Designing Sustainable Copper‐Based Hybrid Framework Catalysts for One‐Pot Multicomponent Organic Reactions

Abstract The recent breakthroughs in heterogeneous catalysis emphasize the need for novel materials capable of driving organic transformations. The present study explores two copper phosphonate hybrid framework materials, 2D Cu 3 [(Hhedp) 2 (C 4 H 4 N 2 )].2H 2 O ( Cu(II)Pyz‐P ) and 3D Cu 3 [(H 3 hedp) 2 (C 4 H 4 N 2 ) 4 (SO 4 )].2H 2 O ( Cu(I/II)Pyz‐P ), as single crystals isolated via hydrothermal synthetic strategy using H 4 hedp (1‐hydroxyethane 1,1‐diphosphonic acid) and N ‐donor secondary ligand (Pyrazine; C 4 H 4 N 2 ). Cu(II)Pyz‐P contains exclusively +2 oxidation state of copper, while Cu(I/II)Pyz‐P is characterized by a mixed oxidation state, where copper +2 phosphonate is embedded within the network formed by copper +1 state. Moreover, magnetic study elucidates the distinct oxidation states of both compounds by showing deviations from each other. The aforementioned compounds are exceedingly effective for catalyzing multicomponent reactions, that is, A 3 coupling reaction and click reaction. Cu(I/II)Pyz‐P ensures the regioselective synthesis of triazole with high purity, while A 3 coupling reaction is facilitated by both the compounds. Solvent‐ and additive‐free efficient multicomponent reactions are explored for the first time in the copper phosphonate hybrid framework structures. The present study reveals the promise of copper‐based hybrid phosphonate frameworks as durable and efficient catalysts for organic synthesis, providing cost‐effective and sustainable ways for advanced catalytic transformations.