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dc.contributor.authorDawson, Daniel M.
dc.contributor.authorJamieson, Lauren E.
dc.contributor.authorMohideen, M. Infas H.
dc.contributor.authorMcKinlay, Alistair C.
dc.contributor.authorSmellie, Iain A.
dc.contributor.authorCadou, Romain
dc.contributor.authorKeddie, Neil S.
dc.contributor.authorMorris, Russell E.
dc.contributor.authorAshbrook, Sharon E.
dc.identifier.citationDawson , D M , Jamieson , L E , Mohideen , M I H , McKinlay , A C , Smellie , I A , Cadou , R , Keddie , N S , Morris , R E & Ashbrook , S E 2012 , ' High-resolution solid-state 13 C NMR spectroscopy of the paramagnetic metal-organic frameworks, STAM-1 and HKUST-1 ' Physical Chemistry Chemical Physics , vol. 15 , no. 3 , pp. 919-929 .
dc.identifier.otherPURE: 46702547
dc.identifier.otherPURE UUID: a33456f4-e93c-4a19-b684-aaa86f992554
dc.identifier.otherWOS: 000312217200025
dc.identifier.otherScopus: 84871303598
dc.identifier.otherORCID: /0000-0002-4538-6782/work/56638913
dc.identifier.otherORCID: /0000-0002-9502-5862/work/35745204
dc.identifier.otherORCID: /0000-0002-8110-4535/work/34029125
dc.description.abstractSolid-state C-13 magic-angle spinning (MAS) NMR spectroscopy is used to investigate the structure of the Cu(II)-based metal-organic frameworks (MOFs), HKUST-1 and STAM-1, and the structural changes occurring within these MOFs upon activation (dehydration). NMR spectroscopy is an attractive technique for the investigation of these materials, owing to its high sensitivity to local structure, without any requirement for longer-range order. However, interactions between nuclei and unpaired electrons in paramagnetic systems (e.g., Cu(II)-based MOFs) pose a considerable challenge, not only for spectral acquisition, but also in the assignment and interpretation of the spectral resonances. Here, we exploit the rapid T-1 relaxation of these materials to obtain C-13 NMR spectra using a spin-echo pulse sequence at natural abundance levels, and employ frequency-stepped acquisition to ensure uniform excitation of resonances over a wide frequency range. We then utilise selective C-13 isotopic labelling of the organic linker molecules to enable an unambiguous assignment of NMR spectra of both MOFs for the first time. We show that the monomethylated linker can be recovered from STAM-1 intact, demonstrating not only the interesting use of this MOF as a protecting group, but also the ability (for both STAM-1 and HKUST-1) to recover isotopically-enriched linkers, thereby reducing significantly the overall cost of the approach.
dc.relation.ispartofPhysical Chemistry Chemical Physicsen
dc.rightsThis is the author's version of this article. The published version © 2013 The Royal Society of Chemistry is available from http://pubs.rsc.orgen
dc.subject1st-principles calculationsen
dc.subjectCO2 adsorptionen
dc.subjectMAS NMRen
dc.subjectQD Chemistryen
dc.titleHigh-resolution solid-state 13C NMR spectroscopy of the paramagnetic metal-organic frameworks, STAM-1 and HKUST-1en
dc.typeJournal articleen
dc.contributor.institutionUniversity of St Andrews.School of Chemistryen
dc.contributor.institutionUniversity of St Andrews.EaSTCHEMen
dc.description.statusPeer revieweden

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