移动反应界面（MRB）的计算机模拟
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摘要
从1970年开始,移动反应界面(MRB)就成了生化分析领域中的一个研究热点,运用MRB理论,在毛细管电泳(CE)中分离和富集各种分析物的研究也取得了很大的进展,但是直到目前为止,对于移动反应界面的数学理论模型的研究依然还有所欠缺。
本论文首先对不同类型的移动反应界面理论以及相关研究历史背景进行简要的介绍,然后着重介绍两种类型的移动反应界面:基于EDTA与金属离子络合反应形成的移动络合界面(MCB)以及由强弱电解质形成的移动中和界面(MNB)。
根据不同的反应体系理论,以及一些相关的电泳动力学方程和电化学方程,本论文开发出相应的软件来模拟移动反应界面。对于移动络合界面MCB,编写的模拟软件可以:(1)动态模拟实验条件下的整个MCB反应和形成的过程,特征峰型以及实验结果。(2)定量计算生成的络合物浓度,相应的界面速度(包括移动络合界面MCB与络合物迁移界面CB),以及所有物质浓度和金属离子的富集效率。所有模拟结果与相应的实验结果吻合较好。因此,本论文开发的软件可以用于预测相关基于EDTA的络合作用来富集金属离子的实验结果并对实验条件进行优化。
对于移动衍生中和界面(dMNB),之前的MNB理论及公式对于反应界面的移动速度的计算存在较大的误差,而根据我们计算机模拟得到的结果与原来的理论相比对于实际实验的吻合度大大提高,这不仅验证了我们理论的正确性,而且该模型及其方法的建立,对于利用毛细管电泳法进行预测和设计样品的富集,具有非常重要的意义。
在移动界面的研究中,Kohlrausch调整函数(KRF)是一个十分重要的数学工具。本文中对移动反应界面的模拟都用到了KRF函数及其相应的衍生函数,模拟结果的正确性也验证了KRF函数对于移动反应界面同样是适用的,在本文中我们将揭示KRF函数及其衍生函数与移动反应界面之间的理论联系:它可以从移动反应界面的理论数学推导出来,但是应当注意它也有一个关键的使用条件,即界面速度不等于0,这些发现已经通过一些理论模拟与实际实验得到证实。
Since 1970, the research for moving reaction boundary has become a hotspot in the analytical chemistry field. By using the theory of MRB, the research for the separation and stacking of samples in the capillary electrophoresis (CE) has been developed. However, up to now, there are only a few reports for the research of mathematical model of MRB.
In this paper, we will first introduce different kinds of MRB theory and the development for the research history. Then we will emphasize on the theories of two kinds of MRB: moving chelation boundary (MCB) based on the continuous sample sweeping for metal ions with EDTA; and moving neutralization boundary (MNB) formed with strong or weak electrolytes.
According to the different theories of MRB system, as well as some related equations for the electrochemistry and dynamics of electrophoresis, corresponding computer softwares can be developed for the simulation of MRB. For the MCB system, the program we compiled can: (1) simulate a dynamic process, characteristic peak shape and relevant electrophoregram of a MCB; (2) quantitatively compute velocities of MRB and complex boundary (CB), all of ionic concentrations (especially the concentration of complex) and sweeping efficiency. These simulation results mentioned above are generally in accordance with the experiments. The simulation software holds evident significances for the study on a MCB and conditional optimization in such an EDTA- based sample sweeping of metal ion in CE.
As for the derivative moving neutralization boundary (dMNB), we found that there are evident systemic errors between the experimental results and theoretical calculations with the original MNB theory. On the contrary, the experiments have much higher agreements with these simulating results relied on the model of derivative MNB theory, which proves the validity of dMNB. And the model of derivative MNB as well as the relative theoretical procedures holds evident significance for the design of new methods for seperation and enrichment of samples in electrophoresis including CE.
Kohlrausch’s regulating function (KRF) plays an important role in the research for moving boundary system. The KRF and its derivative function are used in our simulating programs for both MCB and dMNB. And the simulating results have good agreements with experimental results, which indicated the KRF can be applied in MRB system. In this paper, we reveal that the KRF can be derived from MRB theory. However, it must be paid great attention that KRF should be applied under the condition of nonzero boundary velocity. The theoretical relation is verified by some experimental and simulating results.
