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Marcus Cross-Relationship Probed by Time-Resolved CIDNP.

Maksim P Geniman1,2, Olga B Morozova1, Nikita N Lukzen1,2

  • 1International Tomography Center SB RAS, 630090 Novosibirsk, Russia.

International Journal of Molecular Sciences
|September 28, 2023
PubMed
Summary

Time-resolved CIDNP reveals details of degenerate exchange reactions (DEEs) involving short-lived radicals like GMP and tyrosine. Reorganization energies and electron transfer rates were determined, validating Marcus cross-relation for some reactions.

Keywords:
Marcus theorychemically induced nuclear polarization (CIDNP)degenerate electronic exchangeguanosine monophosphateshort-lived radicalstyrosine anion

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Area of Science:

  • Chemical Kinetics
  • Biophysical Chemistry
  • Radical Chemistry

Background:

  • Degenerate exchange reactions (DEEs) involving short-lived radicals are crucial in biological and chemical processes.
  • Time-resolved chemically induced dynamic nuclear polarization (CIDNP) is a powerful technique for studying transient radical species.

Purpose of the Study:

  • To investigate DEEs of guanosine-5'-monophosphate (GMP) and tyrosine derivatives using time-resolved CIDNP.
  • To determine reorganization energies and electron transfer rate constants for these radical pairs.
  • To evaluate the applicability of the Marcus cross-relation to these electron transfer reactions.

Main Methods:

  • Time-resolved CIDNP spectroscopy was employed to study DEEs.
  • Radicals were generated via quenching of triplet 2,2'-dipyridyl.
  • Arrhenius plots were used to determine reorganization energies.
  • Electron transfer rate constants were measured and compared with Marcus cross-relation predictions.

Main Results:

  • DEEs of GMP(-H)-/GMP(-H)•, N-AcTyrO-/N-AcTyrO•, and TyrO-/TyrO• were studied between 8 and 65 °C.
  • Reorganization energies were successfully obtained from Arrhenius plots.
  • The Marcus cross-relation accurately predicted rate constants for GMP/GMP, N-AcTyrO/N-AcTyrO, and TyrO/TyrO radical pairs.
  • A significant discrepancy (two orders of magnitude) was observed for the GMP(-H)•/TyrO- pair.

Conclusions:

  • Time-resolved CIDNP effectively probes DEEs and electron transfer in radical systems.
  • The Marcus cross-relation is a reliable predictor for some electron transfer reactions but requires careful consideration for others.
  • Temperature-dependent nuclear paramagnetic relaxation rates follow Arrhenius behavior for the studied radicals.