Aqueous-phase tandem catalytic conversion of xylose to furfuryl alcohol over [Al]-SBA-15 molecular sieves
Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis. Incorporation of Al as a heteroatom at different Si/Al ratios was used to tune their surface properties and the catalysts were characterized by SAXRD, ICP-OES, FE-SEM, TEM, FTIR, 29 Si a...
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| Veröffentlicht in: | Catalysis science & technology 2019, Vol.9 (19), p.535-5358 |
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| creator | Perez, Rafael F Albuquerque, Elise M Borges, Luiz E. P Hardacre, Christopher Fraga, Marco A |
| description | Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis. Incorporation of Al as a heteroatom at different Si/Al ratios was used to tune their surface properties and the catalysts were characterized by SAXRD, ICP-OES, FE-SEM, TEM, FTIR,
29
Si and
27
Al CP-NMR, pyridine adsorption and titration in water. Reactivity towards direct conversion of xylose to furfuryl alcohol was systematically investigated. Brønsted acid sites, generated by introducing Al into the siliceous SBA-15 framework, were found to be active for the pentose dehydration reaction, whilst the Lewis acid sites promoted the transfer hydrogenation of the adsorbed furfural intermediate to furfuryl alcohol. A remarkably high selectivity to furfuryl alcohol (90-95%) was observed using the mesoporous catalysts and it was dependent on the Al concentration in the siliceous framework. The vicinity of Brønsted and Lewis acid sites is suggested to be of major concern since the adsorbed furfural species is proposed to be reduced to furfuryl alcohol without being desorbed. The [Al]-SBA-15 molecular sieves were shown to be chemically and structurally stable demonstrating good recyclability in the aqueous-phase upgrading of xylose.
Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis. |
| doi_str_mv | 10.1039/c9cy01235d |
| format | Article |
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29
Si and
27
Al CP-NMR, pyridine adsorption and titration in water. Reactivity towards direct conversion of xylose to furfuryl alcohol was systematically investigated. Brønsted acid sites, generated by introducing Al into the siliceous SBA-15 framework, were found to be active for the pentose dehydration reaction, whilst the Lewis acid sites promoted the transfer hydrogenation of the adsorbed furfural intermediate to furfuryl alcohol. A remarkably high selectivity to furfuryl alcohol (90-95%) was observed using the mesoporous catalysts and it was dependent on the Al concentration in the siliceous framework. The vicinity of Brønsted and Lewis acid sites is suggested to be of major concern since the adsorbed furfural species is proposed to be reduced to furfuryl alcohol without being desorbed. The [Al]-SBA-15 molecular sieves were shown to be chemically and structurally stable demonstrating good recyclability in the aqueous-phase upgrading of xylose.
Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/c9cy01235d</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Alcohol ; Aluminum ; Catalysts ; Catalytic converters ; Dehydration ; Direct conversion ; Furfural ; Furfuryl alcohol ; Lewis acid ; Molecular sieves ; NMR ; Nuclear magnetic resonance ; Organic chemistry ; Pentose ; Recyclability ; Selectivity ; Silicon ; Surface properties ; Titration ; Xylose</subject><ispartof>Catalysis science & technology, 2019, Vol.9 (19), p.535-5358</ispartof><rights>Copyright Royal Society of Chemistry 2019</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c295d-9fb0e5d57d77bac1afacd788a9e299c53ef80482643ffacb52d58d2ac40637a83</citedby><cites>FETCH-LOGICAL-c295d-9fb0e5d57d77bac1afacd788a9e299c53ef80482643ffacb52d58d2ac40637a83</cites><orcidid>0000-0003-1280-608X ; 0000-0001-7256-6765 ; 0000-0002-9768-8360</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,4010,27900,27901,27902</link.rule.ids></links><search><creatorcontrib>Perez, Rafael F</creatorcontrib><creatorcontrib>Albuquerque, Elise M</creatorcontrib><creatorcontrib>Borges, Luiz E. P</creatorcontrib><creatorcontrib>Hardacre, Christopher</creatorcontrib><creatorcontrib>Fraga, Marco A</creatorcontrib><title>Aqueous-phase tandem catalytic conversion of xylose to furfuryl alcohol over [Al]-SBA-15 molecular sieves</title><title>Catalysis science & technology</title><description>Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis. Incorporation of Al as a heteroatom at different Si/Al ratios was used to tune their surface properties and the catalysts were characterized by SAXRD, ICP-OES, FE-SEM, TEM, FTIR,
29
Si and
27
Al CP-NMR, pyridine adsorption and titration in water. Reactivity towards direct conversion of xylose to furfuryl alcohol was systematically investigated. Brønsted acid sites, generated by introducing Al into the siliceous SBA-15 framework, were found to be active for the pentose dehydration reaction, whilst the Lewis acid sites promoted the transfer hydrogenation of the adsorbed furfural intermediate to furfuryl alcohol. A remarkably high selectivity to furfuryl alcohol (90-95%) was observed using the mesoporous catalysts and it was dependent on the Al concentration in the siliceous framework. The vicinity of Brønsted and Lewis acid sites is suggested to be of major concern since the adsorbed furfural species is proposed to be reduced to furfuryl alcohol without being desorbed. The [Al]-SBA-15 molecular sieves were shown to be chemically and structurally stable demonstrating good recyclability in the aqueous-phase upgrading of xylose.
Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis.</description><subject>Alcohol</subject><subject>Aluminum</subject><subject>Catalysts</subject><subject>Catalytic converters</subject><subject>Dehydration</subject><subject>Direct conversion</subject><subject>Furfural</subject><subject>Furfuryl alcohol</subject><subject>Lewis acid</subject><subject>Molecular sieves</subject><subject>NMR</subject><subject>Nuclear magnetic resonance</subject><subject>Organic chemistry</subject><subject>Pentose</subject><subject>Recyclability</subject><subject>Selectivity</subject><subject>Silicon</subject><subject>Surface properties</subject><subject>Titration</subject><subject>Xylose</subject><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNp9kMtLxDAQxoMouKx78S5EvAnVPJq2Odb6hAUP6kFESjYPtku2qUm72P_erCt6cxiYge_HfMwHwDFGFxhRfim5HBEmlKk9MCEoTZM0z_D-787oIZiFsEKxUo5RQSagKT8G7YaQdEsRNOxFq_QaStELO_aNhNK1G-1D41roDPwcrdtSDprBxx4tFFa6pbPQRQy-lfY9eboqE8zg2lktBys8DI3e6HAEDoywQc9-5hS83N48V_fJ_PHuoSrniSScqYSbBdJMsVzl-UJILIyQKi8KwTXhXDKqTYHSgmQpNVFaMKJYoYiQKcpoLgo6BWe7u5138bfQ1ys3-DZa1oQixFLCcBap8x0lvQvBa1N3vlkLP9YY1ds064pXr99pXkf4ZAf7IH-5v7SjfvqfXnfK0C9eVH2b</recordid><startdate>2019</startdate><enddate>2019</enddate><creator>Perez, Rafael F</creator><creator>Albuquerque, Elise M</creator><creator>Borges, Luiz E. P</creator><creator>Hardacre, Christopher</creator><creator>Fraga, Marco A</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><orcidid>https://orcid.org/0000-0003-1280-608X</orcidid><orcidid>https://orcid.org/0000-0001-7256-6765</orcidid><orcidid>https://orcid.org/0000-0002-9768-8360</orcidid></search><sort><creationdate>2019</creationdate><title>Aqueous-phase tandem catalytic conversion of xylose to furfuryl alcohol over [Al]-SBA-15 molecular sieves</title><author>Perez, Rafael F ; Albuquerque, Elise M ; Borges, Luiz E. P ; Hardacre, Christopher ; Fraga, Marco A</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c295d-9fb0e5d57d77bac1afacd788a9e299c53ef80482643ffacb52d58d2ac40637a83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Alcohol</topic><topic>Aluminum</topic><topic>Catalysts</topic><topic>Catalytic converters</topic><topic>Dehydration</topic><topic>Direct conversion</topic><topic>Furfural</topic><topic>Furfuryl alcohol</topic><topic>Lewis acid</topic><topic>Molecular sieves</topic><topic>NMR</topic><topic>Nuclear magnetic resonance</topic><topic>Organic chemistry</topic><topic>Pentose</topic><topic>Recyclability</topic><topic>Selectivity</topic><topic>Silicon</topic><topic>Surface properties</topic><topic>Titration</topic><topic>Xylose</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Perez, Rafael F</creatorcontrib><creatorcontrib>Albuquerque, Elise M</creatorcontrib><creatorcontrib>Borges, Luiz E. P</creatorcontrib><creatorcontrib>Hardacre, Christopher</creatorcontrib><creatorcontrib>Fraga, Marco A</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Perez, Rafael F</au><au>Albuquerque, Elise M</au><au>Borges, Luiz E. P</au><au>Hardacre, Christopher</au><au>Fraga, Marco A</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Aqueous-phase tandem catalytic conversion of xylose to furfuryl alcohol over [Al]-SBA-15 molecular sieves</atitle><jtitle>Catalysis science & technology</jtitle><date>2019</date><risdate>2019</risdate><volume>9</volume><issue>19</issue><spage>535</spage><epage>5358</epage><pages>535-5358</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis. Incorporation of Al as a heteroatom at different Si/Al ratios was used to tune their surface properties and the catalysts were characterized by SAXRD, ICP-OES, FE-SEM, TEM, FTIR,
29
Si and
27
Al CP-NMR, pyridine adsorption and titration in water. Reactivity towards direct conversion of xylose to furfuryl alcohol was systematically investigated. Brønsted acid sites, generated by introducing Al into the siliceous SBA-15 framework, were found to be active for the pentose dehydration reaction, whilst the Lewis acid sites promoted the transfer hydrogenation of the adsorbed furfural intermediate to furfuryl alcohol. A remarkably high selectivity to furfuryl alcohol (90-95%) was observed using the mesoporous catalysts and it was dependent on the Al concentration in the siliceous framework. The vicinity of Brønsted and Lewis acid sites is suggested to be of major concern since the adsorbed furfural species is proposed to be reduced to furfuryl alcohol without being desorbed. The [Al]-SBA-15 molecular sieves were shown to be chemically and structurally stable demonstrating good recyclability in the aqueous-phase upgrading of xylose.
Catalytically active sites were controllably assembled into an SBA-15 framework by direct hydrothermal synthesis.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/c9cy01235d</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0003-1280-608X</orcidid><orcidid>https://orcid.org/0000-0001-7256-6765</orcidid><orcidid>https://orcid.org/0000-0002-9768-8360</orcidid><oa>free_for_read</oa></addata></record> |
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| ispartof | Catalysis science & technology, 2019, Vol.9 (19), p.535-5358 |
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| language | eng |
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| source | Royal Society Of Chemistry Journals 2008- |
| subjects | Alcohol Aluminum Catalysts Catalytic converters Dehydration Direct conversion Furfural Furfuryl alcohol Lewis acid Molecular sieves NMR Nuclear magnetic resonance Organic chemistry Pentose Recyclability Selectivity Silicon Surface properties Titration Xylose |
| title | Aqueous-phase tandem catalytic conversion of xylose to furfuryl alcohol over [Al]-SBA-15 molecular sieves |
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