Origin of macromolecular crowding: Analysis of recognition mechanism of dual-template molecularly imprinted polymers by in silico prediction.
Origin of macromolecular crowding: Analysis of recognition mechanism of dual-template molecularly imprinted polymers by in silico prediction.
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DOI：
10.1016/j.chroma.2021.462695
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发表时间：
2021-12
期刊：
影响因子：
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通讯作者：
Wen-Jing Chen;P. Shang;Sen-Biao Fang;Yanping Huang;Zhaosheng Liu
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文献类型：
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作者：
Wen-Jing Chen;P. Shang;Sen-Biao Fang;Yanping Huang;Zhaosheng Liu
多模板分子印迹技术是分子印迹技术面临的挑战之一，与单模板分子印迹聚合物相比，多模板分子印迹聚合物对每种分析物的选择性和结合亲和力明显降低。本工作尝试利用分子拥挤效应来弥补两种模板竞争导致的印迹降低问题。以甲基丙烯酸（ACR）为功能单体，二甲基丙烯酸乙二酯（EDMA）为交联剂，聚苯乙烯（PS）为大分子拥挤剂。以左氧氟沙星（S-OFX）为第一模板剂，选择多种不同结构的化合物为第二模板剂，研究了双模板剂的印迹效应。当以S-OFX和萘普生（S-NAP）为双模板时，所得分子印迹聚合物对S-OFX的印迹因子（IF）为20.1，对S-NAP的IF为10.9。相比之下，对于单模板MIPs，S-OFX的IF为22.4，S-NAP的IF为11.9。作为比较，在不存在PS的情况下制备的DT-MIP的IF对于S-OFX仅为2.3，对于S-NAP仅为1.0。为了分析分子拥挤印迹体系的识别机理，利用NAMD软件对PS的链结构和模板分子与功能单体的结合方式进行了分子动力学模拟。结果表明，分子拥挤效应是一种很有前途的提高双模板分子印迹聚合物亲和性的方法。
Multi-template imprinting is one of the challenge for molecular imprinting since the selectivity and binding affinity for each analyte decrease significantly compared with the corresponding molecularly imprinting polymers (MIPs) against single template. In this work, molecular crowding effect was tried to remedy the problem of imprinting reduction caused by the competition of two templates. Methacrylic acid (ACR) was used as functional monomer, ethylene dimethacrylate (EDMA) as crosslinker, and polystyrene (PS) as macromolecular crowding agent. With levofloxacin (S-OFX) as the first template, a number of compounds with varied chemical structure were chosen as the second template to investigate the imprinting effect of dual-template. WhenS-OFX and naproxen (S-NAP) was used as the dual-template, the imprinting factor (IF) of the resulting MIP forS-OFX was 20.1 and IF forS-NAP was 10.9. In contrast, for the single-template MIPs, IF forS-OFX was 22.4, and IF forS-NAP was 11.9. As a comparison, the IF of the DT-MIP prepared in absence of PS was only 2.3 forS-OFX and 1.0 forS-NAP. To analyze recognition mechanism of the molecular crowding-based imprinting system, molecular dynamics simulations to the chain structure of PS and binding modes between template and functional monomers was conducted by NAMD software. All the results displayed that molecular crowding is a promising method to improve the affinity of the dual-template imprinted polymer.