高活性Au/SnO_2催化剂的制备及其在1,4-丁二醇氧化制γ-丁内酯反应中的催化应用(英文)  

Preparation and application of highly efficient Au/SnO_2 catalyst in the oxidative lactonization of 1,4-butanediol to γ-butyrolactone

作　　者：李娴[1] 郑嘉旻[1] 杨新丽[2] 戴维林[1] 范康年[1] 

机构地区：[1]复旦大学化学系 上海市分子催化和功能材料重点实验室,上海200433 [2]河南工业大学化学化工学院,河南郑州450001

出　　处：《催化学报》2013年第5期1013-1019,共7页

基　　金：supported by the National Natural Science Foundation of China(20973042,20903035,21173052);the National Basic Research Program of China(973 Program,2012CB224804);the Natural Science Foundation of Shanghai Science and Technology Committee(08DZ2270500)~~

摘　　要：采用沉积沉淀法制备了一系列商业SnO2负载的纳米Au催化剂,通过电感耦合等离子体发射光谱、X射线粉末衍射、透射电镜和X射线光电子能谱等方法研究了溶液酸碱性、沉淀剂种类、Au负载量和焙烧温度等对催化剂性质的影响.结果表明,Au的负载量以及催化剂的焙烧温度对Au颗粒状态有较大影响.其中,于573K焙烧的3%Au/SnO2催化剂在1,4-丁二醇氧化制备γ-丁内酯反应中的催化活性最好,TOF值是Au/TiO2催化剂的15倍.这主要是由于SnO2载体独特的性质对所负载的Au颗粒的影响.A series of gold catalysts supported on commercial SnO2 were synthesized by deposi-tion-precipitation while accurately controlling pH and precipitant species. The supported catalysts were characterized by X-ray diffraction, inductively coupled plasma atomic emission spectrometry, transmission electron microscopy, and X-ray photoelectron spectroscopy. Gold loading and calcina-tion temperature both affected the dispersion and nature of gold species on SnO2 . The performance of the catalysts in the oxidative lactonization of 1,4-butanediol to γ-butyrolactone was investigated. The catalyst with 3% gold that was calcined at 573 K exhibited the highest activity, which was 15 times higher than that of Au/TiO2 . The excellent catalytic performance was attributed to the high dispersion of gold particles and adequate Au0 and Auδ– species formed because of the strong inter-action between Au and SnO2 and the intrinsic properties of SnO2 .

关 键 词：金催化 二氧化锡 沉积沉淀法 1 4-丁二醇 氧化内酯化 焙烧温度 金负载量 

分 类 号：O623.624[理学—有机化学] O643.32[理学—化学]