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Quantum proton tunneling (QPT) significantly impacts electrode reactions like hydrogen evolution and oxygen reduction. Platinum electrodes show weak QPT, while gold electrodes exhibit a transition from classical to QPT with increasing overpotential.

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Area of Science:

  • Electrochemistry
  • Quantum Mechanics
  • Surface Science

Background:

  • Quantum proton tunneling (QPT) plays a role in multi-electron/-proton transfer electrode processes.
  • Understanding QPT is crucial for optimizing reactions like hydrogen evolution (HER) and oxygen reduction (ORR).

Purpose of the Study:

  • Investigate QPT in HER and ORR on platinum (pcPt) and gold (pcAu) electrodes.
  • Determine the influence of overpotential and electrode material on QPT manifestation.
  • Explore the transition between semiclassical transition state theory (SC-TST) and full QPT.

Main Methods:

  • Measurement of hydrogen/deuterium kinetic isotope effect constant ratio (KH/D) under varying conditions.
  • Electrochemical investigation of polycrystalline platinum and gold electrodes at 298 K.
  • Theoretical analysis to interpret QPT phenomena.

Main Results:

  • Platinum electrodes showed negligible to weak QPT in HER (1 < KH/D < 3), indicating SC-TST dominance.
  • Gold electrodes in alkaline conditions displayed a transition from SC-TST to full QPT with increasing overpotential (KH/D > 13).
  • Oxygen reduction on platinum in alkaline conditions showed QPT at low overpotentials, transitioning to classical behavior at higher overpotentials.

Conclusions:

  • QPT in surface electrochemical systems is highly dependent on the specific system and electrode material.
  • Overpotential influences the transition between classical and quantum proton transfer mechanisms.
  • Microscopic proton transfer mechanisms, such as from hydronium ions or water molecules, may affect the QPT pathway.