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Impact of Sulfur Poisoning on the NO x Uptake of a NO x Storage and Reduction (NSR) Model Catalyst
Toward obtaining a more detailed understanding of the influence of SO x poisoning on the mechanism of NO x uptake on a NO x storage and reduction (NSR) catalyst, we have performed a model study under ultrahigh vacuum (UHV) conditions. A supported model catalyst based on a thin well-ordered alumina f...
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Published in: | Journal of physical chemistry. C 2010-03, Vol.114 (10), p.4568-4575 |
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container_title | Journal of physical chemistry. C |
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creator | Happel, Markus Desikusumastuti, Aine Sobota, Marek Laurin, Mathias Libuda, Jörg |
description | Toward obtaining a more detailed understanding of the influence of SO x poisoning on the mechanism of NO x uptake on a NO x storage and reduction (NSR) catalyst, we have performed a model study under ultrahigh vacuum (UHV) conditions. A supported model catalyst based on a thin well-ordered alumina film grown on a NiAl(110) single crystal is used onto which BaO and Pd particles are deposited. Time-resolved (TR) infrared reflection absorption spectroscopy (IRAS) is applied to identify the species formed during NO2 uptake on the catalyst surface, which has been pretreated with SO2. These results are compared to the NO2 uptake on the corresponding fresh samples. It is shown that SO2 readily decomposes upon adsorption on both the pristine Al2O3 surface and the BaO and Pd loaded model systems. NO2 reoxidizes the decomposition products to surface sulfites and sulfates. A pronounced influence of the SO2 species on the interaction with NO2 is observed leading to reduced NO2 uptake and to a change of the preferential adsorption geometry from bridging to monodentate. A comparison of the integral intensity of the nitrate bands on the Ba-free and the Ba-containing samples furthermore suggests that SO2 adsorbs preferentially on Ba2+ centers rather than on the Al3+ centers. |
doi_str_mv | 10.1021/jp910777r |
format | article |
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A supported model catalyst based on a thin well-ordered alumina film grown on a NiAl(110) single crystal is used onto which BaO and Pd particles are deposited. Time-resolved (TR) infrared reflection absorption spectroscopy (IRAS) is applied to identify the species formed during NO2 uptake on the catalyst surface, which has been pretreated with SO2. These results are compared to the NO2 uptake on the corresponding fresh samples. It is shown that SO2 readily decomposes upon adsorption on both the pristine Al2O3 surface and the BaO and Pd loaded model systems. NO2 reoxidizes the decomposition products to surface sulfites and sulfates. A pronounced influence of the SO2 species on the interaction with NO2 is observed leading to reduced NO2 uptake and to a change of the preferential adsorption geometry from bridging to monodentate. A comparison of the integral intensity of the nitrate bands on the Ba-free and the Ba-containing samples furthermore suggests that SO2 adsorbs preferentially on Ba2+ centers rather than on the Al3+ centers.</description><identifier>ISSN: 1932-7447</identifier><identifier>EISSN: 1932-7455</identifier><identifier>DOI: 10.1021/jp910777r</identifier><language>eng</language><publisher>American Chemical Society</publisher><subject>C: Surfaces, Interfaces, Catalysis</subject><ispartof>Journal of physical chemistry. 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A pronounced influence of the SO2 species on the interaction with NO2 is observed leading to reduced NO2 uptake and to a change of the preferential adsorption geometry from bridging to monodentate. 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C</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Happel, Markus</au><au>Desikusumastuti, Aine</au><au>Sobota, Marek</au><au>Laurin, Mathias</au><au>Libuda, Jörg</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Impact of Sulfur Poisoning on the NO x Uptake of a NO x Storage and Reduction (NSR) Model Catalyst</atitle><jtitle>Journal of physical chemistry. C</jtitle><addtitle>J. Phys. Chem. C</addtitle><date>2010-03-18</date><risdate>2010</risdate><volume>114</volume><issue>10</issue><spage>4568</spage><epage>4575</epage><pages>4568-4575</pages><issn>1932-7447</issn><eissn>1932-7455</eissn><abstract>Toward obtaining a more detailed understanding of the influence of SO x poisoning on the mechanism of NO x uptake on a NO x storage and reduction (NSR) catalyst, we have performed a model study under ultrahigh vacuum (UHV) conditions. A supported model catalyst based on a thin well-ordered alumina film grown on a NiAl(110) single crystal is used onto which BaO and Pd particles are deposited. Time-resolved (TR) infrared reflection absorption spectroscopy (IRAS) is applied to identify the species formed during NO2 uptake on the catalyst surface, which has been pretreated with SO2. These results are compared to the NO2 uptake on the corresponding fresh samples. It is shown that SO2 readily decomposes upon adsorption on both the pristine Al2O3 surface and the BaO and Pd loaded model systems. NO2 reoxidizes the decomposition products to surface sulfites and sulfates. A pronounced influence of the SO2 species on the interaction with NO2 is observed leading to reduced NO2 uptake and to a change of the preferential adsorption geometry from bridging to monodentate. A comparison of the integral intensity of the nitrate bands on the Ba-free and the Ba-containing samples furthermore suggests that SO2 adsorbs preferentially on Ba2+ centers rather than on the Al3+ centers.</abstract><pub>American Chemical Society</pub><doi>10.1021/jp910777r</doi><tpages>8</tpages></addata></record> |
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title | Impact of Sulfur Poisoning on the NO x Uptake of a NO x Storage and Reduction (NSR) Model Catalyst |
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