Dynamics of low temperature N2O formation under SCR reaction conditions over a Cu-SSZ-13 catalyst
[Display omitted] •Investigates low T N2O formation under steady-state and transient over Cu-SSZ-13.•DRIFTS results display no nitrates formation under low T standard SCR conditions.•More oxidized Cu-SSZ-13 catalyst leads to higher amount of N2O formation.•Low T N2O formation is associated with SCR...
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Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2021-10, Vol.294, p.120245, Article 120245 |
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creator | Xi, Yuanzhou Ottinger, Nathan A. Keturakis, Christopher J. Liu, Z. Gerald |
description | [Display omitted]
•Investigates low T N2O formation under steady-state and transient over Cu-SSZ-13.•DRIFTS results display no nitrates formation under low T standard SCR conditions.•More oxidized Cu-SSZ-13 catalyst leads to higher amount of N2O formation.•Low T N2O formation is associated with SCR relevant Cu-oxy species.
Small pore Cu-SSZ-13 zeolite can effectively catalyze selective catalytic reduction (SCR) for NOx (NO and NO2) using NH3 as a reductant. However, side reactions leading to the formation of N2O, a greenhouse gas, occur in parallel under SCR reaction conditions. This work investigates the fundamental characteristics of N2O formation during SCR reactions over a Cu-SSZ-13 catalyst under both steady-state and transient conditions during reactant transitions at 200 °C. The absence of nitrate bands from in situ DRIFTS experiments and the inconsistencies between high stability of NH4NO3 and N2O formation at low temperature exclude the formation of surface nitrate or NH4NO3 as a precursor of N2O formation as the major path under standard SCR reaction conditions at 200 °C. The analysis from the transient N2O formation behavior during reactant transitions and NO + NH3 titration experiments indicates that more oxidized Cu-SSZ-13 catalyst, containing higher amount of Cu-oxy species, produces higher amount of N2O. |
doi_str_mv | 10.1016/j.apcatb.2021.120245 |
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•Investigates low T N2O formation under steady-state and transient over Cu-SSZ-13.•DRIFTS results display no nitrates formation under low T standard SCR conditions.•More oxidized Cu-SSZ-13 catalyst leads to higher amount of N2O formation.•Low T N2O formation is associated with SCR relevant Cu-oxy species.
Small pore Cu-SSZ-13 zeolite can effectively catalyze selective catalytic reduction (SCR) for NOx (NO and NO2) using NH3 as a reductant. However, side reactions leading to the formation of N2O, a greenhouse gas, occur in parallel under SCR reaction conditions. This work investigates the fundamental characteristics of N2O formation during SCR reactions over a Cu-SSZ-13 catalyst under both steady-state and transient conditions during reactant transitions at 200 °C. The absence of nitrate bands from in situ DRIFTS experiments and the inconsistencies between high stability of NH4NO3 and N2O formation at low temperature exclude the formation of surface nitrate or NH4NO3 as a precursor of N2O formation as the major path under standard SCR reaction conditions at 200 °C. The analysis from the transient N2O formation behavior during reactant transitions and NO + NH3 titration experiments indicates that more oxidized Cu-SSZ-13 catalyst, containing higher amount of Cu-oxy species, produces higher amount of N2O.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2021.120245</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Ammonia ; Ammonium nitrate ; Catalysts ; Chemical reduction ; Cu-SSZ-13 ; DRIFTS ; Greenhouse gases ; Low temperature ; N2O ; Nitrogen dioxide ; Nitrous oxide ; Reducing agents ; SCR ; Selective catalytic reduction ; Side reactions ; Titration ; TPD ; Transient ; Zeolites</subject><ispartof>Applied catalysis. B, Environmental, 2021-10, Vol.294, p.120245, Article 120245</ispartof><rights>2021 Elsevier B.V.</rights><rights>Copyright Elsevier BV Oct 5, 2021</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c400t-373ae66c1f0ddf784bc37e3c40b78638d51f327539735f1d6a8fb3dc20fd41aa3</citedby><cites>FETCH-LOGICAL-c400t-373ae66c1f0ddf784bc37e3c40b78638d51f327539735f1d6a8fb3dc20fd41aa3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.apcatb.2021.120245$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids></links><search><creatorcontrib>Xi, Yuanzhou</creatorcontrib><creatorcontrib>Ottinger, Nathan A.</creatorcontrib><creatorcontrib>Keturakis, Christopher J.</creatorcontrib><creatorcontrib>Liu, Z. Gerald</creatorcontrib><title>Dynamics of low temperature N2O formation under SCR reaction conditions over a Cu-SSZ-13 catalyst</title><title>Applied catalysis. B, Environmental</title><description>[Display omitted]
•Investigates low T N2O formation under steady-state and transient over Cu-SSZ-13.•DRIFTS results display no nitrates formation under low T standard SCR conditions.•More oxidized Cu-SSZ-13 catalyst leads to higher amount of N2O formation.•Low T N2O formation is associated with SCR relevant Cu-oxy species.
