alcucom准晶合金的制备及催化环己烯氧化性能研究word格式论文.docxVIP

摘 要烯烃的氧化应用广泛，环己烯是一种重要的烯烃，容易氧化形成多种产物，这些 产物多是具有应用价值的有机合成中间体，用于医药、农药、香料、表面活性剂等精 细化工领域。目前，环己烯氧化的过程多采用双氧水及叔丁基过氧化氢等氧化剂，存 在着腐蚀设备和成本昂贵等缺点。从环保及廉价的角度来看，分子氧是比较理想的氧 源，因此设计合成绿色高效的催化剂，使其可以在温和的条件下催化环己烯氧化成为 了研究的重点。金属有机骨架材料（MOFs）具有高的孔隙率及较好的化学稳定性，本文以 2,2′- 联吡啶（2,2′-bipy）和 2,2′-联苯二酸（2,2′-dpa）为配体原料，采用水热法合成了新 型的金属有机骨架化合物{[Co(2,2′-dpa)(2,2′-bipy)]·2H2O}n，表征了其组成和结构特 性。将其作为催化剂，无溶剂条件下，以分子氧作为氧化剂，催化环己烯氧化，考察 了反应时间、温度及催化剂用量等反应条件的影响。研究发现，该新型 MOF 催化剂 在催化环己烯氧化反应中具有较高的转化频率值，即高效的催化活性。准晶其表面特殊的晶粒结构和电子结构决定了它在催化方面有潜在的应用，可能 成为性能独特的催化剂。本文设计合成了系列 Al-Cu-Co-M 合金催化剂，表征其组成和结构。将其作为催化剂，无溶剂条件下，以分子氧作为氧化剂，催化环己烯氧化，考察了反应时间、温度及催化剂用量等反应条件的影响。研究发现，该准晶合金在催 化环己烯氧化反应中具有较高的催化活性，合金组成是影响其催化活性的首要因素。关键词：金属有机骨架材料；准晶；环己烯氧化；催化；氧气IAbstractOxidation of olefins is widely applied. Cyclohexene is an important olefin and easily oxidized to form a variety of products. These products are mostly synthetic organic intermediates which having the application value in fine chemicals fields of pharmaceuticals, pesticides, perfumes, surfactants etc. At present, hydrogen peroxide and t-butyl hydrogen peroxide are used as the oxidants in the process of oxidation of cyclohexene, the process has defects such as corrosion of the equipments and high cost. In terms of environmental protection and cheap price, molecular oxygen is an ideal source of oxygen. Therefore, the design and synthesis of green and efficient catalyst which can catalyze the oxidation of cyclohexene under mild conditions have become the focus of the study.Metal-organic frameworks (MOFs) have high porosity and good chemical stability. A new type of metal-organic framework compound {[Co(2,2′-dpa)(2,2′-bipy)]·2H2O}n was synthesized by hydrothermal method with 2,2′-bipyridine heterocyclic ring and 2,2′-diphenyl carboxylic acid ligands as two raw materials. The composition and structure of the novel compound were characterized. It catalyzed oxidation reaction of cyclohexene with molecular oxygen under solvent-free conditions. The influence of reaction conditions such as reaction time