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Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO
In this work, the poisoning effect of SO 2 was investigated in binary MnTi and ternary MnCeTi mixed oxides for the NH 3 -SCR reaction under conditions relevant for mobile applications. For the binary MnTi sample, catalytic activity increases up to 250 °C, and then drops due to the oxidation of ammon...
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Published in: | Catalysis science & technology 2022-11, Vol.12 (22), p.6838-6848 |
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creator | Ruiz-Martínez, Javier Gevers, Lieven E Enakonda, Linga R Shahid, Ameen Wen, Fei |
description | In this work, the poisoning effect of SO
2
was investigated in binary MnTi and ternary MnCeTi mixed oxides for the NH
3
-SCR reaction under conditions relevant for mobile applications. For the binary MnTi sample, catalytic activity increases up to 250 °C, and then drops due to the oxidation of ammonia to NO
x
. The addition of Ce decreases the catalytic activity at 150 °C but widens the optimal operational temperature and reaches high conversion at 350 C. Upon performing activity test with 100 ppm of SO
2
in the gas stream, catalytic activity drastically decreases in all catalyst samples. The shape of the deactivation curve and SO
2
concentrations at the outlet of the reactor suggest a strong adsorption and poisoning of SO
2
on all the catalysts. Although samples containing large amounts of Ce display a better SO
2
tolerance, this is insufficient to be considered for practical applications. Deactivated samples were investigated by a wide range of characterization tools. N
2
physisorption measurements reveal a drop in the surface area that could partially explain catalyst deactivation. TGA reveals the absence of (NH
4
)
2
SO
4
on the deactivated samples and suggests the formation of Mn and Ce sulfates on the catalyst surface. XPS results confirm the formation of MnSO
4
and also show a decrease in the Mn and Ce oxidation states. Analysis of the redox function by catalytic NO oxidation and H
2
-TPR experiments shows a strong loss of redox function upon SO
2
deactivation, which could explain the decrease of NH
3
-SCR catalytic activity. Upon unraveling the effect and cause of deactivation, a doping study was performed. As in the binary MnTi and ternary MnCeTi, catalytic activity strongly decreases upon the introduction of SO
2
in the gas stream. None of the dopants investigated was able to suppress SO
2
deactivation, which suggest that other dopants or strategies should be pursued to commercialize Mn-based catalysts for low-temperature applications.
In real mobile applications, deactivation of Mn-based catalysts by SO
2
is severe and catalysts underperform at temperatures below 200 °C. SO
2
deactivates the catalysts' redox function and regeneration is cumbersome. |
doi_str_mv | 10.1039/d2cy01151d |
format | article |
fullrecord | <record><control><sourceid>rsc</sourceid><recordid>TN_cdi_rsc_primary_d2cy01151d</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>d2cy01151d</sourcerecordid><originalsourceid>FETCH-rsc_primary_d2cy01151d3</originalsourceid><addsrcrecordid>eNqFjssKwjAQRYMoWNSNe2F-oJq09bWWihvtQvcS85BITUqmFfr3Biy6dDb3cC8chpApo3NG0-1CJqKljC2Z7JEooVkWZ-sV6395mQ7JBPFBw2VbRjdJRHSutRI1OA3nAipn0Flj7-AsNFa6SkngVsKHjja-cQwgeM3LFmsE7TygKoPCvFTX10aAV7IJXdAE86kYk4HmJapJlyMy2-eX3SH2KK6VN0_u2-vv__Tf_gagNEj8</addsrcrecordid><sourcetype>Publisher</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO</title><source>Royal Society of Chemistry</source><creator>Ruiz-Martínez, Javier ; Gevers, Lieven E ; Enakonda, Linga R ; Shahid, Ameen ; Wen, Fei</creator><creatorcontrib>Ruiz-Martínez, Javier ; Gevers, Lieven E ; Enakonda, Linga R ; Shahid, Ameen ; Wen, Fei</creatorcontrib><description>In this work, the poisoning effect of SO
2
was investigated in binary MnTi and ternary MnCeTi mixed oxides for the NH
3
-SCR reaction under conditions relevant for mobile applications. For the binary MnTi sample, catalytic activity increases up to 250 °C, and then drops due to the oxidation of ammonia to NO
x
. The addition of Ce decreases the catalytic activity at 150 °C but widens the optimal operational temperature and reaches high conversion at 350 C. Upon performing activity test with 100 ppm of SO
