MCM-41固载席夫碱钴配合物在环己烷氧化反应中的应用  

MCM-41 supported schiff-base cobalt complexes and its catalytic performance in cyclohexane oxidation

作　　者：单高峰[1] 袁霞[1] 吴剑[1] 罗和安[1] 

机构地区：[1]湘潭大学化工学院,湖南湘潭411105

出　　处：《中南大学学报（自然科学版）》2011年第10期2959-2965,共7页Journal of Central South University:Science and Technology

基　　金：国家自然科学基金资助项目(21006080);湖南省教育厅优秀青年项目(09B099)

摘　　要：制备γ-氨丙基三乙氧基硅烷修饰的MCM-41分子筛固载型双水杨醛缩乙二胺合钴(Cosalen)配合物,采用傅里叶变换红外光谱、X线衍射、比表面积测定、热重-差热(TG-DSC)、紫外-可见光光谱(UV-Vis)、透射电镜等方法对分子筛固载型配合物Cosalen/MCM-41的结构进行表征,并对比Cosalen/MCM-41与Cosalen/NaY的催化性能。研究结果表明:Cosalen已进入分子筛孔道内;在以氧气为氧源的环己烷氧化反应中,Cosalen/MCM-41催化剂具有较好的活性和对环己醇、环已酮的选择性。该催化反应产物中环已基过氧化氢(CHHP)的量很少,表明Cosalen/MCM-41催化剂能加速环已基过氧化氢的分解;以Cosalen/MCM-41为催化剂,在初始氧气压力为0.80 MPa,温度为130℃,环己烷与催化剂的质量比为100,叔丁基过氧化氢0.06 g的相对温和条件下反应2 h,环己烷的转化率达到5.96%,醇酮选择性87.03%。N,N＇-Bis（salicylidene）ethylenediiminocobalt（Cosalen） was encapsulated into the meso-porous molecular sieve（MCM-41） which was modified by 3-triethoxysilylpropylamine.The prepared Cosalen/MCM-41 was characterized by the technique of FT-IR,XRD,BET-BJH,TG-DSC,UV-Vis,TEM and so on.The catalytic performance of the Cosalen/MCM-41 and Cosalen/NaY for the cyclohexane liquid-phase oxidation by oxygen was compared.The oxidation reaction of cyclohexane was studied.The results show that N,N＇-Bis（salicylidene） ethylenediiminocobalt（Cosalen） is incorporated into the pore of the sample.Cosalen/MCM-41 has the better catalytic activity and only small amount of cyclohexyl hydroperoxide（CHHP） is among reaction products which indicates that Cosalen/MCM-41 catalyst is able to accelerate decomposition of CHHP.Under relatively mild conditions,i.e.Cosalen/MCM-41 as catalyst,reaction temperature 130 ℃,initial oxygen pressure 0.80 MPa,mass ratio of catalyst and cyclohexane is 100,0.06 g TBHP and reaction time 2 h,the conversion of cyclohexane is up to 5.96% and cyclohexanol is 87.03%.

关 键 词：环己烷氧化 氧气 Cosalen MCM-41 

分 类 号：TQ032.4[化学工程]