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Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase
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Hangman effect on hydrogen peroxide dismutation by Fe(III) corroles.

Daniel J Graham1, Dilek K Dogutan, Matthias Schwalbe

  • 1Department of Chemistry, 6-335, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.

Chemical Communications (Cambridge, England)
|March 24, 2012
PubMed
Summary

Hangman iron(III) corroles accelerate hydrogen peroxide disproportionation, showing a stronger hangman effect than oxidized versions. This enhanced catalysis stems from the corrole ligand

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Published on: March 15, 2017

Area of Science:

  • Bioinorganic Chemistry
  • Catalysis
  • Oxidation Reactions

Background:

  • Corroles are macrocyclic ligands with diverse applications in catalysis.
  • Hydrogen peroxide disproportionation is a fundamental chemical process with industrial relevance.
  • The 'hangman effect' describes enhanced catalytic activity observed in specific molecular architectures.

Purpose of the Study:

  • To investigate the catalytic activity of Hangman Fe(III) corroles in hydrogen peroxide disproportionation.
  • To compare the catalytic performance and hangman effect of Fe(III) corroles with their one-electron oxidized analogues.
  • To elucidate the mechanism behind the enhanced catalytic activity and hangman effect.

Main Methods:

  • Synthesis and characterization of Hangman Fe(III) corroles and their oxidized analogues.
  • Kinetic studies of hydrogen peroxide disproportionation catalyzed by the synthesized corroles.
  • Computational modeling to understand the electronic structure and reaction mechanism.

Main Results:

  • Hangman Fe(III) corroles exhibited significantly faster rates of H(2)O(2) disproportionation compared to their oxidized counterparts.
  • A more pronounced hangman effect was observed for the Fe(III) corroles, indicating enhanced catalytic efficiency.
  • The corrole ligand's non-innocent nature facilitates redox-leveling, enabling the bypass of high-energy intermediates.

Conclusions:

  • Hangman Fe(III) corroles are superior catalysts for hydrogen peroxide disproportionation.
  • The non-innocent character of the corrole ligand is crucial for the observed enhanced catalytic activity and hangman effect.
  • This study provides insights into catalyst design for efficient oxidation reactions.