选择性降解典型塑化剂可见光光电催化材料的制备与降解机理

Phthalates (PAEs) are worldwide pollutants, which have serious mutagenic effects on male reproduction and growth. Compared with the traditional TiO2 film, the photoelectrocatalytic activity of TiO2 nanotube arrays is higher. However, the pure TiO2 has no visible light response and no selectivity for the degradation of pollutants, thus hindering the degradation of high poisonous PAEs with low concentration. To improve the selectivity and visible-light activity of TiO2 nanotube arrays, Al3+, Fe3+ and Cu2+ will be doped into TiO2 nanotube arrays. This results in formation of Lewis acid sites and the reduction of TiO2 bandgap. The former can enhance absorption of PAEs (Lewis base) selectively due to Lewis acid-base action, and the latter can improve the visible-light activity. The doped TiO2 nanotube arrays will be used to perform selective photoelectrocatalytic degradation of PAEs under irradiation of visible light after a bias potential was applied, which can improve the separation efficiency of photogenerated carriers and the photocatalytic performance of TiO2 nanotube arrays. To investigate the photoelectrocatalytic mechanism of the doped TiO2 nanotube arrays, the generated active radicals will be detected during photoelectrocatalytic degradation. The intermediate products of PAEs in the course of degradation will be determined and analysised to investigate the photoelectrocatalytic degradation mechanism of PAEs. The implementation of this project will provide experimental data for the selective degradation of PAES, and the theoretical foundation for the preparation of photoelectrocatalytic materials for selective degradation of wastewater containing PAEs will be establised.

邻苯二甲酸酯类(PAEs)塑化剂是一种严重影响男性生殖和发育的全球性有毒污染物。TiO2纳米管阵列具有比普通TiO2膜更高的光电催化活性，但TiO2不能吸收可见光，且对污染物的吸附和降解没有选择性，阻碍了它对高毒性低浓度PAEs的高效降解。本项目拟在TiO2纳米管阵列中掺入Al3+、Fe3+和Cu2+，这些离子一方面能形成Lewis酸中心，能选择性吸附PAEs(Lewis碱)；另一方面能降低TiO2的禁带宽度，提高其可见光活性；再在这些掺杂的TiO2纳米管阵列上施加偏压，以提高光生载流子的分离效率和光催化效率，在可见光下选择性光电催化降解水中的PAEs。通过分析检测光电催化过程中的活性基团和PAEs降解过程中的中间产物，揭示这些TiO2纳米管阵列降解PAEs的光电催化机理。本项目的实施和完成将为PAEs污水的选择性降解提供实验数据，为设计、制备选择性降解PAEs的光电催化材料提供理论依据。

邻苯二甲酸酯类(PAEs)塑化剂是一种严重影响男性生殖和发育的全球性有毒污染物。TiO2 纳米管阵列具有比普通TiO2膜更高的光电催化活性，但TiO2不能吸收可见光，且对污染物的吸 附和降解没有选择性，阻碍了它对高毒性低浓度PAEs的高效降解。针对这些问题，本项目开展了如下工作：第一，以PAEs为模板分子，在TiO2纳米管阵列上沉积了能识别PAEs分子的TiO2纳米颗粒，制备了PAEs分子印迹型TiO2纳米管阵列，并通过光电催化选择性降解PAEs；第二，以PAEs为模板剂，在TiO2纳米管阵列中沉积能识别PAEs分子的聚吡咯，制备了PAEs分子印迹型聚吡咯/TiO2纳米管阵列，并通过光电催化选择性降解PAEs；第三，成功制备了ZnFe2O4/ZnO类芬顿光催化材料，并用于降解PAEs。目前已取得了良好的进展，完成了项目的预定研究任务和目标。已成功开发出了几种高效的光催化材料，这些材料可以有效地选择性光电催化降解PAEs。该项目的完成为开发新型选择性光电催化材料的设计和制备提供了新方法。主要研究成果包括有9篇SCI收录论文，发表在《Applied Surface Science》、《Materials Research Bulletin》、《稀有金属材料与工程》、《Materials Letters》、《Journal of Alloys and Compounds》、《Ceramics International》等期刊上。