Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars
Via hydrothermal synthesis of Sn‐Al gels, mild dealumination and ion exchange, a bimetallic Sn‐Ni‐Beta catalyst was prepared which can convert glucose to methyl lactate (MLA) and methyl vinyl glycolate (MVG) in methanol at yields of 71.2 % and 10.2 %, respectively. Results from solid‐state magic‐ang...
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description | Via hydrothermal synthesis of Sn‐Al gels, mild dealumination and ion exchange, a bimetallic Sn‐Ni‐Beta catalyst was prepared which can convert glucose to methyl lactate (MLA) and methyl vinyl glycolate (MVG) in methanol at yields of 71.2 % and 10.2 %, respectively. Results from solid‐state magic‐angle spinning nuclear magnetic resonance, X‐ray photoelectron spectroscopy, transmission electron microscopy, spectroscopic analysis, probe‐temperature‐programmed desorption, and density functional theory calculations conclusively reveal that the openness of the Sn sites, such as by the formation of [(SiO)3−Sn−OH] entities, is governed by an adjacent metal cation such as Ni2+, Co2+, and Mn2+. This relies on the low structure‐defective pore channel, provided by the current synthesis scheme, and the specific silica hydroxyl anchor point is associated with the incorporation of Sn for additional and precise metal ion localization. The presence of metal cations significantly improved the catalytic performance of Sn‐Ni‐Beta for glucose isomerization and conversion to MLA of sugar compared with Sn‐Beta.
Metal ions such as Ni2+, Co2+, and Mn2+ were positioned within Sn‐Beta zeolite to form adjacent bimetallic catalytically active sites with stable open Sn sites. The Sn‐Ni‐Beta catalyst selectively converts glucose to methyl lactate and methyl vinyl glycolate in methanol in high yields of 71.2 % and 10.2 %, respectively. |
doi_str_mv | 10.1002/anie.202215737 |
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Metal ions such as Ni2+, Co2+, and Mn2+ were positioned within Sn‐Beta zeolite to form adjacent bimetallic catalytically active sites with stable open Sn sites. The Sn‐Ni‐Beta catalyst selectively converts glucose to methyl lactate and methyl vinyl glycolate in methanol in high yields of 71.2 % and 10.2 %, respectively.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202215737</identifier><identifier>PMID: 36478093</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Aluminum ; Bimetals ; Carbohydrate Conversion ; Carbon dioxide ; Catalysts ; Catalytic converters ; Cations ; Cobalt ; Conversion ; Density functional theory ; Gels ; Glucose ; Heterogeneous Catalysis ; Ion exchange ; Ions ; Isomerization ; Lactic acid ; Lewis Acid ; Localization ; Metal ions ; Methyl Lactate ; NMR ; Nuclear magnetic resonance ; Photoelectron spectroscopy ; Photoelectrons ; Silica ; Sn-Beta Zeolite ; Sugar ; Transmission electron microscopy ; Zeolites</subject><ispartof>Angewandte Chemie International Edition, 2023-02, Vol.62 (6), p.e202215737-n/a</ispartof><rights>2022 Wiley‐VCH GmbH</rights><rights>2022 Wiley-VCH GmbH.</rights><rights>2023 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3737-c553ed719e9806258ffbb14f0f0edd3c5c5588ab4114c145a930deec329c9d803</citedby><cites>FETCH-LOGICAL-c3737-c553ed719e9806258ffbb14f0f0edd3c5c5588ab4114c145a930deec329c9d803</cites><orcidid>0000-0002-4957-7930 ; 0000-0002-1950-006X ; 0000-0003-1124-7634 ; 0000-0001-9657-1710 ; 0000-0003-0311-8744</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.202215737$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202215737$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1416,27923,27924,45573,45574</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36478093$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Sun, Pengyao</creatorcontrib><creatorcontrib>Liu, Chong</creatorcontrib><creatorcontrib>Wang, Haiyong</creatorcontrib><creatorcontrib>Liao, Yuhe</creatorcontrib><creatorcontrib>Li, Xuning</creatorcontrib><creatorcontrib>Liu, Qiying</creatorcontrib><creatorcontrib>Sels, Bert F.</creatorcontrib><creatorcontrib>Wang, Chenguang</creatorcontrib><title>Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Via hydrothermal synthesis of Sn‐Al gels, mild dealumination and ion exchange, a bimetallic Sn‐Ni‐Beta catalyst was prepared which can convert glucose to methyl lactate (MLA) and methyl vinyl glycolate (MVG) in methanol at yields of 71.2 % and 10.2 %, respectively. Results from solid‐state magic‐angle spinning nuclear magnetic resonance, X‐ray photoelectron spectroscopy, transmission electron microscopy, spectroscopic analysis, probe‐temperature‐programmed desorption, and density functional theory calculations conclusively reveal that the openness of the Sn sites, such as by the formation of [(SiO)3−Sn−OH] entities, is governed by an adjacent metal cation such as Ni2+, Co2+, and Mn2+. This relies on the low structure‐defective pore channel, provided by the current synthesis scheme, and the specific silica hydroxyl anchor point is associated with the incorporation of Sn for additional and precise metal ion localization. The presence of metal cations significantly improved the catalytic performance of Sn‐Ni‐Beta for glucose isomerization and conversion to MLA of sugar compared with Sn‐Beta.
