比率荧光印迹材料的构建及其对微囊藻毒素的快速高灵敏检测研究

Microcystins are a group of toxic and powerful pollutants produced by the outbreak of cyanobacteria bloom. It is urgent to develop a rapid, sensitive and reliable method to detect microcystins in environmental water. To solve the difficulty of analysis and detection of microcystins in complex environmental water matrix, in this project, we purpose to develop molecular imprinting based ratiometric fluorescence materials. The project has two features. Firstly, on fluorescence sensing strategy, by use of quantum dots, carbon dots and gold nanoclusters as fluorescent sources, we plan to explore the reasonable effective combining modes of two fluorescent materials with different emission peaks, and thereby construct fluorescent substrates, which can reduce and even eliminate the influence of the background to achieve high sensitive visual detection. Secondly, on the imprinting strategy, we intend to employ fragment imprinting and dummy imprinting strategies in combination with surface imprinting and nanoimprinting technologies, and screen appropriate functional monomers, to prepare uniform size and controlled nanoscale imprinting materials. Owing to the structure predictability, recognition specificity and high sensitivity, the resultant molecular imprinting based ratiometric fluorescence materials can eliminate matrix interference, realize high selective, sensitive and visual detection of microcystins in complicated environmental water samples, and thereby molecular imprinting based ratiometric fluorescence sensing methods will be developed. The successful implementation of this project has important scientific significance and application values to develop new analysis monitoring methods for microcystin pollution and to ensure the safety of water quality.

微囊藻毒素是由蓝藻水华爆发产生的一类毒性强、危害大的污染物，亟需发展快速、灵敏可靠的检测环境水中微囊藻毒素的方法。本项目拟研发比率荧光印迹材料用于解决复杂环境水基质中微囊藻毒素分析检测这一难题。项目具有两个特色：首先，荧光传感策略上，以量子点、碳点和金纳米簇为荧光信号源，通过探索两种不同发射峰荧光材料的合理有效组合方式，构建比率荧光基底，降低和消除背景影响，实现高灵敏可视化分析检测；其次，印迹策略上，采用片段印迹和虚拟模板印迹，结合表面印迹和纳米印迹技术，筛选合适的功能单体，制备粒径均一、大小可控的纳米尺度印迹材料。所构建的比率荧光印迹传感材料，具有构效预定性、特异识别性和高灵敏度的优势，据此发展基于分子印迹的比率荧光传感方法，消除基质干扰，实现复杂环境水样中微囊藻毒素高选择性、高灵敏度可视化快速检测。本项目对发展微囊藻毒素污染的分析监测新方法和保障水质安全具有重要科学意义和应用价值。

本项目针对复杂环境水样中微囊藻毒素分析检测过程中样品基质复杂、快速检测困难等难题，以量子点、碳点和金纳米簇为荧光信号源构建比率荧光基底，将分子印迹技术与比率荧光检测协同应用，设计合成了比率荧光印迹传感材料，实现了复杂环境水体中微囊藻毒素高选择性、高灵敏度可视化分析检测。项目在执行过程中，通过化学测量学、材料化学和环境科学等多学科交叉，掌握了比率荧光基底的构建方式，基于分子印迹的荧光纳米传感界面的设计原则，功能单体与目标物质选择性的关系以及纳米材料尺寸、修饰基团等因素对荧光纳米材料光学性能以及检测灵敏度的影响，设计合成了高选择性、高灵敏度的荧光纳米传感材料9种，构建了吸附印迹材料等5种，实现了目标物的快速、高灵敏度检测，为今后设计新型荧光纳米探针提供理论和实践指导。相关研究成果在Analytical Chemistry, Biosensors and Bioelectronics,Sensors and Actuators B:Chemical，Nanoscale等期刊发表论文14篇，并基于相关积累应邀为Advanced Materials、科学通报撰写评述性论文2篇。申请中国发明专利1项。项目执行期间培养研究生5人。项目负责人王晓艳，2020年获山东省高等学校科学技术奖一等奖。总之，本项目研究丰富了高灵敏、快速检测的化学测量学的研究内涵，具有重要的科学意义。