Enhanced low-temperature H2-selective catalytic reduction performance and selectivity of Pt/ZSM-5–TiO2 washcoated monolithic catalysts for NOx reduction

Hydrogen-selective catalytic reduction (H2-SCR) is a promising technology for reducing nitrogen oxide (NOx) emissions at low temperatures, but the selectivity of this process is limited by the generation of N2O. To achieve enhanced denitrification (deNOx) performance, H2-SCR catalysts with mixed zeo...

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Veröffentlicht in:Journal of cleaner production 2024-01, Vol.434, p.140333, Article 140333
Hauptverfasser: Lee, Kyungseok, Lee, Kyoungbok, Choi, Byungchul, Oh, Kwangchul
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description Hydrogen-selective catalytic reduction (H2-SCR) is a promising technology for reducing nitrogen oxide (NOx) emissions at low temperatures, but the selectivity of this process is limited by the generation of N2O. To achieve enhanced denitrification (deNOx) performance, H2-SCR catalysts with mixed zeolite and TiO2 supports washcoated on monolithic cordierite were developed. The catalyst support, active metal type and content, and monolithic cordierite cell density significantly influenced the H2-SCR performance. The xPt/TiO2 catalysts (where x is the metal content, wt.%) achieved >90% NOx conversion 135–180 °C, whereas the xPd/TiO2 catalysts exhibited poor H2-SCR activity, with  89% at 140 °C for 0.5Pt/BETA >85% at 150 °C for 0.5Pt/SSZ-13), suggesting that zeolite supports significantly promote H2-SCR activity at low reaction temperatures. For the 0.5Pt/ZSM-5 washcoated monolithic catalyst, increasing the cell density from 400 to 900 cpsi significantly improved the NOx conversion from 52% to 90% at 100 °C owing to the increased geometric surface area and open frontal area of monolithic cordierite. For catalyst with mixed supports (0.5Pt/yZSM-5zTiO2) changing the ZSM-5/TiO2 ratio (y:z) from 25:75 to 90:10 increased the low-temperature NOx conversion from 39% to 89% at 100 °C, indicating that the deNOx characteristics can be tuned. With NO as the reactant, the 0.5Pt/90Z10T catalyst produced the lowest N2O share (8–17%) within the temperature window of maximum NOx conversion, resulting in an increased N2 share (83–88%). Thus, the synergetic effect of mixed ZSM-5/TiO2 catalyst supports can enhance low-temperature NOx conversion and mitigate N2O formation. [Display omitted] •Low-temperature hydrogen-selective catalytic reduction (H2-SCR) was investigated.•Pt or Pd/TiO2 or Pt/zeolite catalysts were washcoated on a monolithic cordierite.•The support, active metal, and cordierite cell density affected H2-SCR performance.•High cell density of cordierite enhanced low-temperature NOx conversion.•Catalysts with mixed supports enhanced NOx conversion and mitigated N2O formation.
