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Title: Atomic structure of Pt nanoclusters supported by graphene/Ir(111) and reversible transformation under CO exposure

Abstract

We investigate the atomic structure of graphene/Ir(111) supported platinum clusters with on average fewer than 40 atoms by means of surface x-ray diffraction (SXRD), grazing incidence small angle x-ray scattering (GISAXS), and normal incidence x-ray standing waves (NIXSW) measurements, in comparison with density functional theory calculations (DFT). GISAXS revealed that the clusters with 1.3 nm diameter form a regular array with domain sizes of 90 nm. SXRD shows that the 1–2 monolayer high, (111) oriented Pt nanoparticles grow epitaxially on the graphene support. From the combined analysis of the SXRD and NIXSW data, a three-dimensional (3D) structural model of the clusters and the graphene support can be deduced which is in line with the DFT results. For the clusters grown in ultrahigh vacuum the lattice parameter is reduced by (4.6±0.1)% compared to bulk platinum. The graphene layer undergoes a strong Pt adsorption induced buckling, caused by a rehybridization of the carbon atoms below the cluster. Lastly, in situ observation of the Pt clusters in CO and O2 environments revealed a reversible change of the clusters' strain state while successively dosing CO at room temperature and O2 at 575 K, pointing to a CO oxidation activity of the Pt clusters.

Authors:
 [1];  [2];  [2];  [3];  [4];  [5];  [4];  [4];  [6];  [7];  [7]
+ Show Author Affiliations
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany); Univ. Siegen, Siegen (Germany)
  2. Univ. Grenoble Alpes, Grenoble (France); CNRS, Inst Neel, Grenoble (France)
  3. Univ. Grenoble Alpes, Grenoble (France); Commissariat a l'Energie Atomique et aux Energies Alternatives (CEA), Grenoble (France)
  4. Univ. zu Koln (Germany)
  5. Univ. zu Koln (Germany); Peter Grunberg Inst., Julich (Germany)
  6. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1248613
Alternate Identifier(s):
OSTI ID: 1236086
Report Number(s):
SAND-2016-0693J
Journal ID: ISSN 2469-9950; 618860
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; Journal Issue: 4; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Franz, Dirk, Blanc, Nils, Coraux, Johann, Renaud, Gilles, Runte, Sven, Gerber, Timm, Busse, Carsten, Michely, Thomas, Feibelman, Peter J., Hejral, Uta, and Stierle, Andreas. Atomic structure of Pt nanoclusters supported by graphene/Ir(111) and reversible transformation under CO exposure. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.93.045426.
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Franz, Dirk, Blanc, Nils, Coraux, Johann, Renaud, Gilles, Runte, Sven, Gerber, Timm, Busse, Carsten, Michely, Thomas, Feibelman, Peter J., Hejral, Uta, & Stierle, Andreas. Atomic structure of Pt nanoclusters supported by graphene/Ir(111) and reversible transformation under CO exposure. United States. https://doi.org/10.1103/PhysRevB.93.045426
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Franz, Dirk, Blanc, Nils, Coraux, Johann, Renaud, Gilles, Runte, Sven, Gerber, Timm, Busse, Carsten, Michely, Thomas, Feibelman, Peter J., Hejral, Uta, and Stierle, Andreas. Tue . "Atomic structure of Pt nanoclusters supported by graphene/Ir(111) and reversible transformation under CO exposure". United States. https://doi.org/10.1103/PhysRevB.93.045426. https://www.osti.gov/servlets/purl/1248613.
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@article{osti_1248613,
title = {Atomic structure of Pt nanoclusters supported by graphene/Ir(111) and reversible transformation under CO exposure},
author = {Franz, Dirk and Blanc, Nils and Coraux, Johann and Renaud, Gilles and Runte, Sven and Gerber, Timm and Busse, Carsten and Michely, Thomas and Feibelman, Peter J. and Hejral, Uta and Stierle, Andreas},
abstractNote = {We investigate the atomic structure of graphene/Ir(111) supported platinum clusters with on average fewer than 40 atoms by means of surface x-ray diffraction (SXRD), grazing incidence small angle x-ray scattering (GISAXS), and normal incidence x-ray standing waves (NIXSW) measurements, in comparison with density functional theory calculations (DFT). GISAXS revealed that the clusters with 1.3 nm diameter form a regular array with domain sizes of 90 nm. SXRD shows that the 1–2 monolayer high, (111) oriented Pt nanoparticles grow epitaxially on the graphene support. From the combined analysis of the SXRD and NIXSW data, a three-dimensional (3D) structural model of the clusters and the graphene support can be deduced which is in line with the DFT results. For the clusters grown in ultrahigh vacuum the lattice parameter is reduced by (4.6±0.1)% compared to bulk platinum. The graphene layer undergoes a strong Pt adsorption induced buckling, caused by a rehybridization of the carbon atoms below the cluster. Lastly, in situ observation of the Pt clusters in CO and O2 environments revealed a reversible change of the clusters' strain state while successively dosing CO at room temperature and O2 at 575 K, pointing to a CO oxidation activity of the Pt clusters.},
doi = {10.1103/PhysRevB.93.045426},
journal = {Physical Review B},
number = 4,
volume = 93,
place = {United States},
year = {Tue Jan 26 00:00:00 EST 2016},
month = {Tue Jan 26 00:00:00 EST 2016}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1103/PhysRevB.93.045426
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Cited by: 20 works
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Figures / Tables:

FIG. 1 FIG. 1: (Color online) Map of reciprocal space: The (1,0), (2,0) and (1,1) rods were measured with GISAXS (green circles). The lines at (9,9) and (9,-9) indicate the first order crystal truncation rods of Ir(111), graphene rods resulting from carbon - carbon spacing are located at (10,0) and (10,-10) (bluemore » circles), grey circles indicate positions of additional cluster lattice rods which were measured.« less
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    Works referencing / citing this record:

    Bimetallic Pd–Pt alloy nanocluster arrays on graphene/Rh(111): formation, stability, and dynamics
    journal, January 2018

    • Düll, Fabian; Bauer, Udo; Späth, Florian
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 33
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    Pseudo-ordered distribution of Ir nanocrystals on h-BN
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    • Martínez-Galera, Antonio J.; Gómez-Rodríguez, José M.
    • Nanoscale, Vol. 11, Issue 5
    • DOI: 10.1039/c8nr08928k

    Growth and stability of Pt nanoclusters from 1 to 50 atoms on h-BN/Rh(111)
    journal, January 2019

    • Düll, Fabian; Meusel, Manuel; Späth, Florian
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 38
    • DOI: 10.1039/c9cp04095a

    Magnetic properties of supported metal atoms and clusters
    journal, October 2016

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