Mn-Al和Cu-Mn-Al复合氧化物催化苯甲醇选择氧化反应  

Selective Catalytic Oxidation of Benzyl Alcohol over Mn-Al and Cu-Mn-Al Composite Oxide Catalysts

作　　者：吴藏藏 郑丽[1] 徐秀峰[1] 

机构地区：[1]烟台大学应用催化研究所,山东烟台264005

出　　处：《分子催化》2016年第6期532-539,共8页Journal of Molecular Catalysis(China)

基　　金：山东省重点研发计划项目(2016GSF117003)~~

摘　　要：用溶胶-凝胶法制备了不同组成的Mn-Al和Cu-Mn-Al复合氧化物两组催化剂,用于苯甲醇选择氧化反应.用X射线衍射(XRD)、N2物理吸附(BET)、扫描电镜(SEM)、H_2程序升温还原(H_2-TPR)、O_2程序升温脱附(O_2-TPD)和X射线光电子能谱(XPS)技术对催化剂进行了结构表征,考察了催化剂组成对催化活性的影响.结果表明:以甲苯为溶剂,O_2为氧化剂,353 K反应5 h,Mn_2Al和Cu_(0.3)Mn_(0.7)Al_2催化剂上的苯甲醇转化率分别为36.6%和40.9%,苯甲醛选择性均为100%.进一步研究表明:催化剂活性与其H2还原性和O_2吸附性有关,高活性的催化剂吸附氧多,生成的活性氧易参与反应.A series of Mn-Al and Cu-Mn-Al composite oxides with different compositions were prepared by sol-gel method and applied in selective oxidation of benzyl alcohol to henzaldehyde. The catalysts were characterized by means of techniques such as X-ray diffraction （XRD） , N2 physisorption （ BET）, Scanning electron microscope （SEM）, Temperature-programmed reduction of hydrogen （H2-TPR）, Temperature-programmed desorption of oxy- gen （O2-TPD）, and X-ray photoelectron spectroscopy （XPS）. The effect of catalyst compositions on catalytic ac- tivity was investigated. It is shown that the high conversion of benzyl alcohol can be obtained under the following re- action conditions ： 02 is used as oxidant, toluene as solvent, the content of benzyl alcohol 1 mmol, reaction tempera- ture 353 K, and reaction time 5 h, thus the 36.6% and 40.9% conversions of henzyl alcohol can be reached on Mn-Al and Cuo.3Mn0.7Al2 catalysts, respectively. Over all catalysts, the selectivity of benzaldehyde maintains 100%. The characterization data indicates that the catalyst with higher activity has more deficit sites and is more facile adsorption of oxygen for benzyl alcohol oxidation reaction.

关 键 词：苯甲醇选择氧化 Mn-Al复合氧化物 Cu-Mn-Al复合氧化物 催化活性 苯甲醛选择性 

分 类 号：O643.3[理学—物理化学]