Abstract
The capacity of the hexahydride complex OsH6(PiPr3)2 (1) to discern between the nitrogen atom and the NH unit in the azole assisted aryl C–H bond activation has been investigated. Complex 1 reacts with 2-phenylimidazole to give OsH3{κ2-C,N-(C6H4-imidazole)}(PiPr3)2 (2), which has been characterized by X-ray diffraction analysis. The structure proves the higher affinity of the metal center for the N atom in the presence of the NH unit, which remains unchanged, and reveals that in the solid state the molecules of this complex form infinite chains by means of intermolecular asymmetric 3-center bifurcated dihydrogen bonds. In solution, 1H-DOSY NMR experiments suggest that the association degree decreases as the temperature increases. The fused six-membered ring of benzimidazole weakens the NH bond, enhancing its reactivity. As a consequence, complex 1 cannot discern between the N atom and the NH unit of 2-phenylbenzimidazole. Thus, the treatment of 1 with this substrate leads to a mixture of OsH3{κ2-C,N-(C6H4...
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