高活性MgO/SnO_2复合金属氧化物催化剂的合成及其在双氧水选择氧化环己酮制ε-己内酯反应中的应用  

Baeyer-Villiger Oxidation of Cyclohexanone to Caprolactone over Highly Efficient MgO/SnO_2 Catalyst Using H_2O_2 as Oxidant

作　　者：李静霞[1] 黄靓[1] 戴维林[1] 范康年[1] 

机构地区：[1]复旦大学化学系上海市分子催化与创新材料重点实验室,上海200433

出　　处：《化学学报》2008年第1期5-9,共5页Acta Chimica Sinica

基　　金：国家自然科学基金(Nos.20407006;20573024);上海市科委基础研究(No.06JC14004)资助项目

摘　　要：通过共沉淀法制备了一系列Mg基复合金属氧化物.采用X射线衍射(XRD)、热重(TG)以及N2吸附(BET)等表征手段对催化剂的结构进行了表征,并研究了其对双氧水体系中环己酮Baeyer-Villiger氧化制己内酯的催化反应性能,考察了不同组成和配比的催化剂以及反应条件对催化活性的影响.结果表明,在以H2O2水溶液为氧化剂,苯甲腈和二氧六环混合溶液为溶剂时,复合金属氧化物MgO/SnO2体现出比MgO/La2O3,MgO/TiO,MgO/ZnO,MgO/ZrO2等催化剂更优异的催化性能.同时发现金属物质的量比为7∶3,焙烧温度为600℃的MgO/SnO2催化剂在优选反应条件下可使环己酮的最高转化率达90.5%,己内酯的选择性达到100%.A series of Mg-based catalysts were prepared by a coprecipitation method and characterized by XRD, BET, and TG-DTA. As compared with other composite catalysts, including MgO/Al2O3, MgO/La2O3, MgO/TiO2, MgO/ZnO and MgO/ZrO2, MgO/SnO2 showed the most efficient catalytic performance in the Baeyer-Villiger oxidation of cyclohexanone to e-caprolactone with aqueous hydrogen peroxide as an oxidant. Under optimal reaction conditions, the as-prepared MgO/SnO2 catalyst after being calcined at 600 ℃ with the Mg/Sn molar ratio of 7 ： 3 presented an excellent performance with the cyclohexanone conversion of 90.5% and the caprolactone selectivity of 100%.

关 键 词：MgO/SnO2复合金属氧化物 环己酮 BAEYER-VILLIGER氧化 

分 类 号：O643.3[理学—物理化学]