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Title: Insight into restructuring of Pd-Au nanoparticles using EXAFS

Abstract

We acquired Pd K-edge and Au L3-edge EXAFS spectra of two libraries of titania-supported Pd-doped Au nanoparticle catalysts representing the as-prepared and post-catalysis state. The nanoparticles have narrow particle size distributions, in the range 2.8–6.6 nm, and were synthesized to preferentially locate the palladium atoms on the surface of a gold core, with Pd mole fractions of 1.4–38%. EXAFS spectra of both the as-prepared samples and post-catalysis Pd-Au particles were collected and modeled. EXAFS refinement of all samples showed contributions from both Pd-Au and Pd-Pd scattering paths, revealing that Pd and Au components alloyed together. Pd was in a partially oxidized state as evidenced by a Pd-O scattering contribution, unlike Au. Overlaying measured coordination numbers from the libraries with predicted values, using models of surface and bulk alloying, showed that Pd restructures among Au as a result of exposure to the reaction conditions.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1]
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  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Stony Brook Univ., NY (United States)
  3. Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis
  4. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1769959
Alternate Identifier(s):
OSTI ID: 1634256
Grant/Contract Number:  
AC02-76SF00515; FG02-03ER15476; AC02-06CH11357; ECCS-1542152
Resource Type:
Accepted Manuscript
Journal Name:
Radiation Physics and Chemistry (1993)
Additional Journal Information:
Journal Name: Radiation Physics and Chemistry (1993); Journal Volume: 175; Journal ID: ISSN 0969-806X
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Dilute alloy; Palladium; Gold; Catalyst; Multi-edge EXAFS; Structural model

Citation Formats

Boubnov, Alexey, Timoshenko, Janis, Wrasman, Cody J., Hoffman, Adam S., Cargnello, Matteo, Frenkel, Anatoly I., and Bare, Simon R. Insight into restructuring of Pd-Au nanoparticles using EXAFS. United States: N. p., 2019. Web. doi:10.1016/j.radphyschem.2019.04.054.
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Boubnov, Alexey, Timoshenko, Janis, Wrasman, Cody J., Hoffman, Adam S., Cargnello, Matteo, Frenkel, Anatoly I., & Bare, Simon R. Insight into restructuring of Pd-Au nanoparticles using EXAFS. United States. https://doi.org/10.1016/j.radphyschem.2019.04.054
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Boubnov, Alexey, Timoshenko, Janis, Wrasman, Cody J., Hoffman, Adam S., Cargnello, Matteo, Frenkel, Anatoly I., and Bare, Simon R. Mon . "Insight into restructuring of Pd-Au nanoparticles using EXAFS". United States. https://doi.org/10.1016/j.radphyschem.2019.04.054. https://www.osti.gov/servlets/purl/1769959.
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@article{osti_1769959,
title = {Insight into restructuring of Pd-Au nanoparticles using EXAFS},
author = {Boubnov, Alexey and Timoshenko, Janis and Wrasman, Cody J. and Hoffman, Adam S. and Cargnello, Matteo and Frenkel, Anatoly I. and Bare, Simon R.},
abstractNote = {We acquired Pd K-edge and Au L3-edge EXAFS spectra of two libraries of titania-supported Pd-doped Au nanoparticle catalysts representing the as-prepared and post-catalysis state. The nanoparticles have narrow particle size distributions, in the range 2.8–6.6 nm, and were synthesized to preferentially locate the palladium atoms on the surface of a gold core, with Pd mole fractions of 1.4–38%. EXAFS spectra of both the as-prepared samples and post-catalysis Pd-Au particles were collected and modeled. EXAFS refinement of all samples showed contributions from both Pd-Au and Pd-Pd scattering paths, revealing that Pd and Au components alloyed together. Pd was in a partially oxidized state as evidenced by a Pd-O scattering contribution, unlike Au. Overlaying measured coordination numbers from the libraries with predicted values, using models of surface and bulk alloying, showed that Pd restructures among Au as a result of exposure to the reaction conditions.},
doi = {10.1016/j.radphyschem.2019.04.054},
journal = {Radiation Physics and Chemistry (1993)},
number = ,
volume = 175,
place = {United States},
year = {Mon Apr 29 00:00:00 EDT 2019},
month = {Mon Apr 29 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1016/j.radphyschem.2019.04.054
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Works referenced in this record:

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journal, December 2018

Uniform Bimetallic Nanocrystals by High-Temperature Seed-Mediated Colloidal Synthesis and Their Catalytic Properties for Semiconducting Nanowire Growth
journal, August 2015

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