基于四环素类抗生素残留光解的嵌入式磁性印迹光催化剂的制备及其选择性吸附/光解行为和机理研究

For the purposes of not only enhancing the photocatalytic activity but also improving the selectivity, meanwhile, simplifying the preparation process; Combining with the characteristics of easy separation and recovery of magnetic fly-ash, the advantages of high efficiency, environment friendly of the photocatalytic technology, the optical response properties of noble metal loaded conductive polymer and the specific recognition properties of surface imprinting technique; This project was designed to use magnetic fly-ash as the carrier, noble metal loaded conductive polymer as the functional monomer and catalytic material, tetracycline antibiotic residues were imprinted onto the magnetic fly-ash by using the surface imprinting technique. Finally, the magnetic imprinted photocatalyst embedded within noble metal loaded conductive polymer was obtained, which solved the problem of the difficult recovery, the tedious preparation process, the poor photocatalytic activity and poor selectivity of common photocatalyst. Researched the different materials and different synthetic methods of the magnetic imprinted photocatalyst embedded within noble metal loaded conductive polymer; researched the energy level structure, the rule of electron transfer, the production rate of radical, the catalytic ability and the embedding mechanism of the noble metal loaded conductive polymer; researched the interface relationship, bonding regularity and mechanism of different layers and different materials; researched the relationship between the selective adsorption and the selective photodegradation; researched the selective adsorption/photodegradation kinetics/thermodynamic behavior, the mechanism of selective adsorption/degradation and the intermediate degradation products onto the tetracycline antibiotic residues.

本着既提高选择性又提高光催化活性，同时简化制备过程的目的，结合磁性粉煤灰易于分离回收的特点，光催化技术高效、环境友好的优点，贵金属负载导电聚合物的光响应性能以及表面印迹技术的专一吸附性能，本课题拟采用磁性粉煤灰为载体，贵金属负载导电聚合物为功能单体及催化物质，利用表面印迹技术印迹四环素类抗生素，来构建贵金属@导电聚合物嵌入式磁性印迹光催化体系，以解决普通光催化剂分离回收难、制备过程繁琐、光催化活性低及光催化降解无选择性等问题。研究不同材料、不同方法制备的贵金属@导电聚合物嵌入式磁性印迹光催化剂；研究贵金属负载导电聚合物的能级结构、电子转移规律、产自由基速率、催化能力及嵌入机制；研究各层、各物质之间的界面关系、作用机理及成键规律；研究选择性吸附和选择性光降解的相互关系；研究选择性吸附/光降解四环素类抗生素残留的动力学/热力学行为、选择性吸附/降解机制以及中间降解产物机理等。

本着既提高选择性又提高光催化活性，同时简化制备过程的目的，结合磁性材料易于分离回收的特点，光催化技术高效、环境友好的优点，导电聚合物的光响应性能以及表面印迹技术的专一吸附性能，本课题以磁性复合光催化材料为基体，再以导电聚合物为功能单体，利用表面印迹技术印迹特定抗生素，构建了一系列具有特定专属活性位点的便于分离回收再利用的嵌入式磁性印迹光催化剂（如：PPy@CdS@MFA印迹光催化剂、Ag-PEDOT/ZnFe2O4有机印迹复合光催化剂、导电印迹Ag@PANI/CoFe2O4/C光催化剂、Ag-POPD/CoFe2O4有机印迹复合光催化剂、导电印迹SiW/Fe3O4/C复合光催化剂、POPD-CdS异质结嵌入式磁性印迹光催化剂），解决了普通光催化材料分离回收难、制备过程繁琐、光催化活性低及光催化降解无选择性等问题。阐述了不同材料、不同方法制备的嵌入式磁性印迹光催化剂；阐明了研究各层、各物质之间的界面关系、作用机理及成键规律；系统研究了光催化材料的能级结构、电子转移规律、产自由基速率、催化能力，以及导电聚合物的嵌入机制；深入考察了选择性吸附和选择性光降解的相互关系、选择性吸附/光降解抗生素残留的动力学/热力学行为、选择性吸附/光降解机理以及抗生素残留的降解中间体等。所制备的一系列嵌入式磁性印迹光催化剂不仅具有较高的光催化活性、较好的稳定性，还对特定目标抗生素具有较强的选择性。通过本课题的实施为嵌入式磁性印迹光催化的研究提供了可靠依据，为印迹光催化领域的发展提供了新思路，并为印迹光催化材料治理其它目标污染物奠定了理论和实践基础。