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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 O 2 environments revealed a reversible change of the clusters' strain state while successively dosing CO at room temperature and O 2 at 575 K, pointing to a CO oxidation activity of the Ptmore » clusters.« less

Authors:
 [1];  [2];  [2];  [3];  [4];  [5];  [4];  [4];  [6];  [7];  [7]
  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) (SC-22)
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.
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. doi:10.1103/PhysRevB.93.045426.
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. doi:10.1103/PhysRevB.93.045426. https://www.osti.gov/servlets/purl/1248613.
@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 = {2016},
month = {1}
}

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Cited by: 5 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 referenced in this record:

A review on non-precious metal electrocatalysts for PEM fuel cells
journal, January 2011

  • Chen, Zhongwei; Higgins, Drew; Yu, Aiping
  • Energy & Environmental Science, Vol. 4, Issue 9
  • DOI: 10.1039/c0ee00558d

Inorganic solid state chemically sensitive devices: electrochemical oxygen gas sensors
journal, October 1987


The Problem with Determining Atomic Structure at the Nanoscale
journal, April 2007


Illuminating surface atoms in nanoclusters by differential X-ray absorption spectroscopy
journal, January 2014

  • Spanjers, Charles S.; Senftle, Thomas P.; van Duin, Adri C. T.
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 48
  • DOI: 10.1039/C4CP02146K

Atomic Structure and Crystalline Order of Graphene-Supported Ir Nanoparticle Lattices
journal, February 2013


Nanoparticle structures served up on a tray
journal, March 2013


Structural Coherency of Graphene on Ir(111)
journal, February 2008

  • Coraux, Johann; N‘Diaye, Alpha T.; Busse, Carsten
  • Nano Letters, Vol. 8, Issue 2
  • DOI: 10.1021/nl0728874

Graphene on Ru(0001): A 25 × 25 Supercell
journal, September 2008


Graphene on metal surfaces
journal, June 2009


Graphene on Ru(0001): a corrugated and chiral structure
journal, April 2010


Structure Determination of the Coincidence Phase of Graphene on Ru(0001)
journal, April 2010


Tunable interfacial properties of epitaxial graphene on metal substrates
journal, February 2010

  • Gao, Min; Pan, Yi; Zhang, Chendong
  • Applied Physics Letters, Vol. 96, Issue 5
  • DOI: 10.1063/1.3309671

Periodically modulated geometric and electronic structure of graphene on Ru(0 0 0 1)
journal, February 2010


Two-Dimensional Ir Cluster Lattice on a Graphene Moiré on Ir(111)
journal, November 2006


A versatile fabrication method for cluster superlattices
journal, October 2009


Pinning of graphene to Ir(111) by flat Ir dots
journal, April 2008


Onset of three-dimensional Ir islands on a graphene/Ir(111) template
journal, August 2009


Clusters binding to the graphene moiré on Ir(111): X-ray photoemission compared to density functional calculations
journal, January 2012


Graphene on Ir(111): Physisorption with Chemical Modulation
journal, July 2011


Surface structure determination with X-ray standing waves
journal, October 1993


Surface diffraction beamline at ESRF
journal, February 1995

  • Ferrer, S.; Comin, F.
  • Review of Scientific Instruments, Vol. 66, Issue 2
  • DOI: 10.1063/1.1145879

Growth of graphene on Ir(111)
journal, February 2009


Integrated Intensities Using a Six-Circle Surface X-ray Diffractometer
journal, October 1997


ROD : a program for surface X-ray crystallography
journal, April 2000


X-ray standing waves and hard X-ray photoelectron spectroscopy at the insertion device beamline ID32
journal, May 2010

  • Zegenhagen, Jörg; Detlefs, Blanka; Lee, Tien-Lin
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 178-179
  • DOI: 10.1016/j.elspec.2009.09.008

Kink ordering and organized growth of Co clusters on a stepped Au(111) surface: A combined grazing-incidence x-ray scattering and STM study
journal, January 2008


Local deformations and incommensurability of high-quality epitaxial graphene on a weakly interacting transition metal
journal, December 2012


IsGISAXS : a program for grazing-incidence small-angle X-ray scattering analysis of supported islands
journal, July 2002


CO-Induced Smoluchowski Ripening of Pt Cluster Arrays on the Graphene/Ir(111) Moiré
journal, February 2013

  • Gerber, Timm; Knudsen, Jan; Feibelman, Peter J.
  • ACS Nano, Vol. 7, Issue 3
  • DOI: 10.1021/nn400082w

High-Pressure CO Oxidation on Pt(111) Monitored with Infrared−Visible Sum Frequency Generation (SFG)
journal, April 1997

  • Su, Xingcai; Cremer, Paul S.; Shen, Y. Ron
  • Journal of the American Chemical Society, Vol. 119, Issue 17
  • DOI: 10.1021/ja9638723

Topography of the graphene/Ir(111) moiré studied by surface x-ray diffraction
journal, June 2015


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