Comparative study on K‐tolerance performance of Fe/ZrO2 and Fe/ZrO2‐W catalysts for NH3‐SCR of NOx
BACKGROUND Selective catalytic reduction (SCR) of nitrous oxides (NOx) with ammonia (NH3) as reductant is used worldwide in mobile and stationary sources to reach strict emission standards. It is a feasible strategy to modify support with acidic metal oxides to improve the alkali metal potassium (K)...
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| Veröffentlicht in: | Journal of chemical technology and biotechnology (1986) 2023-09, Vol.98 (9), p.2343-2353 |
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| container_title | Journal of chemical technology and biotechnology (1986) |
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| creator | Xu, Duo Han, Zhitao Li, Yeshan Lu, Shijian Pan, Xinxiang |
| description | BACKGROUND
Selective catalytic reduction (SCR) of nitrous oxides (NOx) with ammonia (NH3) as reductant is used worldwide in mobile and stationary sources to reach strict emission standards. It is a feasible strategy to modify support with acidic metal oxides to improve the alkali metal potassium (K) tolerance of SCR catalysts. Herein, a comparative investigation was conducted based on iron/zirconium dioxide (Fe/ZrO2)and Fe/ZrO2‐tungsten (W) catalysts to reveal the correlation of support modification with W and K‐tolerance performance.
RESULTS
The NOx conversion for K‐Fe/ZrO2 catalyst was 80%).
CONCLUSION
According to the characterization results, it was found that K‐species impose a negative impact on NH3 adsorption on the surface of the Fe/ZrO2 catalyst, especially drastically preventing the adsorption of NH3 species on Brønsted acid sites, thus inhibiting the occurrence of SCR reactions via the Langmuir–Hinshelwood (L‐H) mechanism. By contrast, W modification resulted in more chemisorbed oxygen, stronger redox capacity and an increased Fe3+/(Fe3++Fe2+) ratio on the surface of the Fe/ZrO2‐W catalyst. More importantly, W modification brought about abundant Brønsted acid sites, significantly promoting NH3 adsorption and activation. W modification also weakened the adsorption stability of NOx species to a certain extent. As a result, SCR reactions over the Fe/ZrO2‐W catalyst could proceed via both Eley–Rideal (E‐R) and L‐H pathways. © 2023 Society of Chemical Industry (SCI). |
| doi_str_mv | 10.1002/jctb.7463 |
| format | Article |
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Selective catalytic reduction (SCR) of nitrous oxides (NOx) with ammonia (NH3) as reductant is used worldwide in mobile and stationary sources to reach strict emission standards. It is a feasible strategy to modify support with acidic metal oxides to improve the alkali metal potassium (K) tolerance of SCR catalysts. Herein, a comparative investigation was conducted based on iron/zirconium dioxide (Fe/ZrO2)and Fe/ZrO2‐tungsten (W) catalysts to reveal the correlation of support modification with W and K‐tolerance performance.
RESULTS
The NOx conversion for K‐Fe/ZrO2 catalyst was <80% across the whole temperature range, and the catalyst was completely deactivated at ≈400 °C. As expected, the Fe/ZrO2‐W catalyst exhibited a much superior anti‐K‐performance in comparison to the Fe/ZrO2 catalyst. The active temperature window for K‐Fe/ZrO2‐W catalyst was 285–485 °C (NOx conversion of >80%).
