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Title: Carbon and oxygen reaction pathways of CO{sub 2} reforming of methane over Ni/La{sub 2}O{sub 3}and Ni/Al{sub 2}O{sub 3} catalysts studied by isotopic tracing techniques

Abstract

Steady-state tracing techniques, using isotopically labeled molecules, were applied to study mechanistic aspects of the carbon and oxygen reaction pathways to form CO over Ni/La{sub 2}O{sub 3} and Ni/Al{sub 2}O{sub 3} catalysts. Over the Ni/La{sub 2}O{sub 3} catalyst, it was found that under steady-state reaction conditions, the quantity of reversibly adsorbed CH{sub 4} and the active carbon-containing intermediate species in the carbon pathway to form CO originating from CH{sub 4} is higher than the respective quantities derived from the CO{sub 2} molecule. Over the Ni/Al{sub 2}O{sub 3} catalyst, much smaller quantities of reversibly adsorbed CH{sub 4} and active carbon-containing species, originated from the CH{sub 4} molecule, which lead to CO formation were detected. It was also determined that a large quantity of oxygen atoms, originating from the La{sub 2}O{sub 3} support of the Ni/La{sub 2}O{sub 3} catalyst, participate in the reaction scheme. It is concluded that La{sub 2}O{sub 2}CO{sub 3}, which form by the interaction of La{sub 2}O{sub 3} and CO{sub 2}, may decompose to produce CO or provide oxygen species which react with carbon accumulated on Ni crystallites due to CH{sub 2} cracking to produce CO. The latter process is very fast over the Ni/La{sub 2}O{sub 3} catalyst, asmore » compared to carbon accumulation, and this imparts this catalyst its special stability characteristics.« less

Authors:
;
Publication Date:
Research Org.:
Univ. of Patras (GR)
OSTI Identifier:
20000961
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; Journal Volume: 187; Journal Issue: 1; Other Information: PBD: 1 Oct 1999
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; 10 SYNTHETIC FUELS; METHANE; REFORMER PROCESSES; CARBON DIOXIDE; NICKEL; CATALYTIC EFFECTS; LANTHANUM OXIDES; ALUMINIUM OXIDES; CHEMICAL REACTION KINETICS; REACTION INTERMEDIATES; SYNTHESIS GAS

Citation Formats

Tsipouriari, V.A., and Verykios, X.E. Carbon and oxygen reaction pathways of CO{sub 2} reforming of methane over Ni/La{sub 2}O{sub 3}and Ni/Al{sub 2}O{sub 3} catalysts studied by isotopic tracing techniques. United States: N. p., 1999. Web. doi:10.1006/jcat.1999.2565.
Tsipouriari, V.A., & Verykios, X.E. Carbon and oxygen reaction pathways of CO{sub 2} reforming of methane over Ni/La{sub 2}O{sub 3}and Ni/Al{sub 2}O{sub 3} catalysts studied by isotopic tracing techniques. United States. doi:10.1006/jcat.1999.2565.
Tsipouriari, V.A., and Verykios, X.E. Fri . "Carbon and oxygen reaction pathways of CO{sub 2} reforming of methane over Ni/La{sub 2}O{sub 3}and Ni/Al{sub 2}O{sub 3} catalysts studied by isotopic tracing techniques". United States. doi:10.1006/jcat.1999.2565.
@article{osti_20000961,
title = {Carbon and oxygen reaction pathways of CO{sub 2} reforming of methane over Ni/La{sub 2}O{sub 3}and Ni/Al{sub 2}O{sub 3} catalysts studied by isotopic tracing techniques},
author = {Tsipouriari, V.A. and Verykios, X.E.},
abstractNote = {Steady-state tracing techniques, using isotopically labeled molecules, were applied to study mechanistic aspects of the carbon and oxygen reaction pathways to form CO over Ni/La{sub 2}O{sub 3} and Ni/Al{sub 2}O{sub 3} catalysts. Over the Ni/La{sub 2}O{sub 3} catalyst, it was found that under steady-state reaction conditions, the quantity of reversibly adsorbed CH{sub 4} and the active carbon-containing intermediate species in the carbon pathway to form CO originating from CH{sub 4} is higher than the respective quantities derived from the CO{sub 2} molecule. Over the Ni/Al{sub 2}O{sub 3} catalyst, much smaller quantities of reversibly adsorbed CH{sub 4} and active carbon-containing species, originated from the CH{sub 4} molecule, which lead to CO formation were detected. It was also determined that a large quantity of oxygen atoms, originating from the La{sub 2}O{sub 3} support of the Ni/La{sub 2}O{sub 3} catalyst, participate in the reaction scheme. It is concluded that La{sub 2}O{sub 2}CO{sub 3}, which form by the interaction of La{sub 2}O{sub 3} and CO{sub 2}, may decompose to produce CO or provide oxygen species which react with carbon accumulated on Ni crystallites due to CH{sub 2} cracking to produce CO. The latter process is very fast over the Ni/La{sub 2}O{sub 3} catalyst, as compared to carbon accumulation, and this imparts this catalyst its special stability characteristics.},
doi = {10.1006/jcat.1999.2565},
journal = {Journal of Catalysis},
number = 1,
volume = 187,
place = {United States},
year = {Fri Oct 01 00:00:00 EDT 1999},
month = {Fri Oct 01 00:00:00 EDT 1999}
}