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Related Experiment Videos

Gas-phase dioxygen activation by binuclear manganese clusters.

Barbara Chiavarino1, Maria Elisa Crestoni, Simonetta Fornarini

  • 1Dipartimento di Studi di Chimica e Tecnologia delle Sostanze Biologicamente Attive Università di Roma La Sapienza Piazzale A. Moro 5, 00185 Roma, Italy.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|October 24, 2002
PubMed
Summary

Gas-phase binuclear manganese oxide cations exhibit diverse reactivity with small molecules and organic compounds. These manganese oxide ions show potential for catalytic cycles through oxidation and ligand exchange reactions.

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Area of Science:

  • Gas-phase inorganic chemistry
  • Organometallic chemistry
  • Catalysis research

Background:

  • Binuclear manganese oxide cations are key intermediates in oxidation reactions.
  • Understanding their reactivity is crucial for developing new catalytic processes.
  • Previous studies have focused on mononuclear species, leaving binuclear systems less explored.

Purpose of the Study:

  • To synthesize and characterize gas-phase binuclear manganese oxide cations (Mn2O2+ and Mn2O+).
  • To investigate the reactivity of these cations with various neutral molecules.
  • To gain insights into reaction mechanisms and potential catalytic applications.

Main Methods:

  • Gas-phase ion preparation via reaction of O2 with ionized [Mn2(CO)10].
  • Reactivity studies using Fourier Transform Ion Cyclotron Resonance (FT-ICR) spectrometry.

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  • Structural analysis through collision-induced dissociation and ion-molecule reaction outcomes.

    • Main Results:

    • Mn2O2+ and Mn2O+ cations were successfully prepared in the gas phase.
    • Reactions with H2O, H2S, and NH3 involved exchange, addition, and oxidation pathways.
    • Oxidative reactions, including dehydrogenation and O-atom transfer, were observed with organic molecules.
    • Dihydrogen showed no reactivity with the manganese oxide cations.

    Conclusions:

    • Binuclear manganese oxide cations display significant oxidative reactivity.
    • The observed reactions suggest potential for catalytic cycles involving these species.
    • Ligand exchange with O2 can regenerate the active manganese oxide cation species.