Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene
The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work...
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creator | de la Croix, Tim Claes, Nathalie Eyley, Samuel Thielemans, Wim Bals, Sara De Vos, Dirk |
description | The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt-Sn/C catalysts were prepared
via
a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored
via
gas-phase FTIR, and distribution of liquid products was analyzed
via
GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn
2
/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
The catalytic transfer dehydrogenation of long-chain alkanes was investigated with simple heterogeneous Pt catalysts under mild conditions and with high selectivity, using ethylene as a cheap and abundant hydrogen acceptor. |
doi_str_mv | 10.1039/d3cy00370a |
format | Article |
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via
a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored
via
gas-phase FTIR, and distribution of liquid products was analyzed
via
GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn
2
/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
The catalytic transfer dehydrogenation of long-chain alkanes was investigated with simple heterogeneous Pt catalysts under mild conditions and with high selectivity, using ethylene as a cheap and abundant hydrogen acceptor.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/d3cy00370a</identifier><identifier>PMID: 38089937</identifier><language>eng</language><publisher>England: Royal Society of Chemistry</publisher><subject>Alkanes ; Alkenes ; Cascade chemical reactions ; Catalysts ; Chemisorption ; Chemistry ; Coking ; Dehydrogenation ; Endothermic reactions ; Ethylene ; NMR ; Nuclear magnetic resonance ; Reaction products</subject><ispartof>Catalysis science & technology, 2023-12, Vol.13 (24), p.7123-7135</ispartof><rights>This journal is © The Royal Society of Chemistry.</rights><rights>Copyright Royal Society of Chemistry 2023</rights><rights>This journal is © The Royal Society of Chemistry 2023 The Royal Society of Chemistry</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c388t-e38d3a6bcd172eaff5614a058507f663ce2bb315a8f874bb4700f17a971f4803</cites><orcidid>0000-0002-4249-8017 ; 0000-0002-1929-8455 ; 0000-0001-9869-8387 ; 0000-0001-6475-0204 ; 0000-0003-0490-9652 ; 0000-0003-4451-1964</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,780,784,885,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38089937$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>de la Croix, Tim</creatorcontrib><creatorcontrib>Claes, Nathalie</creatorcontrib><creatorcontrib>Eyley, Samuel</creatorcontrib><creatorcontrib>Thielemans, Wim</creatorcontrib><creatorcontrib>Bals, Sara</creatorcontrib><creatorcontrib>De Vos, Dirk</creatorcontrib><title>Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene</title><title>Catalysis science & technology</title><addtitle>Catal Sci Technol</addtitle><description>The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt-Sn/C catalysts were prepared
via
a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored
via
gas-phase FTIR, and distribution of liquid products was analyzed
via
GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn
2
/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
The catalytic transfer dehydrogenation of long-chain alkanes was investigated with simple heterogeneous Pt catalysts under mild conditions and with high selectivity, using ethylene as a cheap and abundant hydrogen acceptor.