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Effects of the surface chemistry and structure of carbon nanotubes on the coating of glucose oxidase and electrochemical biosensors performance

机译:碳纳米管的表面化学和结构对葡萄糖氧化酶涂层和电化学生物传感器性能的影响

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Glucose oxidase (GOx) has been immobilized on multiwall and herringbone carbon nanotubes (NTs) for glucose biosensing. Emphasis has been pointed in the effect of the structure and surface chemistry in the biosensor performance. Functionalization with carboxylic moieties renders a better performance than amino groups, and it also improves the performance with respect to that of bare NTs. No relationship was found between sensitivity to glucose and the amount of charge coming from the direct electron transfer between NTs and the flavin adenine dinucleotide (FAD) group of GOx. Based on these results, oxidized herringbones and multiwall NTs were used to prepare electrochemical sensors with different GOx loadings that were tested at positive and negative potentials. At positive potentials, the sensing mechanism is based on the oxidation of H2O2, and differences in sensitivity are related to the amount of active enzyme loaded on the carbon nanotubes surface. This amount seems to be enhanced by the presence of carboxylic moieties on oxidized NTs, as well as by the homogeneous surface structure and higher surface area of multiwall NTs. In this sense, the homogeneous structure of multiwall NTs seems to be more important than their larger surface area. At negative potentials, the detection mechanism is driven by oxygen consumption during the glucose oxidation. Thanks to the aforementioned reasons, multiwall NTs provide a similar sensibility and working range as herringbone NTs while using half the amount of GOx. These results point out the huge impact of NTs structure and surface chemistry upon the activity of GOx for electrochemical sensors.
机译:葡萄糖氧化酶(GOx)已固定在多壁和人字形碳纳米管(NTs)上,用于葡萄糖生物传感。已经着重指出了结构和表面化学对生物传感器性能的影响。与羧基相比,具有羧基的官能团具有更好的性能,并且相对于裸NT而言,其性能也得到了改善。在对葡萄糖的敏感性与NT和GOx的黄素腺嘌呤二核苷酸(FAD)之间直接电子转移产生的电荷量之间没有发现任何关系。根据这些结果,使用氧化的人字形和多壁NT来制备具有不同GOx负载的电化学传感器,并在正电势和负电势下对其进行测试。在正电位下,感测机制基于H 2 O 2 的氧化以及灵敏度的差异与负载在碳纳米管表面上的活性酶的量有关。似乎由于氧化的NTs上存在羧基部分,以及多壁NTs的均质表面结构和较高的表面积而使该量增加。从这个意义上讲,多壁NT的均匀结构似乎比其更大的表面积更重要。在负电位下,检测机制由葡萄糖氧化过程中的氧气消耗驱动。由于上述原因,多壁NT在使用一半量的GOx的同时,提供了与人字形NT相似的灵敏度和工作范围。这些结果指出了NTs结构和表面化学性质对电化学传感器GOx活性的巨大影响。

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