取代基对Ru-Schiff碱配合物/Y催化剂加氢性能的影响  

Effect of Substituents of Ru-Schiff Base/Y Catalysts on Hydrogenation Activity

作　　者：陈萍[1] 范彬彬[1] 宋明纲[1] 晋春[1] 李瑞丰[1] 

机构地区：[1]太原理工大学精细化工研究所煤科学与技术教育部重点实验室,山西太原030024

出　　处：《石油化工》2006年第8期740-744,共5页Petrochemical Technology

基　　金：国家自然科学基金项目(50472083);山西省自然科学基金项目(20051010);山西省留学回国人员基金项目(2004-22)

摘　　要：采用自由配体法将系列Ru(5,5′-X2-salen)(X=H,C l,B r,CH3O;salen为N,N′-双水杨醛亚乙基二亚胺)配合物封装于Y型沸石的孔腔中,制备出系列Ru(5,5′-X2-salen)/Y催化剂。采用X射线衍射、氮吸附、等离子发射光谱、傅里叶变换红外光谱、漫反射紫外可见光谱和差热分析对所制备的催化剂进行了表征,并考察了该系列催化剂对苯加氢反应的催化性能。实验结果表明,不同性质基团对配合物芳环上氢原子的取代不仅可改变封装配合物的电子和光谱性质,而且还对所制备催化剂的加氢活性产生很大影响。具有吸电子基团和给电子基团取代基的催化剂的加氢活性均低于未被取代的催化剂,Ru-salen/Y催化剂的加氢活性最高,苯的转化率可达75.2%。Ru(5,5′-X2-salen)/Y催化剂在苯加氢反应中具有良好的稳定性,可重复使用。A series of Ru（5,5＇-X2-salen） complexes,were encapsulated within cavities of Y zeolite by flexible ligand method, where salen was N, N＇-ethylenebis （ salicydene aminato） and X were H, Cl, Br or CH3O. The prepared Ru （5,5＇-X2-salen）/Y catalysts were characterized by means of XRD, ICP, N2-Adsorption,FTIR, UV-Vis and DTA. The catalysts were evaluated by probe reaction of benzene hydrogenation. Substitution of hydrogen atoms on aryl group in salen ligand of the prepared catalyst by other groups not only changed spectroscopic properties of encapsulated complexes, but also greatly affected hydrogenation activity of the catalyst. The encapsulated catalysts with electron-withdrawing group like CI or Br, or electron-donating group like CH30 exhibited lower activity than the unsubstituted. Hydrogenation activity of Ru-salen/Y catalyst is the highest and benzene conversion can reach 75.2%. The Ru（5,5＇-X2-salen）/Y catalysts are stable in benzene hydrogenation and can be reused.

关 键 词：钌 配合物 Y型沸石 SCHIFF碱 取代基 催化剂 苯加氢 

分 类 号：TQ032[化学工程]