咖啡因替代物(茶碱)分子表面印迹材料的制备及其分子识别特性研究  

PREPARATION OF MOLECULARLY SURFACE-IMPRINTED MATERIAL OF CAFFEINE SUBSTITUTION(THEOPHYLLINE) AND ITS MOLECULE RECOGNITION CHARACTER

作　　者：施雪军[1] 高保娇[1] 赵兴龙[1] 

机构地区：[1]中北大学化学工程系,太原030051

出　　处：《高分子学报》2013年第8期1047-1057,共11页Acta Polymerica Sinica

基　　金：山西省自然科学基金(基金号201002100843)资助项目

摘　　要：采用巯基-过氧化苯甲酰(BPO)氧化还原引发体系,先实现了甲基丙烯酸缩水甘油酯(GMA)在微米级硅胶微粒表面的引发接枝聚合,制得接枝微粒PGMA/SiO2.使接枝大分子PGMA的环氧基团与5-氨基水杨酸(ASA)发生开环反应,将水杨酸基团键合在接枝大分子侧链,制得功能接枝微粒SA-PGMA/SiO2,并对其化学结构与表面电性能进行了表征.考察研究了功能微粒SA-PGMA/SiO2与咖啡因替代物茶碱分子之间的相互作用力.研究表明,微粒SA-PGMA/SiO2与茶碱分子之间存在有强的次价键力(静电和氢键相互作用).在此基础上,采用本课题组建立的新型分子表面印迹技术,以咖啡因替代物茶碱为模板分子,乙二醇二缩水甘油醚(EGDE)为交联剂,对接枝在硅胶表面的功能大分子链SA-PGMA进行了交联印迹,制备了茶碱分子表面印迹材料MIP-SAP/SiO2,深入考察研究了其分子识别特性.实验结果表明,相对于两种对照物甘油茶碱和苦参碱,印迹材料MIP-SAP/SiO2对茶碱分子具有特异的识别选择性与优良的结合亲和性,相对于甘油茶碱,印迹材料对茶碱的识别选择性系数为7.72.By adopting sulfydryl-benzoyl peroxide redox initiating system,the surface-initiated graft-polymerization of glycidyl methacrylate(GMA) on micron-sized silica gel particles was first realized,obtaining grafted particles PGMA/SiO2 with a high grafting degree,and then the ring-opening reaction of the epoxy groups of the grafting macromolecule PGMA with 5-aminosalicylic acid(ASA) was carried out,leading to bonding salicylic acid(SA) onto the side chains of the grafting macromolecule PGMA and resulting in the functional grafting particles SA-PGMA/SiO2.The chemical structure and surface-electrical property of SA-PGMA/SiO2 particles were characterized.The interaction between the functional grafting particles SA-PGMA/SiO2 and theophylline molecule as the substitute of caffeine was examined in depth.The investigation result shows that there exist strong secondary bond forces between the functional grafting particles SA-PGMA/SiO2 and theophylline molecules,including electrostatic interaction and hydrogen bonding.On that basis,the molecular imprinting towards the grafted SA-PGMA was performed with theophylline as template molecule and ethylene glycol diglycidyl ether(EGDE) as crosslinking agent by using the novel surface-molecular imprinting technique established by our research group,and the theophylline molecule-imprinted material MIP-SAP/SiO2 was prepared.With diprophylline and matrine as two contrast compounds,both static and dynamic methods were adopted to investigate the binding properties and molecule recognition character of MIP-SAP/SiO2 for theophylline molecule.The experiment results show that MIP-SAP/SiO2 have specific recognition selectivity and excellent binding affinity for theophylline.Relative to the contrast substance,diprophylline,the coefficient of recognition selectivity of the imprinted material MIP-SAP/SiO2 for theophylline is equal to 7.72,displaying excellent recognition selectivity for the template molecule.

关 键 词：聚甲基丙烯酸缩水甘油酯 硅胶 表面印迹 咖啡因替代物 分子识别 

分 类 号：O631.3[理学—高分子化学]