摘要
在研究大黄酚分子印迹聚合物制备过程中,为选择合适的功能单体,首先采用PM3量化计算方法,得出大黄酚与4-乙烯吡啶、甲基丙烯酸之间的结合能分别为-768.91 kJ/mol和-14.78 kJ/mol,表明4-乙烯吡啶与大黄酚的作用力更强,是较好的功能单体;又采用紫外预组装的实验方法优化选择功能单体,得出与上述一致的结论;同时实验确定大黄酚与4-乙烯吡啶最佳反应比为1:4。因此,以此单体和反应比去合成大黄酚印迹(MIP)和非印迹聚合物(NMIP),采用平衡吸附实验表征MIP的吸附性能和选择性,并推测其作用机理。结果表明:MIP对大黄酚及结构相似物的分配系数均大于NMIP;MIP对大黄酚的结合容量大大高于NMIP,对大黄酚的分配系数大于其结构类似物;由此说明:合成的MIP具有一定的印迹效果,4-乙烯吡啶与大黄酚(及其类似物)的作用可能产生于羟基蒽醌骨架上。研究表明:实验结果和量化计算具有一致性,量化计算方法对分子印迹聚合物合成时功能单体的选择具有很好的指导作用。
During the preparation of chrysophanol molecularly imprinted polymers, PM3 quantum chemical calculations method was used to optimize fuetional monomer. The binding energy between chrysophanol and 4-vinylpyridine （4-VP） or methyl methacrylate （MAA） was - 768.91 k J/tool and - 14. 78 kJ/mol, respectively. It indicated that the force was stronger between ehrysophanol and 4- VP, so 4-VP was superior to MAA. Then UV spectrum experiment was used to optimize fuctional monomer and the result was consistent with the calculation. Meanwhile, the best mole ratio（ 1：4 ）of template to fuctional monomer is determined by pre-UV spectrum experiment. Chrysophanol imprinted and non-imprinted polymer were thus synthesized by 4-VP according to the best mole ratio. The adsorptivity and selectivity of the MIP were evaluated by equilibrium adsorption and mechanism was speculated. The results showed that the distribution coefficients of MIP to chrysophanol and its analogues were larger than that of NMIP. The binding capacity to ehry- sophanol of MIP was much higher than that of NMIP and the distribution coefficients of MIP to chrysophanol is larger than its ana- logues. It indicated that the MIP possessed imprinted speciality and the interaction between 4-VP and chrysophanol （and its analogues） may occur on the role of the skeleton of hydroxyanthraquinonel. The studies have shown that the experimental results were consistent with quantitative calculation. The quantitative method is a good guidance to choose the functional monomer during the synthesis of MIP.
出处
《计算机与应用化学》
CAS
CSCD
北大核心
2010年第5期668-672,共5页
Computers and Applied Chemistry
基金
河北省科学技术研究与发展指导计划项目(07276464)
邯郸市科学技术研究与发展计划项目(072816058-5)
关键词
量化计算
预组装实验
功能单体
分子印迹聚合物
吸附性能
quantum chemical calculation, assembly experiment, functional monomer, molecularly imprinted polymer, adsorptivity