CONCLUSION
According to the characterization results, it was found that K‐species impose a negative impact on NH3 adsorption on the surface of the Fe/ZrO2 catalyst, especially drastically preventing the adsorption of NH3 species on Brønsted acid sites, thus inhibiting the occurrence of SCR reactions via the Langmuir–Hinshelwood (L‐H) mechanism. By contrast, W modification resulted in more chemisorbed oxygen, stronger redox capacity and an increased Fe3+/(Fe3++Fe2+) ratio on the surface of the Fe/ZrO2‐W catalyst. More importantly, W modification brought about abundant Brønsted acid sites, significantly promoting NH3 adsorption and activation. W modification also weakened the adsorption stability of NOx species to a certain extent. As a result, SCR reactions over the Fe/ZrO2‐W catalyst could proceed via both Eley–Rideal (E‐R) and L‐H pathways. © 2023 Society of Chemical Industry (SCI).</description><identifier>ISSN: 0268-2575</identifier><identifier>EISSN: 1097-4660</identifier><identifier>DOI: 10.1002/jctb.7463</identifier><language>eng</language><publisher>Chichester, UK: John Wiley & Sons, Ltd</publisher><subject>Acidic oxides ; Adsorption ; Alkali metals ; Ammonia ; Catalysts ; Chemical reduction ; Comparative studies ; Conversion ; Emission standards ; Fe‐based catalysts ; Iron ; K‐tolerance ; Metal oxides ; NH3‐SCR ; Nitrogen oxides ; Nitrous oxide ; Reducing agents ; Selective catalytic reduction ; Stationary sources ; Surface chemistry ; Tungsten ; W modification ; Zirconium ; Zirconium dioxide ; ZrO2</subject><ispartof>Journal of chemical technology and biotechnology (1986), 2023-09, Vol.98 (9), p.2343-2353</ispartof><rights>2023 Society of Chemical Industry (SCI).</rights><rights>Copyright © 2023 Society of Chemical Industry (SCI)</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-5501-6067</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fjctb.7463$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fjctb.7463$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,776,780,1411,27903,27904,45553,45554</link.rule.ids></links><search><creatorcontrib>Xu, Duo</creatorcontrib><creatorcontrib>Han, Zhitao</creatorcontrib><creatorcontrib>Li, Yeshan</creatorcontrib><creatorcontrib>Lu, Shijian</creatorcontrib><creatorcontrib>Pan, Xinxiang</creatorcontrib><title>Comparative study on K‐tolerance performance of Fe/ZrO2 and Fe/ZrO2‐W catalysts for NH3‐SCR of NOx</title><title>Journal of chemical technology and biotechnology (1986)</title><description>BACKGROUND
Selective catalytic reduction (SCR) of nitrous oxides (NOx) with ammonia (NH3) as reductant is used worldwide in mobile and stationary sources to reach strict emission standards. It is a feasible strategy to modify support with acidic metal oxides to improve the alkali metal potassium (K) tolerance of SCR catalysts. Herein, a comparative investigation was conducted based on iron/zirconium dioxide (Fe/ZrO2)and Fe/ZrO2‐tungsten (W) catalysts to reveal the correlation of support modification with W and K‐tolerance performance.
RESULTS
The NOx conversion for K‐Fe/ZrO2 catalyst was <80% across the whole temperature range, and the catalyst was completely deactivated at ≈400 °C. As expected, the Fe/ZrO2‐W catalyst exhibited a much superior anti‐K‐performance in comparison to the Fe/ZrO2 catalyst. The active temperature window for K‐Fe/ZrO2‐W catalyst was 285–485 °C (NOx conversion of >80%).
CONCLUSION
According to the characterization results, it was found that K‐species impose a negative impact on NH3 adsorption on the surface of the Fe/ZrO2 catalyst, especially drastically preventing the adsorption of NH3 species on Brønsted acid sites, thus inhibiting the occurrence of SCR reactions via the Langmuir–Hinshelwood (L‐H) mechanism. By contrast, W modification resulted in more chemisorbed oxygen, stronger redox capacity and an increased Fe3+/(Fe3++Fe2+) ratio on the surface of the Fe/ZrO2‐W catalyst. More importantly, W modification brought about abundant Brønsted acid sites, significantly promoting NH3 adsorption and activation. W modification also weakened the adsorption stability of NOx species to a certain extent. As a result, SCR reactions over the Fe/ZrO2‐W catalyst could proceed via both Eley–Rideal (E‐R) and L‐H pathways. © 2023 Society of Chemical Industry (SCI).