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Interfacial electrochemical methods focus on the phenomena occurring at the boundary between an electrode and a solution, as opposed to bulk methods that concentrate on the solution's overall properties. These interfacial methods are classified as either static or dynamic based on the presence of a nonzero current in the electrochemical cell and the consistency of analyte concentrations. Static methods, such as potentiometry, measure the cell's potential without any significant current...
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Interfacial Proton Transfer for Hydrogen Evolution at the Sub-Nanometric Platinum/Electrolyte Interface.

Hao Zhang1,2, Lina Cao3, Yanlei Wang4

  • 1Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China.

ACS Applied Materials & Interfaces
|September 21, 2021
PubMed
Summary

Sub-nanometric platinum clusters (SNM-Pt) show excellent hydrogen evolution reaction (HER) activity. A unique Pt-interfacial water configuration facilitates proton transfer, enhancing the catalytic mechanism.

Keywords:
electrode−electrolyte interfacehydrogen evolutioninterfacial wateroperando XASproton transfer

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Area of Science:

  • Electrocatalysis
  • Surface Science
  • Materials Chemistry

Background:

  • Interfacial charge transfer is key to electrocatalysis, with interfacial water playing a role in proton transfer.
  • The complex structure of the electrical double layer (EDL) hinders understanding of interfacial phenomena.
  • Sub-nanometric platinum (Pt) electrocatalysts offer unique properties due to fully exposed atoms.

Purpose of the Study:

  • To investigate the electrode/electrolyte interface during the hydrogen evolution reaction (HER).
  • To identify structural configurations of interfacial water and their impact on catalytic mechanisms.
  • To understand the role of sub-nanometric Pt electrocatalysts in interfacial charge transfer.

Main Methods:

  • Operando X-ray absorption spectroscopy (XAS) was employed to study sub-nanometric Pt electrocatalysts.
  • The hydrogen evolution reaction (HER) was performed under electrochemical conditions.
  • Analysis focused on identifying structural features at the electrode/electrolyte interface.

Main Results:

  • Metallic Pt clusters derived from SNM-Pt demonstrated superior HER activity, with an 18 mV overpotential at 10 mA/cm².
  • The mass activity of SNM-Pt was an order of magnitude higher than commercial Pt/C.
  • A distinct Pt-interfacial water configuration (Pt-O distance ~2.5 Å) was identified as crucial for proton transfer.

Conclusions:

  • SNM-Pt electrocatalysts exhibit remarkable HER performance.
  • The identified Pt-interfacial water structure is fundamental for efficient interfacial proton transfer.
  • Structural evolution of interfacial water at higher overpotentials accelerates proton transfer and increases hydrogen coverage, boosting the reaction rate.