Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR
The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide toleranc...
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Veröffentlicht in: | ACS sustainable chemistry & engineering 2021-01, Vol.9 (2), p.987-997 |
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description | The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide tolerance was successfully applied to low-temperature NH3–SCR in this study. The findings indicate that the Cu x Ce/CAC-CNTs obtained at a 0.2 Cu/Ce molar ratio and the calcination temperature of 450 °C showed the highest 100% NO conversion with 95.8% N2 selectivity at 150 °C and 10 000 h–1. The incorporation of Cu improved the Cu0.2Ce/CAC-CNTs in Lewis acid, lattice oxygen (31.99%), and Ce3+ (26.03%). The accelerated NH3 adsorption on acid sites, the encouraging electron transfer by the Ce4+ + Cu+ ↔ Ce3+ + Cu2+ redox circle, and the more surface chemisorbed oxygen (Oβ) improved the catalytic activity of Cu0.2Ce/CAC-CNTs. The NH3–SCR of Cu0.2Ce/CAC-CNTs largely follows the L–H mechanism, together with a certain degree of “Fast SCR.” The added Cu species effectively prevented surface SO2 adsorption and oxidation, and the Cu0.2Ce/CAC-CNTs restored more than 94% SCR activity after 8 h of poisoning in 50 ppm SO2 and 5 vol % H2O. |
doi_str_mv | 10.1021/acssuschemeng.0c08490 |
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The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide tolerance was successfully applied to low-temperature NH3–SCR in this study. The findings indicate that the Cu x Ce/CAC-CNTs obtained at a 0.2 Cu/Ce molar ratio and the calcination temperature of 450 °C showed the highest 100% NO conversion with 95.8% N2 selectivity at 150 °C and 10 000 h–1. The incorporation of Cu improved the Cu0.2Ce/CAC-CNTs in Lewis acid, lattice oxygen (31.99%), and Ce3+ (26.03%). The accelerated NH3 adsorption on acid sites, the encouraging electron transfer by the Ce4+ + Cu+ ↔ Ce3+ + Cu2+ redox circle, and the more surface chemisorbed oxygen (Oβ) improved the catalytic activity of Cu0.2Ce/CAC-CNTs. The NH3–SCR of Cu0.2Ce/CAC-CNTs largely follows the L–H mechanism, together with a certain degree of “Fast SCR.” The added Cu species effectively prevented surface SO2 adsorption and oxidation, and the Cu0.2Ce/CAC-CNTs restored more than 94% SCR activity after 8 h of poisoning in 50 ppm SO2 and 5 vol % H2O.</description><identifier>ISSN: 2168-0485</identifier><identifier>EISSN: 2168-0485</identifier><identifier>DOI: 10.1021/acssuschemeng.0c08490</identifier><language>eng</language><publisher>American Chemical Society</publisher><ispartof>ACS sustainable chemistry & engineering, 2021-01, Vol.9 (2), p.987-997</ispartof><rights>2021 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-5754-7937 ; 0000-0002-3367-244X ; 0000-0003-2743-758X ; 0000-0003-1327-7159</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acssuschemeng.0c08490$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acssuschemeng.0c08490$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,27053,27901,27902,56713,56763</link.rule.ids></links><search><creatorcontrib>Yang, Lin</creatorcontrib><creatorcontrib>Wang, Pengchen</creatorcontrib><creatorcontrib>Yao, Lu</creatorcontrib><creatorcontrib>Meng, Xiaomi</creatorcontrib><creatorcontrib>Jia, Charles Q</creatorcontrib><creatorcontrib>Jiang, Xia</creatorcontrib><creatorcontrib>Jiang, Wenju</creatorcontrib><title>Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR</title><title>ACS sustainable chemistry & engineering</title><addtitle>ACS Sustainable Chem. Eng</addtitle><description>The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide tolerance was successfully applied to low-temperature NH3–SCR in this study. The findings indicate that the Cu x Ce/CAC-CNTs obtained at a 0.2 Cu/Ce molar ratio and the calcination temperature of 450 °C showed the highest 100% NO conversion with 95.8% N2 selectivity at 150 °C and 10 000 h–1. The incorporation of Cu improved the Cu0.2Ce/CAC-CNTs in Lewis acid, lattice oxygen (31.99%), and Ce3+ (26.03%). The accelerated NH3 adsorption on acid sites, the encouraging electron transfer by the Ce4+ + Cu+ ↔ Ce3+ + Cu2+ redox circle, and the more surface chemisorbed oxygen (Oβ) improved the catalytic activity of Cu0.2Ce/CAC-CNTs. The NH3–SCR of Cu0.2Ce/CAC-CNTs largely follows the L–H mechanism, together with a certain degree of “Fast SCR.” The added Cu species effectively prevented surface SO2 adsorption and oxidation, and the Cu0.2Ce/CAC-CNTs restored more than 94% SCR activity after 8 h of poisoning in 50 ppm SO2 and 5 vol % H2O.