介孔铋系可见光催化材料晶面调控和改性对高效去除水中低浓度典型药物类污染物的作用研究

The photocatalytic degradation of organic contaminants is a promising technology for wastewater treatment. Suffering from low reaction selectivity and photocatalytic efficiency, it is difficult to efficiently remove low concentration refractory organic contaminants such as pharmaceuticals. Hence, it is urgent to design a novel efficient and selective technology for these pollutants. This project is to design and synthesize mesoporous bismuth based visible light photocatalysts such as BiVO4 and BiOX (X=Cl, Br, I) through facet engineering and surface modification. Using a variety of characterization techniques in aid of theoretical chemistry calculation method, the prepared mesoporous bismuth based visible light photocatalysts are explored. The effect of the exposed facet structure, oxygen vacancy concentration, single-atom metal co-catalysts on the selection and formation efficiency of active species formation are investigated. Also, the effects of pore structure, acid-base properties, hydrophobic effect on selective adsorption of typical pharmaceutical contaminants are studied. We try to clarify the nature of the prepared mesoporous bismuth based photocatalysts with high visible light activity, selective adsorption to pollutant molecules, and strength active species formation. A new wastewater treatment method for the removal of low concentration pharmaceutical contaminants with functions of selective adsorption enrichment and visible light photocatalytic degradation. This project is of great theoretical and practical value to solve the problem of environmental pollution and energy shortage.

环境光催化是一种有广泛应用前景的污染去除技术，但是针对水中低浓度难降解有机污染物（如药物类污染物）处理面临选择性不高和光催化效率低的瓶颈，迫切需要建立新型的高效选择性去除污染物的方法。本项目利用晶面调控和表面改性等方法可控制备介孔铋系可见光催化材料（BiVO4和BiOX（X=Cl,Br,I）），采用多种检测技术手段结合理论化学计算方法进行介孔铋系光催化材料性能研究，探索介孔铋系光催化材料的晶面结构、表面氧空位和表面单原子分散金属助催化剂等因素对反应活性物种生成效率的影响规律，考察材料孔道结构、酸碱性和疏水性等特性对典型药物类污染物选择性吸附作用，阐明介孔铋系光催化材料的高可见光活性、污染物分子选择性吸附以及反应活性物种强化生成的微观本质，提出具有选择性吸附富集-可见光催化降解特征的高效去除水中低浓度难降解药物类污染物的新方法，这对解决环境污染和能源短缺问题具有重要的理论意义和实用价值。

本项目针对水中低浓度抗生素等药物类污染物难去除的问题，发展了介孔铋系可见光催化材料形貌和晶面调控方法，提出了具有选择性吸附富集-可见光催化降解特征的高效去除水中低浓度难降解药物类污染物的新方法。首先，基于吸附富集策略，通过表面缺陷构筑、比表面积增加、多级孔道分布和材料复合对铋系材料进行修饰和调控，提高了对特征污染物分子的吸附容量和效率，增强了对水中低浓度药物类污染物去除能力，并为后续的污染物光催化降解提供了基础。其次，通过元素掺杂、氧空位、金属助催化剂、异质结和能带调控等技术方式，增强光催化材料在可见光区的利用效率，同时提高了反应活性物种（超氧自由基、羟基自由基、空穴等）的生成效率，从而实现水中低浓度药物类污染物的高效降解。最后，构建了吸附富集-催化降解污染物的光催化技术，从光能利用、污染物吸附与降解和活性物种生成角度，实现了对水中药物类污染物的有效去除，为绿色光催化净水机制提供了参考。