Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose
The direct one-pot transformation of glucose into γ-valerolactone (GVL) can be accomplished by means of a cascade of reactions in which Brønsted acid-catalyzed transformations are combined with catalytic transfer hydrogenation (CTH) by using 2-propanol as sacrificial alcohol, avoiding the use of hig...
| Autores: | , , , , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Estado: | Versión aceptada para publicación |
| Fecha de publicación: | 2021 |
| País: | España |
| Institución: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/377729 |
| Acceso en línea: | http://hdl.handle.net/10261/377729 https://www.scopus.com/inward/record.uri?eid=2-s2.0-85084217924&doi=10.1016%2fj.cattod.2020.04.025&partnerID=40&md5=6b59b57b6213f158a954f8c50ded4963 |
| Access Level: | acceso abierto |
| Palabra clave: | Beta zeolite Bifunctional catalyst Cascade reaction Gamma-valerolactone Zirconium |
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Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucosePaniagua, MartaMorales, GabrielMelero, Juan AntonioIglesias, JoséLópez-Aguado, ClaraVidal, N.Mariscal López, RafaelLópez Granados, ManuelMartínez-Salazar, IreneBeta zeoliteBifunctional catalystCascade reactionGamma-valerolactoneZirconiumThe direct one-pot transformation of glucose into γ-valerolactone (GVL) can be accomplished by means of a cascade of reactions in which Brønsted acid-catalyzed transformations are combined with catalytic transfer hydrogenation (CTH) by using 2-propanol as sacrificial alcohol, avoiding the use of high-pressure hydrogen. Catalysts containing Zr Lewis acid sites have been successfully applied in CTH reactions while the acid-driven transformations can be preferentially promoted by Brønsted Al-related acidity. Here, we present the combination of Zr and Al as active sites within a BEA zeolite structure as catalyst, with the possibility of adjusting the Al/Zr ratio from ∞ (commercial H-Beta) to 0 (aluminium-free Zr-Beta), which show a scale of Brønsted/Lewis acid sites ratios. The Al/Zr ratio has a strong impact on the products distribution. As the Zr content increases, higher amount of GVL is obtained, leading to a maximum over the catalyst with high amount of Zr and low content of Al acid sites (Al/Zr = 0.2). An increase of reaction temperature, as well as reaction time, allows an enhancement of yields towards the desired products, leading to a maximum yield towards GVL of 24 mol% over Zr-Al-Beta (2.0), and a maximum yield towards isopropyl lactate of 26 mol% over Zr-Beta at 190 °C. © 2020 Elsevier B.V.The Spanish Ministry of Science, Innovation and Universities and the Regional Government of Madrid are kindly acknowledged for funding this research through the projects RTI2018-094918-B-C42, RTI2018-094918-B-C41, S2018/EMT-4344, and PEJD-2019-PRE_IND-15918. Clara López-Aguado acknowledges a FPI grant (BES-2015-072709) from the Government of Spain.Supplementary material related to this article can be found, in the online version, at doi:https://doi.org/10.1016/j.cattod.2020.04.025Peer reviewedElsevier BVConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252021info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/377729https://www.scopus.com/inward/record.uri?eid=2-s2.0-85084217924&doi=10.1016%2fj.cattod.2020.04.025&partnerID=40&md5=6b59b57b6213f158a954f8c50ded4963reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésCatalysis Todayhttps://doi.org/10.1016/j.cattod.2020.04.025Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3777292026-05-22T06:33:51Z |
| dc.title.none.fl_str_mv |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| title |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| spellingShingle |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose Paniagua, Marta Beta zeolite Bifunctional catalyst Cascade reaction Gamma-valerolactone Zirconium |
| title_short |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| title_full |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| title_fullStr |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| title_full_unstemmed |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| title_sort |
