基于模拟体系定量构效（QSAR）与传质模型和动力学分析的黄连解毒汤超滤机理研究
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摘要
本课题尝试将系统模拟的方法和化工过程控制原理引入中药水提液复杂体系的膜工艺研究,将复方中若干主要指标成分及淀粉、果胶、蛋白质等“共性高分子物质”建立两大类不同模拟体系,分别研究其膜过程,探索建立相对可靠和准确的中药药效物质超滤膜透过/截留率的定量构效关系模型,及“共性高分子物质”在膜分离过程的迁移表现,建立相关传递数学模型。为探讨中药水提液超滤机理,对中药膜技术应用系统进行优化设计奠定了基础。
首先以黄连解毒汤中生物碱、环烯醚萜两大类主要药效物质为研究对象,优选偏最小二乘法(PLS)、支持向量机(SVM)、人工神经网络(ANN)等数据挖掘方法作为建模方法,初步建立了五种超滤膜相对可靠和准确的定量构效关系模型。从入选模型的参数可以看出,在超滤膜分离化合物的过程中,影响透过率的因素主要包括化合物的自身性质(包括得失电子能力、亲水/疏水性)与膜性质的相互作用以及化合物的空间结构。
接下来以中药水提液中淀粉、果胶、蛋白质这三种共性高分子物质为研究对象,建立了三种高分子物质模拟体系七种膜的超滤传质模型,对膜过程的浓差极化阻力进行了定量描述,研究了操作压力对高分子物质膜通量和过滤阻力的影响,并对超滤过程动力学行为进行了分析。探讨共性高分子溶液的传质机理和中药水提液超滤过程中造成膜污染的物质基础,为开展膜分离技术应用系统优化设计提供依据。
第三部分对淀粉、果胶、蛋白质三种高分子物质的模拟体系在七种超滤膜上的静态吸附行为进行考察,建立了静态吸附模型,分析比较了这几种共性高分子物质在不同材质及孔径膜上的吸附特性和差异。实验结果表明淀粉、果胶、蛋白质在聚砜、聚醚砜、聚偏氟乙烯三种常用材质的超滤膜上均存在吸附污染,静态吸附均符合Langmuir吸附模型,吸附主要发生在前40min。膜材质对吸附量影响不大,淀粉、果胶在三种不同截留分子量的膜上的吸附量无明显差异;但蛋白质在三种孔径膜上的吸附量随着膜孔径的增大而增大。
最后,在上述研究基础上,依据黄连解毒汤复方中主要药效物质及高分子物质的含量建立模拟体系,对模拟体系膜过程进行研究,以膜过程中通量变化、膜污染度、截留率、小分子物质吸附速率和吸附量等为指标,研究黄连解毒汤复方中高分子物质对小分子药效物质膜过程的影响。研究表明黄连解毒汤中代表性药效物质小檗碱和栀子苷这两种小分子物质的膜透过率较高,但由于高分子物质的存在,与小分子药效物质间产生相互作用、膜过程浓差极化层和凝胶层的形成等因素造成了小分子药效物质的大量损失。黄连解毒汤模拟体系中造成膜污染和通量衰减的主要物质是淀粉和果胶这两种高分子物质。
本文主要创新点:(1)首次将有机化学中定量构效关系研究方法和信息科学中数据挖掘等技术手段引入中药超滤膜分离技术机理研究,初步建立相对可靠和准确的中药药效物质超滤膜透过/截留率的定量构效关系模型。从中药药效物质分子结构的角度探索其截留机理,将中药超滤膜分离技术的研究提高到微观与定量的层次。(2)首次对中药水提液中共性高分子物质进行系统研究,建立了淀粉、果胶、蛋白质三种物质不同膜超滤过程的传质模型、动力学模型和静态吸附模型,为探讨中药水提液超滤过程中造成膜污染的物质基础和对中药膜技术应用系统进行优化设计奠定了基础。
本论文的研究意义:(1)初步建立QSAR应用于中药超滤膜分离技术的研究方法,系统深入研究超滤膜对中药药效物质的截留机理,丰富膜科学与技术的理论,为开展膜系列技术(微滤、超滤、纳滤等技术)精制中药的研究奠定基础。(2)探索“化工过程控制”原理在中药膜分离领域的研究模式,为开展膜分离及相关精制技术应用系统优化设计提供依据。
The study try using the method of systerm simulation and Chemical Process Control principle in the membrane process research of Chinese herbal decoction. Index composition and various macromolecule materials commonly existed in Chinese herbal decoctions are set up as two types of model systerm and their membrane process are researched separately. Try to explore the establishment of UF transmission rate QSAR models of Chinese herbal index composition and transfer characteristic of macromolecule materials.
