几种新型的化学振荡体系在分析化学中的应用研究
摘要
非平衡非线性化学属于一门新的交叉学科，已成为化学研究中一个新的生长点，近年来引起广大科学工作者的广泛兴趣，非线性行为的化学振荡也成为这一领域的研究热点，研究内容主要包括新体系的设计及其机理的研究和振荡体系在分析测定中的应用。本文应用铜振荡体系和B-Z振荡体系分别测定了对硝基苯偶氮萘酚和α-萘酚及联苯胺，并对L-苯丙氨酸参与的油水液膜振荡体系做了比较系统的研究。
第一部分 化学振荡反应及其在分析中的应用
综述了化学振荡反应发展简史，对几类常见的化学振荡反应体系及其机理给予详细的评述，简要展望了化学振荡反应的应用前景。
第二部分 联苯胺对B-Z振荡反应的影响
研究了B-Z振荡体系电位-时间曲线的周期和振幅的改变值与加入联苯胺浓度的关系，实验表明，当加入联苯胺的浓度在3.5×10~(-9)-1×10~(-4)M范围内时，体系振幅的改变量与加入联苯胺的浓度呈良好的线性关系(r=0.9975)，结合FKN模型讨论了联苯胺对BZ振荡反应的影响机理。该方法简单易行，而且灵敏度较高。
第三部分 在铜催化振荡反应中应用脉冲微扰技术检测了对硝基苯偶氮萘酚和α-萘酚
首次应用铜催化振荡反应检测了对硝基苯偶氮萘酚和α-萘酚。对硝基苯偶氮萘酚和α-萘酚都能使铜催化振荡反应的振幅增大，并且对硝基苯偶氮萘酚也能使振荡反应的周期增大，周期和振幅的增大量与对硝基苯偶氮萘酚的浓度呈线性关系，其线性范围为5.2×10~(-7)-3.3×10~(-3)M；振幅的增大量与α-萘酚的线性范围为3.4×10~(-8)-5.3×10~(-4)M(r=0.9991)。应用脉冲微扰技术实现了对硝基苯偶氮萘酚和α-萘酚的连续测定，缩短了检测时间。
第四部分 L-苯丙氨酸参与的新化学振荡器
以十六烷基三甲基溴化铵(CTAB)+乙醇／含L-苯丙氨酸的硝基苯／氯化钠溶液为研究体系，对其在较宽浓度范围内的非线性动力学行为进行了研究，观察到当各组分浓度不同时，体系的化学行为不同，有规则振荡和混沌现象。并对膜电位的振荡反应机理进行了初步探讨。
The subject of nonequilibrium and nonlinear is very usual in the field of science. It has attracted the attention of researchers for many years. One important investigation is that of chemical oscillation. There has been a focus on the theoretical and experimental chemical kinetics in recent years. Studies of oscillating chemical reactions are application of regular chemical reaction to analytical determination and designing new oscillating chemical reaction. The paper report the effect of benzidine on the B-Z oscillating chemical reaction; determination of p-nitrobenzene-azo-naphthol and alpha-naphthol using the H2O2-CUSO4-KSCN oscillating chemical reaction; A novel chemical oscillator with phenylalanine was also represented. Part I Oscillating chemical reactions and their application in the analytical
chemistry
This literature review provides a brief introduction to the development of the oscillating chemical reactions. Some theoretical model, thermodynamic parameters and their applications are described in detail. The perspective of oscillating chemical reactions is discussed to the point. Part II Effect of benzidine on the B-Z oscillating chemical reaction
A simple and sensitive analytical method for the determination of benzidine with the perturbation caused by different amounts of benzidine on the Belousov-Zhabotinskii (BZ) oscillating chemical system, involving the Ce(IV)-catalyzed reaction between potassium bromate and malonic acid in a acidic medium is proposed. Results show a good linear relationship between the change in the oscillation amplitude of the system and the concentration of benzidine. The calibration curve is linearly proportional to the concentration of benzidine over the range 3.5x10-9 -1x10-4M, with a regression coefficient 0.9975. The optimum conditions for the determination have also been investigated in the B-Z reaction system. Influence of temperature, and variable reaction conditions are investigated in detail and the possible mechanism of action of benzidine on the chemical oscillating system is also discussed.
Part III Determination of p-nitrobenzene-azo-naphthol and alpha-naphthol on H2O2-CuSO4-KSCN oscillating chemical reaction
A simple analytical method for the determination of p-nitrobenzene-azo-naphthol and
alpha-naphthol was proposed by a sequential perturbation with different amounts of them on an oscillating chemical system. The method involves a Cu(II)-catalysed oscillating reaction between hydrogen peroxide and sodium thiocyanate in alkaline medium with the aid of continuous-flow stirred tank reactor (CSTR). And it relies on the linear relationship between the changes in the oscillation amplitude and period of chemical system and the concentration of p-nitrobenzene-azo-naphthol. The calibration curve fits a linear equation very well when the concentration of p-nitrobenzene-azo-naphthol ranges from 5.2x10-7 to 3.3x10-3M. It relies on the linear relationship between the changes in the oscillation amplitude of chemical system and the concentration of alpha-naphthol. The calibration curve fits a linear equation very well when the concentration of alpha-naphthol ranges from 3.4x10-8 to 5.3 x10-4M. The use of analyte pulse perturbation technique provides the possibility of sequential determinations in the same o
scillating system, owing to a new steady state was reappeared rapidly after each perturbation. Influence of temperature, injection point, flow rate and reactants variables on this system were investigated in detail
Part IV A novel chemical oscillator with phenylalanine
Studies on nonlinear behavior at oil/water interface membrane were performed. This system showed rhythmic oscillations and chaos of electrical potential in a given concentration domain. The nonlinear behavior response at the liquid membrane apparently resembled that of biological chemoreceptive membrane. The possibility of developing a new type of chemical sensor with the ability to simulate substance equilibrium in living organisms was suggested in the paper.
