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Impact of Zeolite Framework Composition and Flexibility on Methanol-To-Olefins Selectivity: Confinement or Diffusion?

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Impact of Zeolite Framework Composition and Flexibility on Methanol-To-Olefins Selectivity: Confinement or Diffusion?

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dc.contributor.author Ferri-Vicedo, Pau es_ES
dc.contributor.author Li, Chengeng es_ES
dc.contributor.author Millán-Cabrera, Reisel es_ES
dc.contributor.author Martínez-Triguero, Joaquín es_ES
dc.contributor.author Moliner Marin, Manuel es_ES
dc.contributor.author Boronat Zaragoza, Mercedes es_ES
dc.contributor.author Corma Canós, Avelino es_ES
dc.date.accessioned 2021-04-21T03:31:39Z
dc.date.available 2021-04-21T03:31:39Z
dc.date.issued 2020-10-26 es_ES
dc.identifier.issn 1433-7851 es_ES
dc.identifier.uri http://hdl.handle.net/10251/165409
dc.description This is the peer reviewed version of the following article: P. Ferri, C. Li, R. Millán, J. Martínez-Triguero, M. Moliner, M. Boronat, A. Corma, Angew. Chem. Int. Ed. 2020, 59, 19708, which has been published in final form at https://doi.org/10.1002/anie.202007609. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. es_ES
dc.description.abstract [EN] The methanol-to-olefins reaction catalyzed by small-pore cage-based acid zeolites and zeotypes produces a mixture of short chain olefins, whose selectivity to ethene, propene and butene varies with the cavity architecture and with the framework composition. The product distribution of aluminosilicates and silicoaluminophosphates with the CHA and AEI structures (H-SSZ-13, H-SAPO-34, H-SSZ-39 and H-SAPO-18) has been experimentally determined, and the impact of acidity and framework flexibility on the stability of the key cationic intermediates involved in the mechanism and on the diffusion of the olefin products through the8rwindows of the catalysts has been evaluated by means of periodic DFT calculations and ab initio molecular dynamics simulations. The preferential stabilization by confinement of fully methylated hydrocarbon pool intermediates favoring the paring pathway is the main factor controlling the final olefin product distribution. es_ES
dc.description.sponsorship This work has been supported by the European Union through ERC-AdG-2014-671093 (SynCatMatch), Spanish Government through "Severo Ochoa" (SEV-2016-0683, MINECO), MAT2017-82288-C2-1-P (AEI/FEDER, UE) and RTI2018-101033-B-I00 (MCIU/AEI/FEDER, UE), and by Generalitat Valenciana through AICO/2019/060. The Electron Microscopy Service of the UPV is acknowledged for their help in sample characterization. Red Espanola de Supercomputacion (RES) and Servei d'Informatica de la Universitat de Valencia (SIUV) are acknowledged for computational resources and technical support. P.F. and R.M. thank ITQ for their contracts. C.L. acknowledges China Scholarship Council (CSC) for a Ph.D fellowship. es_ES
dc.language Inglés es_ES
dc.publisher John Wiley & Sons es_ES
dc.relation.ispartof Angewandte Chemie International Edition es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Ab initio calculations es_ES
dc.subject Diffusion es_ES
dc.subject MTO es_ES
dc.subject Reaction mechanism es_ES
dc.subject Structure-selectivity relationship es_ES
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title Impact of Zeolite Framework Composition and Flexibility on Methanol-To-Olefins Selectivity: Confinement or Diffusion? es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1002/anie.202007609 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/671093/EU/MATching zeolite SYNthesis with CATalytic activity/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2016-0683/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/MAT2017-82288-C2-1-P/ES/MATERIALES HIBRIDOS MULTIFUNCIONALES BASADOS EN NANO-UNIDADES ESTRUCTURALES ACTIVAS/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-101033-B-I00/ES/DISEÑO DE CATALIZADORES MULTIFUNCIONALES PARA LA CONVERSION EFICIENTE DE BIOGAS Y GAS NATURAL A HIDROCARBUROS DE INTERES INDUSTRIAL/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//AICO%2F2019%2F060/ es_ES
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.contributor.affiliation Universitat Politècnica de València. Departamento de Química - Departament de Química es_ES
dc.description.bibliographicCitation Ferri-Vicedo, P.; Li, C.; Millán-Cabrera, R.; Martínez-Triguero, J.; Moliner Marin, M.; Boronat Zaragoza, M.; Corma Canós, A. (2020). Impact of Zeolite Framework Composition and Flexibility on Methanol-To-Olefins Selectivity: Confinement or Diffusion?. Angewandte Chemie International Edition. 59(44):19708-19715. https://doi.org/10.1002/anie.202007609 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1002/anie.202007609 es_ES
dc.description.upvformatpinicio 19708 es_ES
dc.description.upvformatpfin 19715 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 59 es_ES
dc.description.issue 44 es_ES
dc.identifier.pmid 32597576 es_ES
dc.relation.pasarela S\434188 es_ES
dc.contributor.funder European Commission es_ES
dc.contributor.funder Generalitat Valenciana es_ES
dc.contributor.funder China Scholarship Council es_ES
dc.contributor.funder European Regional Development Fund es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES
dc.contributor.funder Agencia Estatal de Investigación es_ES
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