2
in the gas stream, catalytic activity drastically decreases in all catalyst samples. The shape of the deactivation curve and SO
2
concentrations at the outlet of the reactor suggest a strong adsorption and poisoning of SO
2
on all the catalysts. Although samples containing large amounts of Ce display a better SO
2
tolerance, this is insufficient to be considered for practical applications. Deactivated samples were investigated by a wide range of characterization tools. N
2
physisorption measurements reveal a drop in the surface area that could partially explain catalyst deactivation. TGA reveals the absence of (NH
4
)
2
SO
4
on the deactivated samples and suggests the formation of Mn and Ce sulfates on the catalyst surface. XPS results confirm the formation of MnSO
4
and also show a decrease in the Mn and Ce oxidation states. Analysis of the redox function by catalytic NO oxidation and H
2
-TPR experiments shows a strong loss of redox function upon SO
2
deactivation, which could explain the decrease of NH
3
-SCR catalytic activity. Upon unraveling the effect and cause of deactivation, a doping study was performed. As in the binary MnTi and ternary MnCeTi, catalytic activity strongly decreases upon the introduction of SO
2
in the gas stream. None of the dopants investigated was able to suppress SO
2
deactivation, which suggest that other dopants or strategies should be pursued to commercialize Mn-based catalysts for low-temperature applications.
In real mobile applications, deactivation of Mn-based catalysts by SO
2
is severe and catalysts underperform at temperatures below 200 °C. SO
2
deactivates the catalysts' redox function and regeneration is cumbersome.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/d2cy01151d</identifier><ispartof>Catalysis science & technology, 2022-11, Vol.12 (22), p.6838-6848</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Ruiz-Martínez, Javier</creatorcontrib><creatorcontrib>Gevers, Lieven E</creatorcontrib><creatorcontrib>Enakonda, Linga R</creatorcontrib><creatorcontrib>Shahid, Ameen</creatorcontrib><creatorcontrib>Wen, Fei</creatorcontrib><title>Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO</title><title>Catalysis science & technology</title><description>In this work, the poisoning effect of SO
2
was investigated in binary MnTi and ternary MnCeTi mixed oxides for the NH
3
-SCR reaction under conditions relevant for mobile applications. For the binary MnTi sample, catalytic activity increases up to 250 °C, and then drops due to the oxidation of ammonia to NO
x
. The addition of Ce decreases the catalytic activity at 150 °C but widens the optimal operational temperature and reaches high conversion at 350 C. Upon performing activity test with 100 ppm of SO
2
in the gas stream, catalytic activity drastically decreases in all catalyst samples. The shape of the deactivation curve and SO
2
concentrations at the outlet of the reactor suggest a strong adsorption and poisoning of SO
2
on all the catalysts. Although samples containing large amounts of Ce display a better SO
2
tolerance, this is insufficient to be considered for practical applications. Deactivated samples were investigated by a wide range of characterization tools. N
2
physisorption measurements reveal a drop in the surface area that could partially explain catalyst deactivation. TGA reveals the absence of (NH
4
)
2
SO
4
on the deactivated samples and suggests the formation of Mn and Ce sulfates on the catalyst surface. XPS results confirm the formation of MnSO
4
and also show a decrease in the Mn and Ce oxidation states. Analysis of the redox function by catalytic NO oxidation and H
2
-TPR experiments shows a strong loss of redox function upon SO
2
deactivation, which could explain the decrease of NH
3
-SCR catalytic activity. Upon unraveling the effect and cause of deactivation, a doping study was performed. As in the binary MnTi and ternary MnCeTi, catalytic activity strongly decreases upon the introduction of SO
2
in the gas stream. None of the dopants investigated was able to suppress SO
2
deactivation, which suggest that other dopants or strategies should be pursued to commercialize Mn-based catalysts for low-temperature applications.
