The synthesis of pyridines from dinitrogen in homogeneous solution is known to be challenging considering that an N cleavage step needs to be combined with two N-C coupling steps. Herein, a tungsten complex bearing a tailor-made 2,2'-(BuAs)-substituted tolane ligand scaffold was shown to split N to afford the corresponding tungsten nitride, which is not the case for the corresponding (PrAs)-substituted derivative. The former nitride was then reacted with 2,4,6-trimethylpyrylium triflate, which led to the formation of a tungsten oxo complex, along with collidine. Over the course of this reaction, the O atom of the pyrylium starting material was replaced with an N atom via a hitherto unprecedented skeletal editing process.
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