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基于电子类型分离的碳纳米管电化学生物传感器,结合葡萄糖氧化酶和脱氢酶。

Electronically type-sorted carbon nanotube-based electrochemical biosensors with glucose oxidase and dehydrogenase.

机构信息

Department of Electronic Engineering, Shibaura Institute of Technology , 3-7-5 Toyosu, Koto-ku, Tokyo 135-8548, Japan.

出版信息

ACS Appl Mater Interfaces. 2015 Jan 14;7(1):584-92. doi: 10.1021/am506758u. Epub 2014 Dec 31.

Abstract

An electrochemical enzyme biosensor with electronically type-sorted (metallic and semiconducting) single-walled carbon nanotubes (SWNTs) for use in aqueous media is presented. This research investigates how the electronic types of SWNTs influence the amperometric response of enzyme biosensors. To conduct a clear evaluation, a simple layer-by-layer process based on a plasma-polymerized nano thin film (PPF) was adopted because a PPF is an inactive matrix that can form a well-defined nanostructure composed of SWNTs and enzyme. For a biosensor with the glucose oxidase (GOx) enzyme in the presence of oxygen, the response of a metallic SWNT-GOx electrode was 2 times larger than that of a semiconducting SWNT-GOx electrode. In contrast, in the absence of oxygen, the response of the semiconducting SWNT-GOx electrode was retained, whereas that of the metallic SWNT-GOx electrode was significantly reduced. This indicates that direct electron transfer occurred with the semiconducting SWNT-GOx electrode, whereas the metallic SWNT-GOx electrode was dominated by a hydrogen peroxide pathway caused by an enzymatic reaction. For a biosensor with the glucose dehydrogenase (GDH; oxygen-independent catalysis) enzyme, the response of the semiconducting SWNT-GDH electrode was 4 times larger than that of the metallic SWNT-GDH electrode. Electrochemical impedance spectroscopy was used to show that the semiconducting SWNT network has less resistance for electron transfer than the metallic SWNT network. Therefore, it was concluded that semiconducting SWNTs are more suitable than metallic SWNTs for electrochemical enzyme biosensors in terms of direct electron transfer as a detection mechanism. This study makes a valuable contribution toward the development of electrochemical biosensors that employ sorted SWNTs and various enzymes.

摘要

本文提出了一种在水溶液中使用电子类型分级(金属和半导体)单壁碳纳米管(SWNTs)的电化学酶生物传感器。本研究探讨了 SWNTs 的电子类型如何影响酶生物传感器的电流响应。为了进行清晰的评估,采用了基于等离子体聚合纳米薄膜(PPF)的简单层层工艺,因为 PPF 是一种无活性的基质,可以形成由 SWNTs 和酶组成的具有良好定义的纳米结构。对于存在氧气的葡萄糖氧化酶(GOx)酶的生物传感器,金属 SWNT-GOx 电极的响应是半导体 SWNT-GOx 电极的 2 倍。相比之下,在没有氧气的情况下,半导体 SWNT-GOx 电极的响应得以保留,而金属 SWNT-GOx 电极的响应则显著降低。这表明直接电子转移发生在半导体 SWNT-GOx 电极上,而金属 SWNT-GOx 电极则由酶反应引起的过氧化氢途径主导。对于具有葡萄糖脱氢酶(GDH;无需氧气的催化)酶的生物传感器,半导体 SWNT-GDH 电极的响应是金属 SWNT-GDH 电极的 4 倍。电化学阻抗谱用于表明半导体 SWNT 网络的电子转移电阻小于金属 SWNT 网络。因此,得出结论,在直接电子转移作为检测机制方面,与金属 SWNTs 相比,半导体 SWNTs 更适合用于电化学酶生物传感器。本研究为开发使用分级 SWNTs 和各种酶的电化学生物传感器做出了有价值的贡献。

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