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基于还原氧化石墨烯场效应晶体管的酶-聚电解质多层组装用于生物传感应用。

Enzyme-polyelectrolyte multilayer assemblies on reduced graphene oxide field-effect transistors for biosensing applications.

机构信息

Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA) - Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de La Plata - CONICET, Suc. 4, CC 16, La Plata, Argentina.

Centre of Electrochemical Surface Technology (CEST), Viktor-Kaplan-Straße 2, 2700 Wiener Neustadt, Austria.

出版信息

Biosens Bioelectron. 2017 Jun 15;92:661-667. doi: 10.1016/j.bios.2016.10.035. Epub 2016 Oct 21.

Abstract

We present the construction of layer-by-layer (LbL) assemblies of polyethylenimine and urease onto reduced-graphene-oxide based field-effect transistors (rGO FETs) for the detection of urea. This versatile biosensor platform simultaneously exploits the pH dependency of liquid-gated graphene-based transistors and the change in the local pH produced by the catalyzed hydrolysis of urea. The use of an interdigitated microchannel resulted in transistors displaying low noise, high pH sensitivity (20.3µA/pH) and transconductance values up to 800 µS. The modification of rGO FETs with a weak polyelectrolyte improved the pH response because of its transducing properties by electrostatic gating effects. In the presence of urea, the urease-modified rGO FETs showed a shift in the Dirac point due to the change in the local pH close to the graphene surface. Markedly, these devices operated at very low voltages (less than 500mV) and were able to monitor urea in the range of 1-1000µm, with a limit of detection (LOD) down to 1µm, fast response and good long-term stability. The urea-response of the transistors was enhanced by increasing the number of bilayers due to the increment of the enzyme surface coverage onto the channel. Moreover, quantification of the heavy metal Cu(with a LOD down to 10nM) was performed in aqueous solution by taking advantage of the urease specific inhibition.

摘要

我们构建了聚乙烯亚胺和脲酶的层层组装体,用于基于还原氧化石墨烯的场效应晶体管(rGO FET)上对尿素的检测。这种多功能生物传感器平台同时利用了液体门控石墨烯基晶体管的 pH 依赖性以及尿素催化水解产生的局部 pH 变化。使用叉指微通道使晶体管具有低噪声、高 pH 灵敏度(20.3µA/pH)和高达 800µS 的跨导值。通过静电门控效应的转导特性,弱聚电解质对 rGO FET 的修饰改善了 pH 响应。在存在尿素的情况下,由于靠近石墨烯表面的局部 pH 变化,脲酶修饰的 rGO FET 表现出 Dirac 点的移动。值得注意的是,这些器件在非常低的电压(小于 500mV)下工作,能够在 1-1000µm 范围内监测尿素,检测限(LOD)低至 1µm,具有快速响应和良好的长期稳定性。由于通道表面覆盖的酶增加,晶体管的尿素响应通过增加双层数得到增强。此外,通过利用脲酶的特异性抑制,在水溶液中实现了对重金属 Cu 的定量(检测限低至 10nM)。

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