第一部分 化学振荡反应及其在分析中的应用
综述了化学振荡反应发展简史，对几类常见的化学振荡反应体系及其机理给予详细的评述，简要展望了化学振荡反应的应用前景。
第二部分 联苯胺对B-Z振荡反应的影响
研究了B-Z振荡体系电位-时间曲线的周期和振幅的改变值与加入联苯胺浓度的关系，实验表明，当加入联苯胺的浓度在3.5×10~(-9)-1×10~(-4)M范围内时，体系振幅的改变量与加入联苯胺的浓度呈良好的线性关系(r=0.9975)，结合FKN模型讨论了联苯胺对BZ振荡反应的影响机理。该方法简单易行，而且灵敏度较高。
第三部分 在铜催化振荡反应中应用脉冲微扰技术检测了对硝基苯偶氮萘酚和α-萘酚
首次应用铜催化振荡反应检测了对硝基苯偶氮萘酚和α-萘酚。对硝基苯偶氮萘酚和α-萘酚都能使铜催化振荡反应的振幅增大，并且对硝基苯偶氮萘酚也能使振荡反应的周期增大，周期和振幅的增大量与对硝基苯偶氮萘酚的浓度呈线性关系，其线性范围为5.2×10~(-7)-3.3×10~(-3)M；振幅的增大量与α-萘酚的线性范围为3.4×10~(-8)-5.3×10~(-4)M(r=0.9991)。应用脉冲微扰技术实现了对硝基苯偶氮萘酚和α-萘酚的连续测定，缩短了检测时间。
第四部分 L-苯丙氨酸参与的新化学振荡器
以十六烷基三甲基溴化铵(CTAB)+乙醇／含L-苯丙氨酸的硝基苯／氯化钠溶液为研究体系，对其在较宽浓度范围内的非线性动力学行为进行了研究，观察到当各组分浓度不同时，体系的化学行为不同，有规则振荡和混沌现象。并对膜电位的振荡反应机理进行了初步探讨。
The subject of nonequilibrium and nonlinear is very usual in the field of science. It has attracted the attention of researchers for many years. One important investigation is that of chemical oscillation. There has been a focus on the theoretical and experimental chemical kinetics in recent years. Studies of oscillating chemical reactions are application of regular chemical reaction to analytical determination and designing new oscillating chemical reaction. The paper report the effect of benzidine on the B-Z oscillating chemical reaction; determination of p-nitrobenzene-azo-naphthol and alpha-naphthol using the H2O2-CUSO4-KSCN oscillating chemical reaction; A novel chemical oscillator with phenylalanine was also represented. Part I Oscillating chemical reactions and their application in the analytical
chemistry
This literature review provides a brief introduction to the development of the oscillating chemical reactions. Some theoretical model, thermodynamic parameters and their applications are described in detail. The perspective of oscillating chemical reactions is discussed to the point. Part II Effect of benzidine on the B-Z oscillating chemical reaction
A simple and sensitive analytical method for the determination of benzidine with the perturbation caused by different amounts of benzidine on the Belousov-Zhabotinskii (BZ) oscillating chemical system, involving the Ce(IV)-catalyzed reaction between potassium bromate and malonic acid in a acidic medium is proposed. Results show a good linear relationship between the change in the oscillation amplitude of the system and the concentration of benzidine. The calibration curve is linearly proportional to the concentration of benzidine over the range 3.5x10-9 -1x10-4M, with a regression coefficient 0.9975. The optimum conditions for the determination have also been investigated in the B-Z reaction system. Influence of temperature, and variable reaction conditions are investigated in detail and the possible mechanism of action of benzidine on the chemical oscillating system is also discussed.
Part III Determination of p-nitrobenzene-azo-naphthol and alpha-naphthol on H2O2-CuSO4-KSCN oscillating chemical reaction
A simple analytical method for the determination of p-nitrobenzene-azo-naphthol and
alpha-naphthol was proposed by a sequential perturbation with different amounts of them on an oscillating chemical system. The method involves a Cu(II)-catalysed oscillating reaction between hydrogen peroxide and sodium thiocyanate in alkaline medium with the aid of continuous-flow stirred tank reactor (CSTR). And it relies on the linear relationship between the changes in the oscillation amplitude and period of chemical system and the concentration of p-nitrobenzene-azo-naphthol. The calibration curve fits a linear equation very well when the concentration of p-nitrobenzene-azo-naphthol ranges from 5.2x10-7 to 3.3x10-3M. It relies on the linear relationship between the changes in the oscillation amplitude of chemical system and the concentration of alpha-naphthol. The calibration curve fits a linear equation very well when the concentration of alpha-naphthol ranges from 3.4x10-8 to 5.3 x10-4M. The use of analyte pulse perturbation technique provides the possibility of sequential determinations in the same o
scillating system, owing to a new steady state was reappeared rapidly after each perturbation. Influence of temperature, injection point, flow rate and reactants variables on this system were investigated in detail
Part IV A novel chemical oscillator with phenylalanine
Studies on nonlinear behavior at oil/water interface membrane were performed. This system showed rhythmic oscillations and chaos of electrical potential in a given concentration domain. The nonlinear behavior response at the liquid membrane apparently resembled that of biological chemoreceptive membrane. The possibility of developing a new type of chemical sensor with the ability to simulate substance equilibrium in living organisms was suggested in the paper.
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