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To achieve enhanced denitrification (deNOx) performance, H2-SCR catalysts with mixed zeolite and TiO2 supports washcoated on monolithic cordierite were developed. The catalyst support, active metal type and content, and monolithic cordierite cell density significantly influenced the H2-SCR performance. The xPt/TiO2 catalysts (where x is the metal content, wt.%) achieved &gt;90% NOx conversion 135–180 °C, whereas the xPd/TiO2 catalysts exhibited poor H2-SCR activity, with &lt;30% NOx conversion. In contrast to 0.5Pt/TiO2, the 0.5Pt/zeolite catalysts achieved high NOx conversion at 140–150 °C (91% at 140 °C for 0.5Pt/ZSM-5 &gt; 89% at 140 °C for 0.5Pt/BETA &gt;85% at 150 °C for 0.5Pt/SSZ-13), suggesting that zeolite supports significantly promote H2-SCR activity at low reaction temperatures. For the 0.5Pt/ZSM-5 washcoated monolithic catalyst, increasing the cell density from 400 to 900 cpsi significantly improved the NOx conversion from 52% to 90% at 100 °C owing to the increased geometric surface area and open frontal area of monolithic cordierite. For catalyst with mixed supports (0.5Pt/yZSM-5zTiO2) changing the ZSM-5/TiO2 ratio (y:z) from 25:75 to 90:10 increased the low-temperature NOx conversion from 39% to 89% at 100 °C, indicating that the deNOx characteristics can be tuned. With NO as the reactant, the 0.5Pt/90Z10T catalyst produced the lowest N2O share (8–17%) within the temperature window of maximum NOx conversion, resulting in an increased N2 share (83–88%). Thus, the synergetic effect of mixed ZSM-5/TiO2 catalyst supports can enhance low-temperature NOx conversion and mitigate N2O formation. [Display omitted] •Low-temperature hydrogen-selective catalytic reduction (H2-SCR) was investigated.•Pt or Pd/TiO2 or Pt/zeolite catalysts were washcoated on a monolithic cordierite.•The support, active metal, and cordierite cell density affected H2-SCR performance.•High cell density of cordierite enhanced low-temperature NOx conversion.•Catalysts with mixed supports enhanced NOx conversion and mitigated N2O formation.</description><identifier>ISSN: 0959-6526</identifier><identifier>DOI: 10.1016/j.jclepro.2023.140333</identifier><language>eng</language><publisher>Elsevier Ltd</publisher><subject>catalysts ; cordierite ; denitrification ; geometry ; Hydrogen-selective catalytic reduction ; Nitric oxide ; nitrogen oxides ; Platinum/ZSM-5 ; surface area ; synergism ; temperature ; Titanium dioxide ; Washcoated monolithic catalyst ; zeolites</subject><ispartof>Journal of cleaner production, 2024-01, Vol.434, p.140333, Article 140333</ispartof><rights>2023 Elsevier Ltd</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c290t-8b3ff773fa5270d9f692afddc09e08f147aab2698a91f55e6beb4dc08950f3483</cites><orcidid>0000-0001-7909-9485 ; 0000-0002-4138-6259 ; 0000-0002-6064-6597</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0959652623044918$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>Lee, Kyungseok</creatorcontrib><creatorcontrib>Lee, Kyoungbok</creatorcontrib><creatorcontrib>Choi, Byungchul</creatorcontrib><creatorcontrib>Oh, Kwangchul</creatorcontrib><title>Enhanced low-temperature H2-selective catalytic reduction performance and selectivity of Pt/ZSM-5–TiO2 washcoated monolithic catalysts for NOx reduction</title><title>Journal of cleaner production</title><description>Hydrogen-selective catalytic reduction (H2-SCR) is a promising technology for reducing nitrogen oxide (NOx) emissions at low temperatures, but the selectivity of this process is limited by the generation of N2O. To achieve enhanced denitrification (deNOx) performance, H2-SCR catalysts with mixed zeolite and TiO2 supports washcoated on monolithic cordierite were developed. The catalyst support, active metal type and content, and monolithic cordierite cell density significantly influenced the H2-SCR performance. The xPt/TiO2 catalysts (where x is the metal content, wt.