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用于葡萄糖生物传感器的氧化还原聚合物纳米珠和纳米复合材料的合成。

Synthesis of redox polymer nanobeads and nanocomposites for glucose biosensors.

机构信息

Institute of Polymer Science and Engineering, National Taiwan University, Taipei 10617, Taiwan.

出版信息

ACS Appl Mater Interfaces. 2013 Aug 28;5(16):7852-61. doi: 10.1021/am4018219. Epub 2013 Aug 7.

DOI:10.1021/am4018219
PMID:23845050
Abstract

Redox polymer nanobeads of branched polyethylenimine binding with ferrocene (BPEI-Fc) were synthesized using a simple chemical process. The functionality and morphology of the redox polymer nanobeads were investigated by Fourier transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). This hydrophilic redox nanomaterial could be mixed with glucose oxidase (GOx) for drop-coating on a screen-printed carbon electrode (SPCE) for glucose sensing application. Electrochemical properties of the BPEI-Fc/GOx/SPCE prepared under different conditions were studied by cyclic voltammetry (CV). On the basis of these CV results, the synthetic condition of the BPEI-Fc/GOx/SPCE could be optimized. By incorporating conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), the performance of a redox polymer nanobead–based enzyme electrode could be further improved. The influence of PEDOT:PSS on the nanocomposite enzyme electrode was discussed from the aspects of the apparent electron diffusion coefficient (D(app)) and the charge transfer resistance (R(ct)). The glucose-sensing sensitivity of the BPEI-Fc/PEDOT:PSS/GOx/SPCE is calculated to be 66 μA mM(–1) cm(–2), which is 2.5 times higher than that without PEDOT:PSS. The apparent Michaelis constant (K(M)(app)) of the BPEI-Fc/PEDOT:PSS/GOx/SPCE estimated by the Lineweaver–Burk plot is 2.4 mM, which is much lower than that of BPEI-Fc/GOx/SPCE (11.2 mM). This implies that the BPEI-Fc/PEDOT:PSS/GOx/SPCE can catalytically oxidize glucose in a more efficient way. The interference test was carried out by injection of glucose and three common interferences: ascorbic acid (AA), dopamine (DA), and uric acid (UA) at physiological levels. The interferences of DA (4.2%) and AA (7.8%) are acceptable and the current response to UA (1.6%) is negligible, compared to the current response to glucose.

摘要

采用简单的化学过程合成了具有二茂铁(Fc)的支化聚乙烯亚胺(BPEI-Fc)的氧化还原聚合物纳米珠。通过傅里叶变换红外光谱(FTIR)和透射电子显微镜(TEM)研究了氧化还原聚合物纳米珠的功能和形态。这种亲水性氧化还原纳米材料可与葡萄糖氧化酶(GOx)混合,用于在丝网印刷碳电极(SPCE)上滴涂,用于葡萄糖传感应用。通过循环伏安法(CV)研究了在不同条件下制备的 BPEI-Fc/GOx/SPCE 的电化学性质。基于这些 CV 结果,可以优化 BPEI-Fc/GOx/SPCE 的合成条件。通过掺入导电聚(3,4-亚乙基二氧噻吩):聚(苯乙烯磺酸盐)(PEDOT:PSS),可以进一步提高基于氧化还原聚合物纳米珠的酶电极的性能。从表观电子扩散系数(D(app))和电荷转移电阻(R(ct))两个方面讨论了 PEDOT:PSS 对纳米复合酶电极的影响。BPEI-Fc/PEDOT:PSS/GOx/SPCE 的葡萄糖传感灵敏度计算为 66 μA mM(–1)cm(–2),是没有 PEDOT:PSS 时的 2.5 倍。通过 Lineweaver-Burk 图估计的 BPEI-Fc/PEDOT:PSS/GOx/SPCE 的表观米氏常数(K(M)(app))为 2.4 mM,远低于 BPEI-Fc/GOx/SPCE(11.2 mM)。这意味着 BPEI-Fc/PEDOT:PSS/GOx/SPCE 可以更有效地催化葡萄糖氧化。通过在生理水平下注入葡萄糖和三种常见干扰物:抗坏血酸(AA)、多巴胺(DA)和尿酸(UA)进行干扰测试。与葡萄糖的电流响应相比,DA(4.2%)和 AA(7.8%)的干扰是可以接受的,UA(1.6%)的电流响应可以忽略不计。

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