改性石墨烯/双贵金属复合纳米材料的可控合成及其黄曲霉毒素生物传感器的构建研究

The synthesis and application of composite nano-sensing material related to Graphene noble metals is one of the advanced frontier subjects, which has important theoretical value and potential applications in various fields including food safety monitoring, environmental analysis and tests of clinical medicine, etc. However, the common sensing interface nanomaterials are inactivated by aggregated, difficult to controllable synthesis, and the sensitivity, selectivity, and biocompatibility need to be further improved. In this project, we plan to carry out a series of studies about synthetizing the modification or functionalization of graphene by various methods, explore their synthesis rules, controllable synthesis of functionalized graphene/bimetallic nanomaterials, and discuss their interaction mechanism and properties, constructe electrochemical biosensor and research its electrochemistry performance from the perspective of interdisciplinary. Graphene was functionalized by doping B or N atom, or coating conductive polymer, and to reveal the influence rule between the relevant parameters and the structure propermance of these composite nanomaterials, the relevant parameters including the doping concentrations, the modified density and reaction speed. Through regulate the interaction between graphene and nanoparticles to controlled load bimetallic nanoparticles on the surface of graphene, obtaining various sensing interface composite nanomaterials with higher specific surface area, excellent electronic conductivity, more catalytic activity site and outstanding biocompatibility. Finally, we will utilize the excellent composite nanomaterials to structure electrochemical biosensors, to detect the aflatoxin in complex samples of the food and environment. The research of this project has certain academic significance and important practical value in application subjects based on the new material, electrochemical, materials chemistry, food science, environmental science, and related applications.

基于石墨烯贵金属复合纳米传感材料的合成及应用，是食品安全监控、环境分析、临床医学检测等领域具有理论及应用价值的前沿热点课题。然而，常用传感界面材料存在易聚集失活，难以可控合成以及选择性、生物相容性不够高等问题。我们将从多学科交叉的角度，集中开展石墨烯改性合成及规律、功能化石墨烯/双贵金属复合纳米材料可控合成及作用机制、复合纳米材料电化学生物传感器构建及性能的研究。通过对石墨烯进行无机掺杂及聚合物包覆的功能化修饰，深入探讨掺杂浓度、修饰密度、反应速度等参数对复合纳米材料结构性能的影响规律，实现双金属纳米粒子的可控负载。获得具有更高比表面积、电子传导性、生物相容性及更多催化活性位点的传感界面复合纳米材料，并构建电化学生物传感器用于食品、环境等复杂样品中黄曲霉毒素的分析。本项目的研究，对基于新材料应用的电化学、材料化学、食品科学、环境科学等学科及其相关的应用领域具有重要的科学意义及实际价值。

通过对石墨烯进行无机掺杂、聚合物包覆、金属纳米颗粒负载等功能化修饰，对提高其比表面积、电子传导性、生物相容性及催化活性位点非常有利，可用于构建高灵敏度的电化学传感器，是目前分析学科的重要研究领域之一。本课题研究及优化了通过N、B、S-B掺杂及通过聚苯胺、聚对氨基苯甲酸、硫化钼等修饰的石墨烯功能化改性的方法，有效改进了石墨烯的性能。在此基础上有效负载金属纳米颗粒，制备了一系列具有比表面积、电子传导性、生物相容性及更多催化活性位点的传感界面复合纳米材料。基于这些修饰材料，构建了一系列检测黄曲霉毒素B1、芦丁、茶多酚等分子的电化学传感器。这些传感器具有良好的稳定性、重现性和较高的灵敏度，均用于实际样品的检测，具有良好的应用前景。通过本项目的实施，为石墨烯的功能化改性及其纳米传感界面材料的合成提供了新思路，拓展了黄曲霉素B1、芦丁、茶多酚等分子快速检测的电化学分析途径。同时，还开展了色谱分析、计算化学和活性分子合成方面的研究工作，为后续进一步的分子识别及其相关研究等奠定了前期基础。在本项目的资助下，发表论文近30篇，SCI收录论文23篇，电化学分析领域11篇（SCI收录6篇，按照中科院论文分区，一区1篇，二区2篇）；申请发明专利7项，获得授权3项，4项处于受理状态。对照计划任务，该项目完成了预期研究目标，取得了较好的研究成果。