</description><issn>2168-0485</issn><issn>2168-0485</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><sourceid/><recordid>eNpVkN1KwzAYhoMoOOYuQcgNdMtf0_RwxJ8OyhRXj0uaJltH25SmZXrmPXiHXokVd6AfH3zvyft88ABwi9ESI4JXSns_en0wjWn3S6SRYDG6ADOCuQgQE-Hln3wNFt4f0TRxTInAM9BJ13Wmh3euq9o9fO5d44bKtXBaaVZyLQO5zaBUg6rf_eDhqRoOMKn2B7gbaztOzcq9VaWBmatNr1ptoHU9TN0pyEwzodUw9gZuE_r18bmTLzfgyqram8X5zsHrw30mkyB9etzIdRooHEdDECurOBEEqZIQqjlDESt5WPDQakqwFmVpkOEoIqGlRSGEoIyTglnGcUQooXOAf7mToPzoxr6dvuUY5T_W8n_W8rM1-g3WNmRp</recordid><startdate>20210118</startdate><enddate>20210118</enddate><creator>Yang, Lin</creator><creator>Wang, Pengchen</creator><creator>Yao, Lu</creator><creator>Meng, Xiaomi</creator><creator>Jia, Charles Q</creator><creator>Jiang, Xia</creator><creator>Jiang, Wenju</creator><general>American Chemical Society</general><scope/><orcidid>https://orcid.org/0000-0001-5754-7937</orcidid><orcidid>https://orcid.org/0000-0002-3367-244X</orcidid><orcidid>https://orcid.org/0000-0003-2743-758X</orcidid><orcidid>https://orcid.org/0000-0003-1327-7159</orcidid></search><sort><creationdate>20210118</creationdate><title>Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR</title><author>Yang, Lin ; Wang, Pengchen ; Yao, Lu ; Meng, Xiaomi ; Jia, Charles Q ; Jiang, Xia ; Jiang, Wenju</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a197t-9afa62820ad223c64074d65b65fc321c8dde0e60725f3bb8883462b4f46172323</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yang, Lin</creatorcontrib><creatorcontrib>Wang, Pengchen</creatorcontrib><creatorcontrib>Yao, Lu</creatorcontrib><creatorcontrib>Meng, Xiaomi</creatorcontrib><creatorcontrib>Jia, Charles Q</creatorcontrib><creatorcontrib>Jiang, Xia</creatorcontrib><creatorcontrib>Jiang, Wenju</creatorcontrib><jtitle>ACS sustainable chemistry & engineering</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yang, Lin</au><au>Wang, Pengchen</au><au>Yao, Lu</au><au>Meng, Xiaomi</au><au>Jia, Charles Q</au><au>Jiang, Xia</au><au>Jiang, Wenju</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR</atitle><jtitle>ACS sustainable chemistry & engineering</jtitle><addtitle>ACS Sustainable Chem. Eng</addtitle><date>2021-01-18</date><risdate>2021</risdate><volume>9</volume><issue>2</issue><spage>987</spage><epage>997</epage><pages>987-997</pages><issn>2168-0485</issn><eissn>2168-0485</eissn><abstract>The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide tolerance was successfully applied to low-temperature NH3–SCR in this study. The findings indicate that the Cu x Ce/CAC-CNTs obtained at a 0.2 Cu/Ce molar ratio and the calcination temperature of 450 °C showed the highest 100% NO conversion with 95.8% N2 selectivity at 150 °C and 10 000 h–1. The incorporation of Cu improved the Cu0.2Ce/CAC-CNTs in Lewis acid, lattice oxygen (31.99%), and Ce3+ (26.03%). The accelerated NH3 adsorption on acid sites, the encouraging electron transfer by the Ce4+ + Cu+ ↔ Ce3+ + Cu2+ redox circle, and the more surface chemisorbed oxygen (Oβ) improved the catalytic activity of Cu0.2Ce/CAC-CNTs. The NH3–SCR of Cu0.2Ce/CAC-CNTs largely follows the L–H mechanism, together with a certain degree of “Fast SCR.” The added Cu species effectively prevented surface SO2 adsorption and oxidation, and the Cu0.2Ce/CAC-CNTs restored more than 94% SCR activity after 8 h of poisoning in 50 ppm SO2 and 5 vol % H2O.</abstract><pub>American Chemical Society</pub><doi>10.1021/acssuschemeng.0c08490</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0001-5754-7937</orcidid><orcidid>https://orcid.org/0000-0002-3367-244X</orcidid><orcidid>https://orcid.org/0000-0003-2743-758X</orcidid><orcidid>https://orcid.org/0000-0003-1327-7159</orcidid></addata></record> |
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title | Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR |
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