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Mixed-metal MIL-100(Sc,M) (M=Al, Cr, Fe) for Lewis acid catalysis and tandem C−C bond formation and alcohol oxidation
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dc.contributor.author | Mitchell, Laura | |
dc.contributor.author | Williamson, Patrick | |
dc.contributor.author | Ehrlichova, Barbora | |
dc.contributor.author | Anderson, Amanda Elizabeth | |
dc.contributor.author | Seymour, Valerie Ruth | |
dc.contributor.author | Ashbrook, Sharon Elizabeth | |
dc.contributor.author | Acerbi, Nadia | |
dc.contributor.author | Daniels, Luke | |
dc.contributor.author | Walton, Richard | |
dc.contributor.author | Clarke, Matthew L. | |
dc.contributor.author | Wright, Paul Anthony | |
dc.date.accessioned | 2015-10-27T00:11:25Z | |
dc.date.available | 2015-10-27T00:11:25Z | |
dc.date.issued | 2014-12-05 | |
dc.identifier | 157247904 | |
dc.identifier | d93818fb-fb15-43fb-8aa7-0108c9666c87 | |
dc.identifier | 000346056600044 | |
dc.identifier | 84915747976 | |
dc.identifier.citation | Mitchell , 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 . https://doi.org/10.1002/chem.201404377 | en |
dc.identifier.issn | 0947-6539 | |
dc.identifier.other | ORCID: /0000-0002-4538-6782/work/56638937 | |
dc.identifier.other | ORCID: /0000-0002-2444-1244/work/59464610 | |
dc.identifier.other | ORCID: /0000-0002-4243-9957/work/62668269 | |
dc.identifier.uri | https://hdl.handle.net/10023/7693 | |
dc.description | The 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.abstract | The 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.format.extent | 14 | |
dc.format.extent | 1876737 | |
dc.language.iso | eng | |
dc.relation.ispartof | Chemistry - A European Journal | en |
dc.subject | Bifunctional catalysts | en |
dc.subject | Heterogeneous catalysis | en |
dc.subject | Iron | en |
dc.subject | Scandium | en |
dc.subject | Tandem catalysis | en |
dc.subject | QD Chemistry | en |
dc.subject | BDC | en |
dc.subject.lcc | QD | en |
dc.title | Mixed-metal MIL-100(Sc,M) (M=Al, Cr, Fe) for Lewis acid catalysis and tandem C−C bond formation and alcohol oxidation | en |
dc.type | Journal article | en |
dc.contributor.sponsor | The Leverhulme Trust | en |
dc.contributor.sponsor | EPSRC | en |
dc.contributor.sponsor | EPSRC | en |
dc.contributor.institution | University of St Andrews. School of Chemistry | en |
dc.contributor.institution | University of St Andrews. EaSTCHEM | en |
dc.identifier.doi | 10.1002/chem.201404377 | |
dc.description.status | Peer reviewed | en |
dc.date.embargoedUntil | 2015-10-27 | |
dc.identifier.url | http://onlinelibrary.wiley.com/doi/10.1002/chem.201404377/suppinfo | en |
dc.identifier.grantnumber | F/00 268/BJ | en |
dc.identifier.grantnumber | EP/J501542/1 | en |
dc.identifier.grantnumber | EP/J501542/1 | en |
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