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Pd–Au–Cu Ternary Alloy Nanoparticles: Highly Tunable and Economical Nitrite Reduction Catalysts
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    Pd–Au–Cu Ternary Alloy Nanoparticles: Highly Tunable and Economical Nitrite Reduction Catalysts
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    • Pranaw Kunal
      Pranaw Kunal
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
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    • Chenxu Yan
      Chenxu Yan
      Department of Civil, Architectural and Environmental Engineering, The University of Texas at Austin, 301 E. Dean Keeton Street, Stop C1700, Austin, Texas 78712. United States
      More by Chenxu Yan
    • Hongyu Guo
      Hongyu Guo
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
      More by Hongyu Guo
    • Hao Li
      Hao Li
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
      More by Hao Li
    • Carolyn E. Brady
      Carolyn E. Brady
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
      Department of Civil, Architectural and Environmental Engineering, The University of Texas at Austin, 301 E. Dean Keeton Street, Stop C1700, Austin, Texas 78712. United States
    • Michael Duncan
      Michael Duncan
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
    • Xun Zhan
      Xun Zhan
      Texas Materials Institute, The University of Texas at Austin, 204 E. Dean Keeton St. Stop C2201, Austin, Texas 78712-1591, United States
      More by Xun Zhan
    • Charles J. Werth*
      Charles J. Werth
      Department of Civil, Architectural and Environmental Engineering, The University of Texas at Austin, 301 E. Dean Keeton Street, Stop C1700, Austin, Texas 78712. United States
      *Email: [email protected]
    • Graeme Henkelman*
      Graeme Henkelman
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
      Texas Materials Institute, The University of Texas at Austin, 204 E. Dean Keeton St. Stop C2201, Austin, Texas 78712-1591, United States
      *Email: [email protected]
    • Simon M. Humphrey*
      Simon M. Humphrey
      Department of Chemistry, The University of Texas at Austin, Welch Hall 2.204, 105 E 24th St. Stop A5300, Austin, Texas 78712-1224, United States
      Texas Materials Institute, The University of Texas at Austin, 204 E. Dean Keeton St. Stop C2201, Austin, Texas 78712-1591, United States
      *Email: [email protected]
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    ACS Catalysis

    Cite this: ACS Catal. 2023, 13, 18, 11945–11953
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c01676
    Published August 28, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Solid-solution ternary Pd–Au–Cu nanoparticles (NPs) with broadly tunable compositions (PdxAuyCu100–(x+y); where x = 30–70 and y = 15–35) were prepared by a microwave-assisted polyol reduction method. Commercially available Pd2+, Au3+, and Cu2+ salts were directly co-reduced by ethylene glycol and NaBH4 in a one-pot process to generate near-monodisperse ternary alloy NPs with mean sizes between 2 and 4 nm. Using the same synthetic approach, the corresponding binary alloy PdCu NPs with similar monodispersities and particle sizes were also prepared. The comparative catalytic performances of PdCu NPs and PdAuCu NPs were assessed for the aqueous-phase reduction of nitrate (NO3) anions and were compared to previously published results for analogous binary PdAu NPs. The experimental catalytic results and theoretical studies reveal that the resulting catalytic activity of Pd surface sites are highly sensitive to the relative amounts of Au and Cu also present. We ultimately prove that the hitherto unstudied ternary PdAuCu NPs are highly active and selective as NO2 reduction catalysts and effectively utilize Cu as an economically viable dilutant metal, without sacrificing the activity or stability of industrially important and well-studied PdAu alloy catalysts. From an economic perspective, the ternary alloy nanocatalysts show superior price-to-activity ratios: the measured turnover rates of Pd63Au22Cu16 NPs (3.353 min–1 $–1) outperform not only monometallic Pd NPs (0.797 min–1 $–1) but also binary PdAu NPs and PdCu NPs of all accessible compositions.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.3c01676.

    • Detailed experimental methods, PXRD patterns, TEM images, HRTEM images, EDS mapping, Cu Auger spectra for PdCu and PdAuCuNPs, TEM images for catalysts after nitrite reduction, additional catalysis, and DFT information (PDF)

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    This article is cited by 9 publications.

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    ACS Catalysis

    Cite this: ACS Catal. 2023, 13, 18, 11945–11953
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c01676
    Published August 28, 2023
    Copyright © 2023 American Chemical Society

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