具有可见-近红外光谱响应的碳量子点基复合光电材料合成及构建多氯联苯光电化学传感器研究

Polychlorinated biphenyls (PCBs) and other classic persistent organic pollutants, are one of the major problems of the environment pollution. The target of this project is to establish the trace PCBs detection method using photoelectrochemical technique. We first will design and synthesis carbon quantum dots and its composite photoelectric nanomaterial with spectral absorption in visible and near infrared region and upconversion luminescence properties; and modify these composite photoelectric nanomaterial with functional groups. Combined with the photoelectric catalysis and electrochemistry analysis technique, we will study the dechlorination degradation process and dechlorination mechanism of PCBs using synthesized composite nanomaterials, reveal the photoelectrochemical degradation process, photocurrent signal generation principle and the photocurrent signal sensitive mechanism toward PCBs; and establish a new photoelectrochemical method detecting PCBs rapidly and selectively in the visible and near infrared region. Our research work also provide a technical and theoretical support of the development of photoelectrochemical detection of PCBs directly using of solar light source with high selectivity, fast trace and online. At the same time, we could develop a new photoelectric degradation (management) principle and technology of PCBs based on carbon quantum dot materials through the study of photocatalytic process and the mechanism of PCBs, and provide a new way to explore the photoelectric detection and degradation of PCBs synchronous in environmental water sample.

多氯联苯（以下简称PCBs）等持久性有机污染物是目前面临的环境污染重大问题之一。本项目以建立水体中PCBs快速、痕量光电化学检测新方法为目标，首先设计合成具有可见及近红外区域光吸收和上转换发光性质的碳量子点及其复合光电纳米材料，并进行表面功能化修饰；然后结合光电催化技术和电化学分析技术，研究复合材料对PCBs光电催化降解脱氯的过程和降解机理，揭示光电降解过程中，光生电流信号的产生原理及对PCBs的敏感机制规律；建立在可见及近红外区域对PCBs进行高选择性快速、痕量光电化学检测的新方法，为发展直接利用太阳光源对PCBs进行高选择性快速、痕量、在线光电化学探测提供技术支撑和理论基础。同时本项目通过对PCBs光电催化脱氯降解的过程及机理的研究，也发展了基于新型碳量子点基光电材料催化降解（治理）PCBs的原理和技术，为探索实现环境水体中PCBs的光电检测、治理二位一体同步进行提供了新思路。

本项目执行期间重点开展了针对水体中多氯酚和农药残留等有机污染物和重金属离子的识别与检测研究。运用绿色纳米合成技术等手段，设计并制备了一系列对目标污染物具有高选择性和高灵敏识别能力的碳量子点、超薄二维纳米片等传感材料，并进行功能化和复合化，研究其传感分析性能。主要研究成果包括发展了各种碳源制备碳量子点的方法，制备了几种具有高比表面积的二维类石墨烯材料，发展碳量子点与类石墨烯二维薄片纳米材料的复合光电材料对五氯酚等污染物的光电传感分析的新方法；发展了系列有机-无机杂化纳米结构电化学传感材料方法和原理，构筑应用于水体中污染物电化学传感检测方法；设计制备了几种纳米复合光催化材料，探索其水体中有机污染物的降解治理中应用。通过本项目的研究，为探索制备新型具有高选择性的识别能力的碳量子点基光电化学纳米传感技术，试验水体中有机无机污染物快速、痕量、在线光、电化学探测提供了理论和技术支撑。 上述研究取得了多项具有系统性和创新性的研究成果，在Electrochim. Acta，RSC Advances, J. Electrochemical Society，Anal. Methods和Materials Science & Engineering B等国内外材料和分析化学和材料刊物上发表论文12篇，其中被SCI收录11篇，EI 收录1篇；发表会议论文2篇（墙报）。此外，投稿在审论文2篇；申请国家发明专利1项（实审中）。