高选择性部分氧化催化剂Au-Pd/TiO_(2)-SiO_(2)的设计合成与苯甲醇部分氧化反应  

Design and synthesis of Au-Pd/TiO_(2)-SiO_(2) catalyst with high selectivity for partial oxidation of benzyl alcohol

作　　者：吴萍萍[1] 舒洁 王悦[1] 张永辉[1] 赵联明 白鹏[1] WU Pingping;SHU Jie;WANG Yue;ZHANG Yonghui;ZHAO Lianming;BAI Peng(School of Chemistry and Chemical Engineering in China University of Petroleum(East China),Qingdao 266580,China;School of Material Science and Engineering in China University of Petroleum(East China),Qingdao 266580,China)

机构地区：[1]中国石油大学(华东)化学化工学院,山东青岛266580 [2]中国石油大学(华东)材料科学与工程学院,山东青岛266580

出　　处：《中国石油大学学报（自然科学版）》2024年第1期189-196,共8页Journal of China University of Petroleum(Edition of Natural Science)

基　　金：国家自然科学基金项目(51601223);山东省自然科学基金项目(ZR2021ME020,ZR2022MB094)。

摘　　要：贵金属纳米催化剂在苯甲醇部分氧化制备苯甲醛过程中具有较高的反应活性,产物苯甲醛选择性较低。采用一锅法制备TiO_(2)改性的Au-Pd/TiO_(2)-SiO_(2)纳米合金催化剂并用于苯甲醇部分氧化反应。对催化剂结构表征关联反应进行评价。结果表明:少量TiO_(2)的引入会改善贵金属纳米颗粒在载体表面的分散度,调变了金钯合金表面的电子结构,提高反应活性,并显著提高载体表面Lewis酸位的数量,从而大幅提高苯甲醛选择性;大量TiO_(2)的引入会导致金钯合金程度降低,产生大量的Bronsted酸位,使得反应活性和产物选择性都大幅降低。Noble metal nanoparticle catalysts exhibit high catalytic activity in the partial oxidation of benzyl alcohol to benzaldehyde.However,the selectivity of benzaldehyde is low.TiO_(2) modified Au-Pd/TiO_(2)-SiO_(2) nano alloy catalysts were prepared by a one pot method and applied for benzyl alcohol partial oxidation.It is found that the introduction of a small amount of TiO_(2) increases the metal dispersion on the support surface,and modifies the electronic structure of the Au-Pd alloy surface,and improves the reaction activity.Also,the number of Lewis acid sites on the support surface are increased,which improves benzaldehyde selectivity.However,the introduction of a large amount of TiO_(2) destroys the alloying of Au-Pd and produces a large number of Bronsted acid sites,which greatly reduces the reaction activity and product selectivity.

关 键 词：贵金属纳米催化剂 部分氧化 表面酸性 助剂效应 

分 类 号：O646.7[理学—物理化学]