本论文首先对不同类型的移动反应界面理论以及相关研究历史背景进行简要的介绍,然后着重介绍两种类型的移动反应界面:基于EDTA与金属离子络合反应形成的移动络合界面(MCB)以及由强弱电解质形成的移动中和界面(MNB)。
根据不同的反应体系理论,以及一些相关的电泳动力学方程和电化学方程,本论文开发出相应的软件来模拟移动反应界面。对于移动络合界面MCB,编写的模拟软件可以:(1)动态模拟实验条件下的整个MCB反应和形成的过程,特征峰型以及实验结果。(2)定量计算生成的络合物浓度,相应的界面速度(包括移动络合界面MCB与络合物迁移界面CB),以及所有物质浓度和金属离子的富集效率。所有模拟结果与相应的实验结果吻合较好。因此,本论文开发的软件可以用于预测相关基于EDTA的络合作用来富集金属离子的实验结果并对实验条件进行优化。
对于移动衍生中和界面(dMNB),之前的MNB理论及公式对于反应界面的移动速度的计算存在较大的误差,而根据我们计算机模拟得到的结果与原来的理论相比对于实际实验的吻合度大大提高,这不仅验证了我们理论的正确性,而且该模型及其方法的建立,对于利用毛细管电泳法进行预测和设计样品的富集,具有非常重要的意义。
在移动界面的研究中,Kohlrausch调整函数(KRF)是一个十分重要的数学工具。本文中对移动反应界面的模拟都用到了KRF函数及其相应的衍生函数,模拟结果的正确性也验证了KRF函数对于移动反应界面同样是适用的,在本文中我们将揭示KRF函数及其衍生函数与移动反应界面之间的理论联系:它可以从移动反应界面的理论数学推导出来,但是应当注意它也有一个关键的使用条件,即界面速度不等于0,这些发现已经通过一些理论模拟与实际实验得到证实。
Since 1970, the research for moving reaction boundary has become a hotspot in the analytical chemistry field. By using the theory of MRB, the research for the separation and stacking of samples in the capillary electrophoresis (CE) has been developed. However, up to now, there are only a few reports for the research of mathematical model of MRB.
In this paper, we will first introduce different kinds of MRB theory and the development for the research history. Then we will emphasize on the theories of two kinds of MRB: moving chelation boundary (MCB) based on the continuous sample sweeping for metal ions with EDTA; and moving neutralization boundary (MNB) formed with strong or weak electrolytes.
According to the different theories of MRB system, as well as some related equations for the electrochemistry and dynamics of electrophoresis, corresponding computer softwares can be developed for the simulation of MRB. For the MCB system, the program we compiled can: (1) simulate a dynamic process, characteristic peak shape and relevant electrophoregram of a MCB; (2) quantitatively compute velocities of MRB and complex boundary (CB), all of ionic concentrations (especially the concentration of complex) and sweeping efficiency. These simulation results mentioned above are generally in accordance with the experiments. The simulation software holds evident significances for the study on a MCB and conditional optimization in such an EDTA- based sample sweeping of metal ion in CE.
As for the derivative moving neutralization boundary (dMNB), we found that there are evident systemic errors between the experimental results and theoretical calculations with the original MNB theory. On the contrary, the experiments have much higher agreements with these simulating results relied on the model of derivative MNB theory, which proves the validity of dMNB. And the model of derivative MNB as well as the relative theoretical procedures holds evident significance for the design of new methods for seperation and enrichment of samples in electrophoresis including CE.
Kohlrausch’s regulating function (KRF) plays an important role in the research for moving boundary system. The KRF and its derivative function are used in our simulating programs for both MCB and dMNB. And the simulating results have good agreements with experimental results, which indicated the KRF can be applied in MRB system. In this paper, we reveal that the KRF can be derived from MRB theory. However, it must be paid great attention that KRF should be applied under the condition of nonzero boundary velocity. The theoretical relation is verified by some experimental and simulating results.
引文
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