Hydrothermal stability of CuSSZ13 for reducing NOx by NH3

[Display omitted] •Deactivation of CuSSZ13 by aging becomes more severe as the Cu/Al ratio increases.•Cu2+ ions are first exchanged on the sites on D6R (α) before those in the CHA cage (β).•The β/α ratio reveals a rising trend with increasing Cu/Al ratio.•Cu2+ ions on the CHA sites readily agglomera...

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Veröffentlicht in:Journal of catalysis 2014-03, Vol.311, p.447-457
Hauptverfasser: Kim, Young Jin, Lee, Jun Kyu, Min, Kyung Myung, Hong, Suk Bong, Nam, In-Sik, Cho, Byong K.
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container_end_page 457
container_issue
container_start_page 447
container_title Journal of catalysis
container_volume 311
creator Kim, Young Jin
Lee, Jun Kyu
Min, Kyung Myung
Hong, Suk Bong
Nam, In-Sik
Cho, Byong K.
description [Display omitted] •Deactivation of CuSSZ13 by aging becomes more severe as the Cu/Al ratio increases.•Cu2+ ions are first exchanged on the sites on D6R (α) before those in the CHA cage (β).•The β/α ratio reveals a rising trend with increasing Cu/Al ratio.•Cu2+ ions on the CHA sites readily agglomerate leading to the formation of CuOx.•Collapse of SSZ13 due to CuOx is the primary cause for the hydrothermal deactivation. The hydrothermal stability of CuSSZ13 catalysts with respect to their Cu/Al ratio has been investigated to understand the deactivation mechanism of their catalytic activity for NO reduction by NH3/SCR. The decline of the deNOx activity due to the hydrothermal aging became more severe as the Cu/Al ratio increased. Results of ESR, H2-TPR and DRIFT studies indicated that the D6R sites are occupied first by Cu2+ ions (α species) up to their accommodation capacity, followed by the occupation of the CHA sites (β species) with the increase in the Cu/Al ratio. The β species agglomerate more readily than α species due to their less stable nature, leading to the formation of CuOx. The CuOx may grow to destroy the zeolite cage and channel, resulting in the collapse of the SSZ13 structure, which is believed to be the primary cause for the hydrothermal deactivation of the CuSSZ13 catalyst.
doi_str_mv 10.1016/j.jcat.2013.12.012
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The hydrothermal stability of CuSSZ13 catalysts with respect to their Cu/Al ratio has been investigated to understand the deactivation mechanism of their catalytic activity for NO reduction by NH3/SCR. The decline of the deNOx activity due to the hydrothermal aging became more severe as the Cu/Al ratio increased. Results of ESR, H2-TPR and DRIFT studies indicated that the D6R sites are occupied first by Cu2+ ions (α species) up to their accommodation capacity, followed by the occupation of the CHA sites (β species) with the increase in the Cu/Al ratio. The β species agglomerate more readily than α species due to their less stable nature, leading to the formation of CuOx. The CuOx may grow to destroy the zeolite cage and channel, resulting in the collapse of the SSZ13 structure, which is believed to be the primary cause for the hydrothermal deactivation of the CuSSZ13 catalyst.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2013.12.012</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Catalysis ; Catalysts ; Chemistry ; CuSSZ13 ; ESR ; Exact sciences and technology ; General and physical chemistry ; Hydrothermal stability ; NH3/SCR ; Nitrous oxide ; NOx reduction ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; Thermal energy</subject><ispartof>Journal of catalysis, 2014-03, Vol.311, p.447-457</ispartof><rights>2014 Elsevier Inc.</rights><rights>2015 INIST-CNRS</rights><rights>Copyright © 2014 Elsevier B.V. All rights reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c461t-a47ec5a2d54753bc1956274b2c66028a732d1c03c638a54e966988b56bd038d13</citedby><cites>FETCH-LOGICAL-c461t-a47ec5a2d54753bc1956274b2c66028a732d1c03c638a54e966988b56bd038d13</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0021951713004466$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&amp;idt=28313090$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Kim, Young Jin</creatorcontrib><creatorcontrib>Lee, Jun Kyu</creatorcontrib><creatorcontrib>Min, Kyung Myung</creatorcontrib><creatorcontrib>Hong, Suk Bong</creatorcontrib><creatorcontrib>Nam, In-Sik</creatorcontrib><creatorcontrib>Cho, Byong K.