Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes
The production of conjugated C4–C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)‐atomically doped mesoporous silica, denoted as AlNb‐MCM‐41, which affords quantitative conversion of 2‐met...
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| Veröffentlicht in: | Angewandte Chemie 2022-12, Vol.134 (51), p.e202212164-n/a |
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| creator | Fan, Mengtian Xu, Shaojun An, Bing Sheveleva, Alena M. Betts, Alexander Hurd, Joseph Zhu, Zhaodong He, Meng Iuga, Dinu Lin, Longfei Kang, Xinchen Parlett, Christopher M. A. Tuna, Floriana McInnes, Eric J. L. Keenan, Luke L. Lee, Daniel Attfield, Martin P. Yang, Sihai |
| description | The production of conjugated C4–C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)‐atomically doped mesoporous silica, denoted as AlNb‐MCM‐41, which affords quantitative conversion of 2‐methyltetrahydrofuran (2‐MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of AlIII and NbV sites into the framework of AlNb‐MCM‐41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X‐ray absorption, diffuse reflectance infrared and solid‐state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2‐MTHF over AlNb‐MCM‐41. Specifically, the atomically‐dispersed NbV sites play an important role in binding 2‐MTHF to drive the conversion. Overall, this study highlights the potential of hetero‐atomic mesoporous solids for the manufacture of renewable materials.
The highly selective conversion of biomass‐derived 2‐methyltetrahydrofuran (2‐MTHF) into pentadienes has been achieved over an aluminum and niobium bimetallic atomically doped MCM‐41. The NbV sites enhance the catalytic performance by binding 2‐MTHF. |
| doi_str_mv | 10.1002/ange.202212164 |
| format | Article |
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The highly selective conversion of biomass‐derived 2‐methyltetrahydrofuran (2‐MTHF) into pentadienes has been achieved over an aluminum and niobium bimetallic atomically doped MCM‐41. The NbV sites enhance the catalytic performance by binding 2‐MTHF.</description><identifier>ISSN: 0044-8249</identifier><identifier>EISSN: 1521-3757</identifier><identifier>DOI: 10.1002/ange.202212164</identifier><identifier>PMID: 38505214</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>2-Methyltetrahydrofuran ; Aluminum ; Bimetals ; Biomass ; Chemical synthesis ; Chemistry ; Cleavage of C−O Bond ; Conversion ; Dienes ; Forschungsartikel ; Liquid fuels ; Magnetic resonance spectroscopy ; Niobium ; Niobium Sites ; NMR ; NMR spectroscopy ; Nuclear magnetic resonance ; Pentadienes ; Polymers ; Renewable resources ; Selectivity ; Silica</subject><ispartof>Angewandte Chemie, 2022-12, Vol.134 (51), p.e202212164-n/a</ispartof><rights>2022 The Authors. Angewandte Chemie published by Wiley-VCH GmbH</rights><rights>2022 The Authors. Angewandte Chemie published by Wiley-VCH GmbH.</rights><rights>2022. This article is published under http://creativecommons.org/licenses/by/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><cites>FETCH-LOGICAL-c2694-2cd53f0c04c01fd1ae887aa691ef08fd04dde7a1ae8eed20fac8be98799ddbf23</cites><orcidid>0000-0002-1111-9272 ; 0000-0001-6508-1751</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%2Fange.202212164$$EPDF$$P50$$Gwiley$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fange.202212164$$EHTML$$P50$$Gwiley$$Hfree_for_read</linktohtml><link.rule.ids>230,314,776,780,881,1411,27901,27902,45550,45551</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38505214$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Fan, Mengtian</creatorcontrib><creatorcontrib>Xu, Shaojun</creatorcontrib><creatorcontrib>An, Bing</creatorcontrib><creatorcontrib>Sheveleva, Alena M.