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Reactivity mapping of nanoscale defect chemistry under electrochemical reaction conditions

Author

Listed:
  • Jonas H. K. Pfisterer

    (Max Planck Institute for Polymer Research)

  • Masoud Baghernejad

    (Max Planck Institute for Polymer Research)

  • Giovanni Giuzio

    (Max Planck Institute for Polymer Research)

  • Katrin F. Domke

    (Max Planck Institute for Polymer Research)

Abstract

Electrocatalysts often show increased conversion at nanoscale chemical or topographic surface inhomogeneities, resulting in spatially heterogeneous reactivity. Identifying reacting species locally with nanometer precision during chemical conversion is one of the biggest quests in electrochemical surface science to advance (electro)catalysis and related fields. Here, we demonstrate that electrochemical tip-enhanced Raman spectroscopy can be used for combined topography and reactivity imaging of electro-active surface sites under reaction conditions. We map the electrochemical oxidation of Au nanodefects, a showcase energy conversion and corrosion reaction, with a chemical spatial sensitivity of about 10 nm. The results indicate the reversible, concurrent formation of spatially separated Au2O3 and Au2O species at defect-terrace and protrusion sites on the defect, respectively. Active-site chemical nano-imaging under realistic working conditions is expected to be pivotal in a broad range of disciplines where quasi-atomistic reactivity understanding could enable strategic engineering of active sites to rationally tune (electro)chemical device properties.

Suggested Citation

  • Jonas H. K. Pfisterer & Masoud Baghernejad & Giovanni Giuzio & Katrin F. Domke, 2019. "Reactivity mapping of nanoscale defect chemistry under electrochemical reaction conditions," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-13692-3
    DOI: 10.1038/s41467-019-13692-3
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    Cited by:

    1. Roman M. Wyss & Günter Kewes & Pietro Marabotti & Stefan M. Koepfli & Karl-Philipp Schlichting & Markus Parzefall & Eric Bonvin & Martin F. Sarott & Morgan Trassin & Maximilian Oezkent & Chen-Hsun Lu , 2024. "Bulk-suppressed and surface-sensitive Raman scattering by transferable plasmonic membranes with irregular slot-shaped nanopores," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Linfei Li & Jeremy F. Schultz & Sayantan Mahapatra & Zhongyi Lu & Xu Zhang & Nan Jiang, 2022. "Chemically identifying single adatoms with single-bond sensitivity during oxidation reactions of borophene," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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