%) achieved &gt;90% NOx conversion 135–180 °C, whereas the xPd/TiO2 catalysts exhibited poor H2-SCR activity, with &lt;30% NOx conversion. In contrast to 0.5Pt/TiO2, the 0.5Pt/zeolite catalysts achieved high NOx conversion at 140–150 °C (91% at 140 °C for 0.5Pt/ZSM-5 &gt; 89% at 140 °C for 0.5Pt/BETA &gt;85% at 150 °C for 0.5Pt/SSZ-13), suggesting that zeolite supports significantly promote H2-SCR activity at low reaction temperatures. For the 0.5Pt/ZSM-5 washcoated monolithic catalyst, increasing the cell density from 400 to 900 cpsi significantly improved the NOx conversion from 52% to 90% at 100 °C owing to the increased geometric surface area and open frontal area of monolithic cordierite. For catalyst with mixed supports (0.5Pt/yZSM-5zTiO2) changing the ZSM-5/TiO2 ratio (y:z) from 25:75 to 90:10 increased the low-temperature NOx conversion from 39% to 89% at 100 °C, indicating that the deNOx characteristics can be tuned. With NO as the reactant, the 0.5Pt/90Z10T catalyst produced the lowest N2O share (8–17%) within the temperature window of maximum NOx conversion, resulting in an increased N2 share (83–88%). Thus, the synergetic effect of mixed ZSM-5/TiO2 catalyst supports can enhance low-temperature NOx conversion and mitigate N2O formation. [Display omitted] •Low-temperature hydrogen-selective catalytic reduction (H2-SCR) was investigated.•Pt or Pd/TiO2 or Pt/zeolite catalysts were washcoated on a monolithic cordierite.•The support, active metal, and cordierite cell density affected H2-SCR performance.•High cell density of cordierite enhanced low-temperature NOx conversion.•Catalysts with mixed supports enhanced NOx conversion and mitigated N2O formation.</description><subject>catalysts</subject><subject>cordierite</subject><subject>denitrification</subject><subject>geometry</subject><subject>Hydrogen-selective catalytic reduction</subject><subject>Nitric oxide</subject><subject>nitrogen oxides</subject><subject>Platinum/ZSM-5</subject><subject>surface area</subject><subject>synergism</subject><subject>temperature</subject><subject>Titanium dioxide</subject><subject>Washcoated monolithic catalyst</subject><subject>zeolites</subject><issn>0959-6526</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkMtKxDAUhrtQ8PoIQpZuOubStM1KRLyBOoK6cRMy6QmToW3GJKPOzndw5-P5JKZUcSkEAsn_f4fzZdkBwROCSXm0mCx0C0vvJhRTNiEFZoxtZNtYcJGXnJZb2U4IC4xJhatiO_s86-eq19Cg1r3mEboleBVXHtAlzQO0oKN9AaRVVO06Wo08NKv05nqUksb5bmgj1TfoN23jGjmD7uLR0_1Nzr_ePx7slKJXFebaqZhGda53rY3zhBvBIQaUWOh2-vY3YC_bNKoNsP9z72aP52cPp5f59fTi6vTkOtdU4JjXM2ZMVTGjOK1wI0wpqDJNo7EAXBtSVErNaClqJYjhHMoZzIr0WwuODStqtpsdjtxk7XkFIcrOBg1tq3pwqyAZ4cOpC5KifIxq70LwYOTS2075tSRYDv7lQv74l4N_OfpPveOxB2mPFwteBm1h0G59ciYbZ_8hfAN23Zfh</recordid><startdate>20240101</startdate><enddate>20240101</enddate><creator>Lee, Kyungseok</creator><creator>Lee, Kyoungbok</creator><creator>Choi, Byungchul</creator><creator>Oh, Kwangchul</creator><general>Elsevier Ltd</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0001-7909-9485</orcidid><orcidid>https://orcid.org/0000-0002-4138-6259</orcidid><orcidid>https://orcid.org/0000-0002-6064-6597</orcidid></search><sort><creationdate>20240101</creationdate><title>Enhanced low-temperature H2-selective catalytic reduction performance and selectivity of Pt/ZSM-5–TiO2 washcoated monolithic catalysts for NOx reduction</title><author>Lee, Kyungseok ; Lee, Kyoungbok ; Choi, Byungchul ; Oh, Kwangchul</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c290t-8b3ff773fa5270d9f692afddc09e08f147aab2698a91f55e6beb4dc08950f3483</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>catalysts</topic><topic>cordierite</topic><topic>denitrification</topic><topic>geometry</topic><topic>Hydrogen-selective catalytic reduction</topic><topic>Nitric oxide</topic><topic>nitrogen oxides</topic><topic>Platinum/ZSM-5</topic><topic>surface area</topic><topic>synergism</topic><topic>temperature</topic><topic>Titanium dioxide</topic><topic>Washcoated