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Quantum tunneling significantly impacts proton-coupled electron transfer (PCET) reactions. This study quantifies tunneling

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Area of Science:

  • Physical Chemistry
  • Quantum Mechanics
  • Electrocatalysis

Background:

  • Proton tunneling is crucial in proton-coupled electron transfer (PCET) reactions but challenging to study under ambient conditions.
  • Understanding the contribution of quantum effects like proton tunneling is vital for designing efficient catalysts.

Purpose of the Study:

  • To develop and apply a single-molecule technique for quantifying the role of proton tunneling in PCET reactions.
  • To investigate the mechanistic pathways and kinetics of PCET on a molecular catalyst at room temperature.

Main Methods:

  • Utilized an on-chip electrochemical mechanically controllable break junction to immobilize a single benzothiadiazole molecule.
  • Monitored PCET reactions via conductance tracking and correlated with Raman spectroscopy to identify intermediates.
  • Performed temperature-dependent kinetic experiments to analyze reaction pathways and calculate rate constants and Kinetic Isotope Effects.

Main Results:

  • Identified four key PCET intermediates and quantified elementary step kinetics and pathway evolution probabilities.
  • Revealed an efficient tunneling-mediated pathway competing with the classical thermodynamic pathway.
  • Demonstrated tunable modulation of the tunneling route's population (13% to 42%) at room temperature.

Conclusions:

  • Established a single-molecule platform for mechanistic quantification in room-temperature electrocatalysis.
  • Quantified the significant contribution of proton tunneling, showing its potential for energy-efficient catalysis.
  • This method enables evaluation and promotion of proton tunneling in catalytic systems.