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基于石墨化羟基化多壁碳纳米管/离子液体的电化学传感器对多种抗病毒药物的高灵敏度检测

Highly sensitive detection of multiple antiviral drugs using graphitized hydroxylated multi-walled carbon nanotubes/ionic liquids-based electrochemical sensors.

作者信息

Zhang Zhipeng, Zheng Huizi, Liu Ying, Ma Shuang, Feng Qi, Qu Jiao, Zhu Xiaolin

机构信息

School of Environment, Northeast Normal University, Changchun, 130117, PR China.

School of Environment, Northeast Normal University, Changchun, 130117, PR China.

出版信息

Environ Res. 2024 May 15;249:118466. doi: 10.1016/j.envres.2024.118466. Epub 2024 Feb 12.

Abstract

Global outbreaks and the spread of viral diseases in the recent years have led to a rapid increase in the usage of antiviral drugs (ATVs), the residues and metabolites of which are discharged into the natural environment, posing a serious threat to human health. There is an urgent need to develop sensitive and rapid detection tools for multiple ATVs. In this study, we developed a highly sensitive electrochemical sensor comprising a glassy carbon electrode (GCE) modified with graphitized hydroxylated multi-walled carbon nanotubes (G-MWCNT-OH) and 1-butyl-3-methylimidazolium hexafluorophosphate (BMIMPF, IL) for the detection of six ATVs including famciclovir (FCV), remdesivir (REM), favipiravir (FAV), hydroxychloroquine sulfate (HCQ), cepharanthine (CEP) and molnupiravir (MOL). The morphology and structure of the G-MWCNT-OH/IL nanocomposites were characterized comprehensively, and the electroactive surface area and electron conductivity of G-MWCNT-OH/IL/GCE were determined using cyclic voltammetry and electrochemical impedance spectroscopy. The thermodynamic stability and non-covalent interactions between the G-MWCNT-OH and IL were evaluated through quantum chemical simulation calculations, and the mechanism of ATV detection using the G-MWCNT-OH/IL/GCE was thoroughly examined. The detection conditions were optimized to improve the sensitivity and stability of electrochemical sensors. Under the optimal experimental conditions, the G-MWCNT-OH/IL/GCE exhibited excellent electrocatalytic performance and detected the ATVs over a wide concentration range (0.01-120 μM). The limit of detections (LODs) were 42.3 nM, 55.4 nM, 21.9 nM, 15.6 nM, 10.6 nM, and 3.2 nM for FCV, REM, FAV, HCQ, CEP, and MOL, respectively. G-MWCNT-OH/IL/GCE was also highly stable and selective to the ATVs in the presence of multiple interfering analytes. This sensor exhibited great potential for enabling the quantitative detection of multiple ATVs in actual water environment.

摘要

近年来,全球病毒性疾病的爆发和传播导致抗病毒药物(ATV)的使用量迅速增加,其残留物和代谢产物被排放到自然环境中,对人类健康构成严重威胁。迫切需要开发用于多种ATV的灵敏快速检测工具。在本研究中,我们开发了一种高灵敏度电化学传感器,该传感器由用石墨化羟基化多壁碳纳米管(G-MWCNT-OH)和1-丁基-3-甲基咪唑六氟磷酸盐(BMIMPF,离子液体)修饰的玻碳电极(GCE)组成,用于检测六种ATV,包括泛昔洛韦(FCV)、瑞德西韦(REM)、法匹拉韦(FAV)、硫酸羟氯喹(HCQ)、千金藤素(CEP)和莫努匹拉韦(MOL)。对G-MWCNT-OH/离子液体纳米复合材料的形态和结构进行了全面表征,并采用循环伏安法和电化学阻抗谱测定了G-MWCNT-OH/离子液体/GCE的电活性表面积和电子电导率。通过量子化学模拟计算评估了G-MWCNT-OH与离子液体之间的热力学稳定性和非共价相互作用,并深入研究了使用G-MWCNT-OH/离子液体/GCE检测ATV的机制。对检测条件进行了优化,以提高电化学传感器的灵敏度和稳定性。在最佳实验条件下,G-MWCNT-OH/离子液体/GCE表现出优异的电催化性能,可在较宽的浓度范围(0.01 - 120μM)内检测ATV。FCV、REM、FAV、HCQ、CEP和MOL的检测限分别为42.3 nM、55.4 nM、21.9 nM、15.6 nM、10.6 nM和3.2 nM。在存在多种干扰分析物时G-MWCNT-OH/离子液体/GCE对ATV也具有高度稳定性和选择性。该传感器在实际水环境中对多种ATV进行定量检测方面具有巨大潜力。

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