monolithic catalyst</topic><topic>zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lee, Kyungseok</creatorcontrib><creatorcontrib>Lee, Kyoungbok</creatorcontrib><creatorcontrib>Choi, Byungchul</creatorcontrib><creatorcontrib>Oh, Kwangchul</creatorcontrib><collection>CrossRef</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>Journal of cleaner production</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lee, Kyungseok</au><au>Lee, Kyoungbok</au><au>Choi, Byungchul</au><au>Oh, Kwangchul</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enhanced low-temperature H2-selective catalytic reduction performance and selectivity of Pt/ZSM-5–TiO2 washcoated monolithic catalysts for NOx reduction</atitle><jtitle>Journal of cleaner production</jtitle><date>2024-01-01</date><risdate>2024</risdate><volume>434</volume><spage>140333</spage><pages>140333-</pages><artnum>140333</artnum><issn>0959-6526</issn><abstract>Hydrogen-selective catalytic reduction (H2-SCR) is a promising technology for reducing nitrogen oxide (NOx) emissions at low temperatures, but the selectivity of this process is limited by the generation of N2O. To achieve enhanced denitrification (deNOx) performance, H2-SCR catalysts with mixed zeolite and TiO2 supports washcoated on monolithic cordierite were developed. The catalyst support, active metal type and content, and monolithic cordierite cell density significantly influenced the H2-SCR performance. The xPt/TiO2 catalysts (where x is the metal content, wt.%) achieved &gt;90% NOx conversion 135–180 °C, whereas the xPd/TiO2 catalysts exhibited poor H2-SCR activity, with &lt;30% NOx conversion. In contrast to 0.5Pt/TiO2, the 0.5Pt/zeolite catalysts achieved high NOx conversion at 140–150 °C (91% at 140 °C for 0.5Pt/ZSM-5 &gt; 89% at 140 °C for 0.5Pt/BETA &gt;85% at 150 °C for 0.5Pt/SSZ-13), suggesting that zeolite supports significantly promote H2-SCR activity at low reaction temperatures. For the 0.5Pt/ZSM-5 washcoated monolithic catalyst, increasing the cell density from 400 to 900 cpsi significantly improved the NOx conversion from 52% to 90% at 100 °C owing to the increased geometric surface area and open frontal area of monolithic cordierite. For catalyst with mixed supports (0.5Pt/yZSM-5zTiO2) changing the ZSM-5/TiO2 ratio (y:z) from 25:75 to 90:10 increased the low-temperature NOx conversion from 39% to 89% at 100 °C, indicating that the deNOx characteristics can be tuned. With NO as the reactant, the 0.5Pt/90Z10T catalyst produced the lowest N2O share (8–17%) within the temperature window of maximum NOx conversion, resulting in an increased N2 share (83–88%). Thus, the synergetic effect of mixed ZSM-5/TiO2 catalyst supports can enhance low-temperature NOx conversion and mitigate N2O formation. [Display omitted] •Low-temperature hydrogen-selective catalytic reduction (H2-SCR) was investigated.•Pt or Pd/TiO2 or Pt/zeolite catalysts were washcoated on a monolithic cordierite.•The support, active metal, and cordierite cell density affected H2-SCR performance.•High cell density of cordierite enhanced low-temperature NOx conversion.•Catalysts with mixed supports enhanced NOx conversion and mitigated N2O formation.</abstract><pub>Elsevier Ltd</pub><doi>10.1016/j.jclepro.2023.140333</doi><orcidid>https://orcid.org/0000-0001-7909-9485</orcidid><orcidid>https://orcid.org/0000-0002-4138-6259</orcidid><orcidid>https://orcid.org/0000-0002-6064-6597</orcidid></addata></record>
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subjects catalysts
cordierite
denitrification
geometry
Hydrogen-selective catalytic reduction
Nitric oxide
nitrogen oxides
Platinum/ZSM-5
surface area
synergism
temperature
Titanium dioxide
Washcoated monolithic catalyst
zeolites
title Enhanced low-temperature H2-selective catalytic reduction performance and selectivity of Pt/ZSM-5–TiO2 washcoated monolithic catalysts for NOx reduction
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