分子筛固载型Cosalen的制备、表征及其应用研究

分别采用NaY分子筛、γ-氨丙基三乙氧基硅烷修饰的MCM-41分子筛固载双水杨醛缩乙二胺合钴(Cosahn)配合物,制备了固载型Cosahn/NaY、Cosalen/MCM-41催化剂.采用傅里叶变换红外光谱、热重-差热、X射线衍射、比表面积测定等方法对固载型分子筛催化剂的结构进行表征.结果表明,Cosalen已成功地进入分子筛孔道内.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、环己酮的选择性.该催化反应体系产物中环己基过氧化氢(CHHP)的量很少,表明Cosalen/MCM-41催化剂能加速CHHP的分解.在初始氧气压力0.80 MPa、温度130℃、环己烷用量30 g、Cosalen/MCM-41用量0.30 g、叔丁基过氧化氢0.10 g的条件下反应2 h,环己烷的转化率达到5.96%,醇酮选择性87.03%.

Preparation of molecular sieve immobilized Cosalen and its characterization and application

N,N'-bis(salicylidene)ethylenediiminocobah(Cosalen)is encapsulated into both the supercage of microporous NaY zeolite and the mesoporous molecular sieve(MCM-41)which modified by 3-triethoxysilylpropylamine.The prepared samples are characterized by FT-IR,TG-DSC,XRD,BET.The results show that Cosalen has incorporated into matrix of the both samples.The catalyze performance of the samples for the cyclohcxane hquid-phase oxidation into cyclohexanone and cyclohexanol by oxygen is investigated in the absence of solvents.Only small amount of cyclohexyl hydroperoxide(CHHP)analyzed in products indicates that Cosalen/MCM-41 catalyst can accderate decomposition of CHHP.The oxidation reaction of cyclohexane is studied andthe optimum reaction conditions are obtained asfollows:0.8MPa of initial oxygen pressure,130℃ of temperature,30 g of cyclohexane,0.30 g of Cosalen/MCM-41 used as the catalyst,0.10 g of TBHP and 2 h of reaction time.The conversion of cyclohexane can reach 5.96%and the selectivity of cyclohexanone and cyclohexanol can be up to 87.03%.