Journal
INORGANIC CHEMISTRY
Volume 48, Issue 10, Pages 4514-4523Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic9002466
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Funding
- NIH [GM47365]
- NSF [CHE-0610183]
- REU funds
- NSERC of Canada
- UM Lando Undergraduate Research Program
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Copper(I) complexes of a diketiminate featuring CF3 groups on the backbone and dimethylphenyl substituents (4) and a nitroformazan (5) were synthesized and shown by spectroscopy, X-ray crystallography, cyclic voltammetry, and theory to contain copper(I) sites electron-deficient relative to those supported by previously studied diketiminate complexes comprising alkyl or aryl backbone substituents. Despite their electron-poor nature, oxygenation of LCu(CH3CN) (L = 4 or 5) at room temperature yielded bis(hydroxo)dicopper(II) compounds and at -80 degrees C yielded bis(mu-oxo)dicopper complexes that were identified on the basis of UV-vis and resonance Raman spectroscopy, spectrophotometric titration results (2:1 Cu/O-2 ratio), electron paramagnetic resonance spectroscopy (silent), and density functional theory calculations. The bis(mu-oxo)dicopper complex supported by 5 exhibited unusual spectroscopic properties and decayed via a novel intermediate proposed to be a metallaverdazyl radical complex, findings that highlight the potential for the formazan ligand to exhibit noninnocent behavior.
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