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A new equation explains reaction rates and thermodynamic driving force across all regimes. It reveals three key parameters (minimum preorganizational barrier, reaction symmetry offset, kinetic curvature factor) and clarifies limitations of classical models.

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Area of Science:

  • Physical Chemistry
  • Chemical Kinetics
  • Reaction Rate Theory

Background:

  • Existing rate theories lack a general, physically grounded equation relating reaction rate to thermodynamic driving force across all regimes.
  • Classical models like Marcus and Leffler equations have limitations, relying on unrealistic assumptions or only capturing local behavior.

Purpose of the Study:

  • To derive a general, non-linear equation that accurately relates reaction rate and thermodynamic driving force.
  • To identify and define physically meaningful parameters governing this relationship.
  • To explain the physical origins and limitations of classical rate models.

Main Methods:

  • Derivation of a new rate-driving force equation based on microscopic reversibility.
  • Identification of three key parameters: minimum preorganizational barrier (Emin), reaction symmetry offset (Eeq), and kinetic curvature factor (θ).
  • Analysis of experimental data, including hydrogen atom transfer to Fe(IV)=O, hydride shifts, rearrangements, and cyclizations.

Main Results:

  • A novel, non-linear equation that captures global rate-driving force behavior and recovers known limiting cases.
  • Explanation of the physical basis for the Brønsted slope observed in classical models like the Leffler equation.
  • Demonstration of the model's ability to reinterpret curved rate-driving force plots and predict behavior in highly exergonic regimes.

Conclusions:

  • The new framework provides a physically grounded understanding of the rate-driving force relationship, enhancing existing models without replacing them.
  • Enables chemists to better understand, predict, and design chemical reactions with desired kinetics across diverse systems.
  • Reveals hidden curvature and deeper physical meaning in rate-driving force relationships, even in seemingly linear plots.