化学振荡反应在分析检测中的应用
摘要
第一刊g分化学振荡反脚问理论发展及其在分析检测中的应用
近年末，化学振荡反应己成为化学动力学理沦和实验研究的重点。其卞要任务是
发现新的振荡体系，研究反应机理及探索化学振荡反应与生命有机体的关系。这一部
分主要阐述了化学振荡反应理沦研究的发展历史，各种化学振荡反应的机理以及它们
在分析检测中的应用。最后，简要介绍了化学振荡反应研究的重要意义以及它在化
学，生化，工程等领域的发展前景。
第二部分应用BZ振荡反应检测抗坏血酸
首次应用BZ振荡反应对抗坏血酸进行检测。山于抗坏血酸能够使BZ振荡反应的
振幅发生变化，而振幅的改变与抗坏血酸的浓度呈线性关系，囚此我们可利用BZ振荡
反应来检测抗坏血酸。在 3．5 xlo”‘．4． 7 X 0“M的浓度范围内，振幅的改变与抗坏血酸的
浓度成线性关系，线性方程为：AA＝2 8。2 6741＋10596413531［抗坏血酸］，相关系数为
09975。最后，我们结合FKN模型讨论了抗坏血酸对BZ振荡反应的影响的机理。
第三部分应用脉冲微扰技术在铜催化振荡反应中检测谷氨酸
首次应用铜催化振荡反应对谷氨酸进付检测。谷氨酸使铜催化振荡反应的振幅减
小，其振幅的减小与谷氨酸的浓度呈线性关系，线性范围为 2．5 XIO’‘刁2 xlo“M，相关
系数为0．9987，线性万程为：＊＊＝3．34769伺7允6．驯12时谷氨酸」。找们应用脉仲微扰
技术实现了谷氨酸检测的连续性，缩短了检测时间，并且检测的相对标准偏差小于
068％。最后，结合铜催化振荡反应的机理讨论了谷氨酸对铜催化振荡反应的影响。
第四部分检测BZ振荡反应和铜催化振荡反应的振荡范围
近年来，化学振荡反应已成为化学动力学理论和实验研究的重点。在这些复杂的振
荡体系中，科学工作者研究最多的是BZ振荡反应和铜催化振荡反应。一个化学反应只
有当其处于远离平腼态时才会发生振荡现象。这也就是悦，化学扼荡反应存在着一个
振荡范mn广。该一音卜卜卜．赣仆讨卜H了R7桥俟6向和嗣倔仆彬蕉厂府呐郴兢茹阳扛卅
其影响＊系进付了讨沦。
Part I Theoretical and experimental development of oscillating chemical reactions and their applications in analytical determination
Oscillating chemical reactions have been the focus of much research in the area of theoretical and experimental chemical kinetics in recent years. The major task is to discover new oscillating systems, investigate the mechanisms of these reactions and explore the relationship between oscillating chemical reactions and the living organisms. In this section, we described the theoretical and experimental development of these reactions. The mechanisms of these reactions and their applications in analytical determination were also discussed in brief. Finally, we mentioned the importance of these reactions in the field of chemistry, biochemistry and engineering.
Part II Kinetic determination of ascorbic acid by the BZ oscillating chemical system
A new analytical method for the determination of ascorbic acid by the perturbation caused by different amounts of ascorbic acid on the BZ oscillating chemical system involving the Ce(IV)-catalyzed reaction between potassium bromate and malonic acid in a acidic medium is proposed. The method relies on the linear relationship between the change in the oscillation amplitude of the chemical system and the concentration of ascorbic acid, which is in this work exposed for the first time. The calibration curve is linearly proportional to the concentration of ascorbic acid over the range 3.5x10-6-4.7x10-4M, with the regression coefficient is 0.9975. Two different methodologies were used to address the determination. Some aspects of the potential mechanism of action of ascorbic acid on the BZ oscillating chemical system are discussed in detail.
Part III Determination of glutamic acid by an oscillating chemical reaction using the analyte pulse perturbation technique
An analytical method for the determination of glutamic acid by the sequential perturbation caused by different amounts of glutamic acid on the oscillating chemical system involving the Cu(II)-catalysed oscillating reaction between hydrogen peroxide and sodium thiocyanate in an alkaline medium is proposed. The method relies on the linear relationship
between the changes in the oscillation amplitude of the chemical system and the concentration of glutamic acid. The reaction is implemented in a continuous-flow stirred-tank reactor, and changes in the oscillation amplitude on each perturbation are proportional to the glutamic acid concentration. The use of the analyte pulse perturbation technique permits sequential determinations on the same oscillating system owing to the expeditiousness with which the steady state is regained after each perturbation. The dynamic range lies between 2.5x10-6 and 3.2x10-4M of glutamic acid, with the regression coefficient is 0.9987. The precision is excellent(less than 0.68% as relative standard deviation). Some aspects of the potential mechanism of action of glutamic acid on the oscillating system are discussed.
