基于功能化二硫化钼构筑比率型免疫传感器对赭曲霉毒素广谱性识别的研究

Food security is relative with the public health and life safety. As a kind of mycotoxins, ochratoxins include many compounds with analogous structure such as ochratoxin A(OTA), ochratoxin B(OTB), ochratoxin C(OTC) and so on, which are with similar toxicity but coexist in the contaminated cereals. At present, many researches are concerned with the detection of OTA, but the investigations on other ochratoxins and corresponding derivatives are still scare. In this project, the broad-specificity antigen of ochratoxins are designed and synthesized, while the broad-specificity antibody of ochratoxins are prepared and screened. During this process, the molecular docking model are used to investigate the selection mechanism of half-antigen, while the quantitative structure-activity relationship are used to explore recognition mechanism of antibody with small molecules. Then, the broad-specificity immunosensors are constructed by using multi-functional MoS2 materials with abundant edges as the base, and the ratio-dependence from the DNA amplification as the signal. By using the corresponding chemometrics methods such as multiple linear regression and principal component analysis to analyze the data, the fast, sensitive and selective detection of ochratoxins can be achieved. . The completeness of this project will provide a new detection technology for ochratoxins, a new strategy for the design of the broad-specificity half-antigen and the recognition of broad-specificity antibody of mycotoxins, and a new analytical method for the simultaneous detection of small molecules in food. In addition, by analyzing the amount of ochratoxins in different cereals, we may provide theoretical basis for the assessment of ochratoxins on the safety and risk of human health.

食品安全关乎公众身体健康和生命安全。赭曲霉毒素是一种真菌毒素，包含多种结构类似物，在被污染的谷物中普遍共同存在，且毒性相似。目前，赭曲霉毒素A的检测较多，但其他赭曲霉毒素及代谢衍生物的检测仍较少。本项目将针对赭曲霉毒素类物质，设计和合成广谱性抗原，制备和筛选广谱性抗体，采用分子对接模型建立半抗原的选择机制，采用构效关系建立抗体与小分子的识别机制。在此基础上，研制广谱性免疫传感器，以多功能二硫化钼复合材料作为免疫传感器的基底，以DNA扩增产物构筑比率型信号，结合多元线性回归法等化学计量学手段处理数据，实现多种赭曲霉毒素的快速、灵敏的分型检测。. 本项目的完成，将为谷物中赭曲霉毒素的检测提供新技术，为真菌毒素的广谱性半抗原设计及广谱性抗体识别提供新策略，为食品中多种小分子的同时检测提供新手段。同时，通过分析赭曲霉毒素在不同谷物的分布情况，为评价其对人类健康的安全性和风险性提供理论依据。

食品安全关乎公众身体健康和生命安全。赭曲霉毒素是赭曲霉毒素是一种真菌毒素，包含多种结构类似物，在被污染的谷物中普遍共同存在。本项目以赭曲霉毒素的快速筛查为目标，制备了赭曲霉毒素类物质的抗原和抗体，研究了抗体与小分子的识别机制。合成了多功能二硫化钼复合材料为免疫传感器的基底材料和多样化仿生纳米酶为免疫传感器的标记材料，逐步系统地构筑了系列单模单信号免疫传感器、双模双信号免疫传感器和广谱性免疫传感器。研究过程中，详细探讨了材料的控制合成机理，揭示了材料的高效催化性能，探索了传感器的信号响应机制，先后实现了赭曲霉毒素的特异性识别和广谱性识别，并借助多元线性回归、机器学习等完成了多种赭曲霉毒素的分型检测。为了适应现场检测，进一步深入开发了纸基传感、手机APP识别、便携式小型仪器设备等，实现对食品中多种有害物质的快速检测。.项目执行期间内，在Adv Funct Mater, Anal Chem, J Hazard Mater, Biosens Bioelectron等期刊发表论文37篇；申请专利9项，授权专利7项；获广东省优秀学生（研究生阶段）2名，获国家留学基金委资助出国联合培养1名。撰写了题为"Advances in immunoassay-based strategies for mycotoxin detection in food: from single-mode immunosensors to dual-mode immunosensors"的综述。主持申报“食品危害因子的信号识别、增敏及一体化检测关键技术及应用”，获得2022年度中国分析测试协会科学技术奖CAIA奖一等奖。本项目的完成为谷物中赭曲霉毒素的检测提供了新技术，为抗原抗体识别提供了新策略，为食品中多种危害因子的同时检测提供了新手段。