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dc.contributor.authorMitchell, Laura
dc.contributor.authorWilliamson, Patrick
dc.contributor.authorEhrlichova, Barbora
dc.contributor.authorAnderson, Amanda Elizabeth
dc.contributor.authorSeymour, Valerie Ruth
dc.contributor.authorAshbrook, Sharon Elizabeth
dc.contributor.authorAcerbi, Nadia
dc.contributor.authorDaniels, Luke
dc.contributor.authorWalton, Richard
dc.contributor.authorClarke, Matthew L.
dc.contributor.authorWright, Paul Anthony
dc.identifier.citationMitchell , L , Williamson , P , Ehrlichova , B , Anderson , A E , Seymour , V R , Ashbrook , S E , Acerbi , N , Daniels , L , Walton , R , Clarke , M L & Wright , P A 2014 , ' Mixed-metal MIL-100(Sc,M) (M=Al, Cr, Fe) for Lewis acid catalysis and tandem C−C bond formation and alcohol oxidation ' , Chemistry - A European Journal , vol. 20 , no. 51 , pp. 17185-17197 .
dc.identifier.otherPURE: 157247904
dc.identifier.otherPURE UUID: d93818fb-fb15-43fb-8aa7-0108c9666c87
dc.identifier.otherWOS: 000346056600044
dc.identifier.otherScopus: 84915747976
dc.identifier.otherORCID: /0000-0002-4538-6782/work/56638937
dc.identifier.otherORCID: /0000-0002-2444-1244/work/59464610
dc.identifier.otherORCID: /0000-0002-4243-9957/work/62668269
dc.descriptionThe authors thank Johnson Matthey and the EPSRC for an Industrial CASE award to L.M. We gratefully acknowledge the IAESTE UK for a scholarship to B.E. They also thank the Leverhulme Trust (F/00 268/BJ), EPSRC (EP/J501542/1), and the EaStCHEM Research Computing Facility.en
dc.description.abstractThe trivalent metal cations Al3+, Cr3+, and Fe3+ were each introduced, together with Sc3+, into MIL-100(Sc,M) solid solutions (M=Al, Cr, Fe) by direct synthesis. The substitution has been confirmed by powder X-ray diffraction (PXRD) and solid-state NMR, UV/Vis, and X-ray absorption (XAS) spectroscopy. Mixed Sc/Fe MIL-100 samples were prepared in which part of the Fe is present as α-Fe2O3 nanoparticles within the mesoporous cages of the MOF, as shown by XAS, TGA, and PXRD. The catalytic activity of the mixed-metal catalysts in Lewis acid catalysed Friedel–Crafts additions increases with the amount of Sc present, with the attenuating effect of the second metal decreasing in the order Al>Fe>Cr. Mixed-metal Sc,Fe materials give acceptable activity: 40 % Fe incorporation only results in a 20 % decrease in activity over the same reaction time and pure product can still be obtained and filtered off after extended reaction times. Supported α-Fe2O3 nanoparticles were also active Lewis acid species, although less active than Sc3+ in trimer sites. The incorporation of Fe3+ into MIL-100(Sc) imparts activity for oxidation catalysis and tandem catalytic processes (Lewis acid+oxidation) that make use of both catalytically active framework Sc3+ and Fe3+. A procedure for using these mixed-metal heterogeneous catalysts has been developed for making ketones from (hetero)aromatics and a hemiacetal.
dc.relation.ispartofChemistry - A European Journalen
dc.rights© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. This work is made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at
dc.subjectBifunctional catalystsen
dc.subjectHeterogeneous catalysisen
dc.subjectTandem catalysisen
dc.subjectQD Chemistryen
dc.titleMixed-metal MIL-100(Sc,M) (M=Al, Cr, Fe) for Lewis acid catalysis and tandem C−C bond formation and alcohol oxidationen
dc.typeJournal articleen
dc.contributor.sponsorThe Leverhulme Trusten
dc.contributor.institutionUniversity of St Andrews. School of Chemistryen
dc.contributor.institutionUniversity of St Andrews. EaSTCHEMen
dc.description.statusPeer revieweden
dc.identifier.grantnumberF/00 268/BJen

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