Part IV The detection of the oscillatory domain of the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(II)-catalyzed oscillating chemical reaction
The oscillating chemical reactions have been the focus of much research in the area of theoretical and experimental chemical kinetics in recent years. Among these complex systems of chemical reactions, those that have received the most attention and most thoroughly investigated are the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(II)-catalyzed oscillating chemical reaction. For a chemical reaction to be the source of an auto-oscillating system, it must be far from equilibrium. That is to say, oscillating chemical reactions have their own oscillatory domain. In this section, we investigated the oscillatory domain of the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(ll)-catalyzed oscillating chemical reaction. Some factors which have effects on the oscillatory domain are discussed.
近年末，化学振荡反应己成为化学动力学理沦和实验研究的重点。其卞要任务是
发现新的振荡体系，研究反应机理及探索化学振荡反应与生命有机体的关系。这一部
分主要阐述了化学振荡反应理沦研究的发展历史，各种化学振荡反应的机理以及它们
在分析检测中的应用。最后，简要介绍了化学振荡反应研究的重要意义以及它在化
学，生化，工程等领域的发展前景。
第二部分应用BZ振荡反应检测抗坏血酸
首次应用BZ振荡反应对抗坏血酸进行检测。山于抗坏血酸能够使BZ振荡反应的
振幅发生变化，而振幅的改变与抗坏血酸的浓度呈线性关系，囚此我们可利用BZ振荡
反应来检测抗坏血酸。在 3．5 xlo”‘．4． 7 X 0“M的浓度范围内，振幅的改变与抗坏血酸的
浓度成线性关系，线性方程为：AA＝2 8。2 6741＋10596413531［抗坏血酸］，相关系数为
09975。最后，我们结合FKN模型讨论了抗坏血酸对BZ振荡反应的影响的机理。
第三部分应用脉冲微扰技术在铜催化振荡反应中检测谷氨酸
首次应用铜催化振荡反应对谷氨酸进付检测。谷氨酸使铜催化振荡反应的振幅减
小，其振幅的减小与谷氨酸的浓度呈线性关系，线性范围为 2．5 XIO’‘刁2 xlo“M，相关
系数为0．9987，线性万程为：＊＊＝3．34769伺7允6．驯12时谷氨酸」。找们应用脉仲微扰
技术实现了谷氨酸检测的连续性，缩短了检测时间，并且检测的相对标准偏差小于
068％。最后，结合铜催化振荡反应的机理讨论了谷氨酸对铜催化振荡反应的影响。
第四部分检测BZ振荡反应和铜催化振荡反应的振荡范围
近年来，化学振荡反应已成为化学动力学理论和实验研究的重点。在这些复杂的振
荡体系中，科学工作者研究最多的是BZ振荡反应和铜催化振荡反应。一个化学反应只
有当其处于远离平腼态时才会发生振荡现象。这也就是悦，化学扼荡反应存在着一个
振荡范mn广。该一音卜卜卜．赣仆讨卜H了R7桥俟6向和嗣倔仆彬蕉厂府呐郴兢茹阳扛卅
其影响＊系进付了讨沦。
Part I Theoretical and experimental development of oscillating chemical reactions and their applications in analytical determination
Oscillating chemical reactions have been the focus of much research in the area of theoretical and experimental chemical kinetics in recent years. The major task is to discover new oscillating systems, investigate the mechanisms of these reactions and explore the relationship between oscillating chemical reactions and the living organisms. In this section, we described the theoretical and experimental development of these reactions. The mechanisms of these reactions and their applications in analytical determination were also discussed in brief. Finally, we mentioned the importance of these reactions in the field of chemistry, biochemistry and engineering.
Part II Kinetic determination of ascorbic acid by the BZ oscillating chemical system
A new analytical method for the determination of ascorbic acid by the perturbation caused by different amounts of ascorbic acid on the BZ oscillating chemical system involving the Ce(IV)-catalyzed reaction between potassium bromate and malonic acid in a acidic medium is proposed. The method relies on the linear relationship between the change in the oscillation amplitude of the chemical system and the concentration of ascorbic acid, which is in this work exposed for the first time. The calibration curve is linearly proportional to the concentration of ascorbic acid over the range 3.5x10-6-4.7x10-4M, with the regression coefficient is 0.9975. Two different methodologies were used to address the determination. Some aspects of the potential mechanism of action of ascorbic acid on the BZ oscillating chemical system are discussed in detail.
