CuNaX催化乙苯选择氧化制苯乙酮  

Selective Oxidation of Ethylbenzene to Acetophenone over CuNaX Catalysts

作　　者：汤清虎[1] 胡钰[1] 乔冉[1] 赵培正[1] 赵培真[1] 

机构地区：[1]河南师范大学化学与环境科学学院,河南新乡453007

出　　处：《石油化工》2010年第7期782-788,共7页Petrochemical Technology

基　　金：河南省高校科技创新人才支持计划项目(2010HASTIT028)

摘　　要：采用离子交换法制备了一系列不同铜含量的CuNaX催化剂。该催化剂能有效催化以叔丁基过氧化氢(TBHP)为氧化剂的液相乙苯选择氧化反应,产物以苯乙酮为主。在催化剂用量200mg、乙苯用量6mmol、TBHP用量12mmol、乙腈用量1mL、反应温度80℃、反应时间10h的优化反应条件下,乙苯转化率达到78%,苯乙酮选择性为98%,且催化剂能多次循环使用。XRD,DRS,H2-TPR表征结果表明,当铜质量分数小于6.0%时,交换到NaX分子筛中的铜离子主要位于分子筛的超笼中;而当铜质量分数超过6.0%时,交换到NaX分子筛中的铜离子主要位于分子筛的方钠石笼或六角柱笼中。位于NaX分子筛超笼中的六配位的铜离子是催化以TBHP为氧化剂的乙苯选择氧化制苯乙酮反应的活性组分。A series of CuNaX catalysts with different copper contents were prepared through ion- exchange method and used in selective oxidation of ethylbenzene with ten-butyl hydroperoxide （TBHP） to acetophenone in liquid phase. Under the optimized conditions：CuNaX-6.0 catalyst dosage 200 rag, ethylbenzene dosage 6 mmol, TBHP dosage 12 mmol, acetonitrile volume 1 mL, reaction temperature 80 ℃ and reaction time 10 h, conversion of ethylbenzene and selectivity to acetophenone could reach 78% and 98%, respectively. The catalyst could be recycled for several times without evident loss of the activity. The results of XRD, DRS and Ha-TPR suggested that Cu ions were mainly located in the NaX supercages when Cu mass fraction was lower than 6.0% （w）. But Cu ions would be exchanged into sodalite cages and/or hexagonal prism cages when the Cu mass fraction was higher than 6.0% （w）. The key active component for the selective oxidation was the Cu ions in the supercages of NaX, which mainly existed as six coordination Cu （ II ）.

关 键 词：CuNaX催化剂 乙苯 苯乙酮 选择氧化 叔丁基过氧化氢 

分 类 号：TQ426.8[化学工程]