Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts
Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidenc...
Gespeichert in:
| Veröffentlicht in: | Angewandte Chemie (International ed.) 2020-05, Vol.59 (21), p.8042-8046 |
|---|---|
| Hauptverfasser: | , , , , , , , , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | 8046 |
|---|---|
| container_issue | 21 |
| container_start_page | 8042 |
| container_title | Angewandte Chemie (International ed.) |
| container_volume | 59 |
| creator | Zhang, Xuanyu You, Rui Wei, Zeyue Jiang, Xiao Yang, Jiuzhong Pan, Yang Wu, Peiwen Jia, Qingdong Bao, Zhenghong Bai, Lei Jin, Mingzhou Sumpter, Bobby Fung, Victor Huang, Weixin Wu, Zili |
| description | Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH3.) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C2 and C1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.
ODH over h‐BN: Propane oxidative dehydrogenation over hexagonal boron nitride undergoes both surface‐mediated and gas‐phase radical pathways. Propene is exclusively formed from the surface reaction, while C1 and C2 products are formed via both channels. |
| doi_str_mv | 10.1002/anie.202002440 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_osti_</sourceid><recordid>TN_cdi_osti_scitechconnect_1615043</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2382655390</sourcerecordid><originalsourceid>FETCH-LOGICAL-c4370-5363420b1dd74207e3a0732fe5edf05dfef2a20c507f8305a364ac110f3358203</originalsourceid><addsrcrecordid>eNqFkcFPFDEUxhsjEVy9ejSNXrzM-tpOZ2aPuIKQIBii56a0r2zJ7HRpO8j893RdwMSLp_fy8uv3-r2PkHcM5gyAf9aDxzkHXvq6hhfkgEnOKtG24mXpayGqtpNsn7xO6aYwXQfNK7IvOAfRCH5AxkttvdE9Xa5w7VOOE9WDpZeoTfZhoN_RrMqOtE40OPojho0ekF7ce6uzv0P6FVeTjeEaB_2HD3cY6Qne6-swFNUvIZbhuc_RW6RLnXU_pZzekD2n-4RvH-uM_Do--rk8qc4uvp0uD88qU4sWKln-WHO4Yta2pbYoNLSCO5RoHUjr0HHNwUhoXSdAatHU2jAGTgjZFYsz8mGnG1L2Khmfix0ThgFNVqxhEsqFZuTTDtrEcDtiyqocwmDfF6dhTIqLjjdSisVW7-M_6E0YYzFaqBoW0C3qri7UfEeZGFKK6NQm-rWOk2KgtqmpbWrqObXy4P2j7Hi1RvuMP8VUgMUO-O17nP4jpw7PT4_-ij8A8yCitw</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2409089484</pqid></control><display><type>article</type><title>Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts</title><source>Wiley Online Library Journals Frontfile Complete</source><creator>Zhang, Xuanyu ; You, Rui ; Wei, Zeyue ; Jiang, Xiao ; Yang, Jiuzhong ; Pan, Yang ; Wu, Peiwen ; Jia, Qingdong ; Bao, Zhenghong ; Bai, Lei ; Jin, Mingzhou ; Sumpter, Bobby ; Fung, Victor ; Huang, Weixin ; Wu, Zili</creator><creatorcontrib>Zhang, Xuanyu ; You, Rui ; Wei, Zeyue ; Jiang, Xiao ; Yang, Jiuzhong ; Pan, Yang ; Wu, Peiwen ; Jia, Qingdong ; Bao, Zhenghong ; Bai, Lei ; Jin, Mingzhou ; Sumpter, Bobby ; Fung, Victor ; Huang, Weixin ; Wu, Zili</creatorcontrib><description>Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH3.) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C2 and C1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.
