Austria C-C coupling • cyclization • imidazolidine • molybdenum • metal-template 2 Abstract. Preparation of molybdenum dioxido complexes with novel iminophenolate ligands bearing pendant secondary amide functionalities led to unprecedented C-C and C-N coupling reactions of two α-iminoamides upon coordination. The diastereoselective cyclization to asymmetric imidazolidines occurs at the metal center in two consecutive steps via a mono coupled intermediate. A meaningful mechanism is proposed

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... on full characterization of intermediate and final molybdenum-containing products by spectroscopic means and by singlecrystal X-ray diffraction analyses. This process constitutes the first example of a diastereoselective self-cyclization of two α-iminoamides.