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Title: Gas-Induced Segregation in Pt-Rh Alloy Nanoparticles Observed by In Situ Bragg Coherent Diffraction Imaging

Abstract

Bimetallic catalysts can undergo segregation or redistribution of the metals driven by oxidizing and reducing environments. Bragg coherent diffraction imaging (BCDI) was used to relate displacement fields to compositional distributions in crystalline Pt-Rh alloy nanoparticles. Three-dimensional images of internal composition showed that the radial distribution of compositions reverses partially between the surface shell and the core when gas flow changes between O2 and H2. Our observation suggests that the elemental segregation of nanoparticle catalysts should be highly active during heterogeneous catalysis and can be a controlling factor in synthesis of electrocatalysts. Additionally, our study exemplifies applications of BCDI for in situ 3D imaging of internal equilibrium compositions in other bimetallic alloy nanoparticles.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3];  [3]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [6]; ORCiD logo [2]; ORCiD logo [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Tohoku Univ., Sendai (Japan)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. Hamburg, Hamburg (Germany)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States); Tesla, Inc., Palo Alto, CA (United States)
  6. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); National Research Nuclear Univ. MEPhI, Moscow (Russia)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1579194
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 123; Journal Issue: 24; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Kawaguchi, Tomoya, Keller, Thomas F., Runge, Henning, Gelisio, Luca, Seitz, Christoph, Kim, Young Yong, Maxey, Evan R., Cha, Wonsuk, Ulvestad, Andrew, Hruszkewycz, Stephan O., Harder, Ross, Vartanyants, Ivan A., Stierle, Andreas, and You, Hoydoo. Gas-Induced Segregation in Pt-Rh Alloy Nanoparticles Observed by In Situ Bragg Coherent Diffraction Imaging. United States: N. p., 2019. Web. doi:10.1103/PhysRevLett.123.246001.
Kawaguchi, Tomoya, Keller, Thomas F., Runge, Henning, Gelisio, Luca, Seitz, Christoph, Kim, Young Yong, Maxey, Evan R., Cha, Wonsuk, Ulvestad, Andrew, Hruszkewycz, Stephan O., Harder, Ross, Vartanyants, Ivan A., Stierle, Andreas, & You, Hoydoo. Gas-Induced Segregation in Pt-Rh Alloy Nanoparticles Observed by In Situ Bragg Coherent Diffraction Imaging. United States. doi:10.1103/PhysRevLett.123.246001.
Kawaguchi, Tomoya, Keller, Thomas F., Runge, Henning, Gelisio, Luca, Seitz, Christoph, Kim, Young Yong, Maxey, Evan R., Cha, Wonsuk, Ulvestad, Andrew, Hruszkewycz, Stephan O., Harder, Ross, Vartanyants, Ivan A., Stierle, Andreas, and You, Hoydoo. Fri . "Gas-Induced Segregation in Pt-Rh Alloy Nanoparticles Observed by In Situ Bragg Coherent Diffraction Imaging". United States. doi:10.1103/PhysRevLett.123.246001.
@article{osti_1579194,
title = {Gas-Induced Segregation in Pt-Rh Alloy Nanoparticles Observed by In Situ Bragg Coherent Diffraction Imaging},
author = {Kawaguchi, Tomoya and Keller, Thomas F. and Runge, Henning and Gelisio, Luca and Seitz, Christoph and Kim, Young Yong and Maxey, Evan R. and Cha, Wonsuk and Ulvestad, Andrew and Hruszkewycz, Stephan O. and Harder, Ross and Vartanyants, Ivan A. and Stierle, Andreas and You, Hoydoo},
abstractNote = {Bimetallic catalysts can undergo segregation or redistribution of the metals driven by oxidizing and reducing environments. Bragg coherent diffraction imaging (BCDI) was used to relate displacement fields to compositional distributions in crystalline Pt-Rh alloy nanoparticles. Three-dimensional images of internal composition showed that the radial distribution of compositions reverses partially between the surface shell and the core when gas flow changes between O2 and H2. Our observation suggests that the elemental segregation of nanoparticle catalysts should be highly active during heterogeneous catalysis and can be a controlling factor in synthesis of electrocatalysts. Additionally, our study exemplifies applications of BCDI for in situ 3D imaging of internal equilibrium compositions in other bimetallic alloy nanoparticles.},
doi = {10.1103/PhysRevLett.123.246001},
journal = {Physical Review Letters},
number = 24,
volume = 123,
place = {United States},
year = {2019},
month = {12}
}

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