纳米晶嵌入式生物质碳基气凝胶的构筑及其吸附-光催化协同去除水体中氟喹诺酮抗生素的机制研究

The project is aimed at the efficient removal of fluoroquinolones antibiotics in wastewater using the aerogel materials with adsorption-photocatalytic integration, high efficient and low-cost. The biomass-derived carbonaceous aerogels are constructed by cucurbitaceae plants’ peels. Employing the carbonaceous aerogels acted as carbonaceous skeleton combined with nonhydrolytic sol-gel process to control the synthesis of semiconductor nanocrystals embedded biomass-derived carbonaceous aerogels. Meanwhile, we will propose the formation mechanism of carbonaceous aerogels composite materials to realize the control of microstructure. The relationship among composition, structure and property of semiconductor nanocrystals and carbonaceous aerogels composite will be deeply studied through investigating the effect of crystal forms, size of catalysts on optical property, adsorption property and photodegradation performance. Furthermore, the synergistic effect between the interface of carbonaceous aerogels and nanocrystals will be discussed, and the enhanced adsorption-photocatalytic mechanisms and promoted photoinduced carriers separation will be also investigated. The adsorption-photocatalytic degradation efficiency, conversion process and reaction kinetics of fluoroquinolones antibiotics will be explored. The internal mechanism of removal of fluoroquinolones antibiotics by the carbonaceous aerogels composite photocatalysts will be revealed. These project data can also provide important theory and experimental basis for designing novel aerogel materials.

本项目以水体中氟喹诺酮类抗生素的高效去除为目标，构建吸附-光催化一体化的高效、低成本气凝胶材料。拟使用葫芦科植物果皮构建生物质碳基气凝胶，并以该碳基骨架为基体结合非水解-溶胶法构筑半导体纳米晶嵌入式生物质碳基气凝胶材料，阐明碳基复合气凝胶的形成原理，并实现其微观结构调控。通过研究半导体纳米晶及生物质碳基气凝胶复合材料的晶型、尺寸等微观结构对光学特性、吸附性能和光催化降解性能的作用规律，深入研究其组成-结构-性能三者间的相互关系。研究碳基气凝胶和纳米晶相互协同作用机理和吸附-光催化性能增强原理，分析碳基复合气凝胶中光生载流子分离效率增强的机制，阐明其吸附-光催化协同作用的本质机理。研究纳米晶嵌入式生物质碳基气凝胶复合材料对氟喹诺酮类抗生素的吸附-光催化降解转化过程及其反应动力学模型。揭示碳基气凝胶复合光催化剂去除氟喹诺酮类抗生素的内在机理，为设计新型气凝胶材料提供理论依据和实验参数。

气凝胶是一类具有低密度和高比面积的三维纳米网络结构的新型纳米材料，在环境、催化、能源等领域有着广泛的应用前景。为了解决现有炭气凝胶制备过程中存在合成时间长，干燥成本高、微纳米结构控制难等瓶颈问题。.本项目采用葫芦科植物果皮构建生物质碳基气凝胶，并以该碳基骨架为基体结合原位合成法构筑半导体纳米晶嵌入式生物质碳基气凝胶材料（SN-BCA），致力于新型碳基复合气凝胶材料的创新设计制备及其构效关系研究。.利用溶胶-凝胶法、水热/溶剂热成功实现了纳米晶嵌入式生物质碳基气凝胶的有效合成,并显著提升了气凝胶材料的吸附-光催化降解性能，能有效去除水环境中抗生素类污染物。表征结果显示，此类复合气凝胶具有低密度、大比表面积等显著特征，且半导体纳米晶均匀嵌入在三维网络结构上。同时围绕原位合成控制合成半导体纳米晶，开展了系列工作实现生物质碳基气凝胶复合材料的控制合成，筛选出高能效、高稳定性的光催化材料，应用于高效吸附-光催化协同降解环境有机污染物。.在此基础上，系统研究纳米晶嵌入式生物质碳基气凝胶材料的比表面积与其吸附性能间的关系；探讨复合气凝胶的价带-导带结构对其光化学性能的影响，弄清其协同催化机理以及影响规律。为制备具有制作简单、成本低廉、性能优良的碳基复合气凝胶新材料提供科学支撑。.除此之外，以石墨烯、氧化硅等基础单元为研究对象，制备了半导体纳米晶嵌入石墨烯气凝胶和多元氧化物气凝胶材料，对多组分之间的协同作用和耦合机制进行了系统研究，进一步研究气凝胶在吸附和催化领域性能提升的本质。在本项目资助下，项目组在Appl. Catal. B-Environ., Nanoscale, J. Colloid. Interf. Sci., Adv Powder. Technol., Mater. Sci. Eng. B-Adv., J. Mol. Liq.等国内外学术期刊发表SCI论文34篇，获授权专利2件。