[논문]전도성고분자, 티로시나아제 효소 및 이온성 액체 전해질을 융합한 전압전류법 기반의 비스페놀F 검출 센서

지성은; 이상혁; 이혜진

doi:10.14478/ace.2023.1032

[국내논문] 전도성고분자, 티로시나아제 효소 및 이온성 액체 전해질을 융합한 전압전류법 기반의 비스페놀F 검출 센서
Voltammetric Sensor Incorporated with Conductive Polymer, Tyrosinase, and Ionic Liquid Electrolyte for Bisphenol F 원문보기

공업화학 = Applied chemistry for engineering, v.34 no.3, 2023년, pp.258 - 263

지성은 (경북대학교 화학과) , 이상혁 (경북대학교 화학과) , 이혜진 (경북대학교 화학과)

초록
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본 연구에서는 일회용 센서 칩으로 제작 가능한 스크린 프린팅된 탄소칩 전극(screen printed carbon electrode; SPCE) 표면에 전도성고분자 및 효소 티로시나아제(tyrosinase, Tyr)를 적층하여 전기화학적인 방법으로 남성 질환, 갑상선 질환 등과 연관성이 입증된 내분비계 교란 물질인 비스페놀F (bisphenol F, BPF) 검출에 적용하였다. 산소 플라즈마 처리를 통해 음전하를 띠게 한 SPCE 작업전극 표면에 양전하를 띄는 전도성 고분자인 poly(diallyldimethyl ammonium chloride) (PDDA)과 음전하를 띠는 고분자 화합물 poly(sodium 4-styrenesulfonate) (PSS) 그리고 PDDA 순서대로 정전기적인 인력으로 층을 쌓고, 최종적으로 pH (7.0)를 조절하여 음전하를 띄게 한 효소, Tyr층을 올려 PDDA-PSS-PDDA-Tyr 센서를 제작하였다. 상기 전극 센서를 기질이자 타겟분석물인 BPF 용액에 접촉하면, 전극 표면에서 Tyr 효소와 산화반응에 의해 4,4'-methylenebis(cyclohexa-3,5-diene-1,2-dione)가 생성되고, 순환전압전류법과 시차펄스전압전류법을 이용하여 생성물을 0.1 V (vs. Ag/AgCl)에서 환원하면 4,4'-methylenebis(benzene-1,2-diol)이 생성되면서 발생하는 피크 전류 값의 변화를 측정함으로써, BPF의 농도를 정량적으로 분석하였다. 또한, 기존에 많은 연구에서 사용되는 인산완충생리식염수를 대체할 수 있는 이온성 액체 전해질을 사용하여 BPF의 검출 성능 결과를 비교하였다. 또한 BPF와 유사한 구조를 갖는 방해물질로 작용하는 비스페놀S에 대한 선택성을 확인하였다. 마지막으로 실험실에서 준비한 실제 시료안의 BPF의 농도를 분석하는데 제작한 센서를 적용함으로써 센서의 실제 적용 가능성을 입증하고자 하였다.

Abstract ▼ AI-Helper

In this study, conductive polymers and the enzyme tyrosinase (Tyr) were deposited on the surface of a screen printed carbon electrode (SPCE), which can be fabricated as a disposable sensor chip, and applied to the detection of bisphenol F (BPF), an endocrine disruptor with proven links to male diseases and thyroid disorders, using electrochemical methods. On the surface of the SPCE working electrode, which was negatively charged by oxygen plasma treatment, a positively charged conductive polymer, poly(diallyldimethyl ammonium chloride) (PDDA), a negatively charged polymer compound, poly(sodium 4-styrenesulfonate) (PSS), and another layer of PDDA were layered by electrostatic attraction in the order of PDDA, PSS, and finally PDDA. Then, a layer of Tyr, which was negatively charged due to pH adjustment to 7.0, was added to create a PDDA-PSS-PDDA-Tyr sensor for BPF. When the electrode sensor is exposed to a BPF solution, which is the substrate and target analyte, 4,4'-methylenebis(cyclohexa-3,5-diene-1,2-dione) is generated by an oxidation reaction with the Tyr enzyme on the electrode surface. The reduction process of the product at 0.1 V (vs. Ag/AgCl) generating 4,4'-methylenebis(benzene-1,2-diol) was measured using cyclic and differential pulse voltammetries, resulting in a change in the peak current with respect to the concentration of BPF. In addition, we compared the detection performance of BPF using an ionic liquid electrolyte as an alternative to phosphate-buffered saline, which has been used in many previous sensing studies. Furthermore, the selectivity of bisphenol S, which acts as an interfering substance with a similar structure to BPF, was investigated. Finally, we demonstrated the practical applicability of the sensor by applying it to analyze the concentration of BPF in real samples prepared in the laboratory.

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표/그림 (5)

그림 Figure 1. A simplified scheme showing the procedure of fabricating PDDA-PSS-PDDA-Tyr layered SPCE sensor. Representative SEM image of bare (i) and PDDA-PSS-PDDA-Tyr layered SPCE (v). CV data are also shown in the absence (····) and presence (―) of 20 μM BPF in a [BzBIM]OH ionic liquid electrolyte.
그림 Figure 2. (a) A series of CV data for various concentrations of BPF from 10, 20, 60, 80 and 100 μM in [BzBIM]OH solution using PDDA-PSS-PDDA-Tyr layered SPCE sensor. (b) Linear plots showing the oxidation (i) and reduction (ii) peak currents versus the BPF concentration. The data points were taken from (a).
그림 Figure 3. Representative DPV data for different concentrations of BPF ranging from 1, 5, 10, 15, 20, 40, 60, 80 and 100 μM in (a) [BzBIM]OH and (b) PBS (pH 7.0) using PDDA-PSS-PDDA-Tyr layered SPCE sensor. (c) Comparison of linear plots of DPV peak currents as a function of BPF concentrations in (a) [BzBIM]OH and (b) PBS (pH 7.0). Data points in (c) are taken from (a) and (b).
그림 Figure 4. Representative DPV results for the selectivity test of PDDA-PSS-PDDA-Tyr layered sensor. (i) 1 mM BPS only, (ii) 10 μM BPF only and (iii) a mixture of 1 mM BPS and 10 μM BPF in (a) [BzBIM]OH and (b) PBS (pH 7.0) solution.
그림 Figure 5. (a) A set of DPV data for the analysis of a sample containing components of latex gloves dissolved in [BzBIM]OH electrolyte using PDDA-PSS-PDDA-Tyr layered sensor. The added BPF concentration to the sample was 5, 10, 20, and 30 μM. (b) A plot of DPV peak current versus added BPF concentration. The marker (△) is the sample only.

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