摘要
以双氰胺（DCD）为印迹分子，丙烯酰胺（AM）为功能单体，分别以乙二醇双甲基丙烯酸酯（EGDMA）、二乙烯基苯（DVB）、季戊四醇三丙烯酸酯（PETA）和三羟甲基丙烷三甲基丙烯酸酯（TRIM）为交联剂，借助Gaussian09软件，采用密度泛函理论（DFT）M06-2X方法模拟了DCD与AM的预作用构型，筛选最佳印迹物质的量比例；优化交联剂，揭示DCD与AM间印迹作用的本质．理论研究结果表明，最佳印迹物质的量比例为1：5，PETA更适合作为双氰胺分子印迹聚合物（DCD-MIPs）的交联剂．以计算结果为指导采用沉淀聚合法制备了DCD-MIPs，并进行性能研究．紫外光谱实验表明强吸收峰λ=216nm处印迹物质的量比例为1：5的吸光度最大．吸附实验表明在最佳印迹比例时，以PETA为交联剂且使用量为9．5mmol时制备的DCD-MIPs的吸附量最大，其纳米微球平均粒径为185nm．Scatchard分析结果表明，在研究浓度范围内DCD-MIPs对DCD的结合位点是等价的，其最大表观吸附量Qmax为17．24mg／g，离解平衡常数Kd为65．59mg／L．本文制备的DCD-MIPs对DCD展现出较好的吸附性能，可应用于复杂基质中DCD的分离检测．
Dicyandiamide （DCD） was chosen as the template molecule and acrylamide （AM） as the function monomer, and the ethylene glycol dimethacrylate （EGDMA）, divinylbenzene （DVB）, penta- erythritol triacrylate （PETA） and trimethacrylate （TRIM） as the cross-linking agents, the pre-config- uration between DCD and AM has been simulated with the Gaussian 09 software. The best molar im- printed ratio was selected. The cross-linking agent was optimized. The nature of the imprinting reac- tion was also studied. The theoretical results indicated that the molar ratio of reaction for DCD-AM was 1：5. The PETA was the most suitable cross-linking agent in comparison with the other cross- linking agents. Then, the DCD-MIPs were prepared by precipitation polymerization and their proper- ties were studied. The ultraviolet spectral showed that the complex with the molar ratio 1：5 has the largest absorbance at λ = 216 nm. The adsorption experiments showed that the DCD-MIPs have the largest binding capacity when PETA as the cross-linking agent and the application amount of 9.5 mmol with the molar ratio 1：5, and the average diameter was 185 nm. The analysis of the Scatchard plot revealed that the binding sites of DCD-MIPs to DCD were equal class under the studied concentra- tion range, the apparent maximum adsorption quantity （Qmax） was 17. 24 mg/g, and the dissociation constant （Ka） was 65.59 mg/L. The selective adsorption experiment showed that the adsorption ca- pacity of DCD-MIPs to DCD was the largest compared with that of its structural analogue. In this study, the DCD-MIPs demonstrate good adsorption properties to DCD, which can be applied to the separation and detection of DCD in complex matrix.
作者
王岩
刘俊渤
易灵红
戴丽艳
唐珊珊
靳瑞发
WANG Yan;LIU Jun-bo;YI Ling-hong;DAI Li-yan;TANG Shan-shan;JIN Rui-fa(Guangxi Modern Polytechnic College, Hechi 547000, China;College of Resources and Environment, Jilin Agricultural University, Changchun 130118, China;College of Chemistry and Chemical Engineering, Chifeng University, Chifeng 024000, China)
出处
《分子科学学报》
CAS
CSCD
北大核心
2018年第2期103-110,共8页
Journal of Molecular Science
基金
国家自然科学基金资助项目(21302062,21563002)
吉林省自然科学基金资助项目(201359)
吉林省科技发展计划项目(20130206099SF)
关键词
双氰胺
丙烯酰胺
分子印迹聚合物
交联剂
计算模拟
dicyandiamide
acrylamide
molecularly imprinted polymer
cross-linking agent
computa-tional simulation
