Journal
ORGANOMETALLICS
Volume 30, Issue 17, Pages 4687-4694Publisher
AMER CHEMICAL SOC
DOI: 10.1021/om200527y
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Funding
- National Basic Research Program of China (973 Program) [2011CB808705]
- National Natural Science Foundation of China [21002114, 20872168]
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The unique cobalt(I)-NHC complex [CO(lEt)(4)] [BPh4] (1) (IEt = 1,3-diethyl-4,5-dimethylimidazole-2-ylidene) and its analogues employing other carbene ligands were prepared by the reactions of [Co(PPh3)(3)Cl] with free carbene ligands followed by anion exchange. X-ray diffraction revealed 1 features a homoleptic cation [Co(IEt)(4)](+) with square-planar geometry. Electrochemical studies showed the square-planar complexes support the redox series [Co(IEt)(4)](+/2+3+), of which the divalent cation has been synthesized and structurally characterized as in [Co (IEt)(4)] [BF4](2) (2). Both EPR and DFT studies indicated 2 has a low-spin Co(II) center. 1 can efficiently catalyze the oxidative homocoupling reactions of aryl Grignard reagents. Investigations on the stoichiometric reactions of 1 with organic halides and 2 with aryl Grignard reagents established an interesting radical mechanism involving the [Co (IEt)(4)](+/2+) redox shuttle for these cobalt-NHC complex catalyzed homocoupling reactions.
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