化学反应中的自组织及振荡反应在有机物分析检测中的应用
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摘要
近年来，非生命系统中出现越来越多的自组织现象受到关注，并已成为许多科技工作者研究的热点问题。化学振荡反应即是化学反应中的自组织现象的体现，由于具有特别的宏观现象及特殊的机理，因此成为分析化学进行微量检测的有效工具。本文利用化学振荡反应测定了间苯二酚，建立了麻黄碱的动力学检测方法，结果满意。论文由三部分组成。
第一部分 化学反应中的自组织及振荡反应在有机物分析检测中的应用
综述了化学反应中的自组织现象——化学振荡反应的发展历史，以及与之有关的热力学基本理论和化学振荡反应具备的条件。对几类化学振荡反应机理，特别是B-Z振荡反应机理给予详细阐述。系统地评述了1978—2003年间化学振荡反应在分析检测应用取得的进展。
第二部分 痕量间苯二酚的B-Z振荡反应动力学测定
研究了在封闭体系中B-Z振荡反应测定间苯二酚的条件，建立了测定痕量间苯二酚的新方法。当[KBrO_3]=0.25mol·L~(-1)、[CH_2(COOH)_2]=0.5mol·L~(-1)、[Ce(SO_4)_2]=0.04mol·L~(-1)、[H_2SO_4]=0.8mol·L~(-1)时，间苯二酚在6.5×10~(-7)mol·L~(-1)～1.0×10~(-5)mol·L~(-1)范围内，浓度与振幅改变值ΔA呈线性关系，检出限为6.0×10~(-7)mol·L~(-1)。用于废水中间苯二酚的测定，回收率为99％。
第三部分 使用Cu(Ⅱ)催化振荡反应测定麻黄碱
研究了Cu(Ⅱ)催化振荡反应在封闭体系中测定麻黄碱的条件，建立了测定麻黄碱的新方法，确定了相关的反应条件。在测定条件下，当麻黄碱1.06×10~(-3)mol·L~(-1)—2.5×10~(-6)mol·L~(-1)范围内，具有良好的线性关系，相关系数0.9954，检出限为2.05×10~(-6)mol·L~(-1)。
In recent years,more and more self-organized phenomenon which was obseverd in non-linear system, in particular, have become of great interest across of wide range of scientific research. Oscillating chemical reactions exhibit exotic behavior and unusual mechanisms. Consequently, they have been considered as a useful tool for the determination of trace amounts of chemical compounds This work develops new methods using oscillating chemical reaction for quantitative analytical determinations of resorcinol, and ephedrine, the accuracy and selectivity of these methods are well-pleasing. The main content consists of three parts
Part I Self-organization in the Chemical Reactions and Analytical Applications of Oscillating Chemical Reactions in the Organic Compounds
This literature review provides a simple introduction to the phenomenon of "self-orgnization in chemical reaction" -oscillating chemical reaction., and provides some basic thermodynamic theory related. Mechanisms of some chemical oscillators that were used in analytical determinations are reported in details, especially B-Z chemical oscillation. The research progress in analytical applications from 1978 to 2003 is discussed systematically through representative examples
Part II Kinetic Determimation of Trace Amount of Resorcinol by B-Z Oscillating Chemical Reaction
An analytical method for the determination of trace amount of resorcinol is establishd by studying its pertubation on B-Z oscillating reaction. The best reaction condition and the reactant's concentrations are reported. The amplitude decrease of the poteniometric oscillation is linearly proportional to the concentration of resorcinol in the range of 6.5×10-7 mol·L-1 - 1.0×10*5 mol·L-1, with the correlation coefficien of 0.9989. In the range of 1.5×10-5 mol·L-1 - 6.5 × 10-4 mol·L-1, the decrease in amplitude
versus the concentrations of resorcinol fits a second-order equation, and the correlation coefficient is 0.9949. Detection limite is 6.0×10-7 mol·L-1. The method is used to determine resorcinol in waster water, a satisfactory results are achieude. The mechanism of the pertubation is discussed.
Part III Determination of Ephedrine by an Cu(II) Catalized Oscillating Chemical Reaction
A new analytical method for the determination by the perturbation caused by different amounts of ephedrine on the oscillating chemical system, involving the Cu( II )-catalysed reaction between hydrogen peroxide and sodium thiocyanate in closed system, is proposed. The method relies on the linear relationship between the changes in the oscillating amplitude and the logarthm of concentration of ephedrine. The calibration curve is linear over the range from 1.06×10-3 mol·L*1 - 2.5×10-6 mol·L-1, and the correlation coefficient is 0.9954. Detection limite is 2.05×10-6 mol·L-1. Some aspects of the interaction of ephedrine with the oscillating chemical system are also discussed.
