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Estimating excited-state potentials for iron(III) complexes is unreliable. New findings show potentials are significantly lower than expected, impacting photoredox catalysis design.

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Area of Science:

  • Photochemistry
  • Inorganic Chemistry
  • Catalysis

Background:

  • Reduction potentials of excited states are vital for designing photoredox reactions.
  • These potentials are typically estimated from ground-state values and excited-state energies.
  • This estimation method fails for low-spin d5 iron(III) complexes with photoactive ligand-to-metal charge transfer (LMCT) excited states.

Purpose of the Study:

  • To investigate the accuracy of estimated excited-state reduction potentials for iron(III) complexes.
  • To determine the true reduction potentials of excited-state iron(III) complexes.
  • To understand the implications for photoinduced electron transfer reactions and LMCT photoredox catalysis.

Main Methods:

  • Stern-Volmer luminescence quenching experiments.
  • Photocatalytic reaction studies.
  • Detailed thermodynamic analyses.

Main Results:

  • The commonly applied estimation approach for excited-state potentials breaks down for specific iron(III) complexes.
  • True oxidation potentials for excited-state iron(III) complexes are up to 0.7 V lower than predicted.
  • This leads to significant changes (approx. 70 kJ/mol) in the driving forces for photoinduced electron transfer.

Conclusions:

  • The findings reveal a critical flaw in estimating excited-state potentials for certain metal complexes.
  • This behavior is likely common in other complexes with LMCT-excited states and partially filled d-orbitals.
  • The study has major implications for designing reactions using LMCT-excited states and for LMCT photoredox catalysis.