One‐Pot Room‐Temperature Synthesis of Bicyclic and Tricyclic <i>Ortho</i> ‐Aminocarbonitriles Catalyzed by [2‐HEAF] Ionic Liquid: A Sustainable Approach

ABSTRACT A task‐specific ionic liquid, 2‐hydroxyethylammonium formate [2‐HEAF], has been demonstrated as an efficient and sustainable catalyst for the synthesis of bicyclic and tricyclic ortho‐aminocarbonitrile derivatives via a four‐component condensation reaction under ambient conditions. The reactions proceed smoothly within 40–90 min, affording the desired products in excellent yields (80%–97%). The resulting ortho ‐aminocarbonitriles are valuable intermediates for the synthesis of natural products, polymers, advanced materials, liquid crystals, ligands, and medicinal agents. A key advantage of this protocol is the use of a mild basic ionic liquid, which effectively regulates the reaction pathway, suppresses side‐product formation, and ensures direct and selective transformation. In addition, the method offers operational simplicity, high efficiency, and catalyst recyclability for up to five consecutive cycles without significant loss of activity, making it a cost‐effective and environmentally benign approach. Furthermore, a plausible reaction mechanism is proposed to provide insight into the catalytic process, and green metrics analysis has been performed to evaluate the environmental impact and sustainability of the protocol.