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采用纳米结构聚(3,4-亚乙基二氧噻吩)衍生物作为沟道层的有机电化学晶体管对汗皮质醇的灵敏检测。

Sensitive Detection of Sweat Cortisol Using an Organic Electrochemical Transistor Featuring Nanostructured Poly(3,4-Ethylenedioxythiophene) Derivatives in the Channel Layer.

机构信息

Smart Organic Materials Laboratory, Institute of Chemistry, Academia Sinica, No. 128, Section 2, Research Institute Road, Nankang, Taipei 11529, Taiwan.

Taiwan International Graduate Program (TIGP), Sustainable Chemical Science & Technology (SCST), Academia Sinica, No. 128, Section 2, Research Institute Road, Nankang, Taipei 11529, Taiwan.

出版信息

Anal Chem. 2022 May 31;94(21):7584-7593. doi: 10.1021/acs.analchem.2c00497. Epub 2022 May 19.

Abstract

In this study, we examined the influence of functionalized poly(3,4-ethylenedioxythiophene) (PEDOT) nanostructures decorated on the channel layer of an organic electrochemical transistor (OECT) for the detection of sweat cortisol, an adrenocorticosteroid stress hormone. The OECT device featured a bilayer channel confined by a PEDOT:polystyrenesulfonate (PSS) underlayer and a nanostructure-decorated upper layer engineered from the monomers EDOT-COOH and EDOT-EG3 through template-free electrochemical polymerization. This molecular design allowed antibody conjugation using 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide/-hydroxysulfosuccinimide coupling through the carboxylic acid side chain, with EDOT-EG3 known to minimize nonspecific binding of biomolecules. We also engineered an OECT device having a channel area without any nanostructures to gain insight into the effect of the nanostructures on cortisol sensing. Our new nanostructure-embedded OECT device facilitated real-time detection of cortisol at concentrations ranging from 1 fg/mL to 1 μg/mL with a detection limit of 0.0088 fg/mL with good linearity ( = 0.9566), in addition to excellent selectivity toward cortisol among other structurally similar interfering compounds and high stability and reproducibility. With its rapid response for the detection of 100 ng/mL cortisol-spiked artificial sweat, this nanostructure-decorated OECT device has potential clinical practicality and utility in wearable sensors for future healthcare applications.

摘要

在这项研究中,我们研究了功能化聚(3,4-亚乙基二氧噻吩)(PEDOT)纳米结构在有机电化学晶体管(OECT)通道层上的修饰对汗液皮质醇(一种应激激素)检测的影响。OECT 器件的双层通道由聚(PEDOT:聚苯乙烯磺酸盐)(PSS)底层和通过无模板电化学聚合由单体 EDOT-COOH 和 EDOT-EG3 工程化的纳米结构修饰的上层构成。这种分子设计允许使用 1-乙基-3-(3-二甲基氨基丙基)碳化二亚胺/羟基磺基琥珀酰亚胺通过羧酸侧链进行抗体偶联,已知 EDOT-EG3 可最小化生物分子的非特异性结合。我们还设计了一种没有任何纳米结构的通道区域的 OECT 器件,以深入了解纳米结构对皮质醇传感的影响。我们的新纳米结构嵌入式 OECT 器件能够实时检测皮质醇,浓度范围从 1 fg/mL 到 1 μg/mL,检测限为 0.0088 fg/mL,具有良好的线性度(= 0.9566),此外,与其他结构相似的干扰化合物相比,对皮质醇具有出色的选择性,具有高稳定性和重现性。这种纳米结构修饰的 OECT 器件对 100 ng/mL 皮质醇掺杂人工汗液的快速响应使其在未来医疗保健应用的可穿戴传感器中具有潜在的临床实用性和实用性。

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