Metal-organic frameworks as kinetic modulators for branched selectivity in hydroformylation.

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dc.contributor.authorBauer, Gerald
dc.contributor.authorOngari, Daniele
dc.contributor.authorTiana, Davide
dc.contributor.authorGäumann, Patrick
dc.contributor.authorRohrbach, Thomas
dc.contributor.authorPareras, Gerard
dc.contributor.authorTarik, Mohamed
dc.contributor.authorSmit, Berend
dc.contributor.authorRanocchiari, Marco
dc.contributor.funderETH ZĂĽrich Foundationen
dc.contributor.funderH2020 European Research Councilen
dc.contributor.funderHorizon 2020en
dc.contributor.funderSchweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschungen
dc.contributor.funderEnergy System Integration, Paul Scherrer Instituten
dc.date.accessioned2020-03-02T15:28:27Z
dc.date.available2020-03-02T15:28:27Z
dc.date.issued2020-02-26
dc.date.updated2020-02-28T15:27:21Z
dc.description.abstractFinding heterogeneous catalysts that are superior to homogeneous ones for selective catalytic transformations is a major challenge in catalysis. Here, we show how micropores in metal-organic frameworks (MOFs) push homogeneous catalytic reactions into kinetic regimes inaccessible under standard conditions. Such property allows branched selectivity up to 90% in the Co-catalysed hydroformylation of olefins without directing groups, not achievable with existing catalysts. This finding has a big potential in the production of aldehydes for the fine chemical industry. Monte Carlo and density functional theory simulations combined with kinetic models show that the micropores of MOFs with UMCM-1 and MOF-74 topologies increase the olefins density beyond neat conditions while partially preventing the adsorption of syngas leading to high branched selectivity. The easy experimental protocol and the chemical and structural flexibility of MOFs will attract the interest of the fine chemical industries towards the design of heterogeneous processes with exceptional selectivity.en
dc.description.sponsorshipETH Zürich Foundation (Swiss National Supercomputing Centre (CSCS) under Project no. s765); Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (Swiss National Science Foundation (SNSF) National Centre of Competence in Research (NCCR) “Materials’ Revolution: Computational Design and Discovery of Novel Materials (MARVEL)”);en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.articleid1059en
dc.identifier.citationBauer, G., Ongari, D., Tiana, D., Gäumann, P., Rohrbach, T., Pareras, G., Tarik, M., Smit, B. and Ranocchiari, M. (2020) 'Metal-organic frameworks as kinetic modulators for branched selectivity in hydroformylation', Nature Communications, 11(1), 1059 (8 pp). doi: 10.1038/s41467-020-14828-6en
dc.identifier.doi10.1038/s41467-020-14828-6en
dc.identifier.endpage8en
dc.identifier.issn2041-1723
dc.identifier.issued1en
dc.identifier.journaltitleNature Communicationsen
dc.identifier.startpage1en
dc.identifier.urihttps://hdl.handle.net/10468/9717
dc.identifier.volume11en
dc.language.isoenen
dc.publisherSpringer Natureen
dc.relation.projectinfo:eu-repo/grantAgreement/EC/H2020::ERC::ERC-ADG/666983/EU/The Materials Genome in Action/MaGicen
dc.relation.urihttps://www.nature.com/articles/s41467-020-14828-6#Ack1
dc.rights© The Author(s) 2020. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.en
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.subjectCatalystsen
dc.subjectCatalytic transformationsen
dc.subjectDensity functional theory (DFT)en
dc.subjectHeterogeneous processesen
dc.subjectHeterogeneous catalysisen
dc.subjectHomogeneous catalysisen
dc.subjectMetal–organic frameworksen
dc.titleMetal-organic frameworks as kinetic modulators for branched selectivity in hydroformylation.en
dc.typeArticle (peer-reviewed)en
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