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Correlated solvent coordinates accelerate multi-donor proton-coupled electron transfer.

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Investigating proton-coupled electron transfer (PCET) in ruthenium complexes with multiple donors reveals accelerated rates due to solvent reorganization. This work offers insights into designing efficient synthetic charge transfer systems.

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Area of Science:

  • Inorganic Chemistry
  • Photochemistry
  • Electron Transfer Theory

Background:

  • Semi-classical electron transfer theory accurately describes discrete donor-acceptor (D/A) pairs.
  • The influence of multiple equivalent redox sites on charge transfer rates is less understood.
  • Proton-coupled electron transfer (PCET) is crucial in various chemical and biological processes.

Purpose of the Study:

  • To investigate the effect of increasing the number of identical electron donors (N) on intramolecular PCET rates.
  • To isolate the impact of donor number while maintaining constant geometry, coupling, and driving forces.
  • To elucidate the role of solvent dynamics in supra-statistical acceleration of PCET.

Main Methods:

  • Synthesis of [Ru(L)3-N(OH)N]2+ complexes with N=1, 2, or 3 phenolic donors.
  • Flash photolysis and oxidative quenching with methyl viologen (MV2+).
  • Kinetic analysis of transient Ru(iii) oxidation via PCET.

Main Results:

  • PCET rates increased significantly with increasing donor number (3.4-fold for N=2, 5.7-fold for N=3).
  • Statistically corrected rates showed supra-statistical acceleration (1.7-fold for N=2, 1.9-fold for N=3).
  • Acceleration attributed to reduced outer sphere reorganization energy (λm) from partially shared solvent coordinate.

Conclusions:

  • Multiple equivalent redox sites can accelerate intramolecular PCET rates beyond statistical expectations.
  • Solvent reorganization energy plays a critical role in modulating PCET rates.
  • Provides a strategy for designing synthetic charge transfer systems with enhanced efficiency.