</description><subject>Acidic oxides</subject><subject>Adsorption</subject><subject>Alkali metals</subject><subject>Ammonia</subject><subject>Catalysts</subject><subject>Chemical reduction</subject><subject>Comparative studies</subject><subject>Conversion</subject><subject>Emission standards</subject><subject>Fe‐based catalysts</subject><subject>Iron</subject><subject>K‐tolerance</subject><subject>Metal oxides</subject><subject>NH3‐SCR</subject><subject>Nitrogen oxides</subject><subject>Nitrous oxide</subject><subject>Reducing agents</subject><subject>Selective catalytic reduction</subject><subject>Stationary sources</subject><subject>Surface chemistry</subject><subject>Tungsten</subject><subject>W modification</subject><subject>Zirconium</subject><subject>Zirconium dioxide</subject><subject>ZrO2</subject><issn>0268-2575</issn><issn>1097-4660</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNo1kN9KwzAUh4MoOKcXvkHA62751yS91OI2dWygE8GbkKYpbnRtTTK1dz6Cz-iT2Dq9Oj8O3-8c-AA4x2iEESLjjQnZSDBOD8AAo0REjHN0CAaIcBmRWMTH4MT7DUKIS8IH4CWtt412OqzfLPRhl7ewruDd9-dXqEvrdGUsbKwrarf9zXUBJ3b87JYE6ir_zx3-BI0Oumx98LCj4WJGu-1Det9XFsuPU3BU6NLbs785BI-T61U6i-bL6U16OY8aQiiNMksyQawtrM5jSlgiZWYKiXBcYJMIwzWKRYaYTajNacyNJBkjNMOC066B6RBc7O82rn7dWR_Upt65qnupiGQM0YQmPTXeU-_r0raqceutdq3CSPUWVW9R9RbVbbq66gP9AYMkaIM</recordid><startdate>202309</startdate><enddate>202309</enddate><creator>Xu, Duo</creator><creator>Han, Zhitao</creator><creator>Li, Yeshan</creator><creator>Lu, Shijian</creator><creator>Pan, Xinxiang</creator><general>John Wiley & Sons, Ltd</general><general>Wiley Subscription Services, Inc</general><scope>7QF</scope><scope>7QO</scope><scope>7QQ</scope><scope>7QR</scope><scope>7SC</scope><scope>7SE</scope><scope>7SP</scope><scope>7SR</scope><scope>7T7</scope><scope>7TA</scope><scope>7TB</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>JG9</scope><scope>JQ2</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>P64</scope><orcidid>https://orcid.org/0000-0001-5501-6067</orcidid></search><sort><creationdate>202309</creationdate><title>Comparative study on K‐tolerance performance of Fe/ZrO2 and Fe/ZrO2‐W catalysts for NH3‐SCR of NOx</title><author>Xu, Duo ; Han, Zhitao ; Li, Yeshan ; Lu, Shijian ; Pan, Xinxiang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p2233-be2b72eefead5324988bcf8015f1c97c6a057b04e93ed356c82b423b1763ad513</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Acidic oxides</topic><topic>Adsorption</topic><topic>Alkali metals</topic><topic>Ammonia</topic><topic>Catalysts</topic><topic>Chemical reduction</topic><topic>Comparative studies</topic><topic>Conversion</topic><topic>Emission standards</topic><topic>Fe‐based catalysts</topic><topic>Iron</topic><topic>K‐tolerance</topic><topic>Metal oxides</topic><topic>NH3‐SCR</topic><topic>Nitrogen oxides</topic><topic>Nitrous oxide</topic><topic>Reducing agents</topic><topic>Selective catalytic reduction</topic><topic>Stationary sources</topic><topic>Surface chemistry</topic><topic>Tungsten</topic><topic>W modification</topic><topic>Zirconium</topic><topic>Zirconium dioxide</topic><topic>ZrO2</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Xu, Duo</creatorcontrib><creatorcontrib>Han, Zhitao</creatorcontrib><creatorcontrib>Li, Yeshan</creatorcontrib><creatorcontrib>Lu, Shijian</creatorcontrib><creatorcontrib>Pan, Xinxiang</creatorcontrib><collection>Aluminium Industry Abstracts</collection><collection>Biotechnology Research Abstracts</collection><collection>Ceramic Abstracts</collection><collection>Chemoreception Abstracts</collection><collection>Computer and Information Systems Abstracts</collection><collection>Corrosion Abstracts</collection><collection>Electronics & Communications Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Materials Business File</collection><collection>Mechanical & Transportation Engineering Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>ANTE: Abstracts in New Technology & Engineering</collection><collection>Engineering Research Database</collection><collection>Aerospace Database</collection><collection>Copper Technical Reference Library</collection><collection>Materials Research Database</collection><collection>ProQuest Computer Science Collection</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Computer and Information Systems Abstracts Academic</collection><collection>Computer and Information Systems Abstracts Professional</collection><collection>Biotechnology and BioEngineering Abstracts</collection><jtitle>Journal of chemical technology and biotechnology (1986)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Xu, Duo</au><au>Han, Zhitao</au><au>Li, Yeshan</au><au>Lu, Shijian</au><au>Pan, Xinxiang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Comparative study on K‐tolerance performance of Fe/ZrO2 and Fe/ZrO2‐W catalysts for NH3‐SCR of NOx</atitle><jtitle>Journal of chemical technology and biotechnology (1986)</jtitle><date>2023-09</date><risdate>2023</risdate><volume>98</volume><issue>9</issue><spage>2343</spage><epage>2353</epage><pages>2343-2353</pages><issn>0268-2575</issn><eissn>1097-4660</eissn><abstract>BACKGROUND
Selective catalytic reduction (SCR) of nitrous oxides (NOx) with ammonia (NH3) as reductant is used worldwide in mobile and stationary sources to reach strict emission standards. It is a feasible strategy to modify support with acidic metal oxides to improve the alkali metal potassium (K) tolerance of SCR catalysts. Herein, a comparative investigation was conducted based on iron/zirconium dioxide (Fe/ZrO2)and Fe/ZrO2‐tungsten (W) catalysts to reveal the correlation of support modification with W and K‐tolerance performance.
RESULTS
The NOx conversion for K‐Fe/ZrO2 catalyst was <80% across the whole temperature range, and the catalyst was completely deactivated at ≈400 °C. As expected, the Fe/ZrO2‐W catalyst exhibited a much superior anti‐K‐performance in comparison to the Fe/ZrO2 catalyst. The active temperature window for K‐Fe/ZrO2‐W catalyst was 285–485 °C (NOx conversion of >80%).
CONCLUSION
According to the characterization results, it was found that K‐species impose a negative impact on NH3 adsorption on the surface of the Fe/ZrO2 catalyst, especially drastically preventing the adsorption of NH3 species on Brønsted acid sites, thus inhibiting the occurrence of SCR reactions via the Langmuir–Hinshelwood (L‐H) mechanism. By contrast, W modification resulted in more chemisorbed oxygen, stronger redox capacity and an increased Fe3+/(Fe3++Fe2+) ratio on the surface of the Fe/ZrO2‐W catalyst. More importantly, W modification brought about abundant Brønsted acid sites, significantly promoting NH3 adsorption and activation. W modification also weakened the adsorption stability of NOx species to a certain extent. As a result, SCR reactions over the Fe/ZrO2‐W catalyst could proceed via both Eley–Rideal (E‐R) and L‐H pathways. © 2023 Society of Chemical Industry (SCI).</abstract><cop>Chichester, UK</cop><pub>John Wiley & Sons, Ltd</pub><doi>10.1002/jctb.7463</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0001-5501-6067</orcidid></addata></record> |
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| identifier | ISSN: 0268-2575 |
| ispartof | Journal of chemical technology and biotechnology (1986), 2023-09, Vol.98 (9), p.2343-2353 |
| issn | 0268-2575 1097-4660 |
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| source | Wiley Online Library Journals Frontfile Complete |
| subjects | Acidic oxides Adsorption Alkali metals Ammonia Catalysts Chemical reduction Comparative studies Conversion Emission standards Fe‐based catalysts Iron K‐tolerance Metal oxides NH3‐SCR Nitrogen oxides Nitrous oxide Reducing agents Selective catalytic reduction Stationary sources Surface chemistry Tungsten W modification Zirconium Zirconium dioxide ZrO2 |
| title | Comparative study on K‐tolerance performance of Fe/ZrO2 and Fe/ZrO2‐W catalysts for NH3‐SCR of NOx |
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