</creatorcontrib><title>Hydrothermal stability of CuSSZ13 for reducing NOx by NH3</title><title>Journal of catalysis</title><description>[Display omitted] •Deactivation of CuSSZ13 by aging becomes more severe as the Cu/Al ratio increases.•Cu2+ ions are first exchanged on the sites on D6R (α) before those in the CHA cage (β).•The β/α ratio reveals a rising trend with increasing Cu/Al ratio.•Cu2+ ions on the CHA sites readily agglomerate leading to the formation of CuOx.•Collapse of SSZ13 due to CuOx is the primary cause for the hydrothermal deactivation. The hydrothermal stability of CuSSZ13 catalysts with respect to their Cu/Al ratio has been investigated to understand the deactivation mechanism of their catalytic activity for NO reduction by NH3/SCR. The decline of the deNOx activity due to the hydrothermal aging became more severe as the Cu/Al ratio increased. Results of ESR, H2-TPR and DRIFT studies indicated that the D6R sites are occupied first by Cu2+ ions (α species) up to their accommodation capacity, followed by the occupation of the CHA sites (β species) with the increase in the Cu/Al ratio. The β species agglomerate more readily than α species due to their less stable nature, leading to the formation of CuOx. The CuOx may grow to destroy the zeolite cage and channel, resulting in the collapse of the SSZ13 structure, which is believed to be the primary cause for the hydrothermal deactivation of the CuSSZ13 catalyst.</description><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>CuSSZ13</subject><subject>ESR</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Hydrothermal stability</subject><subject>NH3/SCR</subject><subject>Nitrous oxide</subject><subject>NOx reduction</subject><subject>Theory of reactions, general kinetics. Catalysis. 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Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>Thermal energy</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Kim, Young Jin</creatorcontrib><creatorcontrib>Lee, Jun Kyu</creatorcontrib><creatorcontrib>Min, Kyung Myung</creatorcontrib><creatorcontrib>Hong, Suk Bong</creatorcontrib><creatorcontrib>Nam, In-Sik</creatorcontrib><creatorcontrib>Cho, Byong K.</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Kim, Young Jin</au><au>Lee, Jun Kyu</au><au>Min, Kyung Myung</au><au>Hong, Suk Bong</au><au>Nam, In-Sik</au><au>Cho, Byong K.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Hydrothermal stability of CuSSZ13 for reducing NOx by NH3</atitle><jtitle>Journal of catalysis</jtitle><date>2014-03-01</date><risdate>2014</risdate><volume>311</volume><spage>447</spage><epage>457</epage><pages>447-457</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>[Display omitted] •Deactivation of CuSSZ13 by aging becomes more severe as the Cu/Al ratio increases.•Cu2+ ions are first exchanged on the sites on D6R (α) before those in the CHA cage (β).•The β/α ratio reveals a rising trend with increasing Cu/Al ratio.•Cu2+ ions on the CHA sites readily agglomerate leading to the formation of CuOx.•Collapse of SSZ13 due to CuOx is the primary cause for the hydrothermal deactivation. The hydrothermal stability of CuSSZ13 catalysts with respect to their Cu/Al ratio has been investigated to understand the deactivation mechanism of their catalytic activity for NO reduction by NH3/SCR. The decline of the deNOx activity due to the hydrothermal aging became more severe as the Cu/Al ratio increased. Results of ESR, H2-TPR and DRIFT studies indicated that the D6R sites are occupied first by Cu2+ ions (α species) up to their accommodation capacity, followed by the occupation of the CHA sites (β species) with the increase in the Cu/Al ratio. The β species agglomerate more readily than α species due to their less stable nature, leading to the formation of CuOx. 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subjects Catalysis
Catalysts
Chemistry
CuSSZ13
ESR
Exact sciences and technology
General and physical chemistry
Hydrothermal stability
NH3/SCR
Nitrous oxide
NOx reduction
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
Thermal energy
title Hydrothermal stability of CuSSZ13 for reducing NOx by NH3
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