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Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts
[Display omitted] •CoPt/CeO2, CoMo/CeO2, and NiMo/CeO2 favor the reforming pathway to produce syngas via the C–C bond cleavage.•FeNi/CeO2 shows promising selectivity to the oxidative dehydrogenation pathway to produce ethylene via the C–H bond cleavage.•DFT calculated energy profiles on CoPt/CeO2 an...
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Published in: | Journal of catalysis 2016-11, Vol.343, p.168-177 |
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container_title | Journal of catalysis |
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creator | Myint, MyatNoeZin Yan, Binhang Wan, Jie Zhao, Shen Chen, Jingguang G. |
description | [Display omitted]
•CoPt/CeO2, CoMo/CeO2, and NiMo/CeO2 favor the reforming pathway to produce syngas via the C–C bond cleavage.•FeNi/CeO2 shows promising selectivity to the oxidative dehydrogenation pathway to produce ethylene via the C–H bond cleavage.•DFT calculated energy profiles on CoPt/CeO2 and FeNi/CeO2 support different reaction pathways.
An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts. |
doi_str_mv | 10.1016/j.jcat.2016.02.004 |
format | article |
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•CoPt/CeO2, CoMo/CeO2, and NiMo/CeO2 favor the reforming pathway to produce syngas via the C–C bond cleavage.•FeNi/CeO2 shows promising selectivity to the oxidative dehydrogenation pathway to produce ethylene via the C–H bond cleavage.•DFT calculated energy profiles on CoPt/CeO2 and FeNi/CeO2 support different reaction pathways.
An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2016.02.004</identifier><language>eng</language><publisher>San Diego: Elsevier Inc</publisher><subject>Carbon dioxide ; Catalysts ; CeO2 supports ; Ethanol ; Ethylene ; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ; Oxidative dehydrogenation ; Oxidative stress ; Reforming ; Synthesis gas</subject><ispartof>Journal of catalysis, 2016-11, Vol.343, p.168-177</ispartof><rights>2016 Elsevier Inc.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c506t-70e8c3eeb1e2ee84e9e87cf7ef7aed70763948885e984c15346d990cec46141d3</citedby><cites>FETCH-LOGICAL-c506t-70e8c3eeb1e2ee84e9e87cf7ef7aed70763948885e984c15346d990cec46141d3</cites><orcidid>0000-0002-8731-7742 ; 0000000287317742</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,780,784,885,27915,27916</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1341673$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Myint, MyatNoeZin</creatorcontrib><creatorcontrib>Yan, Binhang</creatorcontrib><creatorcontrib>Wan, Jie</creatorcontrib><creatorcontrib>Zhao, Shen</creatorcontrib><creatorcontrib>Chen, Jingguang G.</creatorcontrib><creatorcontrib>Brookhaven National Lab. (BNL), Upton, NY (United States)</creatorcontrib><title>Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts</title><title>Journal of catalysis</title><description>[Display omitted]
•CoPt/CeO2, CoMo/CeO2, and NiMo/CeO2 favor the reforming pathway to produce syngas via the C–C bond cleavage.•FeNi/CeO2 shows promising selectivity to the oxidative dehydrogenation pathway to produce ethylene via the C–H bond cleavage.•DFT calculated energy profiles on CoPt/CeO2 and FeNi/CeO2 support different reaction pathways.
