文献类型：期刊文献

英文题名：13C NMR aided design of molecularly imprinted adsorbents for selectively preparative separation of erythromycin

作者：Zhang, Yuxin[1,2,3];Qu, Xue[1,3];Yu, Jinpeng[3];Xu, Liancai[4];Zhang, Zhiqiang[4];Hong, Hua[3];Liu, Changsheng[1,2,3]

机构：[1]E China Univ Sci & Technol, State Key Lab Bioreactor Engn, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[3]E China Univ Sci & Technol, Engn Res Ctr Biomed Mat, Minist Educ, Shanghai 200237, Peoples R China;[4]Zhengzhou Univ Light Ind, Dept Mat & Chem Engn, Zhengzhou 450002, Henan, Peoples R China

年份：2014

卷号：2

期号：10

起止页码：1390

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY B

收录：;EI(收录号：20140917378815);WOS:【SCI-EXPANDED(收录号:WOS:000332199900012)】；

基金：We acknowledge the financial support from National Basic Research Program of China (973 Program, 2012CB933600), Shanghai Natural Science Foundation (11ZR1409100), National Natural Science Foundation of China (5110304, U1024209), Innovation Program of Shanghai Municipal Education Commission (14ZZ060) and Fundamental Research Funds for the Central Universities (WD1214056).

语种：英文

外文关键词：Adsorption - Alkalinity - Density functional theory - Separation - Ethylene glycol - Antibiotics - Ethylene - Monomers - Chemical shift - Design for testability - Molecules - Nuclear magnetic resonance spectroscopy - Adsorption isotherms - Chemical analysis - Equilibrium constants

摘要：Molecularly imprinted polymers (MIPs) with high binding performance and good selectivity are of interest not only in the field of analytical chemistry, but also in the bio-pharmaceutical industry because of their potential use as affinity sorbents for selectively preparative separation of drug molecules. The choice of a suitable functional monomer for the template molecule plays a key role in the performance of MIPs. Erythromycin (ERY; C37H67NO13; mol wt 733.9), produced by bio-fermentation, is a representative macrolide antibiotic with multiple polar groups. In the present study, C-13 NMR spectroscopy for the first time was employed to evaluate the interactions between ERY and a set of functional monomers at the atomic level. Based on the C-13 chemical shift changes in the ERY molecular structure when binding with different functional monomers, the optimal monomer of methacrylic acid (MAA) was selected and the rational binding sites were predicted. A sequence regarding the interaction force of these binding sites for MAA was proposed, and Density Functional Theory (DFT) theoretical calculation of Lewis basicity of the O/N atoms located at these sites confirmed its reliability. Molecularly imprinted sorbents (MIAs) for ERY were prepared by a suspension polymerization method using MAA as a functional monomer and ethylene glycol dimethacrylate (EGDMA) as a cross-linker. The effects of the monomer to template ratio and the solvent environment employed during the adsorption on the imprinting efficiency of MIAs were both discussed. The adsorption isotherm of ERY on MIAs was fitted by the Langmuir isotherm model. And the specific selectivity of these materials towards ERY was confirmed. The optimized MIAs as column packing materials can separate ERY from its crystal mother liquid with high recovery and good selectivity, exhibiting a promising capability for productive separation of ERY in a large scale. To the best of our knowledge, these results for the first time indicated that C-13 NMR spectroscopy is a simple and effective method for the rational design of MIAs towards complex template molecules. The separation model built in this study represents a novel application of MIPs for future industrial production.