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Reduction of Oxide Layers on Au(111): The Interplay between Reduction Rate, Dissolution, and Restructuring

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. C 2021, 125, 41, 22698-22704
    C: Physical Properties of Materials and Interfaces

    Reduction of Oxide Layers on Au(111): The Interplay between Reduction Rate, Dissolution, and Restructuring
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    • Corinna Stumm
      Corinna Stumm
      Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany
      More by Corinna Stumm
      Orcidhttps://orcid.org/0000-0003-4646-8234
    • Sebastian Grau
      Sebastian Grau
      Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany
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    • Florian D. Speck
      Florian D. Speck
      Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Cauerstraße 1, 91058 Erlangen, Germany
      More by Florian D. Speck
      Orcidhttps://orcid.org/0000-0002-7649-9261
    • Felix Hilpert
      Felix Hilpert
      Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany
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    • Valentín Briega-Martos
      Valentín Briega-Martos
      Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Cauerstraße 1, 91058 Erlangen, Germany
      More by Valentín Briega-Martos
    • Karl Mayrhofer
      Karl Mayrhofer
      Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Cauerstraße 1, 91058 Erlangen, Germany
      Department Chemie- und Bioingenieurwesen, Friedrich-Alexander-Universität Erlangen-Nürnberg, Cauerstraße 1, 91058 Erlangen, Germany
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      Orcidhttps://orcid.org/0000-0002-4248-0431
    • Serhiy Cherevko
      Serhiy Cherevko
      Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Forschungszentrum Jülich GmbH, Cauerstraße 1, 91058 Erlangen, Germany
      More by Serhiy Cherevko
      Orcidhttps://orcid.org/0000-0002-7188-4857
    • Olaf Brummel*
      Olaf Brummel
      Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-5968-0774
    • Jörg Libuda
      Jörg Libuda
      Interface Research and Catalysis, ECRC, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstraße 3, 91058 Erlangen, Germany
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      Orcidhttps://orcid.org/0000-0003-4713-5941
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2021, 125, 41, 22698–22704
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.1c03969
    Published October 7, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
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    Abstract

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    Dissolution and redeposition processes determine the stability of electrode materials. In this work, we address these processes in situ during oxidation and subsequent reduction of Au(111) electrodes in an acidic electrolyte (0.1 M H2SO4). We used complementary techniques, namely, electrochemical scanning tunneling microscopy (EC-STM) and on-line inductively coupled plasma mass spectrometry (ICP–MS). We observed that the reduction rate distinctively influences dissolution and the resulting morphology of the surface. Slow reduction leads to formation of monoatomic holes with a diameter of 1–9 nm on the surface. Dissolved Au species formed during reduction are detected in the bulk electrolyte. During fast reduction, however, the formed holes are much smaller and additional two-dimensional Au islands are formed. Almost no dissolved Au was detected in the electrolyte during reduction. We assign the observed differences to competing processes, namely, diffusion of the dissolved Au species into the solution and direct renucleation of dissolved Au.

    Copyright © 2021 The Authors. Published by 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/acs.jpcc.1c03969.

    • Tip influence in EC-STM; stability of the surface morphology after reduction by potential jump; integration of cathodic and anodic dissolution signals in EC on-line ICP–MS; and calculation of the mass density of a Au(111) monolayer (PDF)

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    Cited By

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    This article is cited by 8 publications.

    1. Juntao Yang, Felix Hilpert, Yunsheng Qiu, Evanie Franz, Valentín Briega-Martos, Serhiy Cherevko, Karl Mayrhofer, Olaf Brummel, Jörg Libuda. Interactions of the Ionic Liquid [C2C1Im][DCA] with Au(111) Electrodes: Interplay between Ion Adsorption, Electrode Structure, and Stability. The Journal of Physical Chemistry C 2024, 128 (7) , 2834-2843. https://doi.org/10.1021/acs.jpcc.3c07122
    2. Matej Zlatar, Daniel Escalera-López, Miquel Gamón Rodríguez, Tomáš Hrbek, Carina Götz, Rani Mary Joy, Alan Savan, Hoang Phi Tran, Hong Nhan Nong, Paulius Pobedinskas, Valentín Briega-Martos, Andreas Hutzler, Thomas Böhm, Ken Haenen, Alfred Ludwig, Ivan Khalakhan, Peter Strasser, Serhiy Cherevko. Standardizing OER Electrocatalyst Benchmarking in Aqueous Electrolytes: Comprehensive Guidelines for Accelerated Stress Tests and Backing Electrodes. ACS Catalysis 2023, 13 (23) , 15375-15392. https://doi.org/10.1021/acscatal.3c03880
    3. Jonas Mart Linge, Valentín Briega-Martos, Andreas Hutzler, Birk Fritsch, Heiki Erikson, Kaido Tammeveski, Serhiy Cherevko. Stability of Carbon Supported Silver Electrocatalysts for Alkaline Oxygen Reduction and Evolution Reactions. ACS Applied Energy Materials 2023, 6 (22) , 11497-11509. https://doi.org/10.1021/acsaem.3c01717
    4. Valentín Briega-Martos, Serhiy Cherevko. On-Line ICP-MS in Electrocatalysis Research: Platinum Dissolution Studies. 2023, 245-247. https://doi.org/10.1007/978-3-031-17425-4_34
    5. Linnéa Strandberg, Victor Shokhen, Mathilde Luneau, Göran Lindbergh, Carina Lagergren, Björn Wickman. Comparison of Oxygen Adsorption and Platinum Dissolution in Acid and Alkaline Solutions Using Electrochemical Quartz Crystal Microbalance. ChemElectroChem 2022, 9 (22) https://doi.org/10.1002/celc.202200591
    6. Keiko Miyabayashi, Yodai Shirayama, Gupta Surabhi, Hirokazu Tatsuoka. Identical‐location Transmission Electron Microscopy of Pt Nanoparticle Electrocatalysts Using Iridium‐coated Au Grids for Fuel Cell Durability Tests Simulating Start‐up and Shutdown Conditions. Electroanalysis 2022, 132 https://doi.org/10.1002/elan.202200199
    7. Evanie Franz, Anne Kunz, Nils Oberhof, Andreas H. Heindl, Manon Bertram, Lukas Fusek, Nicola Taccardi, Peter Wasserscheid, Andreas Dreuw, Hermann A. Wegner, Olaf Brummel, Jörg Libuda. Electrochemically Triggered Energy Release from an Azothiophene‐Based Molecular Solar Thermal System. ChemSusChem 2022, 15 (18) https://doi.org/10.1002/cssc.202200958
    8. Weiran Zheng, Lawrence Yoon Suk Lee. Observing Electrocatalytic Processes via In Situ Electrochemical Scanning Tunneling Microscopy: Latest Advances. Chemistry – An Asian Journal 2022, 17 (15) https://doi.org/10.1002/asia.202200384
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2021, 125, 41, 22698–22704
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.1c03969
    Published October 7, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
    Request reuse permissions

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