An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts.</description><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>CeO2 supports</subject><subject>Ethanol</subject><subject>Ethylene</subject><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>Oxidative dehydrogenation</subject><subject>Oxidative stress</subject><subject>Reforming</subject><subject>Synthesis gas</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNp9kEFr3DAQhUVJoJukf6An0ZztaGTZlqCXsjRtIBAI6Vko0jgrsyulkrLp_vvKuOee3gx8b3jzCPkMrAUGw83cztaUlte5ZbxlTHwgG2CKNXxQ4oxsGOPQqB7Gj-Qi55kxgL6XGzI94hTTwYcXaoKj8Y93pvgjUoe7k0vxBUPdY6Bxolh2JiB992VHtw-cmkwNzXEqqy1UPWKiz_6Axez33tKayexPueQrcj6ZfcZP__SS_Lr9_rT92dw__LjbfrtvbM-G0owMpe0QnwE5ohSoUI52GnEaDbqRjUOnhJSyRyWFhb4Tg1OKWbRiAAGuuyRf1rsxF6-z9QXtzsYQ0BYNnYBh7Cp0vUKvKf5-w1z0HN9SqLk0yI5zGKBTleIrZVPMOeGkX5M_mHTSwPRSup71UrpeSteM61p6NX1dTVifPHpMSwYMFp1PSwQX_f_sfwFsnIrt</recordid><startdate>20161101</startdate><enddate>20161101</enddate><creator>Myint, MyatNoeZin</creator><creator>Yan, Binhang</creator><creator>Wan, Jie</creator><creator>Zhao, Shen</creator><creator>Chen, Jingguang G.</creator><general>Elsevier Inc</general><general>Elsevier BV</general><general>Elsevier</general><scope>AAYXX</scope><scope>CITATION</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0002-8731-7742</orcidid><orcidid>https://orcid.org/0000000287317742</orcidid></search><sort><creationdate>20161101</creationdate><title>Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts</title><author>Myint, MyatNoeZin ; Yan, Binhang ; Wan, Jie ; Zhao, Shen ; Chen, Jingguang G.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c506t-70e8c3eeb1e2ee84e9e87cf7ef7aed70763948885e984c15346d990cec46141d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>CeO2 supports</topic><topic>Ethanol</topic><topic>Ethylene</topic><topic>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</topic><topic>Oxidative dehydrogenation</topic><topic>Oxidative stress</topic><topic>Reforming</topic><topic>Synthesis gas</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Myint, MyatNoeZin</creatorcontrib><creatorcontrib>Yan, Binhang</creatorcontrib><creatorcontrib>Wan, Jie</creatorcontrib><creatorcontrib>Zhao, Shen</creatorcontrib><creatorcontrib>Chen, Jingguang G.</creatorcontrib><creatorcontrib>Brookhaven National Lab. (BNL), Upton, NY (United States)</creatorcontrib><collection>CrossRef</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Myint, MyatNoeZin</au><au>Yan, Binhang</au><au>Wan, Jie</au><au>Zhao, Shen</au><au>Chen, Jingguang G.</au><aucorp>Brookhaven National Lab. (BNL), Upton, NY (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts</atitle><jtitle>Journal of catalysis</jtitle><date>2016-11-01</date><risdate>2016</risdate><volume>343</volume><spage>168</spage><epage>177</epage><pages>168-177</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><abstract>[Display omitted]
•CoPt/CeO2, CoMo/CeO2, and NiMo/CeO2 favor the reforming pathway to produce syngas via the C–C bond cleavage.•FeNi/CeO2 shows promising selectivity to the oxidative dehydrogenation pathway to produce ethylene via the C–H bond cleavage.•DFT calculated energy profiles on CoPt/CeO2 and FeNi/CeO2 support different reaction pathways.
An efficient mitigation of abundantly available CO2 is critical for sustainable environmental impact as well as for novel industrial applications. Using ethane, CO2 can be catalytically converted into a useful feedstock (synthesis gas) and a value-added monomer (ethylene) via the dry reforming pathway through the C–C bond scission and the oxidative dehydrogenation pathway through the C–H bond scission, respectively. Results from the current flow-reactor study show that the precious metal bimetallic CoPt/CeO2 catalyst undergoes the reforming reaction to produce syngas with enhanced activity and stability compared to the parent monometallic catalysts. In order to replace Pt, the activities of non-precious CoMo/CeO2 and NiMo/CeO2 are investigated and the results indicate that NiMo/CeO2 is nearly as active as CoPt/CeO2 for the reforming pathway. Furthermore, FeNi/CeO2 is identified as a promising catalyst for the oxidative dehydrogenation to produce ethylene. Density functional theory (DFT) calculations are performed to further understand the different pathways of the CoPt/CeO2 and FeNi/CeO2 catalysts.</abstract><cop>San Diego</cop><pub>Elsevier Inc</pub><doi>10.1016/j.jcat.2016.02.004</doi><tpages>10</tpages><orcidid>https://orcid.org/0000-0002-8731-7742</orcidid><orcidid>https://orcid.org/0000000287317742</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Carbon dioxide Catalysts CeO2 supports Ethanol Ethylene INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Oxidative dehydrogenation Oxidative stress Reforming Synthesis gas |
title | Reforming and oxidative dehydrogenation of ethane with CO2 as a soft oxidant over bimetallic catalysts |
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