In this research study we designed and synthesized CoII(macrocyclic Schiff base ligand containing 1,4‐diazepane) immobilized on Fe3O4 nanoparticles as a novel, recyclable, and heterogeneous catalyst. The nanomaterial was fully characterized using various techniques such as Fourier‐transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, X‐ray diffraction, energy‐dispersiveX‐ray spectroscopy, thermogravimetric analysis, vibrating sample magnetometry, differential reflectance spectroscopy, Brunauere–Emmette–Teller method, inductively coupled plasma, and elemental analysis (CHNS). Then, the catalytic performance was successfully investigated in the multicomponent synthesis of 2‐amino‐4‐aryl‐6‐(phenylsulfanyl)pyridine‐3,5‐dicarbonitrile and 2‐amino‐5,10‐dioxo‐4‐aryl‐5,10‐dihydro‐4H‐benzo[g]chromene‐3‐carbonitrile derivatives. Furthermore, the catalyst was isolated using a simple filtration, and recovery of the nanocatalyst was demonstrated five times without any loss of activity.

Fe3O4‐supported copper (II) Schiff‐Base complex has been synthesized through post‐modification with 1,3‐phenylenediamine followed by further post‐modification with salicylaldehyde and coordination with Cu(II) ion. The resulted Fe3O4@SiO2‐imine/phenoxy‐Cu(II) magnetic nanoparticles (MNPs) were characterized by various techniques including SEM, TEM, XRD, XPS, EDX, VSM, FT‐IR, and ICP. The catalytic activity as a magnetically recyclable heterogeneous catalyst for one‐pot, three‐component synthesis of 2‐amino‐4H‐chromene derivatives was examined. The catalyst is efficient in the reaction and can be recovered by magnetic separation and recycled several times without significant loss in the catalytic activity.

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