Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications

Handle URI:
http://hdl.handle.net/10754/625589
Title:
Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications
Authors:
Rondelli, Manuel; Zwaschka, Gregor; Krause, Maximilian; Rötzer, Marian D.; Hedhili, Mohamed N. ( 0000-0002-3624-036X ) ; Hogerl, Manuel Peter; D’Elia, Valerio ( 0000-0002-5881-2496 ) ; Schweinberger, Florian F.; Basset, Jean-Marie ( 0000-0003-3166-8882 ) ; Heiz, Ueli
Abstract:
The use of physicochemical preparation techniques of metal clusters in the ultrahigh vacuum (UHV) allows for high control of cluster nuclearity and size distribution for fundamental studies in catalysis. Surprisingly, the potential of these systems as catalysts for organic chemistry transformations in solution has not been explored. To this end, single Pt atoms and Pt clusters with two narrow size distributions were prepared in the UHV and applied for the hydrogenation of p-chloronitrobenzene to p-chloroaniline in ethanol. Following the observation of very high catalytic turnovers (approaching the million molecules of p-nitroaniline formed per Pt cluster) and of size-dependent activity, this work addresses fundamental questions with respect to the suitability of these systems as heterogeneous catalysts for the conversion of solution-phase reagents. For this purpose, we employ scanning transmission electron microscopy (STEM) and X-ray photoelectron spectroscopy (XPS) characterization before and after reaction to assess the stability of the clusters on the support and the question of heterogeneity versus homogeneity in the catalytic process.
KAUST Department:
Imaging and Characterization Core Lab; KAUST Catalysis Center (KCC)
Citation:
Rondelli M, Zwaschka G, Krause M, Rötzer MD, Hedhili MN, et al. (2017) Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications. ACS Catalysis 7: 4152–4162. Available: http://dx.doi.org/10.1021/acscatal.7b00520.
Publisher:
American Chemical Society (ACS)
Journal:
ACS Catalysis
KAUST Grant Number:
KSA-C0069/UKC0020
Issue Date:
10-May-2017
DOI:
10.1021/acscatal.7b00520
Type:
Article
ISSN:
2155-5435; 2155-5435
Sponsors:
This project was supported through collaboration with the King Abdullah University of Saudi-Arabia (Grant No. KSA-C0069/UKC0020). Further, U.H. and F.F.S. acknowledge financial support through DFG project HE3454/23-1. The authors thank Salim Sioud at the
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/acscatal.7b00520
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorRondelli, Manuelen
dc.contributor.authorZwaschka, Gregoren
dc.contributor.authorKrause, Maximilianen
dc.contributor.authorRötzer, Marian D.en
dc.contributor.authorHedhili, Mohamed N.en
dc.contributor.authorHogerl, Manuel Peteren
dc.contributor.authorD’Elia, Valerioen
dc.contributor.authorSchweinberger, Florian F.en
dc.contributor.authorBasset, Jean-Marieen
dc.contributor.authorHeiz, Uelien
dc.date.accessioned2017-10-03T12:49:27Z-
dc.date.available2017-10-03T12:49:27Z-
dc.date.issued2017-05-10en
dc.identifier.citationRondelli M, Zwaschka G, Krause M, Rötzer MD, Hedhili MN, et al. (2017) Exploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applications. ACS Catalysis 7: 4152–4162. Available: http://dx.doi.org/10.1021/acscatal.7b00520.en
dc.identifier.issn2155-5435en
dc.identifier.issn2155-5435en
dc.identifier.doi10.1021/acscatal.7b00520en
dc.identifier.urihttp://hdl.handle.net/10754/625589-
dc.description.abstractThe use of physicochemical preparation techniques of metal clusters in the ultrahigh vacuum (UHV) allows for high control of cluster nuclearity and size distribution for fundamental studies in catalysis. Surprisingly, the potential of these systems as catalysts for organic chemistry transformations in solution has not been explored. To this end, single Pt atoms and Pt clusters with two narrow size distributions were prepared in the UHV and applied for the hydrogenation of p-chloronitrobenzene to p-chloroaniline in ethanol. Following the observation of very high catalytic turnovers (approaching the million molecules of p-nitroaniline formed per Pt cluster) and of size-dependent activity, this work addresses fundamental questions with respect to the suitability of these systems as heterogeneous catalysts for the conversion of solution-phase reagents. For this purpose, we employ scanning transmission electron microscopy (STEM) and X-ray photoelectron spectroscopy (XPS) characterization before and after reaction to assess the stability of the clusters on the support and the question of heterogeneity versus homogeneity in the catalytic process.en
dc.description.sponsorshipThis project was supported through collaboration with the King Abdullah University of Saudi-Arabia (Grant No. KSA-C0069/UKC0020). Further, U.H. and F.F.S. acknowledge financial support through DFG project HE3454/23-1. The authors thank Salim Sioud at theen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/acscatal.7b00520en
dc.subjectsubnanometer cluster catalystsen
dc.subjectPt atom catalysisen
dc.subjectsingle atom catalysisen
dc.subjecthydrogenationen
dc.subjectsize effectsen
dc.titleExploring the Potential of Different-Sized Supported Subnanometer Pt Clusters as Catalysts for Wet Chemical Applicationsen
dc.typeArticleen
dc.contributor.departmentImaging and Characterization Core Laben
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.identifier.journalACS Catalysisen
dc.contributor.institutionTechnical University of Munich, Catalysis Research Center and Chemistry Department, Chair of Physical Chemistry, Ernst-Otto-Fischer-Straße 1 and Lichtenbergstraße 4, 85748 Garching, Germanyen
dc.contributor.institutionVidyasirimedhi Institute of Science and Technology (VISTEC), School of Materials Science and Engineering, 21210, Payupnai, WangChan, Rayong, Thailanden
kaust.authorHedhili, Mohamed N.en
kaust.authorHogerl, Manuel Peteren
kaust.authorD’Elia, Valerioen
kaust.authorBasset, Jean-Marieen
kaust.grant.numberKSA-C0069/UKC0020en
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