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Insight into lewis acid catalysis with alkaline-earth MOFs: The role of polyhedral symmetry distortions

AuthorsPlatero Prats, Ana Eva ; Snejko, Natalia ; Iglesias, Marta ; Monge, M. Ángeles ; Gutiérrez-Puebla, Enrique
KeywordsAlkaline-earth metals
Green catalysts
Metal–organic frameworks
Symmetry distortions
Issue Date2013
CitationChemistry - A European Journal 19(46): 15572-15582 (2013)
AbstractWe propose a multidisciplinary approach to face the interpretation of heterogeneous catalysis with alkaline-earth metal-organic frameworks (MOFs). Their oxygen-based polyhedra, which do not exhibit regular geometries, do act as very active Lewis acid sites. Four novel alkaline-earth MOFs that belong to three different structural types - Mg-AEPF-11, Mg-APF-12, Ca-AEPF-13 and Sr-APF-13 - are reported, together with their net topologies, and a study of the symmetry distortions around the alkaline-earth metal polyhedra by using a continuous shape mapping (CShM) description. These MOFs are good catalysts in the selective hydrogenation of styrene. Even more, Sr-AEPF-13 shows the best conversions ever published with alkaline-earth MOFs for the hydrogenation of activated alkenes under mild conditions. A combination of crystallographic and topological analysis and theoretical calculations, together with experimental catalytic results, has been applied to understand the catalytic activity of these four novel alkaline-earth MOFs. This work demonstrates that the presence of symmetry-distorted alkaline-earth polyhedra gives rise to highly catalytic-active MOFs in the hydrogenation of activated alkenes. A matter of shape! There are many aspects that remain poorly understood in catalysis with alkaline-earth metal-organic frameworks (MOFs). Their metal polyhedra, which do not exhibit regular geometries, act as very active Lewis acids. In this work a new multidisciplinary approach is proposed to understand the catalytic activity of four novel alkaline-earth MOFs in the selective hydrogenation of alkenes (see figure). Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Identifiersdoi: 10.1002/chem.201302571
issn: 0947-6539
e-issn: 1521-3765
Appears in Collections:(ICMM) Artículos
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