锆基纳米材料的气相制备及其对NOx的消除特性

Zr-based nanomaterials have special structure and function and are applied in catalytic degradation and catalyst carrier, toughening ceramics and other fields,which have a broad prospect in application. In this study, soluble or easily sublimated zirconium salt and oxygen, nitrogen, phosphorus species are chosen as precursors to explore the synthesis of the Zr-based nanoparticles, such as ZrO2, Zr3N4, Zr3P4 and composite nanomaterials using vapor-phase hydro (aminolysis or phosphorus)-lysis method. The law of the stabilized zirconia composites nanomaterials will be achieved by regulating precursor ratio, feeding order and other conditions. The optimal synthesis conditions and factors would also be collected by exploring the impact of vapor-phase hydrolysis on the morphology, size and surface properties of materials. Using the gas-solid catalytic test platform, the catalytic activity of the catalytic active ingredients O2-、N3- and P3- in Zr-based nanoparticles or composite nanomaterials are monitored and compared during innocuous treatment of NOx and other polluting gases. The impact on catalytic properties by the variables, such as before and after compositing, composite volume, tablet hardness, calcination temperature will be compared. The synthetic route and conditions should be timely corrected and adjust. The optimal model of optimal catalytic activity between compositing conditions then would be established, the synthetic route Zr-based nanomaterials be further optimized and the mechanism of nanomaterials for gas-solid catalytic reaction be perfected.

锆基纳米材料具有特殊的结构和功能，在催化降解及催化剂载体、陶瓷增韧等领域具有广泛的应有前景。本研究以易溶或易升华的锆盐以及含氧、氮、磷物种为前驱物，选用气相法探索合成ZrO2、Zr3N4、Zr3P4等锆基纳米粒子及以其为主体的纳米复合物；通过调控前驱物配比、给料顺序等复合条件，获取锆基纳米材料的稳定化规律，探究气相水解（氨解、磷解）法对材料的形貌、尺寸及表面性质等的影响，获得最佳的合成条件及影响因素。利用气固相催化分析测试平台，监测并比较锆基纳米粒子及锆基复合纳米材料中O2-、N3-、P3-等催化活性成分在NOx等污染气体无害化处理体系中的催化活性。比较分析纳米材料复合前后、复合量、压片硬度、焙烧温度等变量对催化特性的影响，及时修正调整合成路线及条件，建立最优的催化活性与最优的合成条件之间的模式，进一步优化锆基纳米材料的合成路线，完善锆基纳米材料的气固相催化反应机理。

纳米材料的特殊结构和功能，使其在降解消除环境污染物等领域具有广泛的应用价值。本课题以易溶或易升华的锆盐ZrCl4以及水、氨气等含氧、氮、磷元素的化合物为原料，选用气相法探索合成了氧化锆、氮化锆、磷化锆以及铈锆氧复合材料、磷化锆-石墨烯复合材料等锆基纳米材料及以其为主体的纳米复合物。研究了锆基纳米材料的稳定化、可控化合成规律，探究元素的气相结合法等方法对材料的微观结构及性能的影响，得到了最佳的锆基纳米材料的合成路线。利用气固相催化分析测试平台，监测并比较合成的纳米材料中阴离子等催化活性成分在消除NO污染气体中的活性。材料合成与性能表征联动反馈，建立最优的活性与最优的合成条件之间的模式。. 此外，课题组成员还研究了多选区、多晶型Mg(OH)2纳米六方盘的制备及对酯交换反应的催化性能；合成了一系列不同尺寸的银纳米多面体、立方体，搭建了银-金-聚合物耦合薄膜器件，测定了器件的光学透过率、SERS性能，并研究了影响因素。