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Treatment of dilithiated nitriles and sulfones with oxalic acid bis(imidoyl) chlorides resulted in a new cyclization reaction which provided a variety of (3-imino-2, 3-dihydro-1H-indol-2-ylidene)acetonitriles and -sulfones in good yields. The reactions proceeded by condensation of the dianions with the first imidoyl chloride group of the bis(imidoyl) chloride, subsequent intramolecular attack of the ortho carbon of the arylimino group onto the second imidoyl chloride group, and final aromatization. Excellent stereoselectivities were observed in most cases.

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Reaction of sterically hindered bis(imidoyl)chlorides of oxalic acid with picolylamine afforded conformationally locked oxalic acid‐derived amidines with pendant pyridine functionalities. Based on this new multivalent ligand system, dimetallic complexes were efficiently prepared.