Progress in Optical and Electrochemical Sensors for Detection of Quinolone Antibiotics in Food
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摘要: 食品中喹诺酮类抗生素的残留危害食品安全，已经引起广泛关注。基于纳米材料制备的传感器具有实时分析、低检测限和分析所需的样品量小等多种优势，是目前喹诺酮类抗生素的现场检测技术研究的热点。本文介绍了荧光、比色、表面增强拉曼散射（SERS）、免疫层析（ICA）等光学传感器和基于不同纳米材料的电化学传感器在喹诺酮类抗生素检测中的应用，比较和分析了不同类型传感器的特点。并对量子点、上转换纳米粒子等纳米材料在光学传感器中的应用，以及碳纳米材料、金属纳米材料和氧化还原介质等在电化学传感器中的应用进行了综述并提出了展望，以期为食品中抗生素的检测和传感器的发展提供新的思路。Abstract: Quinolone antibiotic residues present a high risk for food safety and have gained widespread attention. Nanomaterials based sensors have the advantages of on-site application, sensitivity, and small sample volume requirement and has attracted significant interest in on-site detection technology research for quinolone antibiotics. This paper introduces the application of optical sensors including fluorescence, colorimetry, SERS, ICA and electrochemical sensors based on diverse nanomaterials in quinolone antibiotics detection and summarizes the characteristics of diverse sensors. The application of nanomaterials including quantum dots and upconversion in optical sensors, as well as those of carbon and metal nanomaterials and redox media in electrochemical sensors are reviewed and evaluated. The objective of this work is to provide new concepts for antibiotics detection in food and the development of sensors.
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Key words:
- quinolone antibiotics /
- optical /
- electrochemical /
- sensors /
- nanomaterials
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图 1 基于量子点的荧光法检测喹诺酮类抗生素的原理图
注：QDs：量子点；Excitation：激发光；Emission：发射光；Targets：靶标。
Figure 1. The schematic diagram of fluorescence detection of quinolone antibiotics based on quantum dots
图 2 基于上转换纳米粒子的荧光法检测喹诺酮类抗生素的原理图
注：（a）靶标与适配体结合使包被的UCNPs释放导致荧光恢复，（b）靶标与适配体结合使UCNPs游离引起荧光猝灭。Excitation：激发光；Emission：发射光；Target：靶标；Aptamer：靶标的适配体；Complementary DNA：适配体DNA互补链。
Figure 2. The schematic diagram of fluorescence detection of quinolone antibiotics based on upconversion nanoparticles
图 3 基于AuNPs的比色法检测喹诺酮类抗生素的原理图
注：AuNPs：金纳米粒子；Target：靶标；Aptamer：靶标的适配体。
Figure 3. The schematic diagram of colorimetric detection for detection of quinolone antibiotics based on AuNPs
图 4 基于SERS的光学传感器检测喹诺酮类抗生素的原理图
注：Anti-QNs-mAb：抗喹诺酮类单克隆抗体；Target：靶标；Laser：激光。
Figure 4. The schematic diagram of optical sensor based on SERS for the detection of quinolone antibiotics
图 5 基于免疫层析的光学传感器检测喹诺酮类抗生素的原理图
注：Negative：阴性；Positive：阳性；Sample pad：样品垫；PVC support plate：PVC板；T line：T线；C line：C线；NC membrane：硝酸纤维素膜；Absorbent pad：吸附垫；Gold particles：金属材料；Anti-QNs-mAb：抗喹诺酮类单克隆抗体；Target：靶标；Coating antigen：包被抗原；Coating anti-mouse IgG：二抗。
Figure 5. The schematic diagram of optical sensor based on immunochromatography for detecting quinolone antibiotics
图 6 电化学传感器检测喹诺酮类抗生素的原理图
注：WE：工作电极；CNT：碳纳米材料；Gold particles：金属材料；Aptamer：靶标适配体；Target：靶标。
Figure 6. The principle diagram of electrochemical sensor for detecting quinolone antibiotics
表 1 近年来用于喹诺酮类抗生素检测的光学传感器的实例
Table 1. Examples of optical sensors used for quinolone antibiotics detection in recent years
检测方法 原理 靶标 LOD（ng/mL） 线性范围（ng/mL） 时间 样品 荧光 量子点电子转移导致荧光猝灭 LFO 1.53 730~7300 － 牛奶[23] 与GO结合导致CSUNP荧光猝灭 ENR 0.47 0.976~62.5 2 h 奶粉[26] 分析物和荧光免疫探针与抗体的竞争结合 NOR 0.01 0.01~10 15 min 牛奶，蜂蜜[27] 靶向FQs与AuNPs对单抗连接的UCPs的竞争反应 ENR；CIP；NOR 0.19~0.32 0~80 － 自来水[28] 适配体和上转换纳米粒子的杂交探针与靶标结合后的荧光猝灭 ENR 0.06 1~10 90 min 鲈鱼，蛇头鱼，
鲇鱼[29]对不同靶标的荧光颜色转换 OFL；CIP 0.693；0.802 － 80 min －[45] 比色 AuNPs在盐溶液中聚集 OFL 1.221 7.23~144.55 70 min 自来水[30] 互补DNA链与CIP对适配体的竞争结合 CIP 0.397 1.325~165.67 1 h 牛奶[31] 抗体捕获，比色和光热分析 NOR 0.045 0.05~100 20 min 自来水[33] SERS 分析物和抗原与标记的AuNPs间的竞争 NOR、CIP等 0.00055 0.0001~1 15 min 牛奶[37] 微结构光流控器检测未标记的抗生素拉曼信号 CIP；NOR 0.033；0.003 － － 自来水[46] Au@Ag提供的电磁场对拉曼信号的放大 LEVO 0.00037 0.361~36100 － －[47] ICA 抗原与分析物的竞争策略 CIP，OFL等 0.1~10 1~100 10 min 牛奶[41] 抗体标记的AuNPs对抗生素的特异性识别 OFL 0.16 3.125~100 12 min 牛肉[42] 基于QDM的免疫层析 CIP 0.05 0.1~100 15 min 鱼肉[43] AuNPs，QDs，UCNPs分别标记NOR单克隆抗体 NOR 2.0；2.0；0.5 － 10 min 牛奶[44] 注：表中“－”表示所引文献未提及该内容；表2同。 
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表 2 喹诺酮类抗生素检测的电化学传感器
Table 2. Electrochemical sensors for the detection of quinolone antibiotics
检测方法 原理 靶标 LOD（ng/mL） 线性范围（ng/mL） 时间 样品 EIS 固定于纳米复合基质的适配体对抗生素的特异识别 CIP 0.5 0.5~64 10 min 牛奶[50] SWV OCNTs-PDA-Ag修饰玻碳电极 CIP 1.656 1.656~3313 － 自来水[51] DPV Ni-MOF&AuNPs负载适配体与靶标结合 ENR 5.6×10−6 10-5~1 － －[53] DPV AuNPs，AC修饰玻碳电极 CIP 0.066 0.166~8.284 7 min 牛奶[54] DPV 适配体与OFL结合产生信号变化 OFL 0.361 18.05~7220 － 自来水[55] DPV 特定结合物与游离ENR在固定化抗体上的竞争性结合 ENR 3 5~10 6 min 猪、鸡、牛、羊、鸭[56] DPV 双标记适配体修饰电极 CIP 0.033 99.39~149.09 60 min 牛奶[57] SWV 铋膜电极 CIP 0.003 0.008~0.2 62 s 自来水[59]
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