalyzed by a tetraazamacrocyclic copper (Ⅱ) complex. The oscillating system involves sodium bromate-malic acid [CuL](C104)2-sulfuric acid. Experiments show that formation of the SDBS micelles markedly affects the behaviour of the oscillating reaction. It is found that there is a linear relationship between the change in the oscillation amplitude (AA) and the concentration of SDBS, whereas the change in the oscillation period (△T) is linearly proportional to the SDBS concentration. The most likely mechanism that involves the formation of the SDBS micelles and the effects of the micelles on the oscillating chemical system can be understood through the hypothesis that the SDBS micelles are so negatively charged that they attract more [CuL]3+than [CuL]2+. The hypothesis was confirmed by UV-vis spectrophotometric measurements of a constant concentration of [CuL](ClO4)2in different concentrations of SDBS; as the SDBS concentration increased, the absorbance of [CuL](ClCO4)2increased while the maximum absorption wavelength for [CuL](ClCO4)2remained at502nm.
Keywords/Search Tags:Belousov-Zhbaotinskii oscillating reaction, catalyst [CuL](ClO4)2, phenolic compounds, anion surfactant
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