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Toluene total oxidation over CuO-CeO2/Al2O3: structural and kinetic characterization

Unmesh Menon (2013)
abstract
Catalytic oxidation is an important technique for the destruction of Volatile Organic Compounds (VOCs). Precious metals, and the cheaper transition metal oxides constitute efficient catalysts for such processes. In this work, the total oxidation of toluene as VOC model molecule is studied over the binary metal oxide CuO-CeO2/gamma-Al2O3 using Temporal Analysis of Products (TAP). TAP is a transient pulse response technique with millisecond time resolution which help obtain information on the reactants, intermediates and end-products. Toluene reacts catalytically with oxygen to form CO2 and H2O, while oxygen in the feed re-oxidize the catalyst, according to the mechanism of Mars and van Krevelen. The TAP data allows to illustrate the reaction with a detailed reaction network. In order to elucidate the catalytic structure-activity relationship, the catalyst is characterized by high-resolution transmission electron microscope (HRTEM) and X-ray absorption spectroscopy (XAS). This results in the discovery of the active phase in the catalyst which is a solid solution of ceria with built-in substitutional Cu2+. The interaction between Ce and Cu herein, is responsible for the high reactivity of the bimetallic catalyst in the total oxidation of toluene. The reaction network and the structural information are finally coupled to a microkinetic model that describes the experimental data over a wide range of experimental conditions. Microkinetic modeling of the reaction using the transient response experimental data allows identification of the kinetically significant steps and estimation of the corresponding kinetic parameters.
Please use this url to cite or link to this publication:
author
promoter
UGent and UGent
organization
year
type
dissertation
publication status
published
subject
keyword
Transient response technique, Temporal Analysis of Products (TAP), Copper oxide, Ceria, Binary metal oxide, Reaction network, Structural characterization, Toluene total oxidation, Role of ceria, Microkinetic modeling
pages
169 pages
publisher
Department of Chemical engineering and technical chemistry, Ghent University
place of publication
Ghent, Belgium
defense location
Gent: Jozef-Plateauzaal (Jozef-Plateaustraat 22)
defense date
2013-01-07 14:00
ISBN
9789085785699
language
English
UGent publication?
yes
classification
D1
copyright statement
I have retained and own the full copyright for this publication
id
3095566
handle
http://hdl.handle.net/1854/LU-3095566
date created
2013-01-16 16:39:20
date last changed
2017-03-09 12:42:15
@phdthesis{3095566,
  abstract     = {Catalytic oxidation is an important technique for the destruction of Volatile Organic Compounds (VOCs). Precious metals, and the cheaper transition metal oxides constitute efficient catalysts for such processes. In this work, the total oxidation of toluene as VOC model molecule is studied over the binary metal oxide CuO-CeO2/gamma-Al2O3 using Temporal Analysis of Products (TAP). TAP is a transient pulse response technique with millisecond time resolution which help obtain information on the reactants, intermediates and end-products. Toluene reacts catalytically with oxygen to form CO2 and H2O, while oxygen in the feed re-oxidize the catalyst, according to the mechanism of Mars and van Krevelen. The TAP data allows to illustrate the reaction with a detailed reaction network. In order to elucidate the catalytic structure-activity relationship, the catalyst is characterized by high-resolution transmission electron microscope (HRTEM) and X-ray absorption spectroscopy (XAS). This results in the discovery of the active phase in the catalyst which is a solid solution of ceria with built-in substitutional Cu2+. The interaction between Ce and Cu herein, is responsible for the high reactivity of the bimetallic catalyst in the total oxidation of toluene. The reaction network and the structural information are finally coupled to a microkinetic model that describes the experimental data over a wide range of experimental conditions. Microkinetic modeling of the reaction using the transient response experimental data allows identification of the kinetically significant steps and estimation of the corresponding kinetic parameters.},
  author       = {Menon, Unmesh},
  isbn         = {9789085785699},
  keyword      = {Transient response technique,Temporal Analysis of Products (TAP),Copper oxide,Ceria,Binary metal oxide,Reaction network,Structural characterization,Toluene total oxidation,Role of ceria,Microkinetic modeling},
  language     = {eng},
  pages        = {169},
  publisher    = {Department of Chemical engineering and technical chemistry, Ghent University},
  school       = {Ghent University},
  title        = {Toluene total oxidation over CuO-CeO2/Al2O3: structural and kinetic characterization},
  year         = {2013},
}

Chicago
Menon, Unmesh. 2013. “Toluene Total Oxidation over CuO-CeO2/Al2O3: Structural and Kinetic Characterization”. Ghent, Belgium: Department of Chemical engineering and technical chemistry, Ghent University.
APA
Menon, U. (2013). Toluene total oxidation over CuO-CeO2/Al2O3: structural and kinetic characterization. Department of Chemical engineering and technical chemistry, Ghent University, Ghent, Belgium.
Vancouver
1.
Menon U. Toluene total oxidation over CuO-CeO2/Al2O3: structural and kinetic characterization. [Ghent, Belgium]: Department of Chemical engineering and technical chemistry, Ghent University; 2013.
MLA
Menon, Unmesh. “Toluene Total Oxidation over CuO-CeO2/Al2O3: Structural and Kinetic Characterization.” 2013 : n. pag. Print.