At the beginning of the research, taking Alkaloids and Iridoid these two kinds of compound in Huanglianjiedu Decoction as the study subject, quantitative structure-property relationships in five membranes are developed by the data mining method of PLS or SVM. It shown from the parameters in the models that the main factors which infect the UF transmission rate are interaction of compound property and membrane property and compound spatial structure.
Then taking starch、pectin and protein these three macromolecule materials in Chinese herbal decoctions as the study subject, the mass transfer models of model systerm in seven membranes are formed, the resistances from concent ration polarization were obtained. At the same time kinetics analysis in the ultrafiltration process is studied . The research lays a foundation for the exploring of macromolecule materials transfer mechanism and the substance foudation of membrane fouling, and for the the Optimal Design of ultra-filtration membrane in the production of Chinese drugs preparation.
Part three: Examining the adsorption behavior under static condition of the model systerm of three macromolecule materials in seven UF membranes, setting up adsorption models under static condition, and comparing the adsorption characteristic of the three macromolecule in different membranes. The results show that starch、pectin and protein are all have adsorption fouling in three membranes in common use -PS、PES and PVDF. The adsorption under static condition corresponding in character of Langmuir mode, and the adsorption occur in the first 40 minute. The membrane materials have little effect on the adsorption capacity. There is no significant difference of adsorption capacity of starch and pectin in membranes with different MWCOS. But the adsorption capacity of protein increase as the increasing of membrane MWCOS.
Finally, On the basis of the above study, the UF process of model systerm of Huanglianjiedu Decoction is researched. Using the membrane flux change、the fouling degree of membrane、the preserving degree and adsorption capacity of efficiency components as guide line, trying to find out the influence of macromolecule materials on small molecules in Huanglianjiedu Decoction. The results show that the two small molecules berberine and gardenoside in Huanglianjiedu Decoction have high permeation rate. But for the reasons of interaction of macromolecule materials and small molecules and forming of concentration layer and gel layer, the permeation rate of small molecules reduces greatly. Starch and pectin are the two main macromolecule materials in Huanglianjiedu Decoction which cause membrane fouling and flux falling.
The innovations of this article lie in the following two ways: Firstly, using QSAR and data mining method in the mechanism research of UF technique in Chinese herbal decoction for the first time. Models of quantitative structure-property relationships of effective compounds in Chinese medicine with five membranes are initially developed. Improving the research of UF technology in Chinese herbal decoction to a microcosmic and quantitative level. Secondly, research systematically macromolecule materials commonly existed in Chinese herbal decoctions for the first time, and develop mass transfer models、kinetics models and adsorption models under static condition of starch、pectin and protein. The research lays a foundation for the exploring of the substance foudation of membrane fouling, and for the the optimal design of membrane technology in the production of Chinese drugs preparation.
首先以黄连解毒汤中生物碱、环烯醚萜两大类主要药效物质为研究对象,优选偏最小二乘法(PLS)、支持向量机(SVM)、人工神经网络(ANN)等数据挖掘方法作为建模方法,初步建立了五种超滤膜相对可靠和准确的定量构效关系模型。从入选模型的参数可以看出,在超滤膜分离化合物的过程中,影响透过率的因素主要包括化合物的自身性质(包括得失电子能力、亲水/疏水性)与膜性质的相互作用以及化合物的空间结构。
接下来以中药水提液中淀粉、果胶、蛋白质这三种共性高分子物质为研究对象,建立了三种高分子物质模拟体系七种膜的超滤传质模型,对膜过程的浓差极化阻力进行了定量描述,研究了操作压力对高分子物质膜通量和过滤阻力的影响,并对超滤过程动力学行为进行了分析。探讨共性高分子溶液的传质机理和中药水提液超滤过程中造成膜污染的物质基础,为开展膜分离技术应用系统优化设计提供依据。
第三部分对淀粉、果胶、蛋白质三种高分子物质的模拟体系在七种超滤膜上的静态吸附行为进行考察,建立了静态吸附模型,分析比较了这几种共性高分子物质在不同材质及孔径膜上的吸附特性和差异。实验结果表明淀粉、果胶、蛋白质在聚砜、聚醚砜、聚偏氟乙烯三种常用材质的超滤膜上均存在吸附污染,静态吸附均符合Langmuir吸附模型,吸附主要发生在前40min。膜材质对吸附量影响不大,淀粉、果胶在三种不同截留分子量的膜上的吸附量无明显差异;但蛋白质在三种孔径膜上的吸附量随着膜孔径的增大而增大。
最后,在上述研究基础上,依据黄连解毒汤复方中主要药效物质及高分子物质的含量建立模拟体系,对模拟体系膜过程进行研究,以膜过程中通量变化、膜污染度、截留率、小分子物质吸附速率和吸附量等为指标,研究黄连解毒汤复方中高分子物质对小分子药效物质膜过程的影响。研究表明黄连解毒汤中代表性药效物质小檗碱和栀子苷这两种小分子物质的膜透过率较高,但由于高分子物质的存在,与小分子药效物质间产生相互作用、膜过程浓差极化层和凝胶层的形成等因素造成了小分子药效物质的大量损失。黄连解毒汤模拟体系中造成膜污染和通量衰减的主要物质是淀粉和果胶这两种高分子物质。
