一锅法制备石墨烯三元纳米复合材料及其电化学传感性能

The research on preparation, nanostructure fabrication and properties of novel graphene (GE)-based composites is still the hotspot in the field of GE materials. In comparison with GE binary composites, relatively little attention has been paid to the research of GE ternary composites, due to their relatively tedious and complex preparation process and poor structure and performance controllability. As one facile, rapid and clean synthetic technique, the one-pot method provides new ideas for the fabrication of novel materials with complex and outstanding construction. This project aims to fabricate GE-based ternary nano-composites with 3D, porous and hierarchical structure facilely and rapidly, based on GE, conducting polymers (CPs) and noble metal nano-particles (NMPs) via one-pot method. The obtained composites are used as electrode materials to fabricate electrochemical sensor, and their electrochemical sensing performance will be systematic investigated. Through the design of the experiment program, it is to hope that the obtained NMPs/CPs/GE nanocomposites not only possess typical 3D nano-structure, but also combine the high electrical conductivity, huge specific surface area and high electronic properties of GE, with the characteristic redox reversibility and abundant electronic band structure of CPs and the high electrocatalytic activity of NMPs, achieving the effective complement of the structures and properties of each components. In addition, the influencing factors on the nano-structure fabrication and electrochemical sensing performance and the interactions between NMPs, CPs and GE will be intensively investigated. The obtained results will provide theoretical and experimental supporting for the fabrication of GE-based multivariate composites and their application in electrochemical sensor.

新型石墨烯复合材料的制备、结构及性能依然是石墨烯类材料领域的研究热点。与石墨烯二元复合材料相比，石墨烯三元纳米复合材料由于其制备过程较繁琐、复杂，结构与性能可控性差而研究相对较少。“一锅法”作为一种简便、快速、清洁的合成技术，为新型复杂结构材料的制备提供了新思路。本项目旨在以石墨烯及其衍生物、导电聚合物单体、贵金属前驱体盐为主要原料，通过“一锅法”可控制备具有特定三维多孔纳米结构的新型石墨烯三元复合材料，研究其作为电极材料的电化学传感性能。预期所得复合材料不仅具有特定的三维多孔纳米结构，且能秉承各组分的优异特性（高导电性、大比表面积、优异电化学性能、高电催化活性、高可分散与可加工性能等），进而有助于提高复合材料修饰电极的电化学传感性能，并深入系统研究复合材料结构、组成对其传感性能的影响。本实验所得结果对石墨烯三元纳米复合材料的可控制备及性能研究具有理论和实践借鉴意义。

新型石墨烯复合材料的制备、结构及性能依然是石墨烯类材料领域的研究热点。本项目通过“一锅法”制备出了一系列三元纳米复合材料：Pd-PEDOT/GE、Pt-PEDOT/GE、Au-PEDOT/GE、Pd-Au/PEDOT/GE、SnO2/PEDOT/GE、TiO2/PEDOT/GE、Fe2O3/PEDOT/GE，通过改变制备方法、实验条件及材料各组分间的配比对所得复合材料的形貌、结构及性能进行调控，最终得出Pt-PEDOT/GE、Au-PEDOT/GE、Pd-Au/PEDOT/GE及Fe2O3/PEDOT/GE复合材料均表现出独特的三维、多孔纳米结构，且Pt-PEDOT/GE、Au-PEDOT/GE、Pd-Au/PEDOT/GE对于咖啡酸均表现出较优越的电化学传感性能，而Fe2O3/PEDOT/GE对咖啡因表现出较优异的电化学传感性能。GE较高的比表面积和PEDOT可控的形貌结构提高了贵金属纳米粒子和Fe2O3粒子在PEDOT/GE中的分散性，使其表现出较高的电化学活性面积和电催化活性。另一方面，由于PEDOT较强的电负性和GE较高的导电性能，贵金属纳米粒子和Fe2O3粒子与PEDOT、GE间存在的电子协同效应进一步增强了材料的电催化活性，从而使复合材料的电化学传感性能得到进一步提高。以上所得复合材料的成功制备对未来石墨烯三元纳米复合材料的可控制备及性能研究具有理论和实践借鉴意义。复合材料较高的稳定性和可处理性，使其修饰电极有希望应用于食品中咖啡酸、咖啡因的电化学检测和分析。