铁铈氧化物催化环己酮氧气氧化制ε-己内酯  

Oxidation of cyclohexanone toε-caprolactone with oxygen catalyzed by Fe-Ce oxides

作　　者：王媛媛 张明 胡珊珊 刘赛赛 朱明乔[1] WANG Yuan-yuan;ZHANG Ming;HU Shan-shan;LIU Sai-sai;ZHU Ming-qiao(College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,China;Taizhou Yuanzhong Pharmaceutical Co.Ltd.,Taizhou 318000,China)

机构地区：[1]浙江大学化学工程与生物工程学院,浙江杭州310027 [2]台州市源众药业有限公司,浙江台州318000

出　　处：《高校化学工程学报》2020年第4期996-1002,共7页Journal of Chemical Engineering of Chinese Universities

基　　金：浙江省自然科学基金(Y4080247);浙江省重大科技计划项目(2010C01035);广西石化资源加工及过程强化技术重点实验室开放课题基金(K002);工业控制技术国家重点实验室开放课题基金(ICT1224);浙江台州市源众药业有限公司资助项目。

摘　　要：为了探究环己酮氧气氧化制备ε-己内酯反应高效催化剂,采用共沉淀法制备一系列双金属氧化物催化剂FeCe(x:y-T),用X射线衍射(XRD)、N2吸附-脱附、X射线光电子能谱(XPS)、扫描电镜(SEM)等手段进行了表征,并将催化剂用于催化环己酮氧化反应。考察了溶剂种类、催化剂用量、反应温度、反应时间等反应条件的影响。结果表明Fe2O3和CeO2之间有一定协同作用,铁铈摩尔比和焙烧温度的改变对催化剂活性影响明显,其中FeCe(1:2-500)显示出最佳催化效果。对反应条件进行优化后,环己酮的转化率及ε-己内酯选择性均高于99%,且催化剂可被重复使用5次活性无明显下降。In order to explore high efficient catalysts for the oxidation of cyclohexanone toε-caprolactone with oxygen,bimetallic oxide catalysts FeCe(x:y-T)were synthesized by coprecipitation and characterized by X-ray diffraction(XRD),N2 adsorption-desorption,X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM).The catalysts were used to catalyze the oxidation of cyclohexanone.In addtion,the effects of experimental conditions such as solvent,catalyst dosage,reaction temperature and time were investigated.The results show that there is a synergistic effect between Fe2O3 and CeO2,and the change of Fe/Ce mole ratio and calcination temperature have a significant impact on the activity of catalysts.FeCe(1:2-500)exhibited the best catalytic performance.After optimization of reaction conditions,the conversion of cyclohexanone and the selectivity ofε-caprolactone are both higher than 99%,and the catalyst can be reused for five times without significant decrease of activity.

关 键 词：铁铈氧化物 环己酮 分子氧 Ε-己内酯 

分 类 号：TQ465.92[化学工程—制药化工]