A variety of 18
e ansa-chromocene isocyanide complexes were prepared via ligand substitution on thecarbonyl complexes. The relative
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-accepting character of the different isocyanide ligands was evaluatedfrom the structural, spectroscopic, and electrochemical properties of the complexes. One-electron chemicaloxidation of the complexes generates low-spin, 17
e ansa-chromocene isocyanide cations, the structuraland spectroscopic properties of which were compared with their neutral precursors. Density functionaltheory (DFT) calculations were performed on model complexes in order to elucidate the nature of thebonding between the chromium and the isocyanide ligands and to explain the effects of one-electronoxidation of the complexes.