</creatorcontrib><creatorcontrib>Betts, Alexander</creatorcontrib><creatorcontrib>Hurd, Joseph</creatorcontrib><creatorcontrib>Zhu, Zhaodong</creatorcontrib><creatorcontrib>He, Meng</creatorcontrib><creatorcontrib>Iuga, Dinu</creatorcontrib><creatorcontrib>Lin, Longfei</creatorcontrib><creatorcontrib>Kang, Xinchen</creatorcontrib><creatorcontrib>Parlett, Christopher M. A.</creatorcontrib><creatorcontrib>Tuna, Floriana</creatorcontrib><creatorcontrib>McInnes, Eric J. L.</creatorcontrib><creatorcontrib>Keenan, Luke L.</creatorcontrib><creatorcontrib>Lee, Daniel</creatorcontrib><creatorcontrib>Attfield, Martin P.</creatorcontrib><creatorcontrib>Yang, Sihai</creatorcontrib><title>Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes</title><title>Angewandte Chemie</title><addtitle>Angew Chem Weinheim Bergstr Ger</addtitle><description>The production of conjugated C4–C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)‐atomically doped mesoporous silica, denoted as AlNb‐MCM‐41, which affords quantitative conversion of 2‐methyltetrahydrofuran (2‐MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of AlIII and NbV sites into the framework of AlNb‐MCM‐41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X‐ray absorption, diffuse reflectance infrared and solid‐state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2‐MTHF over AlNb‐MCM‐41. Specifically, the atomically‐dispersed NbV sites play an important role in binding 2‐MTHF to drive the conversion. Overall, this study highlights the potential of hetero‐atomic mesoporous solids for the manufacture of renewable materials.
The highly selective conversion of biomass‐derived 2‐methyltetrahydrofuran (2‐MTHF) into pentadienes has been achieved over an aluminum and niobium bimetallic atomically doped MCM‐41. The NbV sites enhance the catalytic performance by binding 2‐MTHF.</description><subject>2-Methyltetrahydrofuran</subject><subject>Aluminum</subject><subject>Bimetals</subject><subject>Biomass</subject><subject>Chemical synthesis</subject><subject>Chemistry</subject><subject>Cleavage of C−O Bond</subject><subject>Conversion</subject><subject>Dienes</subject><subject>Forschungsartikel</subject><subject>Liquid fuels</subject><subject>Magnetic resonance spectroscopy</subject><subject>Niobium</subject><subject>Niobium Sites</subject><subject>NMR</subject><subject>NMR spectroscopy</subject><subject>Nuclear magnetic resonance</subject><subject>Pentadienes</subject><subject>Polymers</subject><subject>Renewable resources</subject><subject>Selectivity</subject><subject>Silica</subject><issn>0044-8249</issn><issn>1521-3757</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid>24P</sourceid><recordid>eNqFkb9vEzEUx08IRNPCyogssbBcsH2-83lCaQgFqSkMMFuO_dy4urODfReUjbkTfyN_CU5Two-Fyc_25330nr5F8YzgKcGYvlL-GqYUU0ooadiDYkJqSsqK1_xhMcGYsbKlTJwUpyndYIwbysXj4qRqa5w5Niluz10Pg-o6p9GsG3vnx_7Ht-9IeYOuXFi5u-ubsAGDlvNlrhlBNkS0sNZpB35A8-C3EJMLHgWLzl3oVUr7Johum9torpcwrHfdAENU652JwY5ReTQE9DEblMkeSE-KR1Z1CZ7en2fF57eLT_N35eWHi_fz2WWpaSNYSbWpK4s1ZhoTa4iCtuVKNYKAxa01mBkDXO3fAQzFVul2BaLlQhizsrQ6K14fvJtx1YPReYKoOrmJrldxJ4Ny8u8f79byOmwlwYI1teDZ8PLeEMOXEdIge5c0dJ3yEMYkqeCU46Zpqoy--Ae9CWP0eT9JeV3RmuE74fRA6RhSimCP0xAs9znLfc7ymHNueP7nDkf8V7AZEAfgq-tg9x-dnF1dLH7LfwJQX7zb</recordid><startdate>20221219</startdate><enddate>20221219</enddate><creator>Fan, Mengtian</creator><creator>Xu, Shaojun</creator><creator>An, Bing</creator><creator>Sheveleva, Alena M.