可抛式电化学-SERS传感器在水体极性抗生素现场快速检测中的研究

The aquatic samples have the characteristics of complex matrix, poor stability, low analyte concentration with large detection demand. Therefore, it is necessary to develop the rapid in-situ detection methods with high sensitivity for the detection of analytes in water. The appearance of emerging chemical pollutants (ECPs) in water including antibiotics may trigger the ecological deterioration and greatly threaten human health. Benefited from the easy operation, uniform control of the preparation process of screen printing technology，and the products are flexible to design and easy to integrate, this program has been proposed to screen printed electrochemical sensors with excellent SERS activity and highly stability and orderly on disposable matrix materials. The electrochemical method is utilized to regulate the potential of this disposable electrochemical-SERS sensor to realize the in-situ separate and concentrate polar antibiotics molecules in water samples; simultaneously, surface-enhanced Raman scattering (SERS) technique is combined to permit high sensitivity and rapid detection of molecules with same polarity. On this basis, portable electrochemical-Raman system is constructed to carry out the rapid in-situ detection of real water samples contain different polar antibiotics. Based on the experimental results, the new method could be established which can provide the qualitative and quantitative information of each component of polar antibiotics in complex water samples within several minutes. The research results are expected to provide new research ideas for the monitoring and emergency analysis of ECPs in aquatic environment, laid the foundation for the application of SERS in the detection of water pollution.

水环境样品具有基体复杂、稳定性差、分析物浓度低和检测需求量多等特点，因而开发高灵敏的水体分析物现场快速检测方法十分必要。水中抗生素等新兴化学污染物(ECPs)的出现可能导致水环境恶化，影响人类健康。因此，本项目拟借助丝网印刷技术操作简便、制备过程均匀可控、产品设计灵活、易于集成等优势，在可抛式基体材料上丝网印刷稳定有序、表面增强拉曼(SERS)活性好的电化学传感器；采用电化学方法调控该可抛式电化学-SERS传感器的电位，对水中极性抗生素分子进行原位分离富集，联用SERS技术实现相同极性分子的高灵敏快速检测；在此基础上，搭建便携式电化学-拉曼系统，对极性抗生素污染水样及实际河流样品进行现场快速检测研究，进而建立能在数分钟内提供复杂水环境中极性抗生素种类和含量信息的新方法。该项目研究成果可望为水环境中ECPs污染的监测和应急分析提供新手段，并为SERS技术在水污染检测中的应用提供新的研究思路。

水环境样品具有基体复杂、稳定性差、分析物浓度低和检测需求量多等特点，因而开发高灵敏、高选择性的污染物现场快速检测方法十分必要。水中内分泌干扰物等新兴化学污染物（ECPs）的出现可能导致水环境恶化，影响人类健康。因此，本项目借助分子印迹材料对目标物的特异性识别能力和表面增强拉曼光谱（SERS）灵敏度高、检测速度快、可原位分析等优点，在可抛式基体材料上构建了一系列稳定有序、SERS活性好，且制备过程简单环保的多功能传感界面，实现了复杂水体中污染物的高选择性及高灵敏检测，在分子水平上研究了相关的基础科学问题。创新性地利用绿色的电化学技术一步可控制备了分子印迹-SERS传感基底；利用天然贻贝仿生多巴胺分子的自聚特性，制备了聚多巴胺分子印迹-SERS传感界面，实现了内分泌干扰物的高选择性检测，解决了常规分子印迹-SERS基底制备过程繁琐的问题。在此基础上，构建了基于核壳结构的聚多巴胺分子印迹-SERS传感界面，结合电化学富集技术，通过电位和时间的选择性调控，对水中极性内分泌干扰物和抗生素分子等进行了原位分离富集，进一步实现对相同极性分子的高选择性高灵敏快速检测，检测限低至0.01 nM。研究成果大大简化了复杂实际样品的预处理和分离步骤，并为结构类似物对SERS谱峰造成的干扰提供了解决方法。该项目研究成果可望为水环境中ECPs污染的监测和应急分析提供新手段，并为SERS技术在水污染检测中的应用提供新的研究思路。