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dc.contributor.authorCano, Israel
dc.contributor.authorWeilhard, Andreas
dc.contributor.authorMartin, Carmen
dc.contributor.authorPinto, Jose
dc.contributor.authorLodge, Rhys W
dc.contributor.authorSantos, Ana R
dc.contributor.authorRance, Graham A
dc.contributor.authorÅhlgren, Elina Harriet
dc.contributor.authorJónsson, Erlendur
dc.contributor.authorYuan, Jun
dc.contributor.authorLi, Ziyou Y
dc.contributor.authorLicence, Peter
dc.contributor.authorKhlobystov, Andrei N
dc.contributor.authorAlves Fernandes, Jesum
dc.date.accessioned2021-10-25T23:30:32Z
dc.date.available2021-10-25T23:30:32Z
dc.date.issued2021-08-17
dc.identifier.issn2041-1723
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/329865
dc.description.abstractUsing a magnetron sputtering approach that allows size-controlled formation of nanoclusters, we have created palladium nanoclusters that combine the features of both heterogeneous and homogeneous catalysts. Here we report the atomic structures and electronic environments of a series of metal nanoclusters in ionic liquids at different stages of formation, leading to the discovery of Pd nanoclusters with a core of ca. 2 nm surrounded by a diffuse dynamic shell of atoms in [C4C1Im][NTf2]. Comparison of the catalytic activity of Pd nanoclusters in alkene cyclopropanation reveals that the atomically dynamic surface is critically important, increasing the activity by a factor of ca. 2 when compared to compact nanoclusters of similar size. Catalyst poisoning tests using mercury and dibenzo[a,e]cyclooctene show that dynamic Pd nanoclusters maintain their catalytic activity, which demonstrate their combined features of homogeneous and heterogeneous catalysts within the same material. Additionally, kinetic studies of cyclopropanation of alkenes mediated by the dynamic Pd nanoclusters reveal an observed catalyst order of 1, underpinning the pseudo-homogeneous character of the dynamic Pd nanoclusters.
dc.format.mediumElectronic
dc.languageeng
dc.publisherSpringer Science and Business Media LLC
dc.rightsAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.titleBlurring the boundary between homogenous and heterogeneous catalysis using palladium nanoclusters with dynamic surfaces.
dc.typeArticle
prism.issueIdentifier1
prism.publicationDate2021
prism.publicationNameNat Commun
prism.startingPage4965
prism.volume12
dc.identifier.doi10.17863/CAM.77310
dcterms.dateAccepted2021-07-29
rioxxterms.versionofrecord10.1038/s41467-021-25263-6
rioxxterms.versionVoR
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.licenseref.startdate2021-08-17
dc.contributor.orcidMartin, Carmen [0000-0001-8687-6887]
dc.contributor.orcidSantos, Ana R [0000-0003-0998-4571]
dc.contributor.orcidJónsson, Erlendur [0000-0002-7776-0484]
dc.contributor.orcidYuan, Jun [0000-0002-6240-7151]
dc.contributor.orcidLicence, Peter [0000-0003-2992-0153]
dc.contributor.orcidKhlobystov, Andrei N [0000-0001-7738-4098]
dc.contributor.orcidAlves Fernandes, Jesum [0000-0002-0468-7343]
dc.identifier.eissn2041-1723
rioxxterms.typeJournal Article/Review
cam.issuedOnline2021-08-17


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Attribution 4.0 International
Except where otherwise noted, this item's licence is described as Attribution 4.0 International