State Key Laboratory of Heavy Oil Processing, Key Laboratory of Catalysis, College of Chemical Engineering, China University of Petroleum , Qingdao 266580, China.
Petrochina Petrochemical Research Institute , Beijing 102206, China.
ACS Appl Mater Interfaces. 2016 Oct 5;8(39):25979-25990. doi: 10.1021/acsami.6b07779. Epub 2016 Sep 26.
Mesoporous γ-AlO was synthesized via a cation-anion double hydrolysis approach (CADH). The synthesized mesoporous alumina displayed a relatively high surface area, a large pore volume and a narrow pore size distribution. By applying the mesoporous alumina as a support, supported vanadium catalysts were prepared and evaluated in the dehydrogenation of propane, exhibiting a superior catalytic performance over that supported on a commercial alumina. Materials were characterized with a variety of techniques such as X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet-visible spectroscopy, V magnetic angle spinning nuclear magnetic resonance, Raman spectroscopy, Fourier transformed infrared spectroscopy of pyridine adsorption and thermogravimetric-differential thermal analysis. The correlated structure-performance relationship of catalysts reveals that a higher crystallization temperature endows mesoporous alumina materials with more surface acid sites, favoring the formation of polymerized VO species, which are more active than isolated ones in the propane dehydrogenation, resulting in a better catalytic performance. The established relationship between surface chemistry and catalytic performance of supported VO catalysts suggests that a superior vanadium catalyst for propane dehydrogenation could be achieved by rationally enriching the concentration of polymeric VO species on the catalyst, which can be realized by tuning the surface acidity of alumina support.
介孔 γ-AlO 通过阳离子-阴离子双水解法(CADH)合成。所合成的介孔氧化铝表现出较高的比表面积、较大的孔体积和较窄的孔径分布。将介孔氧化铝用作载体,制备并评价了负载型钒催化剂在丙烷脱氢反应中的性能,其催化性能优于负载在商业氧化铝上的催化剂。采用 X 射线衍射、X 射线光电子能谱、紫外-可见光谱、V 魔角旋转核磁共振、拉曼光谱、吡啶吸附傅里叶变换红外光谱和热重-差热分析等多种技术对材料进行了表征。催化剂的结构-性能相关性表明,较高的结晶温度赋予介孔氧化铝材料更多的表面酸性位,有利于聚合 VO 物种的形成,这些物种在丙烷脱氢反应中比孤立物种更活跃,从而表现出更好的催化性能。负载 VO 催化剂的表面化学与催化性能之间的关系表明,通过合理增加催化剂上聚合 VO 物种的浓度,可以实现丙烷脱氢用性能更优的钒催化剂,这可以通过调节氧化铝载体的表面酸度来实现。