Part III Determination of glutamic acid by an oscillating chemical reaction using the analyte pulse perturbation technique
An analytical method for the determination of glutamic acid by the sequential perturbation caused by different amounts of glutamic acid on the oscillating chemical system involving the Cu(II)-catalysed oscillating reaction between hydrogen peroxide and sodium thiocyanate in an alkaline medium is proposed. The method relies on the linear relationship
between the changes in the oscillation amplitude of the chemical system and the concentration of glutamic acid. The reaction is implemented in a continuous-flow stirred-tank reactor, and changes in the oscillation amplitude on each perturbation are proportional to the glutamic acid concentration. The use of the analyte pulse perturbation technique permits sequential determinations on the same oscillating system owing to the expeditiousness with which the steady state is regained after each perturbation. The dynamic range lies between 2.5x10-6 and 3.2x10-4M of glutamic acid, with the regression coefficient is 0.9987. The precision is excellent(less than 0.68% as relative standard deviation). Some aspects of the potential mechanism of action of glutamic acid on the oscillating system are discussed.
Part IV The detection of the oscillatory domain of the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(II)-catalyzed oscillating chemical reaction
The oscillating chemical reactions have been the focus of much research in the area of theoretical and experimental chemical kinetics in recent years. Among these complex systems of chemical reactions, those that have received the most attention and most thoroughly investigated are the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(II)-catalyzed oscillating chemical reaction. For a chemical reaction to be the source of an auto-oscillating system, it must be far from equilibrium. That is to say, oscillating chemical reactions have their own oscillatory domain. In this section, we investigated the oscillatory domain of the Belousov-Zhabotinskii(BZ) oscillating chemical reaction and the Cu(ll)-catalyzed oscillating chemical reaction. Some factors which have effects on the oscillatory domain are discussed.
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82 缪静琪，李湘如，B-Z反应对Ki(T)的影响行为，物理化学学报，1989，5，726．
83 Cun Li, Fuxin Xie, and Shisheng, Ni, Oscillating Reactions Catalyzed by Tetraaza macrocyclic Nickle(Ⅱ) Complex, Anhui Daxue Xuebao, 2000,24,79.
84 Yatsimirskii, K.B., and Tikhonova, L.P., Transition Metal Coordination Copounds in Oscillating Chemical Reaction, Coord. Chcm. Rev.,1985,63.241.
85 徐志强，赵祥大，倪诗圣，环镍配合物参与的新型振荡化学反应，安徽大学学报，1993，1，64．
86 徐济德，倪诗圣，BZ反应体系极限环行为的实验描述，安徽大学学报，1986，1，31．
87 Rastogi, R.P., and Verma, M.K., Role of Molecular Bromine in Belousov-Zhabotinskii Reaction Driven by Bromate Ion, Indian.J.Chem.,1983,22,917.
88 Jinzhang Gao, Hua Yang, Xiuhui Liu, Jie Ren, Qizhi Li and Jingwan Kang, Determination of glutamic acid by an oscillating chemical reaction using the analyte pulse perturbation technique, Talanta, 2002,57,105.
89 Olson, D.L., and Scheeline, A., Theoretical investigation of the peroxidase-oxidase chemical oscillator for quantitative enzyme analysis, Anal. Chim. Acta., 1990,237,381.
90 Yoshikawa, K., and Matsubara, Y., Spontaneous Oscillation of pH and Electrical Potential in an Oil-Water System, J.Am. Chem. Soc., 1983,105,267.
91 Ruoshao Liu, Exploration of Chemical Vibration Experiment in the System of KBrO_3 Reacting With CH_2(COOH)_2,Shandong Qinggongye Xueyuan Xuebao,1995,9,14.
92 Xianan Fang, Congjun An,Yi Liu, Zhixin Ling, and Ruxiu Cai, Kinetic Study of Ag~+ on BZ Chemical Oscillatory, Wuhan Daxue Xuebao, 1994,2,100.
93 Zhenwen Shen, Pingchu Jiang, Hexing Li,Yan Jin, and Yuanchang Xu, Approach to the Application of Chemical Oscillation in Clinical Test-Effects of Human Serum on Chemical Oscillation, Shanghai Shifan Daxue Xuebao,1994,23,57.
94 Xiangda Zhao, Zhiqiang Xu, and Junfa Zhu, Research of Quantitative Relationship between Delayed-time of Chemical Oscillating Reaction and Microquantity Elements Silver and Mercury, Anhui Daxue Xuebao, 1994,2,54.
