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用于电化学发光测量和生物分析应用的便携式硫化镉量子点丝网印刷碳电极平台的开发。

Development of portable CdS QDs screen-printed carbon electrode platform for electrochemiluminescence measurements and bioanalytical applications.

作者信息

Díez-Buitrago Beatriz, Saa Laura, Briz Nerea, Pavlov Valeri

机构信息

Center for Cooperative Research in Biomaterials (CIC BiomaGUNE), Basque Research and Technology Alliance (BRTA), Paseo de Miramon 182, 20014, Donostia San Sebastián, Spain; Tecnalia, Basque Research and Technology Alliance (BRTA), Paseo Mikeletegi 2, 20009, Donostia-San Sebastián, Spain.

Center for Cooperative Research in Biomaterials (CIC BiomaGUNE), Basque Research and Technology Alliance (BRTA), Paseo de Miramon 182, 20014, Donostia San Sebastián, Spain.

出版信息

Talanta. 2021 Apr 1;225:122029. doi: 10.1016/j.talanta.2020.122029. Epub 2020 Dec 17.

Abstract

In this work, a portable and disposable screen-printed electrode-based platform for CdS QDs electrochemiluminescence (ECL) detection is presented. CdS QDs were synthesized in aqueous media and placed on top of carbon electrodes by drop casting. The CdS QDs spherical assemblies consisted of nanoparticles about 4 nm diameters and served as ECL sensitizers to enzymatic assays. The nanoparticles were characterized by optical techniques, TEM and XPS. Besides, the electrode modification process was optimized and further studied by SEM and confocal microscopy. The ECL emission from CdS QDs was triggered with HO as cofactor and enzymatic assays were employed to modulate the CdS QDs ECL signal by blocking the surface or generating HO in situ. Thiol-bearing compounds such as thiocholine generated through the hydrolysis of acetylthiocholine by acetylcholinesterase (AChE) interacted with the surface of CdS QDs thus blocking the ECL. The biosensor showed a linear range up to 5 mU mL and a detection limit of 0.73 mU mL for AChE. Moreover, the inhibition mechanism of the enzyme was studied by using 1,5-bis-(4-allyldimethylammonium-phenyl)pentan-3-one dibromide with a detection limit of 79.22 nM. Furthermore, the natural production of HO from the oxidation of methanol by the action of alcohol oxidase was utilized to carry out the ECL process. This enzymatic assay presented a linear range up to 0.5 mg L and a detection limit of 61.46 μg L for methanol. The reported methodology shows potential applications for the development of sensitive and easy to hand biosensors and was applied to the determination of AChE and methanol in real samples.

摘要

在这项工作中,提出了一种基于便携式一次性丝网印刷电极的平台,用于硫化镉量子点电化学发光(ECL)检测。硫化镉量子点在水介质中合成,并通过滴铸法置于碳电极顶部。硫化镉量子点球形组件由直径约4纳米的纳米颗粒组成,用作酶促分析的ECL敏化剂。通过光学技术、透射电子显微镜(TEM)和X射线光电子能谱(XPS)对纳米颗粒进行了表征。此外,通过扫描电子显微镜(SEM)和共聚焦显微镜对电极修饰过程进行了优化和进一步研究。以过氧化氢(HO)作为辅助因子触发硫化镉量子点的ECL发射,并采用酶促分析通过阻断表面或原位生成HO来调节硫化镉量子点的ECL信号。含硫醇的化合物,如乙酰硫代胆碱经乙酰胆碱酯酶(AChE)水解产生的硫代胆碱,与硫化镉量子点表面相互作用,从而阻断ECL。该生物传感器对AChE的线性范围高达5 mU/mL,检测限为0.73 mU/mL。此外,使用1,5-双-(4-烯丙基二甲基铵苯基)戊烷-3-酮二溴化物研究了该酶的抑制机制,检测限为79.22 nM。此外,利用醇氧化酶作用下甲醇氧化产生HO的天然过程来进行ECL过程。该酶促分析对甲醇的线性范围高达0.5 mg/L,检测限为61.46 μg/L。所报道的方法在开发灵敏且易于操作的生物传感器方面显示出潜在应用,并应用于实际样品中AChE和甲醇的测定。

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