聚集诱导荧光分子设计合成及在地下水砷形态快速分析中的应用

It is important and urgent to develop the field rapid detection methods for arsenic speciation concentrations and distributions determination in groundwater with high sensitivity and selectivity. With the data support of arsenic speciations, we can investigate the arsenic migration and transformation mechanism in groundwater, and the arsenic pollution control remedies. In this project, the fluorescence molecules with aggregation induced emission (AIE) effect are designed and prepared, and the structures of the AIE molecules are optimized based on the theoretical simulation calculations. The as-prepared AIE molecules are applied for the detection of arsenic speciations in groundwater. And the detection sensitivity and selectivity of AIE molecules toward arsenic speciations are studied based on the influence investigations of pH, coexisting ions et al. Thus the arsenic speciations specific reorganization mechanism and AIE molecular luminescence mechanism can be clarified. Furthermore, the principle sensor devices based on AIE molecules can be designed and constructed for the on-site field rapid detection of arsenic speciations in the actual groundwater samples. Our research would provide solid and pivotal data support for the risk assessment and restoration of the arsenic pollution in the groundwater, and the science and technology support for the significant social needs, such as the arsenic pollution emergencies in the groundwater etc.

发展高灵敏度和高选择性的野外快速检测方法，准确得到不同砷形态As(III)/As(V)在地下水中的含量和分布，是研究地下水中砷的迁移转化和污染控制急需解决的关键科学问题。本项目首先设计合成具有聚集诱导发光（AIE）效应的荧光分子，结合理论计算优化分子结构；进一步研究AIE分子对地下水中不同砷形态的检测性能，考察水体pH值、共存离子等因素对砷形态检测灵敏度及选择性的影响，阐明AIE分子对砷形态的特异性识别原理及分子发光机理；设计与构建基于AIE分子的原理性传感器器件，研究其对实际地下水中不同砷形态的野外现场快速检测。本项目的成功实施将为地下水的砷污染风险评估及修复治理提供关键可靠的基础数据，进而为应对地下水砷污染突发事件等重大社会需求提供科技支撑。

地下水砷污染已成为全球性环境地质学问题。地下水中砷以As(V)和As(III)的络阴离子形式存在，其生态毒理效应不仅取决于它们的总量，更取决于其形态分布。要准确得到不同砷形态在地下水中的含量和分布，更好地研究砷在地下水中的循环和迁移转化机制，就必须发展高灵敏度、高选择性的砷形态野外快速检测技术。本项目制备与As(III)及As(V)具有特异性作用的有机官能团和纳米材料，合成有机分子探针及纳米探针，基于荧光增强或淬灭的开关机制，借助紫外、荧光等光谱模式探讨所合成的分子探针及纳米探针对不同砷形态的高灵敏度和高选择性快速检测能力，实现As(III)及As(V)的特异性检测及同时快速分析，检测限达到ppb级乃至ppt级，具有较强的选择性和可视化效果。同时，通过分子空间构象关系、官能团结构调控、分子聚集度和纳米粒子形貌结构等因素的研究，探讨有机分子及纳米探针对不同砷形态的光谱响应原理和识别机理。在所发展的有机分子和纳米探针基础上，构建便携易带的纸质传感器，研究它们对地下水中砷形态的野外快速检测性能。本项目提供了地下水砷形态的野外快速检测方法，为地下水中砷的环境毒性效应及其迁移转化机制的研究提供数据支撑，也为其风险评估及修复治理等重大社会需求提供技术保障。