Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy

Handle URI:
http://hdl.handle.net/10754/622857
Title:
Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy
Authors:
Pump, Eva ( 0000-0003-2810-2546 ) ; Viger-Gravel, Jasmine; Abou-Hamad, Edy; Samantaray, Manoja; Hamzaoui, Bilel; Gurinov, Andrei; Anjum, Dalaver H.; Gajan, David; Lesage, Anne; Bendjeriou-Sedjerari, Anissa; Emsley, Lyndon; Basset, Jean-Marie ( 0000-0003-3166-8882 )
Abstract:
Dynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy (DNP SENS) is an emerging technique that allows access to high-sensitivity NMR spectra from surfaces. However, DNP SENS usually requires the use of radicals as an exogenous source of polarization, which has so far limited applications for organometallic surface species to those that do not react with the radicals. Here we show that reactive surface species can be studied if they are immobilized inside porous materials with suitably small windows, and if bulky nitroxide bi-radicals (here TEKPol) are used as the polarization source and which cannot enter the pores. The method is demonstrated by obtaining significant DNP enhancements from highly reactive complelxes [(equivalent to Si-O-)W(Me)(5)] supported on MCM-41, and effects of pore size (6.0, 3.0 and 2.5 nm) on the performance are discussed.
KAUST Department:
KAUST Catalysis Center (KCC); Imaging and Characterization Core Lab
Citation:
Pump E, Viger-Gravel J, Abou-Hamad E, Samantaray MK, Hamzaoui B, et al. (2017) Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy. Chem Sci 8: 284–290. Available: http://dx.doi.org/10.1039/c6sc02379g.
Publisher:
Royal Society of Chemistry (RSC)
Journal:
Chem. Sci.
Issue Date:
15-Aug-2016
DOI:
10.1039/c6sc02379g
Type:
Article
ISSN:
2041-6520; 2041-6539
Sponsors:
This work received support from the King Abdullah University of Science and Technology (KAUST) and ERC Advanced Grant No. 320860. We thank Dr Olivier Ouari and Paul Tordo from the University of Aix-Marseille, for providing the TEKPol radical.
Additional Links:
http://pubs.rsc.org/en/Content/ArticleLanding/2017/SC/C6SC02379G#!divAbstract
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorPump, Evaen
dc.contributor.authorViger-Gravel, Jasmineen
dc.contributor.authorAbou-Hamad, Edyen
dc.contributor.authorSamantaray, Manojaen
dc.contributor.authorHamzaoui, Bilelen
dc.contributor.authorGurinov, Andreien
dc.contributor.authorAnjum, Dalaver H.en
dc.contributor.authorGajan, Daviden
dc.contributor.authorLesage, Anneen
dc.contributor.authorBendjeriou-Sedjerari, Anissaen
dc.contributor.authorEmsley, Lyndonen
dc.contributor.authorBasset, Jean-Marieen
dc.date.accessioned2017-02-09T12:55:03Z-
dc.date.available2017-02-09T12:55:03Z-
dc.date.issued2016-08-15en
dc.identifier.citationPump E, Viger-Gravel J, Abou-Hamad E, Samantaray MK, Hamzaoui B, et al. (2017) Reactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopy. Chem Sci 8: 284–290. Available: http://dx.doi.org/10.1039/c6sc02379g.en
dc.identifier.issn2041-6520en
dc.identifier.issn2041-6539en
dc.identifier.doi10.1039/c6sc02379gen
dc.identifier.urihttp://hdl.handle.net/10754/622857-
dc.description.abstractDynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy (DNP SENS) is an emerging technique that allows access to high-sensitivity NMR spectra from surfaces. However, DNP SENS usually requires the use of radicals as an exogenous source of polarization, which has so far limited applications for organometallic surface species to those that do not react with the radicals. Here we show that reactive surface species can be studied if they are immobilized inside porous materials with suitably small windows, and if bulky nitroxide bi-radicals (here TEKPol) are used as the polarization source and which cannot enter the pores. The method is demonstrated by obtaining significant DNP enhancements from highly reactive complelxes [(equivalent to Si-O-)W(Me)(5)] supported on MCM-41, and effects of pore size (6.0, 3.0 and 2.5 nm) on the performance are discussed.en
dc.description.sponsorshipThis work received support from the King Abdullah University of Science and Technology (KAUST) and ERC Advanced Grant No. 320860. We thank Dr Olivier Ouari and Paul Tordo from the University of Aix-Marseille, for providing the TEKPol radical.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2017/SC/C6SC02379G#!divAbstracten
dc.rightsThis article is licensed under a Creative Commons Attribution 3.0 Unported Licence.en
dc.rights.urihttp://creativecommons.org/licenses/by/3.0/en
dc.titleReactive surface organometallic complexes observed using dynamic nuclear polarization surface enhanced NMR spectroscopyen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentImaging and Characterization Core Laben
dc.identifier.journalChem. Sci.en
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerlanden
dc.contributor.institutionInstitut de Sciences Analytiques (CNRS/ENS-Lyon/UCB-Lyon 1), Université de Lyon, Centre de RMN à Très Hauts Champs, 69100 Villeurbanne, Franceen
kaust.authorPump, Evaen
kaust.authorAbou-Hamad, Edyen
kaust.authorSamantaray, Manojaen
kaust.authorHamzaoui, Bilelen
kaust.authorGurinov, Andreien
kaust.authorAnjum, Dalaver H.en
kaust.authorBendjeriou-Sedjerari, Anissaen
kaust.authorBasset, Jean-Marieen
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