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Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnOx Supports

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    Electrocatalytic Study of the Oxygen Reduction Reaction at Gold Nanoparticles in the Absence and Presence of Interactions with SnOx Supports
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    • Nevena Ostojic
      Nevena Ostojic
      Department of Chemistry, Center for Electrochemistry, and Texas Materials Institute, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
      More by Nevena Ostojic
    • Zhiyao Duan
      Zhiyao Duan
      Department of Chemistry, Center for Electrochemistry, and Texas Materials Institute, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
      More by Zhiyao Duan
    • Aigerim Galyamova
      Aigerim Galyamova
      Department of Chemistry, Center for Electrochemistry, and Texas Materials Institute, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
      More by Aigerim Galyamova
    • Graeme Henkelman*
      Graeme Henkelman
      Department of Chemistry, Center for Electrochemistry, and Texas Materials Institute, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
      *[email protected]
      More by Graeme Henkelman
      Orcidhttp://orcid.org/0000-0002-0336-7153
    • Richard M. Crooks*
      Richard M. Crooks
      Department of Chemistry, Center for Electrochemistry, and Texas Materials Institute, The University of Texas at Austin, 105 East 24th Street, Stop A5300, Austin, Texas 78712-1224, United States
      *[email protected]
      More by Richard M. Crooks
      Orcidhttp://orcid.org/0000-0001-5186-4878
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 42, 13775–13785
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    https://doi.org/10.1021/jacs.8b08036
    Published October 12, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Here we report that density functional theory (DFT) can be used to accurately predict how Au nanoparticle (NP) catalysts cooperate with SnOx (x = 1.9 or 2.0) supports to carry out the oxygen reduction reaction (ORR). Specifically, dendrimers were used to encapsulate AuNPs and prevent their interactions with the underlying SnOx supports. After removal of the dendrimers, however, the AuNPs are brought into direct contact with the support and hence feel its effect. The results show that both SnO1.9 and SnO2.0 supports strongly enhance the electrocatalytic properties of AuNPs for the ORR. In the case of AuNP interaction with a SnO1.9 support, the number of electrons involved in the ORR (neff) increases from 2.1 ± 0.2 to 2.9 ± 0.1 following removal of the dendrimers, indicating an increased preference for the desired four-electron product (water), while the overpotential decreases by 0.32 V. Similarly, direct interactions between AuNPs and a SnO2.0 support result in an increase in neff from 2.2 ± 0.1 to 3.1 ± 0.1 and a reduction of the overpotential by 0.28 V. These experimental results are in excellent agreement with the theoretically predicted onset potential shift of 0.30 V. According to the DFT calculations, the observed activity enhancements are attributed to the existence of anionic Au resulting from electron transfer from surface oxygen vacancies within the SnOx supports to the AuNPs. This theoretical finding was confirmed experimentally using X-ray photoelectron spectroscopy. Importantly, the calculations reported here were performed prior to the experiments. In other words, this study represents an unusual case of theory accurately predicting the electrocatalytic manifestation of strong metal support interactions.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b08036.

    • Atomic structures, Figure S-1; fabrication of pyrolyzed photoresist film (PPF) electrodes; TEM micrograph and particle-size distribution histogram, Figure S-2; UV/O3 procedure for the removal of G6-NH2 dendrimers from Au147 DENs; stable adsorbate surface structures, Figure S-3; free-energy diagram for oxygen reduction, Figure S-4; free-energy diagram for the ORR, Figures S-5 and S-6; O2 adsorption structures and binding energies, Figure S-7; density of states of AuNP, Figure S-8; plot of ellipsometric thicknesses, Figure S-9; results of a stability test of SnOx thin films, Figure S-10; optical profilometry of PPF electrodes, Figure S-11; high-resolution XPS spectra, Figure S-12; summary of XPS Sn 3d and O 1s atomic % concentrations/ratios, Tables S-1 and S-2; high-resolution XPS spectra, Figures S-13, S-14, S-16, and S-17; plot showing the relationship between iGE and VF1/3, Figure S-15 (PDF)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 42, 13775–13785
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.8b08036
    Published October 12, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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