受限空间下“水”增强石墨烯水凝胶去除典型抗生素类药物的吸附/解吸机理研究

Adsorption technology has broad application prospects in pollution control, and development of new and efficient high-performance adsorbents is the key factor to improve the adsorption process. Graphene-based gels have attracted extensive attention due to its superior properties, including high specific surface area, strong chemical activity, and easy recovery, etc. Although the weight percentage of moisture content for graphene gel can reach up to 90 wt%, basic research concerning the influence of water as the main component in gel on the gel’s adsorption characteristics and environmental behavior is still rare. By controlling different confined sizes and interfacial properties of confined carriers (Graphene), this study plans to explore the influence of “Water” under different confined space on adsorption characteristics and effects of antibiotics through experiments and theoretical simulations. Meanwhile, the relationships of micro/macro structure, interface process, and adsorption characteristics will be illuminated. By utilizing computer simulation and analysis techniques, such as synchrotron radiation, this study will reveal the driving force and adsorption/desorption mechanism of water-enhanced adsorption of antibiotics, clarify the interaction characteristics among antibiotics (collaboration/competition), and provide a theoretical basis for controlling the solid-liquid interface procedures in confined space of gels and improving adsorption properties in combined antibiotic pollution. The project will explore new ideas and methods for gel adsorbent enhanced by water in the compound pollution control, to explain and predict the adsorption in the real water environment, and to provide the theoretical and technical foundation for the removal of compound pollution in water supply and sewage treatment.

吸附技术在污染治理中具有广阔应用前景，研发高效吸附剂是高效能吸附处理技术的关键，石墨烯基复合凝胶因比表面积大、活性强、易回收等优良性能，受到广泛关注。然石墨烯基复合水凝胶含水率高达90 wt%，而对主要组份“水”对凝胶吸附特性的影响极其环境行为缺乏基础性研究。本课题以可控制备各类尺寸、界面性质受限载体（石墨烯）为基础，实验结合理论模拟，探讨受限空间下石墨烯水凝胶中“水”对抗生素的吸附特性影响及规律。阐明凝胶微/宏结构、界面过程及吸附性能间构效关系。利用计算机模拟和同步辐射等分析技术，揭示凝胶水增强吸附抗生素驱动力和吸附/解吸机理，阐明复合抗生素间作用规律(协同/竞争等)，为调控凝胶受限空间下固/液界面过程并提高抗生素复合污染吸附性能提供理论依据；探索“水”增强凝胶吸附特性在复合污染治理中新思路和新方法，解释和预测实际水体中吸附现象，为给水和污水处理中去除复合污染物提供理论指导和技术支持

吸附技术在水污染治理中具有广阔应用前景，研发高效吸附剂是高效能吸附处理技术的关键，石墨烯基复合水凝胶因比表面积大、活性强、易回收等优异性能，受到广泛关注，石墨烯基复合水凝胶含水率高达90 wt%，而对主要组份“水”对凝胶吸附特性影响及其环境行为缺乏研究。本课题研究表明石墨烯水凝胶对多种污染物呈现显著吸附增强行为，归因于限域下“水”对污染物的增强吸附作用。通过调节pH和石墨烯浓度等凝胶主要形成参数，实现对石墨烯水凝胶受限空间和受限水的调控；基于全反射红外和拉曼光谱，建立了石墨烯水凝胶中受限水的定性和定量分析方法，对石墨烯水凝胶受限空间和受限水结构变化进行剖析，明晰受限空间下“水”对抗生素等污染物的吸附特性影响及规律，阐明凝胶微/宏结构、界面过程及吸附性能间构效关系。基于多种表/界面微观分析和分子动力学模拟对石墨烯水凝胶富集抗生素的吸附机理开展研究，提出了氢键畸变、受限传输和骨架支撑三种限域吸附增强作用机制。采用高温水浴法实现石墨烯水凝胶的绿色再生，其原因归结于高温下氢键的破裂和受限水与自由水的转换，进一步采用物化学改性和能量场辅助手段提升石墨烯基复合凝胶对抗生素等污染物的吸附性能。上述工作开展为解释和预测实际水体中吸附行为提供理论指导，为限域下“水”增强凝胶吸附特性在水污染治理中的应用提供新思路和新方法。项目执行期内累计发表SCI论文共计28篇，其中包括Adv. Sci., Nano Let.,Water. Res. Environ. Sci. Technol (2篇), Research, J. Mater. Chem. A (2篇), Chem. Eng. J. (7篇), J. Hazard. Mater. (2篇)等期刊，均为JCR一区，授权中国发明专利共计6项。