Journal
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
Volume 26, Issue 14, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.202200728
Keywords
alkanes; carbene ligands; homogeneous catalysis; iron; oxidation
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Heteroleptic and homoleptic iron(III) complexes supported by a tris(N-heterocyclic carbene) borate ligand have been prepared and characterized. The strong electron-donating character of the tris (carbene) donor was revealed through various measurements and calculations. The catalytic activity of each complex in cyclohexane oxidation was evaluated and both complexes showed high catalytic activity and selectivity, with the homoleptic complex exhibiting more metal-based reactions.
Heteroleptic and homoleptic iron(III) complexes supported by a tris(N-heterocyclic carbene) borate ligand have been prepared and crystallographically characterized. The strong electron-donating character of the tris(carbene) donor was revealed by UV-vis absorption spectroscopy and electrochemical measurements combined with quantum chemical calculations. The catalytic activity of each complex was evaluated in cyclohexane oxidation reaction using meta-chloroperoxybenzoic acid (=mCPBA) as an oxidant, and both complexes show high catalytic activity and selectivity with TON=similar to 350 and A/(K+L)=8-10. Mechanistic studies suggested that radical-chain processes are involved in the reaction due to mCPBA acting as a one-electron oxidant, concomitant with the pathway of metal-based reactive species. Moreover, it was found that the homoleptic and heteroleptic complexes differed significantly in the involvement of metal-based active species, with the homoleptic complex exhibiting more metal-based reactions.
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