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Proton-Coupled Electron Transfer Guidelines, Fair and Square.

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Understanding proton-coupled electron transfer (PCET) mechanisms is key for optimizing energy reactions. This perspective offers guidelines to distinguish between sequential and concerted PCET pathways using kinetic and thermodynamic data.

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Area of Science:

  • Chemical Kinetics and Thermodynamics
  • Catalysis and Synthetic Chemistry
  • Bioinorganic and Organometallic Chemistry

Background:

  • Proton-coupled electron transfer (PCET) reactions are vital in natural and artificial energy conversion systems.
  • PCET reactions exhibit mechanistic complexity due to the interplay of proton and electron transfer.
  • Distinguishing between various PCET mechanisms is critical for reaction design and optimization.

Purpose of the Study:

  • To provide practical guidelines for discerning between sequential and concerted PCET mechanisms.
  • To illustrate how thermodynamic and coupling strengths influence PCET mechanism dominance.
  • To discuss contemporary issues and future directions in PCET research.

Main Methods:

  • Interpretation of thermodynamic data.
  • Analysis of temperature-, pressure-, and isotope-dependent kinetics.
  • Development and application of new PCET-zone diagrams.

Main Results:

  • New PCET-zone diagrams demonstrate how varying thermodynamic and coupling strengths can switch or eliminate mechanisms.
  • Guidelines are presented for differentiating sequential and concerted PCET pathways.
  • The role of asynchronous concerted PCET in organic reactions and its distinction from hydrogen atom transfer are discussed.

Conclusions:

  • Understanding PCET mechanism control is crucial for designing efficient energy transformation processes.
  • Thermodynamic and kinetic analyses, alongside novel diagrams, provide powerful tools for mechanistic elucidation.
  • Further research into PCET is essential for advancing catalysis, synthetic chemistry, and energy science.