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Title: Methane Catalytic Combustion over Hierarchical Pd@CeO 2 /Si‐Al 2 O 3 : Effect of the Presence of Water

Abstract

Abstract The influence of water vapor on methane catalytic combustion was studied over a Pd@CeO 2 /Si‐Al 2 O 3 catalyst, carefully designed to maximize Pd‐CeO 2 interaction and prevent metal sintering and compared to a conventional impregnated catalyst with identical chemical composition. Although the nanostructured Pd@CeO 2 /Si‐Al 2 O 3 catalyst is thermally stable, the addition of water to the reaction feed leads to a transient deactivation at low temperatures, consistent with the well documented competitive adsorption. In addition to this, the hierarchically structured catalyst exhibits an additional severe deactivation after methane oxidation in the presence of water vapor at 600 °C that can be reversed only by heating the catalyst above 700 °C. The presence of water in the reaction feed deactivates the conventional impregnated catalyst less severely and the activity largely returns upon water removal. Catalytic FTIR and CO‐chemisorption data indicate that this severe deactivation process in the hierarchical catalyst is due to the formation of stable OH groups on the surface of the ceria nanoparticles. These hydroxyl groups are suggested to significantly inhibit the oxygen spillover from the CeO 2 nanoparticles to Pd, preventing its efficient re‐oxidation, as observed by operando X‐ray absorption near edge spectroscopy (XANES)more » experiments. At the same time, their presence can contribute to limit the gas phase accessibility of Pd, as indicated by the decrease of CO chemisorption capability. The presence of hydroxyls plays a minor role on the deactivation of the conventional catalyst at 600 °C.« less

Authors:
; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1401827
Grant/Contract Number:  
DE‐FG02‐13ER16380
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Name: ChemCatChem Journal Volume: 7 Journal Issue: 14; Journal ID: ISSN 1867-3880
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Monai, Matteo, Montini, Tiziano, Chen, Chen, Fonda, Emiliano, Gorte, Raymond J., and Fornasiero, Paolo. Methane Catalytic Combustion over Hierarchical Pd@CeO 2 /Si‐Al 2 O 3 : Effect of the Presence of Water. Germany: N. p., 2014. Web. doi:10.1002/cctc.201402717.
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Monai, Matteo, Montini, Tiziano, Chen, Chen, Fonda, Emiliano, Gorte, Raymond J., & Fornasiero, Paolo. Methane Catalytic Combustion over Hierarchical Pd@CeO 2 /Si‐Al 2 O 3 : Effect of the Presence of Water. Germany. https://doi.org/10.1002/cctc.201402717
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Monai, Matteo, Montini, Tiziano, Chen, Chen, Fonda, Emiliano, Gorte, Raymond J., and Fornasiero, Paolo. Thu . "Methane Catalytic Combustion over Hierarchical Pd@CeO 2 /Si‐Al 2 O 3 : Effect of the Presence of Water". Germany. https://doi.org/10.1002/cctc.201402717.
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@article{osti_1401827,
title = {Methane Catalytic Combustion over Hierarchical Pd@CeO 2 /Si‐Al 2 O 3 : Effect of the Presence of Water},
author = {Monai, Matteo and Montini, Tiziano and Chen, Chen and Fonda, Emiliano and Gorte, Raymond J. and Fornasiero, Paolo},
abstractNote = {Abstract The influence of water vapor on methane catalytic combustion was studied over a Pd@CeO 2 /Si‐Al 2 O 3 catalyst, carefully designed to maximize Pd‐CeO 2 interaction and prevent metal sintering and compared to a conventional impregnated catalyst with identical chemical composition. Although the nanostructured Pd@CeO 2 /Si‐Al 2 O 3 catalyst is thermally stable, the addition of water to the reaction feed leads to a transient deactivation at low temperatures, consistent with the well documented competitive adsorption. In addition to this, the hierarchically structured catalyst exhibits an additional severe deactivation after methane oxidation in the presence of water vapor at 600 °C that can be reversed only by heating the catalyst above 700 °C. The presence of water in the reaction feed deactivates the conventional impregnated catalyst less severely and the activity largely returns upon water removal. Catalytic FTIR and CO‐chemisorption data indicate that this severe deactivation process in the hierarchical catalyst is due to the formation of stable OH groups on the surface of the ceria nanoparticles. These hydroxyl groups are suggested to significantly inhibit the oxygen spillover from the CeO 2 nanoparticles to Pd, preventing its efficient re‐oxidation, as observed by operando X‐ray absorption near edge spectroscopy (XANES) experiments. At the same time, their presence can contribute to limit the gas phase accessibility of Pd, as indicated by the decrease of CO chemisorption capability. The presence of hydroxyls plays a minor role on the deactivation of the conventional catalyst at 600 °C.},
doi = {10.1002/cctc.201402717},
journal = {ChemCatChem},
number = 14,
volume = 7,
place = {Germany},
year = {Thu Oct 30 00:00:00 EDT 2014},
month = {Thu Oct 30 00:00:00 EDT 2014}
}
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https://doi.org/10.1002/cctc.201402717
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