Application progress of nano-materials in detection of antibiotics by electrochemical sensors
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摘要: 抗生素自发现至今，由于其可以阻碍细菌的生长，被广泛应用于预防和治疗细菌的感染疾病上。但是抗生素在畜牧业、农业等方面的滥用滥排导致抗生素污染，极大地威胁水源地的安全，导致细菌耐药性增强、给环境及人类健康带来重大的危害。因此，抗生素的检测近年来得到了广泛的关注，而大多抗生素都具有电化学活性。基于此，纳米修饰电极可以使抗生素在电解质中的电化学氧化或还原反应增强，从而促进其灵敏度的提高，使电化学传感器可以检测到各类抗生素。本文详细介绍了用于检测抗生素的各种纳米材料修饰电极的电化学传感器及其性能。最后，讨论了纳米材料电化学传感器在抗生素检测中面临的挑战和发展前景。Abstract: Since the discovery of antibiotics, they have been widely used in the prevention and treatment of bacterial infections because they can hinder the growth of bacteria. However, the abuse of antibiotics in animal husbandry and agriculture leads to antibiotic pollution, which greatly threatens the safety of water sources, increases bacterial drug resistance, and brings great harm to the environment and human health. For these reasons, the detection of antibiotics has attracted extensive attention in recent years. Based on the electrochemical activity of most antibiotics, nano-modified-electrode can improve the sensitivity of electrochemical sensor by enhancing the electrochemical oxidation or reduction reaction of antibiotics in electrolyte. Various electrochemical sensors for the detection of antibiotics are described in detail in this paper, as well as their properties. Finally, the challenges and development prospects of nanomaterial electrochemical sensors in antibiotic detection are discussed.
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图 1 (a) 铂纳米球制备示意图/玻碳电极(GCE)表面修饰；(b) 裸GCE的SEM图像；(c) 聚糠醛膜修饰GCE的SEM图像；((d)、(e)) 铂纳米球/聚糠醛膜修饰GCE的SEM图像；(f) 铂纳米球/聚糠醛膜/GCE的高倍SEM图像；((g)、(h)) 各电极的循环伏安(CV) 和差分脉冲伏安(DPV)曲线
Figure 1. (a) Preparation schematic diagram of platinum nanospheres/glassy carbon electrode (GCE) surface modification; (b) SEM image of naked GCE; (c) SEM image of GCE modified by polyfurfural film; ((d), (e)) SEM images of GCE modified by platinum nanosphere/polyfurfural film; (f) High power SEM image of platinum nanospheres/polyfurfural films /GCE; ((g), (h)) Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) curves of electrodes
1—Bare GCE; 2—Pt nanospheres/GCE; 3—Polyfurfural film/GCE; 4—Pt nanospheres/polyfurfural film/GCE; 5—Pt nanospheres/polyfurfural film/GCE without metronidazole; 6—Bare platinum electrode; I—Current; E—Potential
图 3 ((a)、(b)) CdTe-炭黑(CB)-壳聚糖(CTS)的TEM图像和放大图像；((c)、(d)) CdTe 量子点(QDs)的TEM图像和放大图像；(e) 裸GCE、CB-CTS∶环氧氯丙烷(EPH)/GCE和CdTe CB-CTS∶EPH/GCE电极在0.1 mol·L−1的磷酸盐缓冲液中，pH=6.0的条件下的CV曲线；(f) 诺氟沙星(NOR)的氧化反应
Figure 3. ((a), (b)) TEM image and enlarged image of CdTe-carbon black (CB)-chitosan (CTS); ((c), (d)) TEM image and enlarged image of CdTe quantum dot (QDs); (e) CV curves of naked GCE, CB-CTS∶Epichlorohydrin (EPH)/GCE and CdTe CB-CTS∶EPH/GCE electrodes in 0.1 mol·L−1 phosphate buffer at pH=6.0; (f) Oxidation reaction of norfloxacin (NOR)
1—Naked GCE; 2—CB-CTS∶EPH/GCE; 3—CdTe CB-CTS∶EPH/GCE
图 4 用于检测氨苄青霉素(AMP) 的MIPs EC传感器构造过程示意图[52]：(a) 碳布示意图；(b) AMP与N,N-二甲基丙烯酰胺(NNDMA)自组装机制图
Figure 4. Schematic diagram of MIPs EC sensor construction process for detecting ampicillin (AMP)[52]: (a) Schematic diagram of carbon fiber cloth; (b) Self-assembly mechanism diagram with AMP and N, N-dimethylacrylamide (NNDMA)
CC—Carbon cloth; MIP—Molecularly imprinted polymers; NNDMA—N,N-dimethyl acrylamide; MAA—Methacrylic acid; EDMA—Ethyleneglycol dimethacrylate; AIBN—Azodiisobutyronitrile; NIP—Synthesis of non-template polymers
图 5 石墨烯纳米片(GNPs)和分子印迹聚合物 (MIPs)制备和检测过程示意图[55]
Figure 5. Schematic diagram of preparation and detection process of graphene nanosheets (GNPs) and molecularly imprinted polymers (MIPs)[55]
MNZ—Metronidazole; GQDs—Graphene quantum dots; APTES—3-aminopropyltriethoxysilane; TEOS—Tetraethoxysilane; DPV—Differential pulse voltammetry
表 1 常见抗生素
Table 1. Common antibiotics
Types of antibiotics Name Sulfa[6] Sulfonazole, sulfamethoxazole, sulfadiazine, sulfamethoxazole, etc. Tetracycline class[7] Tetracycline, oxytetracycline, chlortetracycline, etc. Macrolide[8] Erythromycin, roxithromycin, azithromycin, clarithromycin, dirithromycin, fluoroerythromycin, telithromycin, etc. β-lactams[9] penicillin, oxacillin, ampicillin, carbenicillin, piperacillin, cefazolin, cefuroxime, cefotaxime, cefepime, etc. Amino glycosides[10] Streptomycin, kanamycin, neomycin, tobramycin, gentamicin, amikacin, etc. Quinolones[11] Ofloxacin, pefloxacin, norfloxacin and ciprofloxacin, etc. Other Metronidazole, vancomycin, lincomycin, clindamycin, etc. 
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