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Organic amidines are an important class of compounds that have found their application in coordination chemistry, organic synthesis and catalysis. Amidines are also used in medicine to treat a wide class of diseases such as trypanosomiasis, leishmaniasis, keratitis and many others. Therefore, the synthesis of such compounds is highly relevant to modern chemistry. Also, recent researches in the chemistry of the metallocenes 4 group have shown the possibility of synthesizing an amidinate functional group in the coordination sphere of zirconium. It was found that the addition of two nitrile equivalents to zirconacyclopropene complexes leads to the formation of bicyclic amidinate metallacycles. We have studied the interaction of precursors of acetylene complexes: metallacyclopentenes, -pentadienes and aryl metallacycles with dinitriles. It was found that in the case of adiponitrile, as a result of intramolecular cyclization, afford the seven-membered tetrahydroazepine zirconaamidinates. Then organic amidines were isolated by demetallization of the obtained compounds. In summary, the interaction of precursors of acetylene complexes of metallocenes with dinitriles makes it possible to synthesize various organic amidines in the coordination sphere of the metal.