A series of bimetallic of FeCu metal–organic frameworks (MOFs) have been synthesised using a solvothermal process by varying the ratio between the two metals. Further, the bimetallic MOF catalysts were characterised by X-ray powder diffraction, scanning electron microscopy, and infrared spectroscopy techniques. Their catalytic properties for activation of peroxymonosulphate (PMS) have been tested by the removal of a model dye, rhodamine B. As a result, NH2–Fe2.4Cu1-MOF demonstrated the highest degradation, the effect of the ratio NH2–Fe2.4Cu1-MOF/PMS has been studied, and the main reactive species have been assessed. The application of these MOFs in powder form is difficult to handle in successive batch or flow systems. Thus, this study assessed the feasibility of growing NH2–Fe2,4Cu1-MOF on polyacrylonitrile (PAN) spheres using the one-pot solvothermal synthesis method. The optimisation of the catalytic activity of the synthesised composite (NH2–Fe2.4Cu1-MOF@PAN) has been evaluated by response surface methodology using a central composite face-centred experimental design matrix and selecting as independent variables: time, PMS concentration, and catalyst dosage. Based on the results, the optimisation of the operational conditions has been validated. At 2.5 mM PMS, 90 min, and 1.19 g·L−1 of catalyst dosage, maximum degradation (80.92%) has been achieved, which doubles the removal values obtained in previous studies with other MOFs. In addition, under these conditions, the catalyst has been proven to maintain its activity and stability for several cycles without activity loss.
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