碱金属钨青铜@LDHs复合材料的构筑及其对有机染料废水或氮氧化物的光催化降解性能研究

Based on energy, resource and environmental considerations, the catalytic material should be highly selective, highly reactive, low cost and environmentally friendly. In order to avoid the each other’ s shortcomings, this project proposes to construct a high performance photocatalytic composite materials which is applied to the degradation of dyestuff wastewater or nitrogen oxides under visible light, namely, MxWO3@LDHs by combined layered double hydroxides (LDHs) with Alkali metal tungsten bronze（MxWO3，M=Li, Na, K, Rb, Cs）with excellent charge transmission performance. This topic belongs to a stronger prospective, exploratory application of fundamental research. Based on the hydrothermal synthesis of MxWO3 micro-nano material, the MxWO3@LDHs composite materials with high photocatalytic activity will be obtained through one step in-situ hydrothermal method. The effects of prepared process, elemental chemical environment and acidity on the law of photocatalytic process will be detailed investigated. The composition, structure and morphology of the catalytic materials will be known through a variety of structural and performance characterizations. The catalysis-assisted structure-activity relationship will be revealed and the Visible light photocatalytic mechanism will also be explored. The successful implementation of the project will provide theoretical basis and application basis for the preparation of high efficiency “green” catalyst, accelerate the technology extension of the “green” catalyst industry and upgrade the efficient clean catalyst in the chemical industry.

基于能源、资源和环境方面的考虑，催化剂应具有高选择性、高活性、低成本且环境友好等特点。本项目提出将层状双金属氢氧化物（LDHs）与具有优良电荷传输性能的碱金属钨青铜（MxWO3，M=Li, Na, K, Rb, Cs）复合，规避彼此缺点，构筑高性能的MxWO3@LDHs复合结构可见光催化材料，被应用于可见光降解染料废水或氮氧化物，本课题属于有较强前瞻性、探索性的应用基础研究。研究将以水热法合成出MxWO3微纳米材料为基础，进而通过一步原位水热法获得具有高催化活性的MxWO3@LDHs，并研究其制备工艺过程、元素化学环境、酸性等因素对光催化过程的影响规律。基于多种结构与性能表征手段，认识催化材料的组成、结构、形貌等复合结构性质，掲示构效关系，探究可见光催化机制。项目的顺利实施将为制备高效“绿色”催化剂提供理论依据和应用基础，加速化工行业“绿色”催化剂产业化技术推广及高效清洁催化剂升级。

本项目将层状双金属氢氧化物（LDHs）与具有优良电荷传输性能的钨青铜（MxWO3）复合，规避彼此缺点，构筑了高性能的MxWO3@LDHs复合结构材料，被用于可见光降解染料（有机物）废水或固氮。研究以水热法合成出MxWO3微纳米材料为基础，通过一步原位水热法获得具有高催化活性的MxWO3@LDHs，研究了其制备工艺过程、元素化学环境、酸性等因素对光催化过程的影响规律。基于多种结构与性能表征手段，认识了催化材料的组成、结构、形貌等复合结构性质，掲示了其构效关系，探究了可见光催化机制。研究过程中发现，在适宜的催化剂浓度、底物浓度的条件下，催化剂对有机污染物基本全部移除。稳定性测试表明所制备的复合材料在经过多次循环之后仍能表现出较高的光催化活性，有望实现工业化应用。另一方面,通过一种简单的原位水热硫代乙酰胺刻蚀方法，构建了硫代乙酰胺蚀刻处理的NiFe-LDH复合催化剂（[NiFe]S），在可见光下具有显著的光固氮活性。水热硫代乙酰胺蚀刻处理技术可以达到一箭三雕的作用，能明显改善N2的光固定活性。LDH已实现工业化生产，而原位硫代乙酰胺蚀刻工艺相对简单，这对于工业实际应用非常重要。同时，研制了一种光固氮催化反应器，该反应器结构合理、传质效率高、固氮催化效率高。本项目的顺利实施为制备高效“绿色”光催化剂提供理论依据和应用基础，加速化工行业“绿色”光催化剂产业化技术推广及高效清洁光催化剂升级。