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Molybdenum(vi) tris(amidophenoxide) complexes.

Alexander N Erickson1, Seth N Brown

  • 1Department of Chemistry and Biochemistry, 251 Nieuwland Science Hall, University of Notre Dame, Notre Dame, IN 46556-5670, USA. Seth.N.Brown.114@nd.edu.

Dalton Transactions (Cambridge, England : 2003)
|October 23, 2018
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Summary

Molybdenum(VI) tris(amidophenoxide) complexes exhibit a preferred facial geometry, unlike other transition metal complexes. This geometry is influenced by N-aryl substituents and is attributed to enhanced pi bonding.

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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Molybdenum Chemistry

Background:

  • Tris(amidophenoxide) complexes of transition metals are known, but their stereochemistry can vary.
  • Molybdenum complexes with related ligands have been studied, but their specific geometric preferences were less understood.

Purpose of the Study:

  • To synthesize and characterize novel tris(2-(arylamido)-4,6-di-tert-butylphenoxo)molybdenum(VI) complexes.
  • To investigate the stereochemistry and isomerism of these molybdenum complexes in solid state and solution.
  • To explore the influence of N-aryl substituents on the observed geometry and isomerization dynamics.

Main Methods:

  • Synthesis of molybdenum(VI) tris(amidophenoxide) complexes using (cycloheptatriene)Mo(CO)3 and N-aryliminoquinone, or MoO2(acac)2 and aminophenol.
  • Solid-state structural analysis to determine the predominant geometry.
  • Solution studies using spectroscopy to identify and quantify facial (fac) and meridional (mer) isomers.
  • Variable temperature NMR spectroscopy to study the interconversion dynamics between isomers.

Main Results:

  • Molybdenum(VI) tris(amidophenoxide) complexes exclusively adopt a facial geometry in the solid state.
  • In solution, the facial isomer predominates, with a small amount of the meridional isomer detectable at room temperature.
  • Isomerization between fac and mer forms occurs via Rây-Dutt trigonal twists, which are faster than Bailar twists due to steric effects.
  • Electron-withdrawing substituents on the N-aryl ring favor the meridional isomer.
  • The preference for facial geometry is attributed to enhanced pi bonding.

Conclusions:

  • Molybdenum(VI) tris(amidophenoxide) complexes display a distinct preference for facial geometry, contrasting with other transition metal analogues.
  • The observed stereochemistry is tunable via N-aryl substituents, impacting the fac/mer equilibrium.
  • The enhanced pi bonding in the facial isomer is proposed as the driving force for this geometric preference.