Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO
[Display omitted] •Cobalt oxide was deposited on two ceria nanoshapes with various metal precursors.•Nanorod-supported catalysts prepared with Co(acac) are most active for NO reduction.•Activity is dependent on cobalt dispersion and presence of defects. The speciation and catalytic activity of ceria...
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Veröffentlicht in: | Journal of catalysis 2020-01, Vol.381 (C), p.355-362 |
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creator | Savereide, Louisa Gosavi, Abha Hicks, Kenton E. Notestein, Justin M. |
description | [Display omitted]
•Cobalt oxide was deposited on two ceria nanoshapes with various metal precursors.•Nanorod-supported catalysts prepared with Co(acac) are most active for NO reduction.•Activity is dependent on cobalt dispersion and presence of defects.
The speciation and catalytic activity of ceria supported transition metal oxides synthesized via incipient wetness impregnation are highly dependent on synthesis parameters such as the choice of metal precursor and the concentration of defects such as oxygen vacancies in the support. Here, cobalt oxide domains were synthesized on cerium oxide nanorods and commercial nanopowder via incipient wetness impregnation of cobalt (II) nitrate hexahydrate, cobalt (II) acetate, cobalt (III) acetylacetonate, and disodium cobalt (II) ethylenediaminetetraacetic acid at surface densities below monolayer coverage. Their reactivity was tested in the catalytic reduction of NO by CO. The steady-state deNOx activity at 250 °C of the catalyst prepared with cobalt (III) acetylacetonate and ceria nanorods was nearly three times greater than that of the control catalyst. From X-ray absorption spectroscopy it was seen that as-deposited cobalt precursors on a nanorod support were more highly coordinated than were cobalt precursors on comparable commercial ceria nanoparticles, possibly indicating anchoring at defects on the nanorods. A relationship was found between catalyst activity and the cobalt oxidation state of the fully calcined catalysts that suggests that deNOx activity is separately dependent on the cobalt oxide distribution and the presence of defects in the support. Overall, here it is shown that the two critical synthesis parameters of ligand choice and defected supports combine additively to improve reactivity of the supported cobalt oxide. |
doi_str_mv | 10.1016/j.jcat.2019.11.016 |
format | Article |
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•Cobalt oxide was deposited on two ceria nanoshapes with various metal precursors.•Nanorod-supported catalysts prepared with Co(acac) are most active for NO reduction.•Activity is dependent on cobalt dispersion and presence of defects.
The speciation and catalytic activity of ceria supported transition metal oxides synthesized via incipient wetness impregnation are highly dependent on synthesis parameters such as the choice of metal precursor and the concentration of defects such as oxygen vacancies in the support. Here, cobalt oxide domains were synthesized on cerium oxide nanorods and commercial nanopowder via incipient wetness impregnation of cobalt (II) nitrate hexahydrate, cobalt (II) acetate, cobalt (III) acetylacetonate, and disodium cobalt (II) ethylenediaminetetraacetic acid at surface densities below monolayer coverage. Their reactivity was tested in the catalytic reduction of NO by CO. The steady-state deNOx activity at 250 °C of the catalyst prepared with cobalt (III) acetylacetonate and ceria nanorods was nearly three times greater than that of the control catalyst. From X-ray absorption spectroscopy it was seen that as-deposited cobalt precursors on a nanorod support were more highly coordinated than were cobalt precursors on comparable commercial ceria nanoparticles, possibly indicating anchoring at defects on the nanorods. A relationship was found between catalyst activity and the cobalt oxidation state of the fully calcined catalysts that suggests that deNOx activity is separately dependent on the cobalt oxide distribution and the presence of defects in the support. Overall, here it is shown that the two critical synthesis parameters of ligand choice and defected supports combine additively to improve reactivity of the supported cobalt oxide.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2019.11.016</identifier><language>eng</language><publisher>United States: Elsevier Inc</publisher><subject>ceria ; cobalt ; deNOx ; oxygen vacancies ; XANES</subject><ispartof>Journal of catalysis, 2020-01, Vol.381 (C), p.355-362</ispartof><rights>2019 Elsevier Inc.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c408t-a0339a957e3bb55829aaf90b484ad15b32dd3ab937ba176316e671de501ed89f3</citedby><cites>FETCH-LOGICAL-c408t-a0339a957e3bb55829aaf90b484ad15b32dd3ab937ba176316e671de501ed89f3</cites><orcidid>0000-0003-1780-7356 ; 0000000317807356</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jcat.2019.11.016$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>230,314,778,782,883,3539,27911,27912,45982</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1775845$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Savereide, Louisa</creatorcontrib><creatorcontrib>Gosavi, Abha</creatorcontrib><creatorcontrib>Hicks, Kenton E.</creatorcontrib><creatorcontrib>Notestein, Justin M.</creatorcontrib><title>Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO</title><title>Journal of catalysis</title><description>[Display omitted]
•Cobalt oxide was deposited on two ceria nanoshapes with various metal precursors.•Nanorod-supported catalysts prepared with Co(acac) are most active for NO reduction.•Activity is dependent on cobalt dispersion and presence of defects.
