Au／TiO2催化剂制备条件对巴豆醛选择加氢的影响  

Influence of Au/TiO_2 Catalyst Preparation Parameters on the Selective Hydrogenation of Crotonaldehyde

作　　者：杨秋芸[1] 朱渊[1] 田莉[1] 裴燕[1] 乔明华[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

出　　处：《物理化学学报》2009年第9期1853-1860,共8页Acta Physico-Chimica Sinica

基　　金：国家重点基础研究发展计划(973项目)(2006CB202502);国家自然科学基金(20673025,20803011);教育部新世纪优秀人才支持计划;霍英东教育基金(104022);上海市科委科技基金(07ZR14007,08DZ2270500);石油化工催化材料与反应工程国家重点实验室开放基金(RIPP,SINOPEC)资助项目~~

摘　　要：采用沉积-沉淀法制备了纳米Au/TiO2催化剂,以X射线衍射(XRD)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)等手段对催化剂进行了系统的表征,并考察了该催化剂在巴豆醛液相加氢制巴豆醇反应中的催化性能.通过改变活化气氛、负载量和还原温度,能够调节Au粒子的尺寸及金属与载体间的相互作用.在673K还原条件下制备Au质量分数为9.2%的Au/TiO2催化剂上,Au粒子的平均粒径为2nm,初始加氢速率达到13.7×10-5mol·s-1·g-1,同时巴豆醇最高收率可达69.9%.结合表征结果,该催化剂良好的巴豆醛选择加氢性能归属为载体TiO2在还原条件下产生的氧缺陷位对Au纳米粒子的锚定作用及给电子作用.Nanosized Au/TiO2 catalysts were prepared by the deposition-precipitation method. These catalysts were evaluated by a liquid phase hydrogenation of crotonaldehyde to crotyl alcohol and characterized by X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and X-ray photoelectron spectroscopy （XPS）. By changing the activation atmosphere, the Au loading, and the reduction temperature we found that the dimension of the Au particles and the metal-support interaction were readily adjustable. For the Au/TiO2 eatalyst reduced at 673 K with an optimal Au mass fraction of 9.2%, the mean particle size of Au was 2 nm and the initial hydrogenation rate was as high as 13.7×10^-6mol·s^-1·g^-1, while the maximum yield of crotyl alcohol was 69.9%. Combined with the characterization results, the superior performance of this catalyst was attributed to it having an optimal size and to its electronic modification effects on the Au nanoparticles. This was due to oxygen defects generated on the TiO2 during the reduction process.

关 键 词：选择加氢 AU/TIO2 制备条件 巴豆醛 巴豆醇 

分 类 号：O643.32[理学—物理化学]