高孔隙率氧化石墨烯宏观气凝胶对典型抗生素类药物吸附机制研究

About 90% or more of widely used antibiotics cannot be absorbed by organism and discharged into the environment in primary form or as metabolites, leading to increasingly serious antibiotic pollution. The proposed project will investigate and apply new 3D carbon material - graphene oxide macro aerogel (GMA) to protect water environment. We use graphene oxide (GO) to design macro-scale nano-adsorbents, taking advantage of GO characteristics of high reactivity and high specific surface area, to efficiently solve the problems of easy aggregation, separation difficulty and G nano-residual toxicity. We further systematically design GMA structure and chemically modify the structure to develop high adsorption capacity materials for antibiotics. Then we will study the performance and regularity of antibiotics adsorption on GMA under a variety of environmental conditions (heavy metals, natural organic matter etc.), to uncover relationship between the physical and chemical properties of GMA and the adsorption properties of antibiotics. The project will use surface analysis methods such as synchrotron radiation, X-ray photoelectron spectroscopy and high- resolution nuclear magnetic resonance spectrometer, to study the internal and surface adsorption behavior and microcosmic mechanism of antibiotics in GMA in molecular level under the co-existence of heavy metals or natural organic matter. Our study will provide scientific basis and theoretical guidance for the synthesis of high capacity and selective adsorption materials and wide application of GMA in environment adsorption field.

抗生素被广泛应用，约90%以上的抗生素不能完全被机体吸收，以原形或代谢物形式排入环境，导致抗生素污染日趋严重。本项目将新型三维碳纳米材料-氧化石墨烯宏观气凝胶(GMA)应用于抗生素污染治理问题，利用氧化石墨烯(GO)构筑三维宏观气凝胶吸附剂，利用GO高比表面积和高化学活性特性，有效解决GO粉体在水中易团聚、难分离及残留GO纳米毒性等问题。针对GMA开展结构设计和化学修饰等基础研究，实现针对抗生素高容量吸附剂的开发。探讨多种环境因素如重金属、天然有机物影响下，GMA对抗生素吸附性能的影响和变化规律，揭示GMA物化性质与抗生素吸附性能间构效关系。利用同步辐射技术、X射线光电子能谱、高分辨核磁共振谱仪等表面分析方法，从分子水平上探讨重金属或天然有机物共存条件下，抗生素在GMA内部及表面的吸附行为及微观作用机制，为制备高容量、选择性宏观吸附材料及GMA在环境吸附领域的应用提供科学依据和理论指导。

随着抗生素的大量使用，抗生素环境污染问题日趋严重。石墨烯具有优异的物化特性和突出的吸附性能，在吸附领域具有良好的潜在应用前景。本课题针对抗生素污染问题，基于石墨烯纳米材料单元，通过水热还原法自组装构建高孔隙率石墨烯基三维宏观凝胶吸附体系，成功实现碳纳米粉体吸附材料的三维宏观化，有效解决优异碳纳米粉体吸附剂在水中易团聚、难分离等问题，并利用X射线光电子能谱、傅里叶变换红外光谱仪、计算机模拟等多角度探讨了抗生素在石墨烯凝胶内部及表面的吸附行为及微观作用机制。为解决石墨烯水凝胶不易储存而气凝胶吸附性能低的问题，将具有优良吸附性能的碳纳米管掺杂到还原的氧化石墨烯气凝胶中，利用碳纳米管一维纳米材料和石墨烯气凝胶二者的协同增效作用使其吸附性能大幅提高。针对吸附剂循环利用问题，提出光催化再生吸附材料的理念，制备磷酸银改性石墨烯凝胶，有效实现在可见光和紫外光下吸附剂使用后多次再生。通过三维高孔隙率石墨烯基凝胶的构建及其对抗生素微观作用机理研究，为调控石墨烯凝胶界面特性并提高对抗生素类污染物吸附性能提供理论依据，对高容量、选择性石墨烯基复合材料在环境领域的应用及处理实际抗生素废水具有重要的理论价值和现实意义。