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以齐墩果酸(OA)为模板分子,三氟甲基丙烯酸(TFMAA)、α-甲基丙烯酸(MAA)、丙烯酰胺(AM)、4-乙烯基吡啶(4-VP)为功能单体,三氯甲烷、四氢呋喃、乙醇、甲醇和丙酮为溶剂,基于量子化学密度泛函理论(DFT)和ONIOM方法,采用Gaussian09软件模拟计算了模板分子与不同功能单体的印迹聚合物预组装体系的构型,探讨了模板分子与功能单体在不同印迹比例时所形成复合物的成键情况以及反应过程中的结合能,并采用自洽反应场极化连续模型(CPCM)计算了功能单体与模板分子在不同溶剂中的溶剂化能。结果表明,TFMAA与模板分子OA以1:1摩尔比形成复合物的结合能ΔE最高(-70.99kJ·mol~(-1)),结构最稳定,模板分子和功能单体在三氯甲烷中的溶剂化能最小。同时,采用实验方法验证模拟结果,并利用扫描电镜、傅里叶红外光谱仪和静态吸附实验对印迹聚合物的形貌、化学基团和吸附性能等进行表征。结果表明,模拟结果与实验结果完全一致,计算机模拟对分子印迹体系的筛选和机理研究提供了理论依据。
Using OA (oleanolic acid) as the template molecule, trimethylacrylate (TFMAA), α-methacrylic acid (MAA), acrylamide (AM) and 4-vinylpyridine , Chloroform, tetrahydrofuran, ethanol, methanol and acetone were used as solvent. Based on Quantum Chemical Density Functional Theory (DFT) and ONIOM method, Gaussian09 software was used to simulate the interaction between template molecules and different functional monomers The formation and bonding of the complex formed by the template molecule and the functional monomer at different imprinting ratios were discussed. The binding energy of the complex formed during the reaction was also investigated. The functional monomer Solvation energy of template molecules in different solvents. The results showed that the highest binding energy ΔE (-70.99 kJ · mol -1) of the complexes formed by TFMAA and the template molecule OA in 1: 1 molar ratio was the most stable. The template and the functional monomer in chloroform The solvation energy is the smallest. At the same time, the experimental results were used to verify the simulation results. The morphology, chemical groups and adsorption properties of the imprinted polymer were characterized by SEM, FTIR and static adsorption experiments. The results show that the simulation results are in good agreement with the experimental results, and the computer simulation provides a theoretical basis for the screening and mechanism study of molecular imprinting system.