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Intermediate stages of electrochemical oxidation of single-crystalline platinum revealed by in situ Raman spectroscopy

Author

Listed:
  • Yi-Fan Huang

    (Leiden Institute of Chemistry, Leiden University)

  • Patricia J. Kooyman

    (ChemE, Faculty of Applied Sciences, Delft University of Technology
    University of Cape Town)

  • Marc T. M. Koper

    (Leiden Institute of Chemistry, Leiden University)

Abstract

Understanding the atomistic details of how platinum surfaces are oxidized under electrochemical conditions is of importance for many electrochemical devices such as fuel cells and electrolysers. Here we use in situ shell-isolated nanoparticle-enhanced Raman spectroscopy to identify the intermediate stages of the electrochemical oxidation of Pt(111) and Pt(100) single crystals in perchloric acid. Density functional theory calculations were carried out to assist in assigning the experimental Raman bands by simulating the vibrational frequencies of possible intermediates and products. The perchlorate anion is suggested to interact with hydroxyl phase formed on the surface. Peroxo-like and superoxo-like two-dimensional (2D) surface oxides and amorphous 3D α-PtO2 are sequentially formed during the anodic polarization. Our measurements elucidate the process of the electrochemical oxidation of platinum single crystals by providing evidence for the structure-sensitive formation of a 2D platinum-(su)peroxide phase. These results may contribute towards a fundamental understanding of the mechanism of degradation of platinum electrocatalysts.

Suggested Citation

  • Yi-Fan Huang & Patricia J. Kooyman & Marc T. M. Koper, 2016. "Intermediate stages of electrochemical oxidation of single-crystalline platinum revealed by in situ Raman spectroscopy," Nature Communications, Nature, vol. 7(1), pages 1-7, November.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms12440
    DOI: 10.1038/ncomms12440
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    Cited by:

    1. Rubén Rizo & Julia Fernández-Vidal & Laurence J. Hardwick & Gary A. Attard & Francisco J. Vidal-Iglesias & Victor Climent & Enrique Herrero & Juan M. Feliu, 2022. "Investigating the presence of adsorbed species on Pt steps at low potentials," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    2. Nannan Meng & Jiang Shao & Hongjiao Li & Yuting Wang & Xiaoli Fu & Cuibo Liu & Yifu Yu & Bin Zhang, 2022. "Electrosynthesis of formamide from methanol and ammonia under ambient conditions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Benedikt Axel Brandes & Yogeshwaran Krishnan & Fabian Luca Buchauer & Heine Anton Hansen & Johan Hjelm, 2024. "Unifying the ORR and OER with surface oxygen and extracting their intrinsic activities on platinum," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Yunzhou Wen & Cheng Liu & Rui Huang & Hui Zhang & Xiaobao Li & F. Pelayo García de Arquer & Zhi Liu & Youyong Li & Bo Zhang, 2022. "Introducing Brønsted acid sites to accelerate the bridging-oxygen-assisted deprotonation in acidic water oxidation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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