The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts
Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalyst...
Gespeichert in:
| Veröffentlicht in: | Helvetica chimica acta 2024-08, Vol.107 (8), p.n/a |
|---|---|
| Hauptverfasser: | , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | n/a |
|---|---|
| container_issue | 8 |
| container_start_page | |
| container_title | Helvetica chimica acta |
| container_volume | 107 |
| creator | Castro‐Fernández, Pedro Serykh, Alexander I. Yarar, Melis Mance, Deni Abdala, Paula M. Copéret, Christophe Fedorov, Alexey Müller, Christoph R. |
| description | Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalysts reveals that the dispersion on silica increases the Ga‐normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2‐treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mainly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2‐treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga−H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga : Al ratios, give Ga−H bands at ca. 2040 and 2060 cm−1.
@GroupLese, @CoperetGroup, @eth_dmavt, @eth_dchab |
| doi_str_mv | 10.1002/hlca.202400076 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_wiley</sourceid><recordid>TN_cdi_proquest_journals_3094180663</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>3094180663</sourcerecordid><originalsourceid>FETCH-LOGICAL-p2036-c64fcc04707524d3443e751575f861c43fc5fadca7625890658a8eadcd806ee93</originalsourceid><addsrcrecordid>eNo9kcFOGzEQhq0KpAbKlbOlXlqpG8b22rt7jJKWVAoEEZC4rYx3lhi5u8vaKeytj9D36FvxJHUIymk0v77_n5F-Qk4ZjBkAP1s7o8cceAoAmfpARkxynnCVyQMyAmB5Aqy4-0iOvH-MSFFANiL_btZIr9HpYNuG3mN4RmzopQ6bHqluKroK-t46Gwba1nTOX__8nVnvW2Ojo3mgKxvQv4FXfdthg3SFDk2wv7cW20TAWaOjbbXpurYPWNEv5_rbxH3lS0Ev7EsUli-2wrcAHQNmuB6qvn3AZvfUVAftBh_8J3JYa-fx5H0ek9sf32-m82SxPP85nSySjoNQiVFpbQykGWSSp5VIU4GZZDKTda6YSUVtZK0rozPFZV6AkrnOMQpVDgqxEMfk8y6369unDfpQPrabvoknSwFFyiKmRKSKHfVsHQ5l19tfuh9KBuW2jXLbRrlvo5wvppP9Jv4DLDOEIw</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>3094180663</pqid></control><display><type>article</type><title>The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts</title><source>Wiley Online Library - AutoHoldings Journals</source><creator>Castro‐Fernández, Pedro ; Serykh, Alexander I. ; Yarar, Melis ; Mance, Deni ; Abdala, Paula M. ; Copéret, Christophe ; Fedorov, Alexey ; Müller, Christoph R.</creator><creatorcontrib>Castro‐Fernández, Pedro ; Serykh, Alexander I. ; Yarar, Melis ; Mance, Deni ; Abdala, Paula M. ; Copéret, Christophe ; Fedorov, Alexey ; Müller, Christoph R.</creatorcontrib><description>Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalysts reveals that the dispersion on silica increases the Ga‐normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2‐treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mainly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2‐treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga−H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga : Al ratios, give Ga−H bands at ca. 2040 and 2060 cm−1.
@GroupLese, @CoperetGroup, @eth_dmavt, @eth_dchab</description><identifier>ISSN: 0018-019X</identifier><identifier>EISSN: 1522-2675</identifier><identifier>DOI: 10.1002/hlca.202400076</identifier><language>eng</language><publisher>Zürich: Wiley Subscription Services, Inc</publisher><subject>Aluminum oxide ; Amorphous materials ; Catalysts ; Dehydrogenation ; Fourier transforms ; Gallia-alumina catalysts ; hydrogen dissociation ; Mixed oxides ; Nanoparticles ; Propane ; propane dehydrogenation ; Roasting ; Selective surfaces ; Selectivity ; Silica ; Silicon dioxide ; structural evolution ; support effect</subject><ispartof>Helvetica chimica acta, 2024-08, Vol.107 (8), p.n/a</ispartof><rights>2024 The Authors. Helvetica Chimica Acta published by Wiley-VHCA AG</rights><rights>2024. This article is published under http://creativecommons.org/licenses/by-nc-nd/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-8523-2390 ; 0000-0001-9814-6726 ; 0000-0001-7069-1861 ; 0000-0003-1936-7905 ; 0000-0003-2234-6902 ; 0000-0001-9660-3890 ; 0000-0002-8850-9041 ; 0000-0002-2011-1707</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%2Fhlca.202400076$$EPDF$$P50$$Gwiley$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fhlca.202400076$$EHTML$$P50$$Gwiley$$Hfree_for_read</linktohtml><link.rule.ids>314,776,780,1411,27903,27904,45553,45554</link.rule.ids></links><search><creatorcontrib>Castro‐Fernández, Pedro</creatorcontrib><creatorcontrib>Serykh, Alexander I.</creatorcontrib><creatorcontrib>Yarar, Melis</creatorcontrib><creatorcontrib>Mance, Deni</creatorcontrib><creatorcontrib>Abdala, Paula M.</creatorcontrib><creatorcontrib>Copéret, Christophe</creatorcontrib><creatorcontrib>Fedorov, Alexey</creatorcontrib><creatorcontrib>Müller, Christoph R.</creatorcontrib><title>The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts</title><title>Helvetica chimica acta</title><description>Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalysts reveals that the dispersion on silica increases the Ga‐normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2‐treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mainly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2‐treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga−H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga : Al ratios, give Ga−H bands at ca. 2040 and 2060 cm−1.
