四氮杂大环金属配合物催化的化学振荡体系在药物分析中的应用
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摘要
化学振荡可以直观的展现自然界中存在的非线性非平衡现象,近年来引起了广大科学工作者的普遍关注和研究。目前,对振荡化学的研究主要集中在新型化学振荡器的设计、机理模型的研究以及振荡体系在分析检测中的应用这几个方面。本文建立了一种新型的溴酸盐振荡体系,研究了三种药物对该振荡体系的干扰影响。
首先,按文献方法合成了四氮杂大环铜配合物[CuL](C104)2 (L为5,7,7,12,14,14-六甲基-1,4,8,11-四氮环杂十四-4,11-二烯),然后以该四氮杂大环铜配合物为催化剂,以苹果酸为有机底物,建立了一个稳定的溴酸盐振荡体系：NaBrO3-苹果酸-[CuL](ClO4)2-H2SO4。接着研究了异丙肾上腺素、左旋多巴、对氨基水杨酸钠对该振荡体系的干扰影响。在研究异丙肾上腺素对该化学振荡体系的扰动时发现,异丙肾上腺素的加入明显改变了振荡体系的周期和振幅,并且浓度与振幅的改变值△A呈现良好的线性关系,由此,我们建立了一种化学振荡法测定异丙肾上腺素含量的方法。同时研究了该振荡体系和异丙肾上腺素之间的作用机理。
在研究左旋多巴对四氮杂大环催化的化学振荡体系的扰动时,发现在铂电极指示电位最低点注入左旋多巴溶液,振幅突然增大,而后又迅速回到原来状态,继续振荡。在9.90×10-6-2.44×10-4mol/L范围内,浓度的对数值和振幅的改变值△A呈现良好的线性关系,相关系数为0.9933。由此,我们建立了一种化学振荡法测定左旋多巴含量的方法,同时研究了该振荡体系和左旋多巴之间的作用机理。
在研究对氨基水杨酸钠对四氮杂大环催化的化学振荡体系的扰动时,建立了一种化学振荡法测定对氨基水杨酸钠含量的方法。当对氨基水杨酸钠浓度在4.97×10-7-1.96×10mol/L范围内,浓度的对数值和振幅的改变值成良好的线性关系,相关系数为0.9915,检测下限为1.96 x 10-7mol/L。同时考察了一些常见离子的干扰,最后研究了该振荡体系和对氨基水杨酸钠可能的作用机理。
Chemical oscillation could reveal the phenomenon of nonlinearity and nonequilibrium which existed in the nature, and it has attracted considerable attention and extensive study of researchers in recent years. At present, the research for the oscillation chemistry mainly focus on the design of new oscillator, the upbuild of mechanism model and the application on the analytical determination. In this paper, we set up a new bromate oscillating system which involves macrocyclic complex [CuL](ClO4)2 as catalyst and malic acid as organic substrate, and studied the disturbing effect of medicine on this system.
Firstly, The catalyst macrocyclic complex [CuL](ClO4)2 was synthesized according to literature and was identified by I.R. spectrum and elemental analyses. The ligand L in the complex is 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetra deca-4,11-dine. Then, the stable bromate oscillating system:NaBrO3-malic acid-[CuL](ClO4)2-H2S04 was established. When the Isoproterenol was injected into the system, it disturbs the oscillation and results in an increaser oscillation amplitude. The change of the oscillating amplitude is linearly proportional to the logarithm of the Isoproterenol. A new analytical method for the determination of Isoproterenol was proposed. The possible perturbation mechanism of Isoproterenol on the oscillating system is also discussed.
The effect of the Levodopa on the [CuL](ClO4)2-catalyzed oscillating reaction was studied. When the Levodopa was injected into the system at the bottom of the potentionmetric cycle, the potential dropped gradually to a minimum and then increased sharply to normal oscillation. In the range of 9.90×10-6 to 2.44×10-4 M, the concentration of Levodop was linear to the change of amplitude with a correlation coefficient of 0.9933. A new analytical method for the determination of Levodopa was proposed.
A novel methodological approach for the determination of PAS-Na based on its perturbation effect on [CuL](ClO4)2-catalyzed oscillating reaction was proposed. Under the optimal conditions, different of PAS-Na concentrations were injected into the system. The results show that the changes of the oscillating amplitude is linearly proportional to the PAS-Na concentration in the range 4.97×10-7 to 1.96×10-4 M, with the correlation coefficient being 0.9915. The detection limit is 1.96×10-7 M. And the effects of some foreign species were studied.
