Improved gate effect enantioselectivity of phenylalanine-imprinted polymers in water by blending crosslinkers
Improved gate effect enantioselectivity of phenylalanine-imprinted polymers in water by blending crosslinkers
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DOI：
10.1016/j.aca.2015.01.001
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发表时间：
2015-03-03
影响因子：
6.2
通讯作者：
Ishii, Noriyuki
中科院分区：
文献类型：
--
作者：
Yoshimi, Yasuo;Ishii, Noriyuki
在这项工作中，与分子印迹聚合物（MIP）接枝通过疏水性乙二醇二甲基丙烯酸酯（EDMA）和亲水性亚甲基双丙烯酰胺（MBAA）的组合交联的电极上的阳极电流被发现表现出对苯丙氨酸模板在水溶液中的对映体选择性的敏感性。用EDMA和MBAA的2：1混合物交联的MIP接枝电极被观察到以最高的对映体选择性响应于模板，使得由印迹模板诱导的电流变化是由模板的对映体诱导的电流变化的四倍以上。使用最佳交联剂混合比制备的MIP涂覆的电极上的水滴的接触角也对模板敏感，并再次表现出手性选择性。由模板诱导的接触角的变化是从模板的对映体获得的接触角的变化的两倍多。原子力显微镜显示，使用交联剂的混合物制造的MIP层的表面比用单一交联剂制成的更粗糙，尽管该层的粗糙度和对映选择性之间没有明显的相关性。这些结果表明，交联剂的适当组合能够通过调节MIP层的柔性和亲水性来实现手性选择性栅极效应。因此，本文所述的方法代表了通过共混具有不同化学性质的交联剂来改善MIP的选择性的新手段。(C)2015 Elsevier B.V.版权所有。
In this work, the anodic current at an electrode grafted with a molecularly imprinted polymer (MIP) crosslinked via a combination of hydrophobic ethyleneglycol dimethacrylate (EDMA) and hydrophilic methylene bisacrylamide (MBAA) was found to exhibit enantioselective sensitivity to the phenylalanine template in aqueous solution. An MIP-grafted electrode crosslinked with a 2: 1 mixture of EDMA and MBAA was observed to respond to the template with the highest enantioselectivity, such that the change in current induced by the imprinted template was more than four times that induced by the enantiomer of the template. The contact angle of a water droplet on an MIP-coated electrode prepared using the optimal crosslinker blending ratio was also sensitive to the template and again exhibited chiral selectivity. The change in the contact angle induced by the template was more than twice as large as that obtained from the template's enantiomer. Atomic force microscopy showed that the surface of the MIP layer fabricated using a mixture of crosslinkers was rougher than that made with a single crosslinking agent, although there was no apparent correlation between the roughness and the enantioselectivity of the layer. These results indicate that the appropriate combination of crosslinkers enables the chiral-selective gate effect by modulating the flexibility and hydrophilicity of the MIP layer. The approach described herein therefore represents a new means of improving the selectivity of MIPs by blending crosslinkers having different chemical properties. (C) 2015 Elsevier B.V. All rights reserved.