</creator><creator>Betts, Alexander</creator><creator>Hurd, Joseph</creator><creator>Zhu, Zhaodong</creator><creator>He, Meng</creator><creator>Iuga, Dinu</creator><creator>Lin, Longfei</creator><creator>Kang, Xinchen</creator><creator>Parlett, Christopher M. A.</creator><creator>Tuna, Floriana</creator><creator>McInnes, Eric J. L.</creator><creator>Keenan, Luke L.</creator><creator>Lee, Daniel</creator><creator>Attfield, Martin P.</creator><creator>Yang, Sihai</creator><general>Wiley Subscription Services, Inc</general><general>John Wiley and Sons Inc</general><scope>24P</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-1111-9272</orcidid><orcidid>https://orcid.org/0000-0001-6508-1751</orcidid></search><sort><creationdate>20221219</creationdate><title>Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes</title><author>Fan, Mengtian ; Xu, Shaojun ; An, Bing ; Sheveleva, Alena M. ; Betts, Alexander ; Hurd, Joseph ; Zhu, Zhaodong ; He, Meng ; Iuga, Dinu ; Lin, Longfei ; Kang, Xinchen ; Parlett, Christopher M. 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A.</au><au>Tuna, Floriana</au><au>McInnes, Eric J. L.</au><au>Keenan, Luke L.</au><au>Lee, Daniel</au><au>Attfield, Martin P.</au><au>Yang, Sihai</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes</atitle><jtitle>Angewandte Chemie</jtitle><addtitle>Angew Chem Weinheim Bergstr Ger</addtitle><date>2022-12-19</date><risdate>2022</risdate><volume>134</volume><issue>51</issue><spage>e202212164</spage><epage>n/a</epage><pages>e202212164-n/a</pages><issn>0044-8249</issn><eissn>1521-3757</eissn><abstract>The production of conjugated C4–C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)‐atomically doped mesoporous silica, denoted as AlNb‐MCM‐41, which affords quantitative conversion of 2‐methyltetrahydrofuran (2‐MTHF) to pentadienes with a high selectivity of 91 %. The incorporation of AlIII and NbV sites into the framework of AlNb‐MCM‐41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X‐ray absorption, diffuse reflectance infrared and solid‐state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2‐MTHF over AlNb‐MCM‐41. Specifically, the atomically‐dispersed NbV sites play an important role in binding 2‐MTHF to drive the conversion. Overall, this study highlights the potential of hetero‐atomic mesoporous solids for the manufacture of renewable materials.
The highly selective conversion of biomass‐derived 2‐methyltetrahydrofuran (2‐MTHF) into pentadienes has been achieved over an aluminum and niobium bimetallic atomically doped MCM‐41. The NbV sites enhance the catalytic performance by binding 2‐MTHF.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>38505214</pmid><doi>10.1002/ange.202212164</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0002-1111-9272</orcidid><orcidid>https://orcid.org/0000-0001-6508-1751</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | 2-Methyltetrahydrofuran Aluminum Bimetals Biomass Chemical synthesis Chemistry Cleavage of C−O Bond Conversion Dienes Forschungsartikel Liquid fuels Magnetic resonance spectroscopy Niobium Niobium Sites NMR NMR spectroscopy Nuclear magnetic resonance Pentadienes Polymers Renewable resources Selectivity Silica |
| title | Bimetallic Aluminum‐ and Niobium‐Doped MCM‐41 for Efficient Conversion of Biomass‐Derived 2‐Methyltetrahydrofuran to Pentadienes |
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