Co-APO-5分子筛催化的环己烷选择氧化:溶剂和改性方法对其催化性能的影响（英文）  

Selective oxidation of cyclohexane over Co-APO-5:Effects of solvent and modification method on the catalytic performance

作　　者：荆补琴[1,2,3] 李俊汾[1] 秦张峰[1] 

机构地区：[1]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001 [2]山西大同大学化学与环境工程学院,山西大同037009 [3]中国科学院大学,北京100049

出　　处：《燃料化学学报》2016年第10期1249-1258,共10页Journal of Fuel Chemistry and Technology

基　　金：the National Natural Science Foundation of China(21403268,21603254);Natural Science Foundation of Shanxi Province of China(201601D202014,2015021003);the CAS/SAFEA International Partnership Program for Creative Research Teams~~

摘　　要：通过合成改性制备了系列Co-APO-5分子筛催化剂,用于环己烷选择氧化,研究了溶剂和改性方法对其催化性能的影响。结果表明,含有π键的极性溶剂对环己烷选择氧化反应有利,环己烷转化率随着π键极性的增加而提高。引入Si和F降低了Co-APO-5分子筛骨架中四配位钴的含量;引入F后Co-APO-5分子筛的结晶度有所提高,而引入Si则能改善Co物种的氧化和还原性,提升其催化反应活性。同时,Co-APO-5的催化活性与其骨架中四配位Co(II)的含量相关,说明骨架Co(II)是环己烷选择氧化的催化活性中心。A series of Co-APO-5 molecular sieves were prepared and used as the catalysts in the selective oxidation of cyclohexane; the effects of solvent and modification method on the catalytic performance of Co-APO-5 were investigated. The results illustrated that polar solvents containing π-bonds are favorable for the oxidation reaction and the conversion of cyclohexane increases with the increase of solvent polarity. The introduction of Si and F leads to a decrease of the tetrahedral cobalt content in the Co-APO-5 framework. However, introducing F can improve the crystallinity of Co-APO-5, whereas adding Si may promote the oxidation and reduction of cobalt species and then enhance the catalytic activity in oxidation. In general, the activity of Co-APO-5 catalysts is related to the content of tetrahedral cobalt in the framework, suggesting that the framework Co（Ⅱ） is probably the catalytically active species for the oxidation of cyclohexane.

关 键 词：Co-APO-5 环己烷 选择氧化 环己醇 环己酮 溶剂效应 分子筛改性 

分 类 号：O643.32[理学—物理化学]