95 Rongming Guan, Non-Linear Phenomenon in Chemical Reactions,Shandong Qinggongye Xueyuan Xuebao, 1996,10,15.
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98 贺占博，化学振荡反应的研究方向，化学通报，2000，8，54．
99 Chenxin Cai, and Cuihong Huang, Oscillating Chemical Reaction, Nanjin Shida Xuebao,Oscillating Chemical Reaction, Coord. Chcm. Rev.,1985,63.241.
100 Zhanbo He, Application of Surfactants in the Study of Nonlinear Chemical Kinetics,Huaxue Gongye yu Gongcheng, 2001,18,93.
101 Jintian Yang, A Survey on the Theory of the Dissipative Structure and Its Philosophical Meaning in the Chemical Field, Huzhou Shifan Xueyuan Xuebao, 2000,22,26.
102 Congjun An, Nanqing Gan, Yi Liu, and Ruxiu Cai, The New Characteristics and Kinetics of Diacetone-Malic Acid-BrO_3~--Mn~(2+)-H_2SO_4 Nonlinear Chemical Reaction, Wuhan Daxue Xuebao,1999,45,411.
103 Guozhi Lu, Yuncheng Cui, and Renzhang Wang, The Oscillatory Reaction Using LLeucine as Organic Compound, Songliao Xuekan, 2000,2,37.
104 Ruxiu Cai, Ke Zhang, Wanhong Ma, Nanqing Gan, and Zhixin Lin, Nonlinear Chemical Reaction Characteristics of Diacetone-Malic Acid-BrO_3~--Mn~(2+)-H_2SO_4 and the Application in Biological Antioxidation, Fuzhou Daxue Xuebao,1999,27,249.
105 Xiaoyan Jin, Lihua Liu, Milin Zhang, and Shunlong Liu, The Investigation of Oscillating Chemical Reaction with the SO and MO as Organic Compound, Haerbin Gongcheng Daxue Xuebao,2001,22,71.
106 Fuxin Xie, Shengli Li, Zhiqiang Xu, Ming Wu, and Shisheng Ni, Chemical Oscillation of NaBrO_3-Pyr-[NiDTH](ClO_4)_2-H_2SO_4 Systems, Zhongguo Kexue Jishu Daxue Xuebao,1998,28,368.
107 Baohua Qian, Studies on Chemical Oscillation in NH_2CH_2COOH-CH_3COCH_3-KBrO_3MnSO_4-H_2SO_4 System by Spectrophotometric Method, Journal of Huaihai Institute of Technology, 1998,3,37.
108 Tinxian Tao, Oscillation Reaction in Tartaric Acid-KBrO_3-MnSO_4-H_2SO_4-Propanone System, Anhui Shida Xuebao,1997,20,291.
109 Guozhi Lu, Yuncheng Cui, Renzhang Wang, Yanfei Xu, and Na Miao,The Oscillatory Reaction of Organic Complex Compound,Songliao Xuekan,1998,1,53.
110 Guozhi Lu, Renzhang Wang, Yuncheng Cui, Ying Lan, and Bin Zhang, The Oscillatory Reaction of Organic Complex Compound, Songliao Xuekan, 1997,1,57.
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81 徐志强，谢复新，杨光，倪诗圣，大环四烯镍催化溴酸氧化丙酮酸的振荡化学反应，无机化学学报，1994，10，75．
82 缪静琪，李湘如，B-Z反应对Ki(T)的影响行为，物理化学学报，1989，5，726．
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86 徐济德，倪诗圣，BZ反应体系极限环行为的实验描述，安徽大学学报，1986，1，31．
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88 Jinzhang Gao, Hua Yang, Xiuhui Liu, Jie Ren, Qizhi Li and Jingwan Kang, Determination of glutamic acid by an oscillating chemical reaction using the analyte pulse perturbation technique, Talanta, 2002,57,105.
89 Olson, D.L., and Scheeline, A., Theoretical investigation of the peroxidase-oxidase chemical oscillator for quantitative enzyme analysis, Anal. Chim. Acta., 1990,237,381.
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103 Guozhi Lu, Yuncheng Cui, and Renzhang Wang, The Oscillatory Reaction Using LLeucine as Organic Compound, Songliao Xuekan, 2000,2,37.
104 Ruxiu Cai, Ke Zhang, Wanhong Ma, Nanqing Gan, and Zhixin Lin, Nonlinear Chemical Reaction Characteristics of Diacetone-Malic Acid-BrO_3~--Mn~(2+)-H_2SO_4 and the Application in Biological Antioxidation, Fuzhou Daxue Xuebao,1999,27,249.
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108 Tinxian Tao, Oscillation Reaction in Tartaric Acid-KBrO_3-MnSO_4-H_2SO_4-Propanone System, Anhui Shida Xuebao,1997,20,291.
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