高效选择性吸附有机物的三维柱撑石墨烯复合材料的可控组装及其吸附作用机制研究

Synthesis of adsorption materials with high efficiency, good selectivity and recoverability is the key problem in removing organics from water environment. Graphene has large specific surface area, however, it shows low adsorption selectivity, and it is also easy to be aggregated and difficult to recycle, which raises a lot of practical problems. By assembly of nanoparticles, polymers or carbon nanotubes into the layers of graphene, this project brings forward a new conception of construction of novel three-dimensional pillared graphene composites with high efficiency and excellent selectivity for adsorption of organics. As for controllable synthesis of graphene oxide, microwave assisted stripping of graphite oxide is to be further studied. The controllable synthesis of reduced graphene and functionalized graphene is also to be investigated. Systematic studies are carried out for the assembly of three-dimensional pillared graphene composites, and some novel approaches and methodologies for regulating and controlling their chemical compositions, structural morphologies are expected. To explain the relationship of "pillaring materials-microstructure-structure morphology-adsorption performance" and uncover the selective adsorption mechanisms, the correlation between chemical composition,structure morphology and adsorption performance is to be analyzed. The key scientific problems are to be solved include establishing a controlled assembly method for preparation of three-dimensional pillared graphene composites and construction of composite models with excellent adsorption performance. The achievements of the project are of great significance in developing novel adsorbing materials and promoting the development of related research fields.

合成选择性良好、可回收利用的高效吸附材料是吸附分离水环境中有机物的关键技术难题。基于石墨烯具有巨大比表面积但易团聚、吸附选择性较差、不易回收等实际问题，本项目提出将纳米粒子、聚合物、碳纳米管等分别组装至石墨烯片层间，构建可高效选择性吸附有机物的新型三维柱撑石墨烯复合材料。深入研究微波辅助法剥离氧化石墨制备氧化石墨烯的可控合成方法，探讨还原石墨烯、功能化石墨烯的可控合成，系统研究三维柱撑石墨烯复合材料的组装工艺，找到调控其化学组成、结构形态的途径与方法。通过分析三维柱撑石墨烯复合材料的化学组成、结构形态与其吸附性能的关系，解析"柱撑材料-微观结构-结构形态-吸附性能"之间的相关性，揭示其选择性吸附有机物的机理机制。拟解决的关键科学问题是建立三维柱撑石墨烯复合材料的可控组装方法，以及构建吸附性能优良的复合材料模型。项目成果对于开发新型高效选择性吸附材料，推动相关研究领域的发展等有重要意义。

完成了氧化石墨烯的制备工艺改良，该工艺路线稳定，所制得的氧化石墨烯层数可控，分散性良好。探讨了卤化石墨烯的制备工艺，研究了不同卤化官能团对其吸附性能的影响。探讨了无机粒子与石墨烯/氧化石墨烯/功能化石墨烯的组装，表征了复合材料的结构和化学组成，考察了材料的吸附性能/电化学识别性能。将生物有机聚合物分子与氧化石墨烯水热组装，制备了多种新型3D石墨烯复合材料，表征了复合材料的结构和化学组成，考察了材料的吸附性能/电化学识别性能。研究了碳纳米管与氧化石墨烯/功能化石墨烯的自组装，所得复合材料可用于吸附/电化学传感。深入分析了3D石墨烯复合材料的组成、结构形态等与其对不同有机物的吸附性能，研究了结构与吸附特性的相互关系与规律，揭示了吸附机理机制，为构筑吸附性能优异、可回收利用的高效吸附材料提供了有用参考。