</description><subject>Alkanes</subject><subject>Alkenes</subject><subject>Cascade chemical reactions</subject><subject>Catalysts</subject><subject>Chemisorption</subject><subject>Chemistry</subject><subject>Coking</subject><subject>Dehydrogenation</subject><subject>Endothermic reactions</subject><subject>Ethylene</subject><subject>NMR</subject><subject>Nuclear magnetic resonance</subject><subject>Reaction products</subject><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpdkUuLFDEURoMozjDOxr1S4EaE0ptKqpKsZGgfIwzoYkBchVTqpqvG6mRM0kr56013j-0jmwTu4fDdfIQ8pvCSAlOvBmYXACbA3COnDXBec9HR-8d3y07IeUo3UA5XFGTzkJwwCVIpJk7J50vMGMMaPYZtqj7l2pps5uUnDlWOxieHsRpwXIY9ZPIUfBVcNQe_ru1oJl-Z-avxmKofUx4rzOMyF9kj8sCZOeH53X1Grt-9vV5d1lcf339YXVzVlkmZa2RyYKbr7UBFg8a5tqPcQCtbEK7rmMWm7xltjXRS8L7nAsBRYZSgjktgZ-T1QXu77Tc4WPQl9Kxv47QxcdHBTPrfiZ9GvQ7fNQVBm0bSYnh-Z4jh2xZT1pspWZxns_8R3ShoVNe2XBb02X_oTdhGX9bbUQVTndoJXxwoG0NKEd0xDQW9q0y_Yasv-8ouCvz07_xH9HdBBXhyAGKyx-mfztkvN5ecRA</recordid><startdate>20231211</startdate><enddate>20231211</enddate><creator>de la Croix, Tim</creator><creator>Claes, Nathalie</creator><creator>Eyley, Samuel</creator><creator>Thielemans, Wim</creator><creator>Bals, Sara</creator><creator>De Vos, Dirk</creator><general>Royal Society of Chemistry</general><general>The Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-4249-8017</orcidid><orcidid>https://orcid.org/0000-0002-1929-8455</orcidid><orcidid>https://orcid.org/0000-0001-9869-8387</orcidid><orcidid>https://orcid.org/0000-0001-6475-0204</orcidid><orcidid>https://orcid.org/0000-0003-0490-9652</orcidid><orcidid>https://orcid.org/0000-0003-4451-1964</orcidid></search><sort><creationdate>20231211</creationdate><title>Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene</title><author>de la Croix, Tim ; Claes, Nathalie ; Eyley, Samuel ; Thielemans, Wim ; Bals, Sara ; De Vos, Dirk</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c388t-e38d3a6bcd172eaff5614a058507f663ce2bb315a8f874bb4700f17a971f4803</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Alkanes</topic><topic>Alkenes</topic><topic>Cascade chemical reactions</topic><topic>Catalysts</topic><topic>Chemisorption</topic><topic>Chemistry</topic><topic>Coking</topic><topic>Dehydrogenation</topic><topic>Endothermic reactions</topic><topic>Ethylene</topic><topic>NMR</topic><topic>Nuclear magnetic resonance</topic><topic>Reaction products</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>de la Croix, Tim</creatorcontrib><creatorcontrib>Claes, Nathalie</creatorcontrib><creatorcontrib>Eyley, Samuel</creatorcontrib><creatorcontrib>Thielemans, Wim</creatorcontrib><creatorcontrib>Bals, Sara</creatorcontrib><creatorcontrib>De Vos, Dirk</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>de la Croix, Tim</au><au>Claes, Nathalie</au><au>Eyley, Samuel</au><au>Thielemans, Wim</au><au>Bals, Sara</au><au>De Vos, Dirk</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene</atitle><jtitle>Catalysis science & technology</jtitle><addtitle>Catal Sci Technol</addtitle><date>2023-12-11</date><risdate>2023</risdate><volume>13</volume><issue>24</issue><spage>7123</spage><epage>7135</epage><pages>7123-7135</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt-Sn/C catalysts were prepared
via
a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored
via
gas-phase FTIR, and distribution of liquid products was analyzed
via
GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn
2
/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.
The catalytic transfer dehydrogenation of long-chain alkanes was investigated with simple heterogeneous Pt catalysts under mild conditions and with high selectivity, using ethylene as a cheap and abundant hydrogen acceptor.</abstract><cop>England</cop><pub>Royal Society of Chemistry</pub><pmid>38089937</pmid><doi>10.1039/d3cy00370a</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0002-4249-8017</orcidid><orcidid>https://orcid.org/0000-0002-1929-8455</orcidid><orcidid>https://orcid.org/0000-0001-9869-8387</orcidid><orcidid>https://orcid.org/0000-0001-6475-0204</orcidid><orcidid>https://orcid.org/0000-0003-0490-9652</orcidid><orcidid>https://orcid.org/0000-0003-4451-1964</orcidid><oa>free_for_read</oa></addata></record> |
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source | Royal Society Of Chemistry Journals 2008- |
subjects | Alkanes Alkenes Cascade chemical reactions Catalysts Chemisorption Chemistry Coking Dehydrogenation Endothermic reactions Ethylene NMR Nuclear magnetic resonance Reaction products |
title | Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene |
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