本文主要创新点:(1)首次将有机化学中定量构效关系研究方法和信息科学中数据挖掘等技术手段引入中药超滤膜分离技术机理研究,初步建立相对可靠和准确的中药药效物质超滤膜透过/截留率的定量构效关系模型。从中药药效物质分子结构的角度探索其截留机理,将中药超滤膜分离技术的研究提高到微观与定量的层次。(2)首次对中药水提液中共性高分子物质进行系统研究,建立了淀粉、果胶、蛋白质三种物质不同膜超滤过程的传质模型、动力学模型和静态吸附模型,为探讨中药水提液超滤过程中造成膜污染的物质基础和对中药膜技术应用系统进行优化设计奠定了基础。
本论文的研究意义:(1)初步建立QSAR应用于中药超滤膜分离技术的研究方法,系统深入研究超滤膜对中药药效物质的截留机理,丰富膜科学与技术的理论,为开展膜系列技术(微滤、超滤、纳滤等技术)精制中药的研究奠定基础。(2)探索“化工过程控制”原理在中药膜分离领域的研究模式,为开展膜分离及相关精制技术应用系统优化设计提供依据。
The study try using the method of systerm simulation and Chemical Process Control principle in the membrane process research of Chinese herbal decoction. Index composition and various macromolecule materials commonly existed in Chinese herbal decoctions are set up as two types of model systerm and their membrane process are researched separately. Try to explore the establishment of UF transmission rate QSAR models of Chinese herbal index composition and transfer characteristic of macromolecule materials.
At the beginning of the research, taking Alkaloids and Iridoid these two kinds of compound in Huanglianjiedu Decoction as the study subject, quantitative structure-property relationships in five membranes are developed by the data mining method of PLS or SVM. It shown from the parameters in the models that the main factors which infect the UF transmission rate are interaction of compound property and membrane property and compound spatial structure.
Then taking starch、pectin and protein these three macromolecule materials in Chinese herbal decoctions as the study subject, the mass transfer models of model systerm in seven membranes are formed, the resistances from concent ration polarization were obtained. At the same time kinetics analysis in the ultrafiltration process is studied . The research lays a foundation for the exploring of macromolecule materials transfer mechanism and the substance foudation of membrane fouling, and for the the Optimal Design of ultra-filtration membrane in the production of Chinese drugs preparation.
Part three: Examining the adsorption behavior under static condition of the model systerm of three macromolecule materials in seven UF membranes, setting up adsorption models under static condition, and comparing the adsorption characteristic of the three macromolecule in different membranes. The results show that starch、pectin and protein are all have adsorption fouling in three membranes in common use -PS、PES and PVDF. The adsorption under static condition corresponding in character of Langmuir mode, and the adsorption occur in the first 40 minute. The membrane materials have little effect on the adsorption capacity. There is no significant difference of adsorption capacity of starch and pectin in membranes with different MWCOS. But the adsorption capacity of protein increase as the increasing of membrane MWCOS.
Finally, On the basis of the above study, the UF process of model systerm of Huanglianjiedu Decoction is researched. Using the membrane flux change、the fouling degree of membrane、the preserving degree and adsorption capacity of efficiency components as guide line, trying to find out the influence of macromolecule materials on small molecules in Huanglianjiedu Decoction. The results show that the two small molecules berberine and gardenoside in Huanglianjiedu Decoction have high permeation rate. But for the reasons of interaction of macromolecule materials and small molecules and forming of concentration layer and gel layer, the permeation rate of small molecules reduces greatly. Starch and pectin are the two main macromolecule materials in Huanglianjiedu Decoction which cause membrane fouling and flux falling.
The innovations of this article lie in the following two ways: Firstly, using QSAR and data mining method in the mechanism research of UF technique in Chinese herbal decoction for the first time. Models of quantitative structure-property relationships of effective compounds in Chinese medicine with five membranes are initially developed. Improving the research of UF technology in Chinese herbal decoction to a microcosmic and quantitative level. Secondly, research systematically macromolecule materials commonly existed in Chinese herbal decoctions for the first time, and develop mass transfer models、kinetics models and adsorption models under static condition of starch、pectin and protein. The research lays a foundation for the exploring of the substance foudation of membrane fouling, and for the the optimal design of membrane technology in the production of Chinese drugs preparation.
引文
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