Fabrication of polymeric electron-transfer mediator/enzyme hydrogel multilayer on an Au electrode in a layer-by-layer process.
Fabrication of polymeric electron-transfer mediator/enzyme hydrogel multilayer on an Au electrode in a layer-by-layer process.
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DOI：
10.1016/j.bios.2012.01.042
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发表时间：
2012-04
影响因子：
12.6
通讯作者：
Ziyin Li;T. Konno;M. Takai;K. Ishihara
中科院分区：
文献类型：
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作者：
Ziyin Li;T. Konno;M. Takai;K. Ishihara
研究了由聚合物电子传递介质和聚合物修饰酶交替组成的多层结构覆盖的酶电极的逐层结构。合成了聚（2-甲基丙烯酰氧乙基磷酸胆碱-co-p-乙烯基苯基硼酸-co-乙烯基二茂铁）（PMVF），并将其用作聚合物电子传递介质。选择葡萄糖氧化酶（GOx）作为模型酶，在温和条件下将聚乙烯醇（PVA）链与GOx （GOx-PVA）结合。PMVF和PVA通过两种聚合物中苯硼酸单元和羟基之间的选择性反应自发形成凝胶。利用自旋镀膜技术，在Au电极表面制备了一层重复的PMVF/GOx-PVA多层膜。PMVF/GOx- pva各层厚度在5.8nm左右，与GOx的尺寸相对应。在葡萄糖浓度测量中评价了电极的电化学性能。葡萄糖被GOx氧化的电流为0.38V（相对于Ag/AgCl），验证了水凝胶PMVF中的二茂铁单元将固定的GOx电连接起来。此外，电流随PMVF/GOx-PVA层数的增加而增加。也就是说，每个单独层之间的分子间电子转移和水凝胶中自由扩散的底物的存在都实现了。我们得出结论，由PMVF和pva修饰的酶构建的LBL结构可以有效地用于开发使用酶分子的生物电子器件。
The layer-by-layer (LBL) construction of an enzyme electrode covered with a multilayer structure alternately composed of a polymeric electron transfer mediator and a polymer-modified enzyme was examined. Poly(2-methacryloyloxyethyl phosphorylcholine-co-p-vinylphenylboronic acid-co-vinylferrocene) (PMVF) was synthesized and used as a polymeric electron transfer mediator. Glucose oxidase (GOx) was selected as a model enzyme and poly(vinyl alcohol) (PVA) chains were bound to the GOx (GOx-PVA) under mild conditions. The PMVF and PVA formed a gel spontaneously through a selective reaction between phenylboronic acid units and hydroxyl groups in both polymers. Using the spin coating technique, a repeating PMVF/GOx-PVA multilayer was fabricated on the surface of an Au electrode. The thickness of each PMVF/GOx-PVA layer was around 5.8nm, corresponding to the dimensions of GOx. The electrochemical performance of the electrode was evaluated in glucose concentration measurement. The oxidation current of glucose by GOx was measured at 0.38V (vs. Ag/AgCl), verifying that ferrocene units in the PMVF of the hydrogel electrically wired the immobilized GOx. Moreover, the current increased with the number of PMVF/GOx-PVA layers. That is, both intermolecular electron transfer between each individual layer and the presence of a freely diffusing substrate in the hydrogel were achieved. We conclude that a LBL structure constructed from PMVF and a PVA-modified enzyme is effective for use in developing bioelectronic devices that employ enzyme molecules.