层间掺杂碱/碱土金属离子g-C3N4可见光催化去除NOx的性能增强机制

项目名称： 层间掺杂碱/碱土金属离子g-C3N4可见光催化去除NOx的性能增强机制

项目编号： No.51478070

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 其他

项目作者： 董帆

作者单位： 重庆工商大学

项目金额： 82万元

中文摘要： 在初步实现高活性层间掺杂碱/碱土金属离子g-C3N4的原位制备基础上，本项目针对电子结构特征、性能增强机制、净化NOx反应机理等关键科学问题，系统优化制备工艺条件，建立制备条件-微结构关系。采用第一性原理计算模拟优化碱/碱土金属离子掺杂g-C3N4的几何结构和电子结构，结合实验表征确定掺杂方式、位置和形态；系统研究掺杂离子对晶体结构、π共轭体系、禁带结构和电荷有效质量的影响，综合光吸收特性、光生电荷迁移转化行为、活性自由基俘获等结果，揭示碱/碱土金属离子掺杂提高g-C3N4光催化性能的作用机制；比较同族不同元素的掺杂效应的异同，揭示掺杂效应差异的本质原因。将制备的催化剂应用于气相低浓度NOx净化，构建微结构-可见光催化性能构效关系；分析光催化反应过程中间产物和终产物的浓度及分布，从分子水平明晰碱/碱土金属离子掺杂g-C3N4光催化净化NOx反应机理，为其走向应用提供技术基础。

中文关键词： 环境催化；氮氧化物；光催化；碳化氮；掺杂

英文摘要： The applicant have initially realized in-situ preparation of interlayer-doped g-C3N4 with alkaline/alkaline-earth metal ions for high photocatalytic activity. On the basis of the exploration, the present project aims to solve the key scientific issues in electronic structure characterization, activity enhancement mechanism and reaction mechanism of NOx purification. The proposal will optimize the synthesis conditions systematically and establish the relationship between preparaiton conditions and microstructure. The doping mode, position and chemical state of the alkaline/alkaline-earth metal ions will be determined by calculation of the geometry and electronic structure using first principle method and experimental characterizations. The proposal will also investigate the effects of doped ions on the crystal structure, π congugated system, band structure and effective mass of carriers. Considering the research results of light absorption characteristics, transfer and transportation behaviors of photo-induced charge carriers and trapping of reactive radicals, the activity enhancement mechanism of alkaline/alkaline-earth metal ions doped g-C3N4 will be revealed.Through comparison of the differences of doping effects induced by different metals in the same group, the essence of the differences in doping effects will be revealed.The as-synthesized catalysts will be applied in purification of NOx at low concentration. Combining the results of structural characterization, the relationship between catalysts microstructure and visible light photocatalytic activity will be established.By analyzing the concentration and distributoin of reaction intermediates and final products, the reaction mechanism of photocatalytic purification of NOx by alkaline/alkaline-earth metal ions doped g-C3N4 will be elucidated, which could provide technological basis for the future application.

英文关键词： Envirenmental catalysis;NOx;Photocatalysis;Carbon nitride;Doping