Oxidative dehydrogenation of ethane over Ni-W-O mixed metal oxide catalysts

被引:111
|
作者
Solsona, B. [2 ]
Lopez Nieto, J. M. [1 ]
Concepcion, P. [1 ]
Dejoz, A. [2 ]
Ivars, F. [1 ]
Vazquez, M. I. [2 ]
机构
[1] Univ Politecn Valencia, CSIC, Inst Tecnol Quim, Valencia 46022, Spain
[2] Univ Valencia, Dep Ingn Quim, E-46100 Burjassot, Spain
关键词
Nickel tungsten metal oxide catalysts; Oxidative dehydrogenation of ethane; Ethylene oxidation; Catalyst characterization; XPS; TPR; XRD; Raman; FTIR of adsorbed CO; Oxygen isotopic exchange; TEMPERATURE-PROGRAMMED-REDUCTION; RAY PHOTOEMISSION-SPECTROSCOPY; PHOTOELECTRON-SPECTROSCOPY; SUPPORTED CATALYSTS; SELECTIVE CATALYSTS; ETHENE PRODUCTION; ETHYLENE; SURFACE; ACTIVATION; PROPANE;
D O I
10.1016/j.jcat.2011.02.010
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ni-W-O mixed oxides were prepared through the evaporation of aqueous solutions of nickel nitrate and ammonium tungstate and calcined in air at 500 degrees C for 2 h. The catalysts were characterized by several techniques (N-2 adsorption, X-ray diffraction, temperature-programmed reduction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy of adsorbed CO, and O-18/O-16 isotope exchange) and tested in the oxidative dehydrogenation of ethane. The catalytic activity and catalyst reducibility decrease when the W content increases. Thus, nickel sites seem to be the active centers for ethane activation in these catalysts. However, the selectivity to ethylene strongly changes depending on the Ni/W ratio. In W-rich catalysts, in which NiWO4 and WO3 are mainly observed, a strong influence of ethane conversion on the selectivity to ethylene is observed. However, in Ni-rich catalysts, in which NiO crystallites and WOx nanoparticles are mainly observed, ethane conversion hardly influences the selectivity to ethylene. It has been demonstrated that the nature of the Ni sites and the characteristics and number of the acid sites determine the catalytic behavior of these catalysts. The presence of Lewis acid sites with high acid strength in W-rich catalysts facilitates the decomposition of ethylene during ethane oxidation. (C) 2011 Elsevier Inc. All rights reserved.
引用
收藏
页码:28 / 39
页数:12
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