The speciation and catalytic activity of ceria supported transition metal oxides synthesized via incipient wetness impregnation are highly dependent on synthesis parameters such as the choice of metal precursor and the concentration of defects such as oxygen vacancies in the support. Here, cobalt oxide domains were synthesized on cerium oxide nanorods and commercial nanopowder via incipient wetness impregnation of cobalt (II) nitrate hexahydrate, cobalt (II) acetate, cobalt (III) acetylacetonate, and disodium cobalt (II) ethylenediaminetetraacetic acid at surface densities below monolayer coverage. Their reactivity was tested in the catalytic reduction of NO by CO. The steady-state deNOx activity at 250 °C of the catalyst prepared with cobalt (III) acetylacetonate and ceria nanorods was nearly three times greater than that of the control catalyst. From X-ray absorption spectroscopy it was seen that as-deposited cobalt precursors on a nanorod support were more highly coordinated than were cobalt precursors on comparable commercial ceria nanoparticles, possibly indicating anchoring at defects on the nanorods. A relationship was found between catalyst activity and the cobalt oxidation state of the fully calcined catalysts that suggests that deNOx activity is separately dependent on the cobalt oxide distribution and the presence of defects in the support. Overall, here it is shown that the two critical synthesis parameters of ligand choice and defected supports combine additively to improve reactivity of the supported cobalt oxide.</description><subject>ceria</subject><subject>cobalt</subject><subject>deNOx</subject><subject>oxygen vacancies</subject><subject>XANES</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNp9kEtLxDAUhYMoOI7-AVfBfTu5fQfcSPExMNiNwuxCmtyOGcamJHGk_97Wce3qwrnnHD4OIbfAYmBQrPbxXskQJwx4DBBP0hlZAOMsSgqenZMFYwlEPIfyklx5v2cMIM-rBdmtNfbBdKPpd3RwdkAXDHpqO3qw39HBSo2a1rbZrmpsEno0km4jJ0cqW2_dEIztqR9QBWe9ssNIO-voa0Md6i_1-21HWjfX5KKTB483f3dJ3p8e3-qXaNM8r-uHTaQyVoVIsjTlkuclpm07ASZcyo6zNqsyqSFv00TrVLY8LVsJZZFCgUUJGnMGqCvepUtyd-q1PhjhlQmoPpTt-4lQQFnmVZZPpuRkUhO0d9iJwZlP6UYBTMx7ir2Y9xTzngJATNIUuj-FcMI_GnRzO_YKtXFzubbmv_gPHvd-lg</recordid><startdate>202001</startdate><enddate>202001</enddate><creator>Savereide, Louisa</creator><creator>Gosavi, Abha</creator><creator>Hicks, Kenton E.</creator><creator>Notestein, Justin M.</creator><general>Elsevier Inc</general><general>Elsevier</general><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0003-1780-7356</orcidid><orcidid>https://orcid.org/0000000317807356</orcidid></search><sort><creationdate>202001</creationdate><title>Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO</title><author>Savereide, Louisa ; Gosavi, Abha ; Hicks, Kenton E. ; Notestein, Justin M.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c408t-a0339a957e3bb55829aaf90b484ad15b32dd3ab937ba176316e671de501ed89f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>ceria</topic><topic>cobalt</topic><topic>deNOx</topic><topic>oxygen vacancies</topic><topic>XANES</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Savereide, Louisa</creatorcontrib><creatorcontrib>Gosavi, Abha</creatorcontrib><creatorcontrib>Hicks, Kenton E.</creatorcontrib><creatorcontrib>Notestein, Justin M.</creatorcontrib><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Savereide, Louisa</au><au>Gosavi, Abha</au><au>Hicks, Kenton E.</au><au>Notestein, Justin M.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO</atitle><jtitle>Journal of catalysis</jtitle><date>2020-01</date><risdate>2020</risdate><volume>381</volume><issue>C</issue><spage>355</spage><epage>362</epage><pages>355-362</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><abstract>[Display omitted]
•Cobalt oxide was deposited on two ceria nanoshapes with various metal precursors.•Nanorod-supported catalysts prepared with Co(acac) are most active for NO reduction.•Activity is dependent on cobalt dispersion and presence of defects.
The speciation and catalytic activity of ceria supported transition metal oxides synthesized via incipient wetness impregnation are highly dependent on synthesis parameters such as the choice of metal precursor and the concentration of defects such as oxygen vacancies in the support. Here, cobalt oxide domains were synthesized on cerium oxide nanorods and commercial nanopowder via incipient wetness impregnation of cobalt (II) nitrate hexahydrate, cobalt (II) acetate, cobalt (III) acetylacetonate, and disodium cobalt (II) ethylenediaminetetraacetic acid at surface densities below monolayer coverage. Their reactivity was tested in the catalytic reduction of NO by CO. The steady-state deNOx activity at 250 °C of the catalyst prepared with cobalt (III) acetylacetonate and ceria nanorods was nearly three times greater than that of the control catalyst. From X-ray absorption spectroscopy it was seen that as-deposited cobalt precursors on a nanorod support were more highly coordinated than were cobalt precursors on comparable commercial ceria nanoparticles, possibly indicating anchoring at defects on the nanorods. A relationship was found between catalyst activity and the cobalt oxidation state of the fully calcined catalysts that suggests that deNOx activity is separately dependent on the cobalt oxide distribution and the presence of defects in the support. Overall, here it is shown that the two critical synthesis parameters of ligand choice and defected supports combine additively to improve reactivity of the supported cobalt oxide.</abstract><cop>United States</cop><pub>Elsevier Inc</pub><doi>10.1016/j.jcat.2019.11.016</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0003-1780-7356</orcidid><orcidid>https://orcid.org/0000000317807356</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | ceria cobalt deNOx oxygen vacancies XANES |
title | Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO |
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