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dc.contributor.authorPump, Eva
dc.contributor.authorBendjeriou-Sedjerari, Anissa
dc.contributor.authorViger-Gravel, Jasmine
dc.contributor.authorGajan, David
dc.contributor.authorScotto, Baptiste
dc.contributor.authorSamantaray, Manoja
dc.contributor.authorAbou-Hamad, Edy
dc.contributor.authorGurinov, Andrei
dc.contributor.authorAlmaksoud, Walid
dc.contributor.authorCao, Zhen
dc.contributor.authorLesage, Anne
dc.contributor.authorCavallo, Luigi
dc.contributor.authorEmsley, Lyndon
dc.contributor.authorBasset, Jean-Marie
dc.date.accessioned2018-09-03T13:25:04Z
dc.date.available2018-09-03T13:25:04Z
dc.date.issued2018
dc.identifier.citationPump E, Bendjeriou-Sedjerari A, Viger-Gravel J, Gajan D, Scotto B, et al. (2018) Predicting the DNP-SENS efficiency in reactive heterogeneous catalysts from hydrophilicity. Chemical Science 9: 4866–4872. Available: http://dx.doi.org/10.1039/c8sc00532j.
dc.identifier.issn2041-6520
dc.identifier.issn2041-6539
dc.identifier.doi10.1039/c8sc00532j
dc.identifier.urihttp://hdl.handle.net/10754/628455
dc.description.abstractIdentification of surfaces at the molecular level has benefited from progress in dynamic nuclear polarization surface enhanced NMR spectroscopy (DNP SENS). However, the technique is limited when using highly sensitive heterogeneous catalysts due to secondary reaction of surface organometallic fragments (SOMFs) with stable radical polarization agents. Here, we observe that in non-porous silica nanoparticles (NPs) (d = 15 nm) some DNP enhanced NMR or SENS characterizations are possible, depending on the metal-loading of the SOMF and the type of SOMF substituents (methyl, isobutyl, neopentyl). This unexpected observation suggests that aggregation of the nanoparticles occurs in non-polar solvents (such as ortho-dichlorobenzene) leading to (partial) protection of the SOMF inside the interparticle space, thereby preventing reaction with bulky polarization agents. We discover that the DNP SENS efficiency is correlated with the hydrophilicity of the SOMF/support, which depends on the carbon and SOMF concentration. Nitrogen sorption measurements to determine the BET constant (C) were performed. This constant allows us to predict the aggregation of silica nanoparticles and consequently the efficiency of DNP SENS. Under optimal conditions, C > 60, we found signal enhancement factors of up to 30.
dc.description.sponsorshipThis work received support from the King Abdullah University of Science and Technology (KAUST) and the European Research Council (ERC Advanced Grant No. 320860).
dc.publisherRoyal Society of Chemistry (RSC)
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2018/SC/C8SC00532J#!divAbstract
dc.rightsThis Open Access Article is licensed under a Creative Commons Attribution-Non Commercial 3.0 Unported Licence
dc.rights.urihttp://creativecommons.org/licenses/by-nc/3.0/
dc.titlePredicting the DNP-SENS efficiency in reactive heterogeneous catalysts from hydrophilicity
dc.typeArticle
dc.contributor.departmentChemical Science Program
dc.contributor.departmentImaging and Characterization Core Lab
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentNMR
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalChemical Science
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionInstitut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne, CH-1015, , , Switzerland
dc.contributor.institutionInstitut de Sciences Analytiques (CNRS/ENS-Lyon/UCB-Lyon 1), Université de Lyon, Centre de RMN À Très Hauts Champs, Villeurbanne, 69100, , , , France
kaust.personPump, Eva
kaust.personBendjeriou-Sedjerari, Anissa
kaust.personScotto, Baptiste
kaust.personSamantaray, Manoja
kaust.personAbou-Hamad, Edy
kaust.personGurinov, Andrei
kaust.personAlmaksoud, Walid
kaust.personCao, Zhen
kaust.personCavallo, Luigi
kaust.personBasset, Jean-Marie
refterms.dateFOA2018-09-05T12:48:11Z


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This Open Access Article is licensed under a Creative Commons Attribution-Non Commercial 3.0 Unported Licence
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