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Title: Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts

Abstract

Dilute alloy materials hold great promise for enhancing selectivity in catalytic reactions. A major challenge with such catalytic materials is developing supported alloy nanoparticles (NPs) with a catalytically optimal composition that are stable with respect to sintering. Here, we demonstrate that NP Pd/Au catalysts with minor concentrations of Pd prepared by a colloid-templating approach are active for oxygen dissociation and catalytic oxidation, as exemplified by CO oxidation. Using electron microscopic imaging, infrared spectroscopy, and X-ray photoelectron spectroscopy, we demonstrate that Pd is stabilized within the Au nanoparticle in its metallic state with minor amounts of Pd at the surface. The Pd–Au nanoparticles are embedded in the colloidally templated silica and form a thermally stable catalyst at high temperature. Surface analysis by diffuse reflectance infrared spectroscopy indicates that the Pd atomic distribution at the surface varies with the bulk concentration, forming isolated Pd atoms at 2% Pd and a mixture of Pd monomers and small Pd clusters at 9% Pd. X-ray absorption fine structure analysis indicates that Pd is well distributed in the bulk of the nanoparticle. In conclusion, in-depth understanding of this new class of catalytic materials opens the way to a wide array of possibilities for crucial enhancement ofmore » activity and selectivity in catalysis.« less

Authors:
 [1];  [1];  [1];  [2]; ORCiD logo [1];  [3];  [3];  [1]; ORCiD logo [4];  [1]; ORCiD logo; ORCiD logo
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  1. Harvard Univ., Cambridge, MA (United States)
  2. Stony Brook Univ., NY (United States)
  3. Tufts Univ., Medford, MA (United States)
  4. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1560004
Report Number(s):
BNL-212061-2019-JAAM
Journal ID: ISSN 0897-4756; TRN: US2000442
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 15; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY

Citation Formats

Luneau, Mathilde, Shirman, Tanya, Filie, Amanda, Timoshenko, Janis, Chen, Wei, Trimpalis, Antonios, Flytzani-Stephanopoulos, Maria, Kaxiras, Efthimios, Frenkel, Anatoly I., Aizenberg, Joanna, Friend, Cynthia M., and Madix, Robert J. Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b01779.
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Luneau, Mathilde, Shirman, Tanya, Filie, Amanda, Timoshenko, Janis, Chen, Wei, Trimpalis, Antonios, Flytzani-Stephanopoulos, Maria, Kaxiras, Efthimios, Frenkel, Anatoly I., Aizenberg, Joanna, Friend, Cynthia M., & Madix, Robert J. Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts. United States. https://doi.org/10.1021/acs.chemmater.9b01779
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Luneau, Mathilde, Shirman, Tanya, Filie, Amanda, Timoshenko, Janis, Chen, Wei, Trimpalis, Antonios, Flytzani-Stephanopoulos, Maria, Kaxiras, Efthimios, Frenkel, Anatoly I., Aizenberg, Joanna, Friend, Cynthia M., and Madix, Robert J. Wed . "Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts". United States. https://doi.org/10.1021/acs.chemmater.9b01779. https://www.osti.gov/servlets/purl/1560004.
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@article{osti_1560004,
title = {Dilute Pd/Au Alloy Nanoparticles Embedded in Colloid-Templated Porous SiO2 : Stable Au-Based Oxidation Catalysts},
author = {Luneau, Mathilde and Shirman, Tanya and Filie, Amanda and Timoshenko, Janis and Chen, Wei and Trimpalis, Antonios and Flytzani-Stephanopoulos, Maria and Kaxiras, Efthimios and Frenkel, Anatoly I. and Aizenberg, Joanna and Friend, Cynthia M. and Madix, Robert J.},
abstractNote = {Dilute alloy materials hold great promise for enhancing selectivity in catalytic reactions. A major challenge with such catalytic materials is developing supported alloy nanoparticles (NPs) with a catalytically optimal composition that are stable with respect to sintering. Here, we demonstrate that NP Pd/Au catalysts with minor concentrations of Pd prepared by a colloid-templating approach are active for oxygen dissociation and catalytic oxidation, as exemplified by CO oxidation. Using electron microscopic imaging, infrared spectroscopy, and X-ray photoelectron spectroscopy, we demonstrate that Pd is stabilized within the Au nanoparticle in its metallic state with minor amounts of Pd at the surface. The Pd–Au nanoparticles are embedded in the colloidally templated silica and form a thermally stable catalyst at high temperature. Surface analysis by diffuse reflectance infrared spectroscopy indicates that the Pd atomic distribution at the surface varies with the bulk concentration, forming isolated Pd atoms at 2% Pd and a mixture of Pd monomers and small Pd clusters at 9% Pd. X-ray absorption fine structure analysis indicates that Pd is well distributed in the bulk of the nanoparticle. In conclusion, in-depth understanding of this new class of catalytic materials opens the way to a wide array of possibilities for crucial enhancement of activity and selectivity in catalysis.},
doi = {10.1021/acs.chemmater.9b01779},
journal = {Chemistry of Materials},
number = 15,
volume = 31,
place = {United States},
year = {Wed Jul 10 00:00:00 EDT 2019},
month = {Wed Jul 10 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.chemmater.9b01779
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Cited by: 36 works
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Figures / Tables:

Table 1 Table 1: PdxAu1-x nanoparticles size is preserved after final calcination at 500°C in air
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    Works referencing / citing this record:

    New Role of Pd Hydride as a Sensor of Surface Pd Distributions in Pd−Au Catalysts
    journal, December 2019

    • Guan, Erjia; Foucher, Alexandre C.; Marcella, Nicholas
    • ChemCatChem, Vol. 12, Issue 3
    • DOI: 10.1002/cctc.201901847

    Au/TiO2 for Ethane Dehydrogenation: Effect of Silica Doping
    journal, February 2020

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