期刊
JOURNAL OF CATALYSIS
卷 271, 期 2, 页码 370-385出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2010.02.026
关键词
Alkane aromatization; Propane; Gallium; ZSM-5; Kinetic modeling
资金
- Department of Energy, Office of the Basic Energy Sciences [DE-FG02-03ER15466]
Ga/HZSM-5 catalysts, synthesized by the incipient wetness impregnation technique, showed a steady decline in Brensted acidity with gallium addition. A maximum in propane conversion and aromatics selectivity at a Ga/Al ratio of about 0.5 suggests synergy between proton and gallium sites. A microkinetic model using 312 elementary steps and 25 rate and equilibrium parameters to describe the aromatization of propane over HZSM-5 with Si/Al of 16 is the base case against which the effects of Ga are compared. Kinetic models based on two different Ga active sites, including GaH2+ and GaH2+, were first used individually to describe the diverse dataset that includes conversion to 10 different products as a function of temperature (510-540 degrees C), space time (2-8 g(cat) h/mol), and Ga/Al (0-1) variations. An evaluation of these models based on an assigned catalytic functionality for these sites and the associated parameters showed that both sites are required to provide a unified description of the catalytic behavior across gallium content with monohydridic Ga-sites being predominantly prevalent at low Ga/Al ratio and dihydridic Gasites at high Ga/Al ratios. In this paper, we address the ability to discriminate between the models and their implications for the primarily dehydrogenation nature of the Ga active sites. (C) 2010 Elsevier Inc. All rights reserved.
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