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Gas-Phase Characterization of Redox-Active Manganese Complexes.

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Summary

This study explores manganese complexes in the gas phase, revealing that manganese(II) is the most stable oxidation state. The manganese(IV) complex acts as a strong oxidant, reacting with triethylamine to form manganese(III) species.

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Area of Science:

  • Inorganic Chemistry
  • Coordination Chemistry
  • Mass Spectrometry

Background:

  • Manganese complexes exhibit diverse redox chemistry, often involving structural changes and ligand dynamics.
  • The 2,6-diguanidylpyridine (dgpy) ligand stabilizes manganese in +II, +III, and +IV oxidation states in condensed phase complexes.
  • The manganese(IV) complex is a potent oxidant in solution.

Purpose of the Study:

  • To investigate the gas-phase stability and redox behavior of manganese-dgpy complexes with hexafluorophosphate counterions.
  • To compare gas-phase properties with known condensed-phase behavior.
  • To elucidate the reactivity of manganese complexes with triethylamine in the gas phase.

Main Methods:

  • Utilized two modified 3D Paul ion trap mass spectrometers for gas-phase ion analysis.
  • Employed collision-induced dissociation (CID) and UV/vis photodissociation to assess stability.
  • Recorded gas-phase UV/vis spectra and studied reactions with triethylamine.

Main Results:

  • Observed six cationic species of [Mnx(dgpy)2(PF6)y]n+ across Mn(II), Mn(III), and Mn(IV) oxidation states, including a reduced dgpy ligand complex.
  • Mn(II) species demonstrated the highest stability under dissociation experiments.
  • Gas-phase UV/vis spectra mirrored condensed-phase features, with variations in relative band intensities.
  • The Mn(IV) complex oxidized triethylamine to Mn(III), while Mn(III) showed limited reactivity.

Conclusions:

  • Gas-phase studies provide insights into the intrinsic stability and redox properties of manganese-dgpy complexes.
  • Stability is influenced by oxidation state and the presence of counterions, with Mn(II) being the most robust.
  • The observed gas-phase reactivity of Mn(IV) with triethylamine aligns with its strong oxidizing nature.