基于双功能纳米材料的农药残留快速检测电化学发光共振能量转移传感技术研究

High sensitive and rapid detection technique is a powerful guarantee to monitor pesticide residues in foods. But the complicated sample matrix makes the sample preparation necessary and pretreatment time consuming in the analytical process, and it’s difficult to obtain satisfying sensitivity when detecting some trace pesticide residues even adopting high specific immune detection technology. Electrochemical luminescence resonance energy transfer technology (ECRET) will provide a new method to detect trace pesticide residues, but the low efficiency of energy transfer between energy donors and receptors is a key problem that impedes the development of the technology. This research is to establish an electrochemical luminescence resonance energy transfer immunosensing system integrating sample separation, enrichment and high sensitive detection for a variety of pesticides (atrazine etc.). Core/shell iron oxide/Au nanoparticles with magnetic and tunable plasmonic properties are prepared and coupled with targets antibodies in its surface to form the bifunctiones nanoparticle-antibody bioconjugates. The bioconjugates are used as energy receptor and also a material to separate and enrich the target analyte. Quantum dots are deposited on the electrode surface as the energy donor and recognition element. The regulatory mechanism of ECRET will be illuminated. The matching conditions between donor and receptor will be optimized to improve the efficiency of energy transfer. After the optimization of detection conditions, the electrochemical luminescence resonance energy transfer immunosensing method for sensitive and rapid detection of trace pesticide residues in foods is established. This project is an interdisciplinary.forefront research related with electroanalytical chemistry, immunology and materials science.The results of this research can be utilized in environment pollutants monitoring, food safety and medical diagnosis, and will promote the development of relative field analyzing techniques. Furthermore, it has an important theoretical significance and broad application prospects。

高灵敏快速检测技术是农药残留监管的有力保障,但样品基质复杂，前处理费时；农药残留量低，即使特异性强的免疫检测技术在灵敏度方面仍有待提高。电化学发光共振能量转移（ECRET）技术可为农残检测提供新的解决方案，但供受体间能量转移效率不足是该技术发展的障碍之一。本研究以多种农药（阿特拉津等）为靶标，制备铁氧化物/金磁性等离子共振可调复合纳米颗粒，在其表面偶联抗体形成双功能纳米颗粒作为能量受体和特异识别元件（又作为靶标物的分离富集材料），电极表面沉积量子点作为能量供体，构建集分离富集、高灵敏检测于一体的ECRET传感系统；优化供受体匹配条件提高能量转移效率，阐明ECRET调控机制，实现农药残留痕量快速检测。该项目是电分析化学、免疫学、材料学多学科交叉的前沿性研究，既为环境与食品安全、检验检疫和医学诊断等领域提供新的高灵敏分析手段，又可推动ECRET技术的发展，具有重要的理论意义和和广阔的应用前景。

高灵敏快速检测技术是农兽药残留监管的有力保障,但样品基质复杂，前处理费时；农兽药残留量低，即使特异性强的免疫检测技术在灵敏度方面仍有待提高。电化学发光共振能量转移（ECRET）技术可为农兽药残检测提供新的解决方案。开展了不同磁性纳米颗粒的制备，并进一步合成了铁氧化物/金磁性等离子共振可调复合纳米颗粒，通过调节配体的量实现了复合纳米颗粒的光谱调控；以硫化镉量子点为发光体，多壁碳纳米管为信号放大材料，构建了新型量子点电化学发光体系。采用了逐步电极修饰方式，研究了量子点电化学发光机理，探讨多壁碳纳米管，壳聚糖对量子点电化学发光的影响，考察两种碳纳米管对ECL信号的影响，优化了发光条件，实现了多壁碳纳米管对电化学发光信号的放大。以磁性纳米复合物颗粒作为电化学发光能量受体，量子点为能量供体，利用间接竞争免疫法，构建了灵敏的阿特拉津、雌二醇的ECL-RET免疫传感器技术，为高灵敏检测痕量污染物提供了一个富有前景的应用平台。该平台也可为环境检测、检验检疫和医学诊断等领域提供新的高灵敏分析手段具有较好的应用前景。