ODH over h‐BN: Propane oxidative dehydrogenation over hexagonal boron nitride undergoes both surface‐mediated and gas‐phase radical pathways. Propene is exclusively formed from the surface reaction, while C1 and C2 products are formed via both channels.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202002440</identifier><identifier>PMID: 32203632</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Boron ; Boron nitride ; Catalysts ; Dehydrogenation ; Density functional theory ; hexagonal boron nitride ; mass spectrometry ; Mass spectroscopy ; Methyl radicals ; oxidative dehydrogenation ; Photoionization ; Propane ; Reaction mechanisms ; reaction pathways ; Vacuum</subject><ispartof>Angewandte Chemie (International ed.), 2020-05, Vol.59 (21), p.8042-8046</ispartof><rights>2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c4370-5363420b1dd74207e3a0732fe5edf05dfef2a20c507f8305a364ac110f3358203</citedby><cites>FETCH-LOGICAL-c4370-5363420b1dd74207e3a0732fe5edf05dfef2a20c507f8305a364ac110f3358203</cites><orcidid>0000-0002-3347-6983 ; 0000-0002-4902-1828 ; 0000-0002-2387-8129 ; 0000-0002-4615-9741 ; 0000-0001-6341-0355 ; 0000-0002-5025-3124 ; 0000-0002-4458-674X ; 0000-0002-4468-3240 ; 0000000223878129 ; 0000000233476983 ; 0000000250253124 ; 0000000249021828 ; 0000000244683240 ; 0000000246159741 ; 0000000163410355 ; 000000024458674X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.202002440$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202002440$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>230,314,776,780,881,1411,27901,27902,45550,45551</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/32203632$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1615043$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhang, Xuanyu</creatorcontrib><creatorcontrib>You, Rui</creatorcontrib><creatorcontrib>Wei, Zeyue</creatorcontrib><creatorcontrib>Jiang, Xiao</creatorcontrib><creatorcontrib>Yang, Jiuzhong</creatorcontrib><creatorcontrib>Pan, Yang</creatorcontrib><creatorcontrib>Wu, Peiwen</creatorcontrib><creatorcontrib>Jia, Qingdong</creatorcontrib><creatorcontrib>Bao, Zhenghong</creatorcontrib><creatorcontrib>Bai, Lei</creatorcontrib><creatorcontrib>Jin, Mingzhou</creatorcontrib><creatorcontrib>Sumpter, Bobby</creatorcontrib><creatorcontrib>Fung, Victor</creatorcontrib><creatorcontrib>Huang, Weixin</creatorcontrib><creatorcontrib>Wu, Zili</creatorcontrib><title>Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts</title><title>Angewandte Chemie (International ed.)</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH3.) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C2 and C1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.
ODH over h‐BN: Propane oxidative dehydrogenation over hexagonal boron nitride undergoes both surface‐mediated and gas‐phase radical pathways. Propene is exclusively formed from the surface reaction, while C1 and C2 products are formed via both channels.</description><subject>Boron</subject><subject>Boron nitride</subject><subject>Catalysts</subject><subject>Dehydrogenation</subject><subject>Density functional theory</subject><subject>hexagonal boron nitride</subject><subject>mass spectrometry</subject><subject>Mass spectroscopy</subject><subject>Methyl radicals</subject><subject>oxidative dehydrogenation</subject><subject>Photoionization</subject><subject>Propane</subject><subject>Reaction mechanisms</subject><subject>reaction pathways</subject><subject>Vacuum</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFkcFPFDEUxhsjEVy9ejSNXrzM-tpOZ2aPuIKQIBii56a0r2zJ7HRpO8j893RdwMSLp_fy8uv3-r2PkHcM5gyAf9aDxzkHXvq6hhfkgEnOKtG24mXpayGqtpNsn7xO6aYwXQfNK7IvOAfRCH5AxkttvdE9Xa5w7VOOE9WDpZeoTfZhoN_RrMqOtE40OPojho0ekF7ce6uzv0P6FVeTjeEaB_2HD3cY6Qne6-swFNUvIZbhuc_RW6RLnXU_pZzekD2n-4RvH-uM_Do--rk8qc4uvp0uD88qU4sWKln-WHO4Yta2pbYoNLSCO5RoHUjr0HHNwUhoXSdAatHU2jAGTgjZFYsz8mGnG1L2Khmfix0ThgFNVqxhEsqFZuTTDtrEcDtiyqocwmDfF6dhTIqLjjdSisVW7-M_6E0YYzFaqBoW0C3qri7UfEeZGFKK6NQm-rWOk2KgtqmpbWrqObXy4P2j7Hi1RvuMP8VUgMUO-O17nP4jpw7PT4_-ij8A8yCitw</recordid><startdate>20200518</startdate><enddate>20200518</enddate><creator>Zhang, Xuanyu</creator><creator>You, Rui</creator><creator>Wei, Zeyue</creator><creator>Jiang, Xiao</creator><creator>Yang, Jiuzhong</creator><creator>Pan, Yang</creator><creator>Wu, Peiwen</creator><creator>Jia, Qingdong</creator><creator>Bao, Zhenghong</creator><creator>Bai, Lei</creator><creator>Jin, Mingzhou</creator><creator>Sumpter, Bobby</creator><creator>Fung, Victor</creator><creator>Huang, Weixin</creator><creator>Wu, Zili</creator><general>Wiley