Metal ions such as Ni2+, Co2+, and Mn2+ were positioned within Sn‐Beta zeolite to form adjacent bimetallic catalytically active sites with stable open Sn sites. The Sn‐Ni‐Beta catalyst selectively converts glucose to methyl lactate and methyl vinyl glycolate in methanol in high yields of 71.2 % and 10.2 %, respectively.</description><subject>Aluminum</subject><subject>Bimetals</subject><subject>Carbohydrate Conversion</subject><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>Catalytic converters</subject><subject>Cations</subject><subject>Cobalt</subject><subject>Conversion</subject><subject>Density functional theory</subject><subject>Gels</subject><subject>Glucose</subject><subject>Heterogeneous Catalysis</subject><subject>Ion exchange</subject><subject>Ions</subject><subject>Isomerization</subject><subject>Lactic acid</subject><subject>Lewis Acid</subject><subject>Localization</subject><subject>Metal ions</subject><subject>Methyl Lactate</subject><subject>NMR</subject><subject>Nuclear magnetic resonance</subject><subject>Photoelectron spectroscopy</subject><subject>Photoelectrons</subject><subject>Silica</subject><subject>Sn-Beta Zeolite</subject><subject>Sugar</subject><subject>Transmission electron microscopy</subject><subject>Zeolites</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkUtP6zAQhS0EAi6wZYkssWGT4kfcxEuoyqUSL1HYsIkcZ4KM0rjYCaj319-JykNiw8pHo2-OPOcQcsjZiDMmTk3rYCSYEFxlMtsgu1wJnsgsk5uoUymTLFd8h_yJ8QX5PGfjbbIjx2mWMy13yeu96ZxvTUPvfHSDdO0z9TW9hg6HM99G2nk670zpGvcP6O0SWvrgWjp3HUSK4hxJ-gS-wQGtfaATg6urzlk68e0bhIiug-W8fzYh7pOt2jQRDj7ePfJ4MX2YXCZXt39nk7OrxEq8JLFKSagyrkHjn4XK67oseVqzmkFVSasQyHNTppynlqfKaMkqACuFtrrKmdwjJ2vfZfCvPcSuWLhooWlMC76PhciUlHysRYro8Q_0xfcBQxmoscbQZKqRGq0pG3yMAepiGdzChFXBWTGUUQxlFF9l4MLRh21fLqD6wj_TR0CvgXfXwOoXu-LsZjb9Nv8Pf0-VvQ</recordid><startdate>20230201</startdate><enddate>20230201</enddate><creator>Sun, Pengyao</creator><creator>Liu, Chong</creator><creator>Wang, Haiyong</creator><creator>Liao, Yuhe</creator><creator>Li, Xuning</creator><creator>Liu, Qiying</creator><creator>Sels, Bert F.</creator><creator>Wang, Chenguang</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-4957-7930</orcidid><orcidid>https://orcid.org/0000-0002-1950-006X</orcidid><orcidid>https://orcid.org/0000-0003-1124-7634</orcidid><orcidid>https://orcid.org/0000-0001-9657-1710</orcidid><orcidid>https://orcid.org/0000-0003-0311-8744</orcidid></search><sort><creationdate>20230201</creationdate><title>Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars</title><author>Sun, Pengyao ; Liu, Chong ; Wang, Haiyong ; Liao, Yuhe ; Li, Xuning ; Liu, Qiying ; Sels, Bert F. ; Wang, Chenguang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3737-c553ed719e9806258ffbb14f0f0edd3c5c5588ab4114c145a930deec329c9d803</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Aluminum</topic><topic>Bimetals</topic><topic>Carbohydrate Conversion</topic><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>Catalytic converters</topic><topic>Cations</topic><topic>Cobalt</topic><topic>Conversion</topic><topic>Density functional theory</topic><topic>Gels</topic><topic>Glucose</topic><topic>Heterogeneous Catalysis</topic><topic>Ion exchange</topic><topic>Ions</topic><topic>Isomerization</topic><topic>Lactic acid</topic><topic>Lewis Acid</topic><topic>Localization</topic><topic>Metal ions</topic><topic>Methyl Lactate</topic><topic>NMR</topic><topic>Nuclear magnetic resonance</topic><topic>Photoelectron spectroscopy</topic><topic>Photoelectrons</topic><topic>Silica</topic><topic>Sn-Beta Zeolite</topic><topic>Sugar</topic><topic>Transmission electron microscopy</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Sun, Pengyao</creatorcontrib><creatorcontrib>Liu, Chong</creatorcontrib><creatorcontrib>Wang, Haiyong</creatorcontrib><creatorcontrib>Liao, Yuhe</creatorcontrib><creatorcontrib>Li, Xuning</creatorcontrib><creatorcontrib>Liu, Qiying</creatorcontrib><creatorcontrib>Sels, Bert F.