In real mobile applications, deactivation of Mn-based catalysts by SO
2
is severe and catalysts underperform at temperatures below 200 °C. SO
2
deactivates the catalysts' redox function and regeneration is cumbersome.</description><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid/><recordid>eNqFjssKwjAQRYMoWNSNe2F-oJq09bWWihvtQvcS85BITUqmFfr3Biy6dDb3cC8chpApo3NG0-1CJqKljC2Z7JEooVkWZ-sV6395mQ7JBPFBw2VbRjdJRHSutRI1OA3nAipn0Flj7-AsNFa6SkngVsKHjja-cQwgeM3LFmsE7TygKoPCvFTX10aAV7IJXdAE86kYk4HmJapJlyMy2-eX3SH2KK6VN0_u2-vv__Tf_gagNEj8</recordid><startdate>20221114</startdate><enddate>20221114</enddate><creator>Ruiz-Martínez, Javier</creator><creator>Gevers, Lieven E</creator><creator>Enakonda, Linga R</creator><creator>Shahid, Ameen</creator><creator>Wen, Fei</creator><scope/></search><sort><creationdate>20221114</creationdate><title>Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO</title><author>Ruiz-Martínez, Javier ; Gevers, Lieven E ; Enakonda, Linga R ; Shahid, Ameen ; Wen, Fei</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-rsc_primary_d2cy01151d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><creationdate>2022</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ruiz-Martínez, Javier</creatorcontrib><creatorcontrib>Gevers, Lieven E</creatorcontrib><creatorcontrib>Enakonda, Linga R</creatorcontrib><creatorcontrib>Shahid, Ameen</creatorcontrib><creatorcontrib>Wen, Fei</creatorcontrib><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ruiz-Martínez, Javier</au><au>Gevers, Lieven E</au><au>Enakonda, Linga R</au><au>Shahid, Ameen</au><au>Wen, Fei</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO</atitle><jtitle>Catalysis science & technology</jtitle><date>2022-11-14</date><risdate>2022</risdate><volume>12</volume><issue>22</issue><spage>6838</spage><epage>6848</epage><pages>6838-6848</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>In this work, the poisoning effect of SO
2
was investigated in binary MnTi and ternary MnCeTi mixed oxides for the NH
3
-SCR reaction under conditions relevant for mobile applications. For the binary MnTi sample, catalytic activity increases up to 250 °C, and then drops due to the oxidation of ammonia to NO
x
. The addition of Ce decreases the catalytic activity at 150 °C but widens the optimal operational temperature and reaches high conversion at 350 C. Upon performing activity test with 100 ppm of SO
2
in the gas stream, catalytic activity drastically decreases in all catalyst samples. The shape of the deactivation curve and SO
2
concentrations at the outlet of the reactor suggest a strong adsorption and poisoning of SO
2
on all the catalysts. Although samples containing large amounts of Ce display a better SO
2
tolerance, this is insufficient to be considered for practical applications. Deactivated samples were investigated by a wide range of characterization tools. N
2
physisorption measurements reveal a drop in the surface area that could partially explain catalyst deactivation. TGA reveals the absence of (NH
4
)
2
SO
4
on the deactivated samples and suggests the formation of Mn and Ce sulfates on the catalyst surface. XPS results confirm the formation of MnSO
4
and also show a decrease in the Mn and Ce oxidation states. Analysis of the redox function by catalytic NO oxidation and H
2
-TPR experiments shows a strong loss of redox function upon SO
2
deactivation, which could explain the decrease of NH
3
-SCR catalytic activity. Upon unraveling the effect and cause of deactivation, a doping study was performed. As in the binary MnTi and ternary MnCeTi, catalytic activity strongly decreases upon the introduction of SO
2
in the gas stream. None of the dopants investigated was able to suppress SO
2
deactivation, which suggest that other dopants or strategies should be pursued to commercialize Mn-based catalysts for low-temperature applications.
In real mobile applications, deactivation of Mn-based catalysts by SO
2
is severe and catalysts underperform at temperatures below 200 °C. SO
2
deactivates the catalysts' redox function and regeneration is cumbersome.</abstract><doi>10.1039/d2cy01151d</doi><tpages>11</tpages></addata></record> |
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source | Royal Society of Chemistry |
title | Effect of SO poisoning on undoped and doped Mn-based catalysts for selective catalytic reduction of NO |
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