首先,按文献方法合成了四氮杂大环铜配合物[CuL](C104)2 (L为5,7,7,12,14,14-六甲基-1,4,8,11-四氮环杂十四-4,11-二烯),然后以该四氮杂大环铜配合物为催化剂,以苹果酸为有机底物,建立了一个稳定的溴酸盐振荡体系：NaBrO3-苹果酸-[CuL](ClO4)2-H2SO4。接着研究了异丙肾上腺素、左旋多巴、对氨基水杨酸钠对该振荡体系的干扰影响。在研究异丙肾上腺素对该化学振荡体系的扰动时发现,异丙肾上腺素的加入明显改变了振荡体系的周期和振幅,并且浓度与振幅的改变值△A呈现良好的线性关系,由此,我们建立了一种化学振荡法测定异丙肾上腺素含量的方法。同时研究了该振荡体系和异丙肾上腺素之间的作用机理。
在研究左旋多巴对四氮杂大环催化的化学振荡体系的扰动时,发现在铂电极指示电位最低点注入左旋多巴溶液,振幅突然增大,而后又迅速回到原来状态,继续振荡。在9.90×10-6-2.44×10-4mol/L范围内,浓度的对数值和振幅的改变值△A呈现良好的线性关系,相关系数为0.9933。由此,我们建立了一种化学振荡法测定左旋多巴含量的方法,同时研究了该振荡体系和左旋多巴之间的作用机理。
在研究对氨基水杨酸钠对四氮杂大环催化的化学振荡体系的扰动时,建立了一种化学振荡法测定对氨基水杨酸钠含量的方法。当对氨基水杨酸钠浓度在4.97×10-7-1.96×10mol/L范围内,浓度的对数值和振幅的改变值成良好的线性关系,相关系数为0.9915,检测下限为1.96 x 10-7mol/L。同时考察了一些常见离子的干扰,最后研究了该振荡体系和对氨基水杨酸钠可能的作用机理。
Chemical oscillation could reveal the phenomenon of nonlinearity and nonequilibrium which existed in the nature, and it has attracted considerable attention and extensive study of researchers in recent years. At present, the research for the oscillation chemistry mainly focus on the design of new oscillator, the upbuild of mechanism model and the application on the analytical determination. In this paper, we set up a new bromate oscillating system which involves macrocyclic complex [CuL](ClO4)2 as catalyst and malic acid as organic substrate, and studied the disturbing effect of medicine on this system.
Firstly, The catalyst macrocyclic complex [CuL](ClO4)2 was synthesized according to literature and was identified by I.R. spectrum and elemental analyses. The ligand L in the complex is 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetra deca-4,11-dine. Then, the stable bromate oscillating system:NaBrO3-malic acid-[CuL](ClO4)2-H2S04 was established. When the Isoproterenol was injected into the system, it disturbs the oscillation and results in an increaser oscillation amplitude. The change of the oscillating amplitude is linearly proportional to the logarithm of the Isoproterenol. A new analytical method for the determination of Isoproterenol was proposed. The possible perturbation mechanism of Isoproterenol on the oscillating system is also discussed.
The effect of the Levodopa on the [CuL](ClO4)2-catalyzed oscillating reaction was studied. When the Levodopa was injected into the system at the bottom of the potentionmetric cycle, the potential dropped gradually to a minimum and then increased sharply to normal oscillation. In the range of 9.90×10-6 to 2.44×10-4 M, the concentration of Levodop was linear to the change of amplitude with a correlation coefficient of 0.9933. A new analytical method for the determination of Levodopa was proposed.
A novel methodological approach for the determination of PAS-Na based on its perturbation effect on [CuL](ClO4)2-catalyzed oscillating reaction was proposed. Under the optimal conditions, different of PAS-Na concentrations were injected into the system. The results show that the changes of the oscillating amplitude is linearly proportional to the PAS-Na concentration in the range 4.97×10-7 to 1.96×10-4 M, with the correlation coefficient being 0.9915. The detection limit is 1.96×10-7 M. And the effects of some foreign species were studied.
引文
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