Oxidation Events Were Attributed To The Mo0/MoI redox Couple
【China Molybdenum Industry News Network】
A series of bimetallic silyl halido cuprates consisting of the new tripodal silicon-based metalloligand [κ3N-Si(3,5-Me2pz)3Mo(CO)3]− is presented (pz=pyrazolyl). This metalloligand is straightforwardly accessible by reacting the ambidentate ligand tris(3,5-dimethylpyrazolyl)silanide ({Si(3,5-Me2pz)3}−) with [Mo(CO)3(η6-toluene)].
The compound features a fac-coordinated tripodal chelating ligand and an outward pointing, “free” pyramidal silyl donor, which is easily accessible for a secondary coordination to other metal centers. Several bimetallic silyl halido cuprates of the general formula [CuX{μ-κ1Si:κ3N-Si(3,5-Me2pz)3Mo(CO)3}]− (X=Cl, Br, I) have been synthesized. The electronic and structural properties of these complexes were probed in detail by X-ray diffraction analysis, electrospray mass spectrometry, infrared-induced multiphoton dissociation studies, cyclic voltammetry, spectroelectrochemistry, gas-phase photoelectron spectroscopy, as well as UV/Vis and fluorescence spectroscopy.
The heterobimetallic complexes contain linear two-coordinate copper(I) entities with the shortest silicon–copper distances reported so far. Oxidation of the anionic complexes in methylene chloride and acetonitrile solutions at =−0.60 and −0.44 V (vs. ferrocene/ferrocenium (Fc/Fc+)), respectively, shows substantial reversibility. Based on various results obtained from different characterization methods, as well as density functional theory calculations, these oxidation events were attributed to the Mo0/MoI redox couple
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