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A New Thiolate-Bound Dimanganese Cluster as a Structural and Functional Model for Class Ib Ribonucleotide Reductases.

Beatrice Battistella1, Thomas Lohmiller1,2, Beatrice Cula1

  • 1Institut für Chemie, Humboldt-Universität zu Berlin, Brook-Taylor-Straße 2, 12489, Berlin, Germany.

Angewandte Chemie (International Ed. in English)
|December 30, 2022
PubMed
Summary

Researchers developed a biomimetic dimanganese complex that mimics class Ib ribonucleotide reductases (RNRs). This complex activates superoxide to form a high-valent Mn(III)-O2-Mn(IV) species, acting as an effective oxidant in chemical reactions.

Keywords:
Bioinorganic ChemistryDimanganese CofactorEnzyme ModelsPhenol OxidationRibonucleotide Reductases

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Area of Science:

  • Bioinorganic Chemistry
  • Enzyme Mimicry
  • Oxidation Chemistry

Background:

  • Class Ib ribonucleotide reductases (RNRs) utilize a dimanganese cluster to activate superoxide, not dioxygen, for biological oxidation reactions.
  • The active species in RNRs is a high-valent Mn(III)-O2-Mn(IV) intermediate, crucial for generating tyrosyl radicals.
  • Developing biomimetic models is key to understanding RNR mechanisms and designing novel catalysts.

Purpose of the Study:

  • To synthesize a biomimetic dimanganese complex that models the active site of class Ib RNRs.
  • To investigate the reaction of this complex with superoxide and characterize the resulting manganese-oxygen species.
  • To evaluate the oxidative capabilities of the biomimetic complex in relevant chemical transformations.

Main Methods:

  • Synthesis of a thiolate-bound dimanganese complex, [MnII2(BPMT)(OAc)2](ClO4) (1).
  • Reaction of complex 1 with superoxide (O2•−) to generate a dimanganese-oxygen species, [(BPMT)MnO2Mn]2+ (2).
  • Characterization using Resonance Raman spectroscopy to detect the O-O bond and Electron Paramagnetic Resonance (EPR) spectroscopy to determine the oxidation state and spin state.

Main Results:

  • The reaction yielded complex 2, confirmed to contain an O-O bond via Resonance Raman spectroscopy.
  • EPR analysis revealed a Mn(III)-Mn(IV) core (St=1/2), consistent with the active species in class Ib RNRs.
  • Complex 2 demonstrated electrophilic oxidant activity in aldehyde deformylation and phenol oxidation, outperforming other reported Mn-O2-Mn complexes.

Conclusions:

  • The synthesized dimanganese complex serves as a highly effective structural and functional biomimetic model for class Ib RNRs.
  • The study highlights the ability of biomimetic complexes to activate superoxide and perform challenging oxidation reactions.
  • This work provides valuable insights into the mechanism of RNRs and opens avenues for designing new oxidation catalysts.