@GroupLese, @CoperetGroup, @eth_dmavt, @eth_dchab</description><subject>Aluminum oxide</subject><subject>Amorphous materials</subject><subject>Catalysts</subject><subject>Dehydrogenation</subject><subject>Fourier transforms</subject><subject>Gallia-alumina catalysts</subject><subject>hydrogen dissociation</subject><subject>Mixed oxides</subject><subject>Nanoparticles</subject><subject>Propane</subject><subject>propane dehydrogenation</subject><subject>Roasting</subject><subject>Selective surfaces</subject><subject>Selectivity</subject><subject>Silica</subject><subject>Silicon dioxide</subject><subject>structural evolution</subject><subject>support effect</subject><issn>0018-019X</issn><issn>1522-2675</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>24P</sourceid><sourceid>WIN</sourceid><recordid>eNo9kcFOGzEQhq0KpAbKlbOlXlqpG8b22rt7jJKWVAoEEZC4rYx3lhi5u8vaKeytj9D36FvxJHUIymk0v77_n5F-Qk4ZjBkAP1s7o8cceAoAmfpARkxynnCVyQMyAmB5Aqy4-0iOvH-MSFFANiL_btZIr9HpYNuG3mN4RmzopQ6bHqluKroK-t46Gwba1nTOX__8nVnvW2Ojo3mgKxvQv4FXfdthg3SFDk2wv7cW20TAWaOjbbXpurYPWNEv5_rbxH3lS0Ev7EsUli-2wrcAHQNmuB6qvn3AZvfUVAftBh_8J3JYa-fx5H0ek9sf32-m82SxPP85nSySjoNQiVFpbQykGWSSp5VIU4GZZDKTda6YSUVtZK0rozPFZV6AkrnOMQpVDgqxEMfk8y6369unDfpQPrabvoknSwFFyiKmRKSKHfVsHQ5l19tfuh9KBuW2jXLbRrlvo5wvppP9Jv4DLDOEIw</recordid><startdate>202408</startdate><enddate>202408</enddate><creator>Castro‐Fernández, Pedro</creator><creator>Serykh, Alexander I.</creator><creator>Yarar, Melis</creator><creator>Mance, Deni</creator><creator>Abdala, Paula M.</creator><creator>Copéret, Christophe</creator><creator>Fedorov, Alexey</creator><creator>Müller, Christoph R.</creator><general>Wiley Subscription Services, Inc</general><scope>24P</scope><scope>WIN</scope><scope>7QL</scope><scope>7QO</scope><scope>7T7</scope><scope>7U9</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>H94</scope><scope>M7N</scope><scope>P64</scope><orcidid>https://orcid.org/0000-0002-8523-2390</orcidid><orcidid>https://orcid.org/0000-0001-9814-6726</orcidid><orcidid>https://orcid.org/0000-0001-7069-1861</orcidid><orcidid>https://orcid.org/0000-0003-1936-7905</orcidid><orcidid>https://orcid.org/0000-0003-2234-6902</orcidid><orcidid>https://orcid.org/0000-0001-9660-3890</orcidid><orcidid>https://orcid.org/0000-0002-8850-9041</orcidid><orcidid>https://orcid.org/0000-0002-2011-1707</orcidid></search><sort><creationdate>202408</creationdate><title>The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts</title><author>Castro‐Fernández, Pedro ; Serykh, Alexander I. ; Yarar, Melis ; Mance, Deni ; Abdala, Paula M. ; Copéret, Christophe ; Fedorov, Alexey ; Müller, Christoph R.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p2036-c64fcc04707524d3443e751575f861c43fc5fadca7625890658a8eadcd806ee93</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Aluminum oxide</topic><topic>Amorphous materials</topic><topic>Catalysts</topic><topic>Dehydrogenation</topic><topic>Fourier transforms</topic><topic>Gallia-alumina catalysts</topic><topic>hydrogen dissociation</topic><topic>Mixed oxides</topic><topic>Nanoparticles</topic><topic>Propane</topic><topic>propane dehydrogenation</topic><topic>Roasting</topic><topic>Selective surfaces</topic><topic>Selectivity</topic><topic>Silica</topic><topic>Silicon dioxide</topic><topic>structural evolution</topic><topic>support effect</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Castro‐Fernández, Pedro</creatorcontrib><creatorcontrib>Serykh, Alexander I.</creatorcontrib><creatorcontrib>Yarar, Melis</creatorcontrib><creatorcontrib>Mance, Deni</creatorcontrib><creatorcontrib>Abdala, Paula M.</creatorcontrib><creatorcontrib>Copéret, Christophe</creatorcontrib><creatorcontrib>Fedorov, Alexey</creatorcontrib><creatorcontrib>Müller, Christoph R.