三维石墨烯基光电多元化重金属富集传感器的构建及应用研究

Nowadays, human existence and health are being severely threatened by more and more serious soil, food and water pollution by heavy metal ions. So, to develop a novel method for rapidly and efficiently detecting heavy metal ions will be of great consequence, which is necessary to protect the environment and to promote the social sustainable development..On the basis of photoelectric sensor theory, surface science, separation science and nano effects, some recognition groups will be constructed to coordinate with the heavy metal ions selectively on the Gaussian 09 software suite with a B3LYP/6-31G level of theory, which are further to be modified onto the three-dimensional graphene substrate by d-π-conjugation, π-π stacking or coordination bond self-assembly. All the composites are of environmentally friendly, high stability, strong adsorption capacity, and especially taking photoelectric chemical reaction before or after heavy metal adsorption or desorption occurred on the surfaces of the functionalized porous graphene composite. All the effect of the morphology of the substrate, chromophore species and the interaction between components on selective adsorption properties of heavy metal and the photoelectric property will be investigated in detail for revealing the mechanism of synergetic photoelectric sensing for offering the theoretical foundation to construct new sensing materials in future. We also explore carefully the influence factors on enrichment capacity to optimize experimental conditions for realizing efficient photoelectric enrichment and detection of heavy metal contamination by paper-based sensors, electrochemical sensors and traditional colorimetric sensors as well. Combined with nano effect, the adsorption/desorption mechanism will be further explored to achieve the purposes for separating heavy metal contamination and recycling sorbents. .In conclusion, a novel preparation and application technology of three-dimensional porous graphene functionalized by different chromophores for synergistic enriching, sensing and separating heavy metal ions have been developed, accordingly, which aims to protect human living environment, and to promote social sustainable development.

研究开发一类快捷高效富集检测与分离重金属污染的光电传感新技术，是有效防控日趋严重的重金属污染关键环节之一。项目依据光电传感理论、表面科学、分离技术和纳米效应，优化设计系列选择性配位识别重金属的功能生色团，通过配位键或d-π共轭、π-π堆叠自组装将生色团可控修饰到三维石墨烯多孔纳米基底上，构筑一类选择性高、吸附能力强、特别是能因重金属的吸附或脱附发生光、电化学信号协同增强的三维石墨烯基复合材料；探讨基底的形貌、生色团种类、作用力方式等对选择性富集识别重金属的影响，揭示组分间协同光电富集传感的机理，为高性能光电传感材料的构筑奠定理论基础；探讨复杂样品（土壤、食品或污水）预处理的方法及富集吸附/脱附的机制；探索除传统比色传感方法外，将复合材料修饰到普通滤纸上做成便携式纸基传感器或修饰到玻碳工作电极上作为电化学传感器，实现快捷高效地光电化学法富集传感与分离重金属和循环利用传感材料的目的。

设计合成系列光电性能良好、能选择性配位识别重金属的Schiff 碱、偶氮、荧光素、贵金属纳米和纳米Ag2S，Co3O4，IrO2等有机、无机生色团，进一步通过d-π共轭、π-π堆叠和配位键等非共价键自组装或共价键修饰到高分子壳聚糖、聚丙烯酰胺、石墨烯、二维氧化物或普通试纸上，可控构筑一类能选择性富集识别重金属，尤其是能因重金属等污染物的吸附或脱附而发生显著光电化性能改变的感材料；在对其材料的结构、性能详细表征和测试的基础上，从反应原理入手，讨论了体系的pH值、离子强度、反应时间及共存物质的干扰等影响因素，成功地应用于对重金属Hg2+、Cu2+、Co2+、Fe3+、Fe2+以及S2–、NO2–、F–、H+和有机污染物氨基苯酚、尿素等的光电检测上，检测线均满足国际卫生组织所规定的健康标准，通过简单物理方法实现富集分离重金属污染物和回收再利用传感材料的目的，开发一类新型协同增强重金属富集传感光电材料的制备与应用新技术。已培养硕士研究生2名（参与研究生共6名），优秀本科毕业论文3人次，获得大学生挑战杯山东省一等奖1次；发表SCI 论文22 篇（SCI>3 的18 篇，其中SCI 二区 TOP以上11篇），申请国家发明专利8 项（已授权4 项）。