期刊
SENSORS AND ACTUATORS B-CHEMICAL
卷 290, 期 -, 页码 378-386出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.snb.2019.03.138
关键词
Amphetamines; Computational modelling; Electroanalysis; Modified working electrode; Molecular recognition; Non-labelled sensing of recreational drugs
资金
- FEDER [PT2020-UID/QUI/50006/2013-POCI/01/0145/FEDER/007265]
- FCT from the PhD Programme in Medicines and Pharmaceutical Innovation (i3DU) [PD/BD/127797/2016]
- Sao Paulo Research Foundation (FAPESP) [2014/25770-6, 2015/01491-3, 2018/14425-7]
- Brazilian National Research Council (CNPq) [309715/2017-2]
- Coordenacao de Aperfeicoamento de Pessoal de Nivel Superior -Brasil (CAPES) [001]
- FCT/MCTES
- Fundação para a Ciência e a Tecnologia [PD/BD/127797/2016] Funding Source: FCT
This study demonstrates the ability of an electrochemical sensor based on molecularly imprinted polymers (MIPs) to selectively quantify 3,4-methylenedioxymethamphetamine (MDMA), also known as ecstasy, in bio-logical samples. The device was constructed using ortho-phenylenediamine (o-PD) as the MIP's building monomer at the surface of a screen-printed carbon electrode (SPCE). The step-by-step construction of the SPCE-MIP sensor was characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). Density functional theory (DFT) calculations and modelling were performed not only to understand template-monomer interaction but also to comprehend which possible polymer structure - linear or ramified poly(o-PD) - indeed interacts with the analyte. The prepared sensor worked by directly measuring the MDMA oxidation signal through square-wave voltammetry (SWV) after an incubation period of 10 min. Several parameters were optimized, such as the monomer/template ratio, the number of electropolymerization scanning cycles, and the incubation period, to obtain the best sensing efficiency. Optimized sensors exhibited suitable selectivity, repeatability (2.6%), reproducibility (7.7%) and up to one month of stable response. A linear range up to 0.2 mmol L-1 was found with an r(2) of 0.9990 and a limit of detection (LOD) and quantification (LOQ) of 0.79 and 2.6 mu mol L-1 (0.15 and 0.51 mu g mL(-1)), respectively. The proposed sensor was successfully applied to human blood serum and urine samples, showing its potential for application in medicine and in forensic sciences.
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