Subscription Services, Inc</general><general>Wiley Blackwell (John Wiley & Sons)</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0002-3347-6983</orcidid><orcidid>https://orcid.org/0000-0002-4902-1828</orcidid><orcidid>https://orcid.org/0000-0002-2387-8129</orcidid><orcidid>https://orcid.org/0000-0002-4615-9741</orcidid><orcidid>https://orcid.org/0000-0001-6341-0355</orcidid><orcidid>https://orcid.org/0000-0002-5025-3124</orcidid><orcidid>https://orcid.org/0000-0002-4458-674X</orcidid><orcidid>https://orcid.org/0000-0002-4468-3240</orcidid><orcidid>https://orcid.org/0000000223878129</orcidid><orcidid>https://orcid.org/0000000233476983</orcidid><orcidid>https://orcid.org/0000000250253124</orcidid><orcidid>https://orcid.org/0000000249021828</orcidid><orcidid>https://orcid.org/0000000244683240</orcidid><orcidid>https://orcid.org/0000000246159741</orcidid><orcidid>https://orcid.org/0000000163410355</orcidid><orcidid>https://orcid.org/000000024458674X</orcidid></search><sort><creationdate>20200518</creationdate><title>Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts</title><author>Zhang, Xuanyu ; You, Rui ; Wei, Zeyue ; Jiang, Xiao ; Yang, Jiuzhong ; Pan, Yang ; Wu, Peiwen ; Jia, Qingdong ; Bao, Zhenghong ; Bai, Lei ; Jin, Mingzhou ; Sumpter, Bobby ; Fung, Victor ; Huang, Weixin ; Wu, Zili</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4370-5363420b1dd74207e3a0732fe5edf05dfef2a20c507f8305a364ac110f3358203</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Boron</topic><topic>Boron nitride</topic><topic>Catalysts</topic><topic>Dehydrogenation</topic><topic>Density functional theory</topic><topic>hexagonal boron nitride</topic><topic>mass spectrometry</topic><topic>Mass spectroscopy</topic><topic>Methyl radicals</topic><topic>oxidative dehydrogenation</topic><topic>Photoionization</topic><topic>Propane</topic><topic>Reaction mechanisms</topic><topic>reaction pathways</topic><topic>Vacuum</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Xuanyu</creatorcontrib><creatorcontrib>You, Rui</creatorcontrib><creatorcontrib>Wei, Zeyue</creatorcontrib><creatorcontrib>Jiang, Xiao</creatorcontrib><creatorcontrib>Yang, Jiuzhong</creatorcontrib><creatorcontrib>Pan, Yang</creatorcontrib><creatorcontrib>Wu, Peiwen</creatorcontrib><creatorcontrib>Jia, Qingdong</creatorcontrib><creatorcontrib>Bao, Zhenghong</creatorcontrib><creatorcontrib>Bai, Lei</creatorcontrib><creatorcontrib>Jin, Mingzhou</creatorcontrib><creatorcontrib>Sumpter, Bobby</creatorcontrib><creatorcontrib>Fung, Victor</creatorcontrib><creatorcontrib>Huang, Weixin</creatorcontrib><creatorcontrib>Wu, Zili</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV</collection><jtitle>Angewandte Chemie (International ed.)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Xuanyu</au><au>You, Rui</au><au>Wei, Zeyue</au><au>Jiang, Xiao</au><au>Yang, Jiuzhong</au><au>Pan, Yang</au><au>Wu, Peiwen</au><au>Jia, Qingdong</au><au>Bao, Zhenghong</au><au>Bai, Lei</au><au>Jin, Mingzhou</au><au>Sumpter, Bobby</au><au>Fung, Victor</au><au>Huang, Weixin</au><au>Wu, Zili</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts</atitle><jtitle>Angewandte Chemie (International ed.)</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2020-05-18</date><risdate>2020</risdate><volume>59</volume><issue>21</issue><spage>8042</spage><epage>8046</epage><pages>8042-8046</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Although hexagonal boron nitride (h‐BN) has recently been identified as a highly efficient catalyst for the oxidative dehydrogenation of propane (ODHP) reaction, the reaction mechanisms, especially regarding radical chemistry of this system, remain elusive. Now, the first direct experimental evidence of gas‐phase methyl radicals (CH3.) in the ODHP reaction over boron‐based catalysts is achieved by using online synchrotron vacuum ultraviolet photoionization mass spectroscopy (SVUV‐PIMS), which uncovers the existence of gas‐phase radical pathways. Combined with density functional theory (DFT) calculations, the results demonstrate that propene is mainly generated on the catalyst surface from the C−H activation of propane, while C2 and C1 products can be formed via both surface‐mediated and gas‐phase pathways. These observations provide new insights towards understanding the ODHP reaction mechanisms over boron‐based catalysts.