Understanding the role of Al/Zr ratio in Zr-Al-Beta zeolite: Towards the one-pot production of GVL from glucose |
| dc.creator.none.fl_str_mv |
Paniagua, Marta Morales, Gabriel Melero, Juan Antonio Iglesias, José López-Aguado, Clara Vidal, N. Mariscal López, Rafael López Granados, Manuel Martínez-Salazar, Irene |
| author |
Paniagua, Marta |
| author_facet |
Paniagua, Marta Morales, Gabriel Melero, Juan Antonio Iglesias, José López-Aguado, Clara Vidal, N. Mariscal López, Rafael López Granados, Manuel Martínez-Salazar, Irene |
| author_role |
author |
| author2 |
Morales, Gabriel Melero, Juan Antonio Iglesias, José López-Aguado, Clara Vidal, N. Mariscal López, Rafael López Granados, Manuel Martínez-Salazar, Irene |
| author2_role |
author author author author author author author author |
| dc.contributor.none.fl_str_mv |
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72] |
| dc.subject.none.fl_str_mv |
Beta zeolite Bifunctional catalyst Cascade reaction Gamma-valerolactone Zirconium |
| topic |
Beta zeolite Bifunctional catalyst Cascade reaction Gamma-valerolactone Zirconium |
| description |
The direct one-pot transformation of glucose into γ-valerolactone (GVL) can be accomplished by means of a cascade of reactions in which Brønsted acid-catalyzed transformations are combined with catalytic transfer hydrogenation (CTH) by using 2-propanol as sacrificial alcohol, avoiding the use of high-pressure hydrogen. Catalysts containing Zr Lewis acid sites have been successfully applied in CTH reactions while the acid-driven transformations can be preferentially promoted by Brønsted Al-related acidity. Here, we present the combination of Zr and Al as active sites within a BEA zeolite structure as catalyst, with the possibility of adjusting the Al/Zr ratio from ∞ (commercial H-Beta) to 0 (aluminium-free Zr-Beta), which show a scale of Brønsted/Lewis acid sites ratios. The Al/Zr ratio has a strong impact on the products distribution. As the Zr content increases, higher amount of GVL is obtained, leading to a maximum over the catalyst with high amount of Zr and low content of Al acid sites (Al/Zr = 0.2). An increase of reaction temperature, as well as reaction time, allows an enhancement of yields towards the desired products, leading to a maximum yield towards GVL of 24 mol% over Zr-Al-Beta (2.0), and a maximum yield towards isopropyl lactate of 26 mol% over Zr-Beta at 190 °C. © 2020 Elsevier B.V. |
| publishDate |
2021 |
| dc.date.none.fl_str_mv |
2021 2025 2025 |
| dc.type.none.fl_str_mv |
info:eu-repo/semantics/article http://purl.org/coar/resource_type/c_6501 Postprint info:eu-repo/semantics/acceptedVersion |
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article |
| status_str |
acceptedVersion |
| dc.identifier.none.fl_str_mv |
http://hdl.handle.net/10261/377729 https://www.scopus.com/inward/record.uri?eid=2-s2.0-85084217924&doi=10.1016%2fj.cattod.2020.04.025&partnerID=40&md5=6b59b57b6213f158a954f8c50ded4963 |
| url |
http://hdl.handle.net/10261/377729 https://www.scopus.com/inward/record.uri?eid=2-s2.0-85084217924&doi=10.1016%2fj.cattod.2020.04.025&partnerID=40&md5=6b59b57b6213f158a954f8c50ded4963 |
| dc.language.none.fl_str_mv |
Inglés |
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Inglés |
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Catalysis Today https://doi.org/10.1016/j.cattod.2020.04.025 Sí |
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info:eu-repo/semantics/openAccess |
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openAccess |
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Elsevier BV |
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Elsevier BV |
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reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC instname:Consejo Superior de Investigaciones Científicas (CSIC) |
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Consejo Superior de Investigaciones Científicas (CSIC) |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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DIGITAL.CSIC. Repositorio Institucional del CSIC |
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15,811543 |