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Magnetically recoverable Fe3O4 nanoparticles have been synthesized as a catalyst for the cyclocondensation of 1,2-phenylenediamines with orthoesters under solvent-free conditions.Catalyst loadings can be as low as 1 mol% to give high yields of the corresponding benzimidazole derivative at 80 ℃.This green method offers significant advantages in terms of its simplicity,low catalyst loadings,high product yields,and non-toxic nature.The Fe3O4 nanoparticles were characterized by X-ray diffraction,transmission electron microscopy,and Fourier transform infrared spectroscopy.