Mechanochemical Near-Ambient Synthesis of C₂N Materials From HAT-CN and its Precursors

C₂N-type carbon materials are typically obtained through high-temperature treatment of nitrogen-rich molecular precursors under inert atmosphere. Herein, we demonstrate mechanochemical approaches that enable the synthesis of C₂N materials, namely by (i) the conversion of hexaazatriphenylenehexacarbonitrile (HAT-CN) and by (ii) a one-pot route starting from its molecular precursors, hexaketocyclohexane, and diaminomaleonitrile. Compared with conventional pyrolytic methods, mechanochemical approaches afford higher yields while significantly reducing energy input, thereby improving overall sustainability. The results highlight the decisive role of mechanical energy in directing carbon-nitrogen framework formation and demonstrate mechanochemistry as a versatile alternative to thermal routes for C₂N synthesis.