Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina
Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). R...
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Veröffentlicht in: | The journal of physical chemistry letters 2021-03, Vol.12 (10), p.2536-2546 |
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creator | Zhao, Yutong Wang, Lizhuo Kochubei, Alena Yang, Wenjie Xu, Haimei Luo, Yongming Baiker, Alfons Huang, Jun Wang, Zichun Jiang, Yijiao |
description | Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of CO groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2. |
doi_str_mv | 10.1021/acs.jpclett.1c00139 |
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Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of CO groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.</description><identifier>ISSN: 1948-7185</identifier><identifier>EISSN: 1948-7185</identifier><identifier>DOI: 10.1021/acs.jpclett.1c00139</identifier><identifier>PMID: 33683898</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Physical Insights into Chemistry, Catalysis, and Interfaces</subject><ispartof>The journal of physical chemistry letters, 2021-03, Vol.12 (10), p.2536-2546</ispartof><rights>2021 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a345t-b0d14242e11ae83f298d7231c64c4f51f81a47aaf88921ac6f5029c3dbdf6ae73</citedby><cites>FETCH-LOGICAL-a345t-b0d14242e11ae83f298d7231c64c4f51f81a47aaf88921ac6f5029c3dbdf6ae73</cites><orcidid>0000-0003-1408-464X ; 0000-0001-8704-605X ; 0000-0002-9930-261X ; 0000-0002-6191-9825 ; 0000-0002-4280-2787</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/acs.jpclett.1c00139$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.jpclett.1c00139$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/33683898$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhao, Yutong</creatorcontrib><creatorcontrib>Wang, Lizhuo</creatorcontrib><creatorcontrib>Kochubei, Alena</creatorcontrib><creatorcontrib>Yang, Wenjie</creatorcontrib><creatorcontrib>Xu, Haimei</creatorcontrib><creatorcontrib>Luo, Yongming</creatorcontrib><creatorcontrib>Baiker, Alfons</creatorcontrib><creatorcontrib>Huang, Jun</creatorcontrib><creatorcontrib>Wang, Zichun</creatorcontrib><creatorcontrib>Jiang, Yijiao</creatorcontrib><title>Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina</title><title>The journal of physical chemistry letters</title><addtitle>J. Phys. Chem. Lett</addtitle><description>Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of CO groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.</description><subject>Physical Insights into Chemistry, Catalysis, and Interfaces</subject><issn>1948-7185</issn><issn>1948-7185</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kEtOwzAQhi0EolA4ARLKkk1bP_Kwl1VFoVIlKhXWkeMHpErsYDuL7rgDN-QkGBoQK1Zjj75_7PkAuEJwiiBGMy78dNeJRoUwRQJCRNgROEMspZMC0ez4z3kEzr3fQZgzSItTMCIkp4QyegbM0rqWh9qahBuZrK04XKxONiHZ1ua5UbEE5ZOVkb1QMqn2yUaZwIW1TtaGh9ibN8m2U6KOWAzPW-u6F9v7mGxqwT_e3udN30b2Apxo3nh1OdQxeFrePi7uJ-uHu9Vivp5wkmZhUkGJUpxihRBXlGjMqCwwQSJPRaozpCniacG5ppRhxEWuM4iZILKSOueqIGNwc5jbOfvaKx_KtvZCNQ03Kv6rxCljUQBmWUTJARXOeu-ULjtXt9ztSwTLL9FlFF0OostBdExdDw_0Vavkb-bHbARmB-A7bXtn4r7_jvwE6T6OgA</recordid><startdate>20210318</startdate><enddate>20210318</enddate><creator>Zhao, Yutong</creator><creator>Wang, Lizhuo</creator><creator>Kochubei, Alena</creator><creator>Yang, Wenjie</creator><creator>Xu, Haimei</creator><creator>Luo, Yongming</creator><creator>Baiker, Alfons</creator><creator>Huang, Jun</creator><creator>Wang, Zichun</creator><creator>Jiang, Yijiao</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0003-1408-464X</orcidid><orcidid>https://orcid.org/0000-0001-8704-605X</orcidid><orcidid>https://orcid.org/0000-0002-9930-261X</orcidid><orcidid>https://orcid.org/0000-0002-6191-9825</orcidid><orcidid>https://orcid.org/0000-0002-4280-2787</orcidid></search><sort><creationdate>20210318</creationdate><title>Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina</title><author>Zhao, Yutong ; Wang, Lizhuo ; Kochubei, Alena ; Yang, Wenjie ; Xu, Haimei ; Luo, Yongming ; Baiker, Alfons ; Huang, Jun ; Wang, Zichun ; Jiang, Yijiao</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a345t-b0d14242e11ae83f298d7231c64c4f51f81a47aaf88921ac6f5029c3dbdf6ae73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Physical Insights into Chemistry, Catalysis, and Interfaces</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhao, Yutong</creatorcontrib><creatorcontrib>Wang, Lizhuo</creatorcontrib><creatorcontrib>Kochubei, Alena</creatorcontrib><creatorcontrib>Yang, Wenjie</creatorcontrib><creatorcontrib>Xu, Haimei</creatorcontrib><creatorcontrib>Luo, Yongming</creatorcontrib><creatorcontrib>Baiker, Alfons</creatorcontrib><creatorcontrib>Huang, Jun</creatorcontrib><creatorcontrib>Wang, Zichun</creatorcontrib><creatorcontrib>Jiang, Yijiao</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>The journal of physical chemistry letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhao, Yutong</au><au>Wang, Lizhuo</au><au>Kochubei, Alena</au><au>Yang, Wenjie</au><au>Xu, Haimei</au><au>Luo, Yongming</au><au>Baiker, Alfons</au><au>Huang, Jun</au><au>Wang, Zichun</au><au>Jiang, Yijiao</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina</atitle><jtitle>The journal of physical chemistry letters</jtitle><addtitle>J. Phys. Chem. Lett</addtitle><date>2021-03-18</date><risdate>2021</risdate><volume>12</volume><issue>10</issue><spage>2536</spage><epage>2546</epage><pages>2536-2546</pages><issn>1948-7185</issn><eissn>1948-7185</eissn><abstract>Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of CO groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>33683898</pmid><doi>10.1021/acs.jpclett.1c00139</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0003-1408-464X</orcidid><orcidid>https://orcid.org/0000-0001-8704-605X</orcidid><orcidid>https://orcid.org/0000-0002-9930-261X</orcidid><orcidid>https://orcid.org/0000-0002-6191-9825</orcidid><orcidid>https://orcid.org/0000-0002-4280-2787</orcidid></addata></record> |
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title | Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina |
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