g-C3N4/Ag2ZrO3复合材料的构建及其对含氮杂环化合物的光催化降解机理研究

The wastewater from military energetic material production is a kind of special wastewater with less consideration. Nitrogen heterocyclic compounds are common organic pollutants in the wastewater. The chemicals with this type of structure often have the properties of good chemical stability, bad biodegradability, with the toxicities of mutagenic, teratogenic and carcinogenic. The conventional technologies for common wastewater treatment may not work properly and effectively. Therefore, construction and preparation of composite photocatalytic materials with high efficiency of solar energy utilization and good effect of degradation for this type of special chemicals has practical significance..Taking g-C3N4 and Ag2ZrO3 as the basic materials, this project is aimed at the construction for serials of g-C3N4/Ag2ZrO3 composite catalytic materials. The structure and the appearance of the materials may be evaluated by using apparatus such as XRD, SEM and EDX. The material properties of response to UV-Vis, degradation effect, the relationship with the constitution, make up technologies may be revealed by the degradation test of colorful organic substance. The specification technology of the composite material preparation therefore is determined. .Using the composite material prepared by the standard process, the degradation process and the effectiveness of nitrogen heterocyclic compound will be discussed. The degradation detailed steps of nitrogen heterocyclic chemicals under the mentioned catalytic materials may be studied by the debris monitoring and QC calculation..The achievements of the program will be helpful to the design, construction and application of a composite photocatalysts which are specially useful for the wastewater treatment from new energetic material production.

军用含能材料的生产废水是一类尚未受到广泛关注的特殊废水，含氮杂环化合物是新型军用含能材料制备废水中的常见有机污染物，其化学稳定性好、三致毒性强、难生物降解，对此常规的处理方法成本高、效果差。构建光能利用率高、降解效果好的复合光催化材料对此类特殊废水的治理具有实际意义。本项目以g-C3N4和Ag2ZrO3为基础构建g-C3N4/Ag2ZrO3系列复合催化材料；用XRD、SEM、EDX等表征材料的结构和表观形态；通过对有色有机物的降解试验检测材料的紫外和可见光响应活性，评价材料的催化效果，总结复合材料的性能与组成、构筑方式及制备工艺的关系，规范制备工艺；将通过规范工艺制得的复合材料用于含氮杂环化合物的降解，探讨光催化降解效果，通过降解碎片的监测和QC计算，探索在该催化材料作用下含氮杂环有机物的降解机理。为新型高效光催化降解材料的设计、构建及在新型含能材料制备废水处理中的应用提供理论和实验依据。

石墨相氮化碳(g-C3N4)由于具有可调控带隙宽度、半导体能带结构、对环境友好和高的热稳定性等优点，在光催化方面具有潜在的应用价值，但催化过程中g-C3N4存在光生载流子迁移率小，光生电子-空穴对复合率高等问题。本项目通过体相g-C3N4改性、g-C3N4结构形貌控制及半导体复合，成功制备了介孔g-C3N4、g-C3N4纳米线、新型管状g-C3N4、蜂窝状多孔g-C3N4、卷曲叶片形g-C3N4纳米片、片层g-C3N4/CdS、两种氮化碳的异质结、g-C3N4/BiOCl 、Ag3PO4@g-C3N4核壳光催化剂、g-C3N4/石墨烯片状纳米颗粒复合材料、红磷/ g-C3N4复合材料、CNS/TNS/ CuBA及g-C3N4/Bi2WO6/WO3三元复合材料。利用UV-Vis、FTIR、XRD、TEM、HRTEM、SEM、EDS、XPS、PL、时间分辨PL和BET等表征手段对制备的光催化剂进行了表征。这些经过改性的g-C3N4或者具有特定形貌的g-C3N4及其复合材料对有机和难降解污染物具有优异的光催化降解性能，并通过清除实验和EPR实验解释了其降解机理。本项目制备的石墨相碳化氮及其复合材料在有机污染物及含能材料废水降解、治理方面有应用前景；本项目的研究不仅拓展了g-C3N4的应用领域，也为g-C3N4 基复合材料的构建设计提供了新思路，具有重要的科学意义和实际使用价值。发表SCI收录学术论文44篇，申请发明专利7项，培养博士研究生3名，硕士研究生7名。