纳米金属/合金的原位形貌调控制备及酚类污染物电化学传感

In order to develop highly sensitive and catalytic electrochemcial sensing materials for the rapid detection of trace phenolic pollutants, metal and alloy nanoparticles (such as Pt, Pd, Pt-Cu) with high stability and reproducibility, would be in-situ prepared on the surface of traditional electrodes based on the electrochemical reduction. Moreover, the shape and particle size would be tuned through electrochemical/chemical methods, and the mechanism and technology are to be developed for the preparation of morphology-controlled metal/alloy nanoparticles. To obtain the unique enhancement effects, facilitating electron transfer and accumulation, the electrochemical sensing properties of different-shaped metal/alloy nanoparticles are going to be investigated in detail. As a result, the morphology-dependent electrochemical sensing theory for metal/alloy nanoparticles would be developed. After that, the electrochemical behavior, sensing and signal transfer mechanisms of phenolic pollutants, including bisphenol A, chlorophenol and so on, could be studied on the surface of different-shaped metal/alloy nanoparticles. Finally, novel theory and method for the highly-sensitive electrochemical detection of phenolic pollutants is going to be established, then the new nano-electrochemical sensors would be constructed for the rapid and in-site determination of phenolic pollutants, which could be used in environmental water samples. In this work, the obtained morphology-controlled preparation method, morphology-dependent sensing theory and enhancement mechanism are helpful to develop novel electrochemical sensors. Meanwhile, it is of great theoretical and practical significance to develope new method and new technology for the rapid and in-situ detection of environmental pollutants.

为研发高灵敏、高催化活性的优控酚类污染物电化学传感材料，实现痕量快速检测，基于电化学还原在常规电极表面原位制备出高稳定性、高重现性的纳米Pt、Pd、Pt-Cu等敏感材料，利用电化学/化学手段调控其形状及颗粒大小，获得形貌可控纳米金属/合金的原位制备原理和技术。系统研究不同形貌纳米金属/合金的电化学传感特性，深入认识二者内在规律，获得纳米增强效应、纳米界面加速电子转移效应和纳米富集效应，建立纳米形貌电化学传感新理论。研究优控酚类污染物（如双酚A、氯酚等）在不同形貌纳米金属/合金表面的电化学行为、敏感机理和信号转换机制，建立高灵敏电化学检测新理论和新方法，构建新型酚类污染物现场快速监测的纳米电化学传感器，用于环境水体分析。 课题所获得的形貌可控制备原理、纳米形貌传感理论和增敏机理有利于构筑更广泛的纳米电化学传感器。同时，为环境污染物的现场快速检测提供新方法和新技术，具有重要的理论和现实意义。

通过电化学方法制备了纳米碳管/金复合材料；通过热解法制备了生物碳/金复合材料和三维相互连通的多孔碳。利用电镜、XPS、XRD、红外光谱、拉曼光谱、N2吸附-解吸等实验手段，对这些材料进行了表征。通过调控电化学参数、热解温度、热解时间等条件获得了重现性好，性能优良的材料。这次材料被用于电化学测定酚类污染物。研究结果发现碳纳米管/金、生物碳/金和三维相互连通的多孔碳修饰电极对对苯二酚和邻苯二酚等酚类污染物检测限度低，灵敏度高，且可以用于环境水体的分析。课题所获得材料的制备方法和增敏机理有利于构筑更广泛的纳米电化学传感器。同时，为环境污染物的现场快速检测提供新方法和新技术，具有重要的理论和现实意义。