Small pore Cu-SSZ-13 zeolite can effectively catalyze selective catalytic reduction (SCR) for NOx (NO and NO2) using NH3 as a reductant. However, side reactions leading to the formation of N2O, a greenhouse gas, occur in parallel under SCR reaction conditions. This work investigates the fundamental characteristics of N2O formation during SCR reactions over a Cu-SSZ-13 catalyst under both steady-state and transient conditions during reactant transitions at 200 °C. The absence of nitrate bands from in situ DRIFTS experiments and the inconsistencies between high stability of NH4NO3 and N2O formation at low temperature exclude the formation of surface nitrate or NH4NO3 as a precursor of N2O formation as the major path under standard SCR reaction conditions at 200 °C. The analysis from the transient N2O formation behavior during reactant transitions and NO + NH3 titration experiments indicates that more oxidized Cu-SSZ-13 catalyst, containing higher amount of Cu-oxy species, produces higher amount of N2O.</description><subject>Ammonia</subject><subject>Ammonium nitrate</subject><subject>Catalysts</subject><subject>Chemical reduction</subject><subject>Cu-SSZ-13</subject><subject>DRIFTS</subject><subject>Greenhouse gases</subject><subject>Low temperature</subject><subject>N2O</subject><subject>Nitrogen dioxide</subject><subject>Nitrous oxide</subject><subject>Reducing agents</subject><subject>SCR</subject><subject>Selective catalytic reduction</subject><subject>Side reactions</subject><subject>Titration</subject><subject>TPD</subject><subject>Transient</subject><subject>Zeolites</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9UE1LxDAQDaLguvoPPAQ8t-ajbbIXQeoniAuuXryENB-Qsm1q0q7svzdrPXuZGebNezPzALjEKMcIV9dtLgclxyYniOAcp1iUR2CBOaMZ5ZwegwVakSqjlNFTcBZjixAilPAFkHf7XnZORegt3PpvOJpuMEGOUzDwlayh9aGTo_M9nHptAtzUbzAYqX5byvfaHapE3yVQwnrKNpvPDFOYDpLbfRzPwYmV22gu_vISfDzcv9dP2cv68bm-fclUgdCYpdOkqSqFLdLaMl40ijJDE9gwXlGuS2wpYSVdMVparCvJbUO1IsjqAktJl-Bq1h2C_5pMHEXrp9CnlYKURUlKVmGUpop5SgUfYzBWDMF1MuwFRuJgpmjFbKY4mClmMxPtZqaZ9MHOmSCicqZXRrtg1Ci0d_8L_AAJD34i</recordid><startdate>20211005</startdate><enddate>20211005</enddate><creator>Xi, Yuanzhou</creator><creator>Ottinger, Nathan A.</creator><creator>Keturakis, Christopher J.</creator><creator>Liu, Z. Gerald</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope><scope>SOI</scope></search><sort><creationdate>20211005</creationdate><title>Dynamics of low temperature N2O formation under SCR reaction conditions over a Cu-SSZ-13 catalyst</title><author>Xi, Yuanzhou ; Ottinger, Nathan A. ; Keturakis, Christopher J. ; Liu, Z. Gerald</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c400t-373ae66c1f0ddf784bc37e3c40b78638d51f327539735f1d6a8fb3dc20fd41aa3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Ammonia</topic><topic>Ammonium nitrate</topic><topic>Catalysts</topic><topic>Chemical reduction</topic><topic>Cu-SSZ-13</topic><topic>DRIFTS</topic><topic>Greenhouse gases</topic><topic>Low temperature</topic><topic>N2O</topic><topic>Nitrogen dioxide</topic><topic>Nitrous oxide</topic><topic>Reducing agents</topic><topic>SCR</topic><topic>Selective catalytic reduction</topic><topic>Side reactions</topic><topic>Titration</topic><topic>TPD</topic><topic>Transient</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Xi, Yuanzhou</creatorcontrib><creatorcontrib>Ottinger, Nathan A.</creatorcontrib><creatorcontrib>Keturakis, Christopher J.</creatorcontrib><creatorcontrib>Liu, Z. Gerald</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Environment 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>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>Applied catalysis. B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Xi, Yuanzhou</au><au>Ottinger, Nathan A.</au><au>Keturakis, Christopher J.</au><au>Liu, Z. Gerald</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Dynamics of low temperature N2O formation under SCR reaction conditions over a Cu-SSZ-13 catalyst</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2021-10-05</date><risdate>2021</risdate><volume>294</volume><spage>120245</spage><pages>120245-</pages><artnum>120245</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted]
•Investigates low T N2O formation under steady-state and transient over Cu-SSZ-13.•DRIFTS results display no nitrates formation under low T standard SCR conditions.•More oxidized Cu-SSZ-13 catalyst leads to higher amount of N2O formation.•Low T N2O formation is associated with SCR relevant Cu-oxy species.
Small pore Cu-SSZ-13 zeolite can effectively catalyze selective catalytic reduction (SCR) for NOx (NO and NO2) using NH3 as a reductant. However, side reactions leading to the formation of N2O, a greenhouse gas, occur in parallel under SCR reaction conditions. This work investigates the fundamental characteristics of N2O formation during SCR reactions over a Cu-SSZ-13 catalyst under both steady-state and transient conditions during reactant transitions at 200 °C. The absence of nitrate bands from in situ DRIFTS experiments and the inconsistencies between high stability of NH4NO3 and N2O formation at low temperature exclude the formation of surface nitrate or NH4NO3 as a precursor of N2O formation as the major path under standard SCR reaction conditions at 200 °C. The analysis from the transient N2O formation behavior during reactant transitions and NO + NH3 titration experiments indicates that more oxidized Cu-SSZ-13 catalyst, containing higher amount of Cu-oxy species, produces higher amount of N2O.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2021.120245</doi></addata></record> |
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subjects | Ammonia Ammonium nitrate Catalysts Chemical reduction Cu-SSZ-13 DRIFTS Greenhouse gases Low temperature N2O Nitrogen dioxide Nitrous oxide Reducing agents SCR Selective catalytic reduction Side reactions Titration TPD Transient Zeolites |
title | Dynamics of low temperature N2O formation under SCR reaction conditions over a Cu-SSZ-13 catalyst |
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