ODH over h‐BN: Propane oxidative dehydrogenation over hexagonal boron nitride undergoes both surface‐mediated and gas‐phase radical pathways. Propene is exclusively formed from the surface reaction, while C1 and C2 products are formed via both channels.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>32203632</pmid><doi>10.1002/anie.202002440</doi><tpages>5</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-3347-6983</orcidid><orcidid>https://orcid.org/0000-0002-4902-1828</orcidid><orcidid>https://orcid.org/0000-0002-2387-8129</orcidid><orcidid>https://orcid.org/0000-0002-4615-9741</orcidid><orcidid>https://orcid.org/0000-0001-6341-0355</orcidid><orcidid>https://orcid.org/0000-0002-5025-3124</orcidid><orcidid>https://orcid.org/0000-0002-4458-674X</orcidid><orcidid>https://orcid.org/0000-0002-4468-3240</orcidid><orcidid>https://orcid.org/0000000223878129</orcidid><orcidid>https://orcid.org/0000000233476983</orcidid><orcidid>https://orcid.org/0000000250253124</orcidid><orcidid>https://orcid.org/0000000249021828</orcidid><orcidid>https://orcid.org/0000000244683240</orcidid><orcidid>https://orcid.org/0000000246159741</orcidid><orcidid>https://orcid.org/0000000163410355</orcidid><orcidid>https://orcid.org/000000024458674X</orcidid></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 1433-7851 |
| ispartof | Angewandte Chemie (International ed.), 2020-05, Vol.59 (21), p.8042-8046 |
| issn | 1433-7851 1521-3773 |
| language | eng |
| recordid | cdi_osti_scitechconnect_1615043 |
| source | Wiley Online Library Journals Frontfile Complete |
| subjects | Boron Boron nitride Catalysts Dehydrogenation Density functional theory hexagonal boron nitride mass spectrometry Mass spectroscopy Methyl radicals oxidative dehydrogenation Photoionization Propane Reaction mechanisms reaction pathways Vacuum |
| title | Radical Chemistry and Reaction Mechanisms of Propane Oxidative Dehydrogenation over Hexagonal Boron Nitride Catalysts |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-02-11T02%3A34%3A10IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_osti_&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Radical%20Chemistry%20and%20Reaction%20Mechanisms%20of%20Propane%20Oxidative%20Dehydrogenation%20over%20Hexagonal%20Boron%20Nitride%20Catalysts&rft.jtitle=Angewandte%20Chemie%20(International%20ed.)&rft.au=Zhang,%20Xuanyu&rft.date=2020-05-18&rft.volume=59&rft.issue=21&rft.spage=8042&rft.epage=8046&rft.pages=8042-8046&rft.issn=1433-7851&rft.eissn=1521-3773&rft_id=info:doi/10.1002/anie.202002440&rft_dat=%3Cproquest_osti_%3E2382655390%3C/proquest_osti_%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2409089484&rft_id=info:pmid/32203632&rfr_iscdi=true |