固载于SBA-15分子筛中的同双核金属配合物催化剂  

Homodinuclear Metal Complexes Encapsulated in SBA-15 Molecular Sieve as Catalyst

作　　者：高丽娟[1] 李瑞丰[1] 田永华[2] 

机构地区：[1]太原理工大学精细化工研究所,山西太原030024 [2]宁夏大学化学化工学院,宁夏银川750021

出　　处：《石油化工》2006年第11期1038-1043,共6页Petrochemical Technology

基　　金：宁夏大学自然科学基金项目(LG0501)

摘　　要：合成了3种同双核金属配合物[M2LCl3]Cl(L代表配体三亚乙基四胺,M代表Co,Cu,Cr),采用微波加热法合成了SBA-15分子筛,采用浸渍法将3种同双核金属配合物分别固载在表面官能化的SBA-15分子筛(SBA-15-NH2分子筛)中制得负载型催化剂。傅里叶变换红外光谱、X射线衍射、紫外可见光谱和热分析表征结果表明,同双核金属配合物被固载后,其结构仍保持完整。以环己烷氧化反应为探针反应,考察了[Co2LCl3]Cl/SBA-15-NH2,[Cu2LCl3]Cl/SBA-15-NH2,[Cr2LCl3]Cl/SBA-15-NH2催化剂的活性,环己烷转化率分别为11.0%,49.5%,57.9%;对于[Cr2LCl3]Cl/SBA-15-NH2催化剂,当分别以乙睛、丙酮和冰醋酸为溶剂时,环己烷转化率分别为57.9%,52.1%,34.2%,3次重复实验的环己烷转化率分别为57.9%,47.8%,46.5%,表明该催化剂具有较好的活性和重复使用性。Three homodinuclear metal complexes [ M2LCl3 ] Cl （L stands for triethylenetetramine ligand,and M stands for Co, Cu or Cr）were synthesized, and SBA-15 molecular sieve was prepared by microwave heating method and were functionalized by y-aminopropyl to produce SBA-15-NH2 molecular sieve. The homodinuclear metal complexes were then immobilized on SBA-15-NH2 by impregnation and used as catalysts for cyclohexane oxidation. The samples were characterized by means of FTIR, UV-Vis, XRD and TG-DTA. Structure of homodinuclear metal complexes remains unchanged after being immobilized. Catalytic activities of [ Co2LCl3] Cl/SBA-15-NH2, [ Cu2LCl3]Cl/SBA-15- NH2 and [ Cr2LC13 ] C1/SBA-15-NH2 were studied by cyclohexane oxidation with H2O2 as oxidant. When [ Cr2LC13 ] Cl/SBA-15-NH2 is used as catalyst and acetonitrile as solvent, cyclohexane conversions can reach 57.9%. After being used for three times, activity of[ Cr2LC13 ] Cl/SBA-15-NH2 catalyst can still keep at 46.5%.

关 键 词：同双核金属配合物 SBA-15分子筛 微波 固载 催化剂 环己烷 氧化反应 

分 类 号：TQ426.61[化学工程]