论文部分内容阅读
合成了3种含氮、氧配体的Ni(Ⅱ)配合物,并把它们担载于不同的载体上.在无有机溶剂及无相转移剂存在时,考察了在用NaOCl作为氧源时它们对苯乙烯环氧化的催化活性.用共沉淀法将微水溶性的Ni(PA)2(H2O)2固载于硅溶胶上;利用两种水溶性的新催化剂(Ni(C12H12N2O2)Cl2和Ni(C16H12N2O2)Cl2)离子型的特性,可以顺利的将它们固载于NaY型分子筛、Na基蒙脱土和离子交换树脂上,固载后催化剂的催化效果以固载于NaY型分子筛上为较佳.催化剂在固载后,苯乙烯的转化率和环氧选择性无明显降低.反应中加入一些氧化吡啶类添加剂,可以明显加快反应速度.其中对苯乙烯环氧化的转化率及选择性的影响,则以4-乙基氧化吡啶为最好.在适宜的反应条件下,固载后的催化剂(A-S)可使苯乙烯环氧化转化率达到83.0%,环氧化物选择性达67.4%.
Three Ni (Ⅱ) complexes containing nitrogen and oxygen ligands were synthesized and supported on different supports. In the absence of organic solvents and no phase transfer agent, the catalytic activity of their epoxidation of styrene in the presence of NaOCl as the oxygen source was investigated. The water-soluble Ni (PA) 2 (H2O) 2 was immobilized on silica sol by coprecipitation method. By using the properties of two kinds of water-soluble new catalysts (Ni (C12H12N2O2) Cl2 and Ni (C16H12N2O2) Cl2) , They can be successfully carried on NaY zeolite, Na-montmorillonite and ion-exchange resin, and the catalytic effect of the catalyst immobilized on the NaY-type molecular sieve is better. After the catalyst was immobilized, the styrene conversion and epoxy selectivity were not significantly reduced. The reaction of adding some pyridine oxide additives, can significantly speed up the reaction rate. Among them, the conversion and selectivity of styrene epoxidation, the 4-ethyl pyridine is the best. Under appropriate reaction conditions, the catalyst (A-S) immobilized on the styrene epoxidation conversion rate of 83.0%, the epoxide selectivity of 67.4%.