Fine-Tuning of Acidity in Hierarchical Zeolites for the Efficient Prins Cyclization Yielding Florol
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| dc.contributor.author | Sánchez-Velandia, Julián E.
|
es_ES |
| dc.contributor.author | Kurmach, Mykhailo
|
es_ES |
| dc.contributor.author | Shvets, Oleksiy
|
es_ES |
| dc.contributor.author | Garcia-Baldovi, Hermenegildo
|
es_ES |
| dc.contributor.author | García-Verdugo, Eduardo
|
es_ES |
| dc.contributor.author | Murzin, Dmitry Yu
|
es_ES |
| dc.contributor.author | Shcherban, Nataliya
|
es_ES |
| dc.date.accessioned | 2024-11-21T19:11:14Z | |
| dc.date.available | 2024-11-21T19:11:14Z | |
| dc.date.issued | 2024-10-22 | es_ES |
| dc.identifier.issn | 2168-0485 | es_ES |
| dc.identifier.uri | http://hdl.handle.net/10251/212134 | |
| dc.description.abstract | [EN] In this contribution, several hierarchical zeolites comprising mainly Br & oslash;nsted acid sites with different morphologies (nanosheets, nanoparticles, nanorods) were synthesized and applied to the efficient synthesis of the perfume Florol (2-isobutyl-4-methyl-tetrahydro-2H-pyran-4-ol) via Prins cyclization of isoprenol and isovaraldehyde. Tuning the acidity in a zeolite was done by either incorporating metal centers or changing the initial composition and crystallization time. Furthermore, the interplay among the pore structure, specific mesoporosity, and accessibility of acidic sites is crucial for optimizing Florol synthesis. Strong Br & oslash;nsted acid sites enhance the formation of the dehydration products, while mild-acidic Br & oslash;nsted acid sites with a medium strength of accessible acid sites improve the formation of Florol. A maximum Florol yield of ca. 80% was achieved with Al-MFI and Al-FER (only 30 min) with typical nanosheet (nsh) morphology; in addition, values of TOF in the order of 1121 and 2655 h(-1), respectively, were also achieved. Al-FER-nsh showed itself to be robust, because it can be reused several times without any apparent loss of its catalytic activity. Finally, different green chemistry parameters were also applied to the studied zeolites in the synthesis of Florol, suggesting the high efficiency of the best catalyst (Al-MFI-nsh). | es_ES |
| dc.description.sponsorship | J.E.S.-V. is grateful to Universidad Jaume I for the postdoctoral position during 2022-2023 (programa Propi UJI) and the project (PID2020-11962RB-C33), MCIN/AEI/10.13039/501100011033/European Union NextGeneration EU/PRTP. N.S., O.S., and M.K. acknowledge the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Science, under Award Number DE-SC0021041 for supporting X-ray diffraction, nitrogen physisorption, and pyridine adsorption with FTIR-spectral analysis, and the National Research Foundation of Ukraine, which funded the material synthesis through the project "Creation of new bifunctional zeolite catalysts for one-pot cascade processes of conversion of platform molecules from biomass into fuels and industrially valuable organic compounds" (Project Number 238/0139). N.S. is grateful to the Verkhovna Rada of Ukraine for a personal scholarship for young scientists-doctors of sciences for 2024. M.K. thanks a Grant to a research group of young scientists "Development of new catalysts for the conversion of mono-, diatomic (bio)alcohols into important dienes, hydrocarbons, oxygenates, pharmaceutical ingredients" (0124U002117). | es_ES |
| dc.language | Inglés | es_ES |
| dc.publisher | American Chemical Society | es_ES |
| dc.relation.ispartof | ACS Sustainable Chemistry & Engineering | es_ES |
| dc.rights | Reserva de todos los derechos | es_ES |
| dc.subject | Hierarchical zeolites | es_ES |
| dc.subject | Prins cyclization | es_ES |
| dc.subject | Tetrahydropyranol | es_ES |
| dc.subject | Florol | es_ES |
| dc.subject | Acid sites | es_ES |
| dc.title | Fine-Tuning of Acidity in Hierarchical Zeolites for the Efficient Prins Cyclization Yielding Florol | es_ES |
| dc.type | Artículo | es_ES |
| dc.identifier.doi | 10.1021/acssuschemeng.4c05535 | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/DOE//DE-SC0021041/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//PID2020-11962RB-C33/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/VRU//0124U002117/ | es_ES |
| dc.relation.projectID | info:eu-repo/grantAgreement/NRFU//238%2F0139/ | es_ES |
| dc.rights.accessRights | Cerrado | es_ES |
| dc.contributor.affiliation | Universitat Politècnica de València. Departamento de Química - Departament de Química | es_ES |
| dc.description.bibliographicCitation | Sánchez-Velandia, JE.; Kurmach, M.; Shvets, O.; Garcia-Baldovi, H.; García-Verdugo, E.; Murzin, DY.; Shcherban, N. (2024). Fine-Tuning of Acidity in Hierarchical Zeolites for the Efficient Prins Cyclization Yielding Florol. ACS Sustainable Chemistry & Engineering. 12(44):16283-16296. https://doi.org/10.1021/acssuschemeng.4c05535 | es_ES |
| dc.description.accrualMethod | S | es_ES |
| dc.relation.publisherversion | https://doi.org/10.1021/acssuschemeng.4c05535 | es_ES |
| dc.description.upvformatpinicio | 16283 | es_ES |
| dc.description.upvformatpfin | 16296 | es_ES |
| dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
| dc.description.volume | 12 | es_ES |
| dc.description.issue | 44 | es_ES |
| dc.relation.pasarela | S\531805 | es_ES |
| dc.contributor.funder | U.S. Department of Energy | es_ES |
| dc.contributor.funder | Supreme Council of Ukraine | es_ES |
| dc.contributor.funder | Ministerio de Ciencia e Innovación | es_ES |
| dc.contributor.funder | National Research Foundation of Ukraine | es_ES |
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