</creatorcontrib><collection>Wiley Online Library Open Access</collection><collection>Wiley Online Library Free Content</collection><collection>Bacteriology Abstracts (Microbiology B)</collection><collection>Biotechnology Research Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Virology and AIDS Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>AIDS and Cancer Research Abstracts</collection><collection>Algology Mycology and Protozoology Abstracts (Microbiology C)</collection><collection>Biotechnology and BioEngineering Abstracts</collection><jtitle>Helvetica chimica acta</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Castro‐Fernández, Pedro</au><au>Serykh, Alexander I.</au><au>Yarar, Melis</au><au>Mance, Deni</au><au>Abdala, Paula M.</au><au>Copéret, Christophe</au><au>Fedorov, Alexey</au><au>Müller, Christoph R.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts</atitle><jtitle>Helvetica chimica acta</jtitle><date>2024-08</date><risdate>2024</risdate><volume>107</volume><issue>8</issue><epage>n/a</epage><issn>0018-019X</issn><eissn>1522-2675</eissn><abstract>Colloidal solutions of gallia‐alumina (Ga,Al)2O3(x:y) solid‐solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica‐supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica‐supported catalysts reveals that the dispersion on silica increases the Ga‐normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2‐treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mainly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2‐treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga−H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga : Al ratios, give Ga−H bands at ca. 2040 and 2060 cm−1.
@GroupLese, @CoperetGroup, @eth_dmavt, @eth_dchab</abstract><cop>Zürich</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/hlca.202400076</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0002-8523-2390</orcidid><orcidid>https://orcid.org/0000-0001-9814-6726</orcidid><orcidid>https://orcid.org/0000-0001-7069-1861</orcidid><orcidid>https://orcid.org/0000-0003-1936-7905</orcidid><orcidid>https://orcid.org/0000-0003-2234-6902</orcidid><orcidid>https://orcid.org/0000-0001-9660-3890</orcidid><orcidid>https://orcid.org/0000-0002-8850-9041</orcidid><orcidid>https://orcid.org/0000-0002-2011-1707</orcidid><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 0018-019X |
| ispartof | Helvetica chimica acta, 2024-08, Vol.107 (8), p.n/a |
| issn | 0018-019X 1522-2675 |
| language | eng |
| recordid | cdi_proquest_journals_3094180663 |
| source | Wiley Online Library - AutoHoldings Journals |
| subjects | Aluminum oxide Amorphous materials Catalysts Dehydrogenation Fourier transforms Gallia-alumina catalysts hydrogen dissociation Mixed oxides Nanoparticles Propane propane dehydrogenation Roasting Selective surfaces Selectivity Silica Silicon dioxide structural evolution support effect |
| title | The Relation between Nature and Stability of H2‐Dissociating Sites and Propene Selectivity in Silica‐Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-24T11%3A18%3A37IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_wiley&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=The%20Relation%20between%20Nature%20and%20Stability%20of%20H2%E2%80%90Dissociating%20Sites%20and%20Propene%20Selectivity%20in%20Silica%E2%80%90Supported%20(Ga,Al)2O3%20Mixed%20Oxide%20Propane%20Dehydrogenation%20Catalysts&rft.jtitle=Helvetica%20chimica%20acta&rft.au=Castro%E2%80%90Fern%C3%A1ndez,%20Pedro&rft.date=2024-08&rft.volume=107&rft.issue=8&rft.epage=n/a&rft.issn=0018-019X&rft.eissn=1522-2675&rft_id=info:doi/10.1002/hlca.202400076&rft_dat=%3Cproquest_wiley%3E3094180663%3C/proquest_wiley%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=3094180663&rft_id=info:pmid/&rfr_iscdi=true |