</creatorcontrib><creatorcontrib>Wang, Chenguang</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Sun, Pengyao</au><au>Liu, Chong</au><au>Wang, Haiyong</au><au>Liao, Yuhe</au><au>Li, Xuning</au><au>Liu, Qiying</au><au>Sels, Bert F.</au><au>Wang, Chenguang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2023-02-01</date><risdate>2023</risdate><volume>62</volume><issue>6</issue><spage>e202215737</spage><epage>n/a</epage><pages>e202215737-n/a</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Via hydrothermal synthesis of Sn‐Al gels, mild dealumination and ion exchange, a bimetallic Sn‐Ni‐Beta catalyst was prepared which can convert glucose to methyl lactate (MLA) and methyl vinyl glycolate (MVG) in methanol at yields of 71.2 % and 10.2 %, respectively. Results from solid‐state magic‐angle spinning nuclear magnetic resonance, X‐ray photoelectron spectroscopy, transmission electron microscopy, spectroscopic analysis, probe‐temperature‐programmed desorption, and density functional theory calculations conclusively reveal that the openness of the Sn sites, such as by the formation of [(SiO)3−Sn−OH] entities, is governed by an adjacent metal cation such as Ni2+, Co2+, and Mn2+. This relies on the low structure‐defective pore channel, provided by the current synthesis scheme, and the specific silica hydroxyl anchor point is associated with the incorporation of Sn for additional and precise metal ion localization. The presence of metal cations significantly improved the catalytic performance of Sn‐Ni‐Beta for glucose isomerization and conversion to MLA of sugar compared with Sn‐Beta.
Metal ions such as Ni2+, Co2+, and Mn2+ were positioned within Sn‐Beta zeolite to form adjacent bimetallic catalytically active sites with stable open Sn sites. The Sn‐Ni‐Beta catalyst selectively converts glucose to methyl lactate and methyl vinyl glycolate in methanol in high yields of 71.2 % and 10.2 %, respectively.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>36478093</pmid><doi>10.1002/anie.202215737</doi><tpages>8</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-4957-7930</orcidid><orcidid>https://orcid.org/0000-0002-1950-006X</orcidid><orcidid>https://orcid.org/0000-0003-1124-7634</orcidid><orcidid>https://orcid.org/0000-0001-9657-1710</orcidid><orcidid>https://orcid.org/0000-0003-0311-8744</orcidid></addata></record> |
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subjects | Aluminum Bimetals Carbohydrate Conversion Carbon dioxide Catalysts Catalytic converters Cations Cobalt Conversion Density functional theory Gels Glucose Heterogeneous Catalysis Ion exchange Ions Isomerization Lactic acid Lewis Acid Localization Metal ions Methyl Lactate NMR Nuclear magnetic resonance Photoelectron spectroscopy Photoelectrons Silica Sn-Beta Zeolite Sugar Transmission electron microscopy Zeolites |
title | Rational Positioning of Metal Ions to Stabilize Open Tin Sites in Beta Zeolite for Catalytic Conversion of Sugars |
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