Self‐Assembled Flake‐Like Pd‐Doped CuCo ₂ O ₄ Nanomaterial for Efficient Microwave‐Assisted Cyanation of Aryl Halides Using K ₄ [Fe(CN) ₆ ]

Abstract Here, we demonstrate the synthesis of self‐assembled flake‐like Pd‐doped CuCo 2 O 4 , characterized by powder X‐ray diffraction (PXRD), field emission scanning electron microscopy (FESEM), energy dispersive X‐ray analysis (EDX), and high‐resolution transmission electron microscopy (HRTEM) with EDX and elemental mapping. The absence of peaks of Pd in the PXRD confirms the uniform and complete incorporation of Pd into cubic CuCo 2 O 4 . The crystallite size of 92 nm was calculated from PXRD while HRTEM reveals formation of nanosized particles with an average size of 16 nm. These particles were self‐assembled into a flake‐like structure with 0.32 µm‐thickness as evident from the FESEM study. The presence of Cu, Co, Pd, and O elements in the material was confirmed from FESEM‐EDX and TEM elemental mapping. The Pd‐doped CuCo 2 O 4 exhibits excellent catalytic activity for the cyanation of aryl halides using K 4 [Fe(CN) 6 ] as a non‐toxic, nonhygroscopic cyanide source, under microwave irradiation conditions. This protocol enables the cyanation of aryl chlorides, bromides, and iodides with good yields (60%–88%). The catalyst remains stable under reaction conditions and was reused for seven times. Finally, cyanoarenes were converted to various valuable products such as aromatic aldehydes, carboxylic acids, and esters. Remarkably, 1,3‐dicyanobenzene was used to synthesize a novel self‐assembled covalent organic cage.