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Hydrolase-like catalysis and structural resolution of natural products by a metal-organic framework

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Hydrolase-like catalysis and structural resolution of natural products by a metal-organic framework

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dc.contributor.author Mon-Conejero, Marta es_ES
dc.contributor.author Bruno, Rosaria es_ES
dc.contributor.author Sanz-Navarro, Sergio es_ES
dc.contributor.author Negro, Cristina es_ES
dc.contributor.author Ferrando-Soria, Jesus es_ES
dc.contributor.author Bartella, Lucia es_ES
dc.contributor.author Di Donna, Leonardo es_ES
dc.contributor.author Prejano, Mario es_ES
dc.contributor.author Marino, Tiziana es_ES
dc.contributor.author Leyva Perez, Antonio es_ES
dc.contributor.author Armentano, Donatella es_ES
dc.contributor.author Pardo, Emilio es_ES
dc.date.accessioned 2022-06-01T18:07:07Z
dc.date.available 2022-06-01T18:07:07Z
dc.date.issued 2020-06-17 es_ES
dc.identifier.issn 2041-1723 es_ES
dc.identifier.uri http://hdl.handle.net/10251/183032
dc.description.abstract [EN] The exact chemical structure of non-crystallising natural products is still one of the main challenges in Natural Sciences. Despite tremendous advances in total synthesis, the absolute structural determination of a myriad of natural products with very sensitive chemical functionalities remains undone. Here, we show that a metal-organic framework (MOF) with alcohol-containing arms and adsorbed water, enables selective hydrolysis of glycosyl bonds, supramolecular order with the so-formed chiral fragments and absolute determination of the organic structure by single-crystal X-ray crystallography in a single operation. This combined strategy based on a biomimetic, cheap, robust and multigram available solid catalyst opens the door to determine the absolute configuration of ketal compounds regardless degradation sensitiveness, and also to design extremely-mild metal-free solid-catalysed processes without formal acid protons. Elucidation of the chemical structure of natural products constitutes one of the main challenges in Natural Sciences. Here, the authors show that an amino acid-based metal-organic framework exhibits hydrolase-like catalytic activity and crystallographic determination of the resulting products es_ES
dc.description.sponsorship This work was supported by the Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy) and the MINECO (Spain) (Projects CTQ2016-75671-P, CTQ 2017-86735-P, RTC-2017-6331-5, Severo Ochoa program SEV-2016-0683 and Excellence Unit "Maria de Maeztu" MDM-2015-0538). R.B. thanks the MIUR (Project PON R&I FSE-FESR 2014-2020) for grant. L.B wishes to thank Italian MIUR for grant n. AIM1899391-1 in the framework of the project "Azione I.2, Mobilita dei Ricercatori, PON R&I 2014-2020". Thanks are also extended to the "2019 Post-doctoral Junior Leader-Retaining Fellowship, la Caixa Foundation (ID100010434 and fellowship code LCF/BQ/PR19/11700011" (J. F.-S.). S. S.-N. thanks ITQ for the concession of a contract. D.A. acknowledges the financial support of the Fondazione CARIPLO/"Economia Circolare: ricerca per un futuro sostenibile" 2019, Project code: 2019-2090, MOCA. E.P. acknowledges the financial support of the European Research Council under the European Union's Horizon 2020 research and innovation program/ERC Grant Agreement No. 814804, MOF-reactors. es_ES
dc.language Inglés es_ES
dc.publisher Nature Publishing Group es_ES
dc.relation.ispartof Nature Communications es_ES
dc.rights Reconocimiento (by) es_ES
dc.title Hydrolase-like catalysis and structural resolution of natural products by a metal-organic framework es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1038/s41467-020-16699-3 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/CTQ2017-86735-P/ES/CATALISIS CON ATOMOS METALICOS AISLADOS Y CLUSTERES ULTRAPEQUEÑOS BIEN DEFINIDOS, SIN LIGANDOS Y CONFINADOS/
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//RTC-2017-6331-5//NUEVA SINTESIS DEL OLIGOMERO CLAVE EN TINTAS DIGITALES/
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2016-75671-P/
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2016-0683/
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//MDM-2015-0538/ES/INSTITUTO DE CIENCIA MOLECULAR/
dc.relation.projectID info:eu-repo/grantAgreement/Fundació Bancària Caixa d'Estalvis i Pensions de Barcelona//LCF%2FBQ%2FPR19%2F11700011/
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/814804/EU
dc.relation.projectID info:eu-repo/grantAgreement/Fondazione Cariplo//2019-2090/
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química es_ES
dc.description.bibliographicCitation Mon-Conejero, M.; Bruno, R.; Sanz-Navarro, S.; Negro, C.; Ferrando-Soria, J.; Bartella, L.; Di Donna, L.... (2020). Hydrolase-like catalysis and structural resolution of natural products by a metal-organic framework. Nature Communications. 11(1):1-9. https://doi.org/10.1038/s41467-020-16699-3 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1038/s41467-020-16699-3 es_ES
dc.description.upvformatpinicio 1 es_ES
dc.description.upvformatpfin 9 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 11 es_ES
dc.description.issue 1 es_ES
dc.identifier.pmid 32555154 es_ES
dc.identifier.pmcid PMC7300120 es_ES
dc.relation.pasarela S\461657 es_ES
dc.contributor.funder Agencia Estatal de Investigación
dc.contributor.funder Ministero dell'Istruzione, dell'Università e della Ricerca
dc.contributor.funder Fundació Bancària Caixa d'Estalvis i Pensions de Barcelona
dc.contributor.funder Fondazione Cariplo
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