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Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites

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Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites

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dc.contributor.author Bermejo-Deval, Ricardo es_ES
dc.contributor.author Assary, Rajeev S. Assary es_ES
dc.contributor.author Nikolla, Eranda es_ES
dc.contributor.author Moliner Marin, Manuel es_ES
dc.contributor.author Roman, Yuriy es_ES
dc.contributor.author Hwang, Son-Jong es_ES
dc.contributor.author Palsdottir, Arna Palsdottir es_ES
dc.contributor.author Silverman, Dorothy es_ES
dc.contributor.author RAUL F. LOBO es_ES
dc.contributor.author Lobo, Raul F. es_ES
dc.contributor.author Curtiss, Larry A. es_ES
dc.contributor.author Davis, Mark E. es_ES
dc.date.accessioned 2017-07-19T10:46:47Z
dc.date.available 2017-07-19T10:46:47Z
dc.date.issued 2012-05-19
dc.identifier.issn 0027-8424
dc.identifier.uri http://hdl.handle.net/10251/85445
dc.description.abstract [EN] Isomerization of sugars is used in a variety of industrially relevant processes and in glycolysis. Here, we show that hydrophobic zeolite beta with framework tin or titanium Lewis acid centers isomerizes sugars, e.g., glucose, via reaction pathways that are analogous to those of metalloenzymes. Specifically, experimental and theoretical investigations reveal that glucose partitions into the zeolite in the pyranose form, ring opens to the acyclic form in the presence of the Lewis acid center, isomerizes into the acyclic form of fructose, and finally ring closes to yield the furanose product. The zeolite catalysts provide processing advantages over metalloenzymes such as an ability to work at higher temperatures and in acidic conditions that allow for the isomerization reaction to be coupled with other important conversions. es_ES
dc.description.sponsorship The work at Caltech and the University of Delaware was financially supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award DE-SC0001004. M.M acknowledges the Fundacion Ramon Areces Postdoctoral Research Fellowship Program and the "Subprograma Ramon y Cajal" for Contract RYC-2011-08972 for financial support. R.B.D. acknowledges the Obra Social "la Caixa" for a graduate fellowship. A.P. acknowledges the Caltech Summer Undergraduate Research Fellowship program(SURF) for financial support. The computational studies for this work were supported by the U.S. Department of Energy under Contract DE-AC0206CH11357 and this material is based upon work supported as part of the Institute for Atom-efficient Chemical Transformations (IACT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. We gratefully acknowledge grants of computer time from the ANL Laboratory Computing Resource Center (LCRC), and the ANL Center for Nanoscale Materials. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Sciences of the U.S. Department of Energy under Contract DE-AC02-05CH11231. en_EN
dc.language Inglés es_ES
dc.publisher National Academy of Sciences es_ES
dc.relation.ispartof Proceedings of the National Academy of Sciences es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Glucose isomerization es_ES
dc.subject Heterogeneus catalysis es_ES
dc.subject Reaction mechanism es_ES
dc.title Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1073/pnas.1206708109
dc.relation.projectID info:eu-repo/grantAgreement/DOE//DE-SC0001004/
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//RYC-2011-08972/ES/RYC-2011-08972/
dc.relation.projectID info:eu-repo/grantAgreement/DOE//DE-AC0206CH11357/
dc.relation.projectID info:eu-repo/grantAgreement/DOE//DE-AC02-05CH11231/
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 Bermejo-Deval, R.; Assary, RSA.; Nikolla, E.; Moliner Marin, M.; Roman, Y.; Hwang, S.; Palsdottir, AP.... (2012). Metalloenzyme-like catalyzed isomerizations of sugars by Lewis acid zeolites. Proceedings of the National Academy of Sciences. 109(25):9727-9732. https://doi.org/10.1073/pnas.1206708109 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion http://doi.org/10.1073/pnas.1206708109 es_ES
dc.description.upvformatpinicio 9727 es_ES
dc.description.upvformatpfin 9732 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 109 es_ES
dc.description.issue 25 es_ES
dc.relation.senia 237715 es_ES
dc.identifier.pmcid PMC3382492
dc.contributor.funder Energy Frontier Research Centers, EEUU
dc.contributor.funder U.S. Department of Energy
dc.contributor.funder Fundación Ramón Areces
dc.contributor.funder Ministerio de Ciencia e Innovación
dc.contributor.funder Argonne National Laboratory
dc.contributor.funder Fundació Bancària Caixa d'Estalvis i Pensions de Barcelona


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