第一部分 化学反应中的自组织及振荡反应在有机物分析检测中的应用
综述了化学反应中的自组织现象——化学振荡反应的发展历史，以及与之有关的热力学基本理论和化学振荡反应具备的条件。对几类化学振荡反应机理，特别是B-Z振荡反应机理给予详细阐述。系统地评述了1978—2003年间化学振荡反应在分析检测应用取得的进展。
第二部分 痕量间苯二酚的B-Z振荡反应动力学测定
研究了在封闭体系中B-Z振荡反应测定间苯二酚的条件，建立了测定痕量间苯二酚的新方法。当[KBrO_3]=0.25mol·L~(-1)、[CH_2(COOH)_2]=0.5mol·L~(-1)、[Ce(SO_4)_2]=0.04mol·L~(-1)、[H_2SO_4]=0.8mol·L~(-1)时，间苯二酚在6.5×10~(-7)mol·L~(-1)～1.0×10~(-5)mol·L~(-1)范围内，浓度与振幅改变值ΔA呈线性关系，检出限为6.0×10~(-7)mol·L~(-1)。用于废水中间苯二酚的测定，回收率为99％。
第三部分 使用Cu(Ⅱ)催化振荡反应测定麻黄碱
研究了Cu(Ⅱ)催化振荡反应在封闭体系中测定麻黄碱的条件，建立了测定麻黄碱的新方法，确定了相关的反应条件。在测定条件下，当麻黄碱1.06×10~(-3)mol·L~(-1)—2.5×10~(-6)mol·L~(-1)范围内，具有良好的线性关系，相关系数0.9954，检出限为2.05×10~(-6)mol·L~(-1)。
In recent years,more and more self-organized phenomenon which was obseverd in non-linear system, in particular, have become of great interest across of wide range of scientific research. Oscillating chemical reactions exhibit exotic behavior and unusual mechanisms. Consequently, they have been considered as a useful tool for the determination of trace amounts of chemical compounds This work develops new methods using oscillating chemical reaction for quantitative analytical determinations of resorcinol, and ephedrine, the accuracy and selectivity of these methods are well-pleasing. The main content consists of three parts
Part I Self-organization in the Chemical Reactions and Analytical Applications of Oscillating Chemical Reactions in the Organic Compounds
This literature review provides a simple introduction to the phenomenon of "self-orgnization in chemical reaction" -oscillating chemical reaction., and provides some basic thermodynamic theory related. Mechanisms of some chemical oscillators that were used in analytical determinations are reported in details, especially B-Z chemical oscillation. The research progress in analytical applications from 1978 to 2003 is discussed systematically through representative examples
Part II Kinetic Determimation of Trace Amount of Resorcinol by B-Z Oscillating Chemical Reaction
An analytical method for the determination of trace amount of resorcinol is establishd by studying its pertubation on B-Z oscillating reaction. The best reaction condition and the reactant's concentrations are reported. The amplitude decrease of the poteniometric oscillation is linearly proportional to the concentration of resorcinol in the range of 6.5×10-7 mol·L-1 - 1.0×10*5 mol·L-1, with the correlation coefficien of 0.9989. In the range of 1.5×10-5 mol·L-1 - 6.5 × 10-4 mol·L-1, the decrease in amplitude
versus the concentrations of resorcinol fits a second-order equation, and the correlation coefficient is 0.9949. Detection limite is 6.0×10-7 mol·L-1. The method is used to determine resorcinol in waster water, a satisfactory results are achieude. The mechanism of the pertubation is discussed.
Part III Determination of Ephedrine by an Cu(II) Catalized Oscillating Chemical Reaction
A new analytical method for the determination by the perturbation caused by different amounts of ephedrine on the oscillating chemical system, involving the Cu( II )-catalysed reaction between hydrogen peroxide and sodium thiocyanate in closed system, is proposed. The method relies on the linear relationship between the changes in the oscillating amplitude and the logarthm of concentration of ephedrine. The calibration curve is linear over the range from 1.06×10-3 mol·L*1 - 2.5×10-6 mol·L-1, and the correlation coefficient is 0.9954. Detection limite is 2.05×10-6 mol·L-1. Some aspects of the interaction of ephedrine with the oscillating chemical system are also discussed.
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