Exploring Low-Temperature Dehydrogenation at Ionic Cu Sites in Beta Zeolite To Enable Alkane Recycle in Dimethyl Ether Homologation
Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Brønsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/...
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| Veröffentlicht in: | ACS catalysis 2017-05, Vol.7 (5), p.3662-3667 |
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| container_title | ACS catalysis |
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| creator | Farberow, Carrie A Cheah, Singfoong Kim, Seonah Miller, Jeffrey T Gallagher, James R Hensley, Jesse E Schaidle, Joshua A Ruddy, Daniel A |
| description | Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Brønsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C–H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. These results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield. |
| doi_str_mv | 10.1021/acscatal.6b03582 |
| format | Article |
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(NREL), Golden, CO (United States)</creatorcontrib><description>Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Brønsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C–H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. These results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield.</description><identifier>ISSN: 2155-5435</identifier><identifier>EISSN: 2155-5435</identifier><identifier>DOI: 10.1021/acscatal.6b03582</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>09 BIOMASS FUELS ; C-H activation ; copper ; dehydrogenation ; heterogeneous catalysis ; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ; zeolites</subject><ispartof>ACS catalysis, 2017-05, Vol.7 (5), p.3662-3667</ispartof><rights>Copyright © 2017 American Chemical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a349t-5d3e294f293b25671afafe2ebe85151ea7ce9b3824be3e87eddfa82ab4545b533</citedby><cites>FETCH-LOGICAL-a349t-5d3e294f293b25671afafe2ebe85151ea7ce9b3824be3e87eddfa82ab4545b533</cites><orcidid>0000-0001-9846-7140 ; 0000-0003-2654-3778 ; 0000000326543778 ; 0000000198467140</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/acscatal.6b03582$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acscatal.6b03582$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,778,782,883,2754,27059,27907,27908,56721,56771</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1357736$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Farberow, Carrie A</creatorcontrib><creatorcontrib>Cheah, Singfoong</creatorcontrib><creatorcontrib>Kim, Seonah</creatorcontrib><creatorcontrib>Miller, Jeffrey T</creatorcontrib><creatorcontrib>Gallagher, James R</creatorcontrib><creatorcontrib>Hensley, Jesse E</creatorcontrib><creatorcontrib>Schaidle, Joshua A</creatorcontrib><creatorcontrib>Ruddy, Daniel A</creatorcontrib><creatorcontrib>National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><title>Exploring Low-Temperature Dehydrogenation at Ionic Cu Sites in Beta Zeolite To Enable Alkane Recycle in Dimethyl Ether Homologation</title><title>ACS catalysis</title><addtitle>ACS Catal</addtitle><description>Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Brønsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C–H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. These results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C5+) hydrocarbon yield.</description><subject>09 BIOMASS FUELS</subject><subject>C-H activation</subject><subject>copper</subject><subject>dehydrogenation</subject><subject>heterogeneous catalysis</subject><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>zeolites</subject><issn>2155-5435</issn><issn>2155-5435</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNp1UD1PwzAQjRBIVKU7o8VMILbjJhlLW2ilSkhQFhbr4l7alMSubFeQmT-OoUVi4Zb7eu_p7kXRJU1uaMLoLSinwENzMywTLnJ2EvUYFSIWKRenf-rzaODcNgmRimGeJb3oc_qxa4yt9ZoszHu8xHaHFvzeIpngpltZs0YNvjaagCdzo2tFxnvyXHt0pNbkDj2QVzRNGJClIVMNZYNk1LyBRvKEqlOhDcBJ3aLfdA2Z-g1aMjOtacz6R_kiOqugcTg45n70cj9djmfx4vFhPh4tYuBp4WOx4siKtGIFL5kYZhQqqJBhibmggiJkCouS5ywtkWOe4WpVQc6gTEUqSsF5P7o66Brna-lUOFltlNEalZeUiyzjwwBKDiBljXMWK7mzdQu2kzSR32bLX7Pl0exAuT5QwkZuzd7q8MX_8C-FGYTj</recordid><startdate>20170505</startdate><enddate>20170505</enddate><creator>Farberow, Carrie A</creator><creator>Cheah, Singfoong</creator><creator>Kim, Seonah</creator><creator>Miller, Jeffrey T</creator><creator>Gallagher, James R</creator><creator>Hensley, Jesse E</creator><creator>Schaidle, Joshua A</creator><creator>Ruddy, Daniel A</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>AAYXX</scope><scope>CITATION</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-9846-7140</orcidid><orcidid>https://orcid.org/0000-0003-2654-3778</orcidid><orcidid>https://orcid.org/0000000326543778</orcidid><orcidid>https://orcid.org/0000000198467140</orcidid></search><sort><creationdate>20170505</creationdate><title>Exploring Low-Temperature Dehydrogenation at Ionic Cu Sites in Beta Zeolite To Enable Alkane Recycle in Dimethyl Ether Homologation</title><author>Farberow, Carrie A ; Cheah, Singfoong ; Kim, Seonah ; Miller, Jeffrey T ; Gallagher, James R ; Hensley, Jesse E ; Schaidle, Joshua A ; Ruddy, Daniel A</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a349t-5d3e294f293b25671afafe2ebe85151ea7ce9b3824be3e87eddfa82ab4545b533</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><topic>09 BIOMASS FUELS</topic><topic>C-H activation</topic><topic>copper</topic><topic>dehydrogenation</topic><topic>heterogeneous catalysis</topic><topic>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</topic><topic>zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Farberow, Carrie A</creatorcontrib><creatorcontrib>Cheah, Singfoong</creatorcontrib><creatorcontrib>Kim, Seonah</creatorcontrib><creatorcontrib>Miller, Jeffrey T</creatorcontrib><creatorcontrib>Gallagher, James R</creatorcontrib><creatorcontrib>Hensley, Jesse E</creatorcontrib><creatorcontrib>Schaidle, Joshua A</creatorcontrib><creatorcontrib>Ruddy, Daniel A</creatorcontrib><creatorcontrib>National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><collection>CrossRef</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>ACS catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Farberow, Carrie A</au><au>Cheah, Singfoong</au><au>Kim, Seonah</au><au>Miller, Jeffrey T</au><au>Gallagher, James R</au><au>Hensley, Jesse E</au><au>Schaidle, Joshua A</au><au>Ruddy, Daniel A</au><aucorp>National Renewable Energy Lab. 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| subjects | 09 BIOMASS FUELS C-H activation copper dehydrogenation heterogeneous catalysis INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY zeolites |
| title | Exploring Low-Temperature Dehydrogenation at Ionic Cu Sites in Beta Zeolite To Enable Alkane Recycle in Dimethyl Ether Homologation |
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