In this work, a novel magnetic carbon nanotube@zeolitic imidazolate framework-67 (MCNT@ZIF-67) composite was prepared facilely by a one-pot method using Fe3O4@SiO2 as the magnetic element, CNTs as the carbon matrix, and 2-methylimidazole (2-MIM) and cobaltous nitrate (Co(NO3)2·6H2O) as the organic and inorganic elements, respectively. The obtained MCNT@ZIF-67 composite was characterized by transmission electron microscopy (TEM), Fourier transform-infrared spectroscopy (FT-IR), X-ray diffraction (XRD), and vibrating sample magnetometry (VSM). Static adsorption experiments demonstrated that the maximum adsorption capacity of MCNTs@ZIF-67 for tetrabromobisphenol A (TBBPA) is 83.23 mg g-1, and the sorption isotherm was fitted well by the Freundlich adsorption model. Dynamic adsorption experiments illustrated that the adsorption of TBBPA on MCNTs@ZIF-67 can reach equilibrium in 20 min, and the adsorption kinetics of TBBPA were fitted well by a pseudo-second-order kinetic model. The adsorption of TBBPA on MCNTs@ZIF-67 showed favorable selectivity. The pH and the NaCl and NH4Cl common salts did not affect the TBBPA adsorption. Then, the proposed magnetic composite was applied as the adsorbent for the rapid removal of TBBPA in water samples, and the removal ratio of MCNTs@ZIF-67 for TBBPA in different spiked water samples with different volumes was above 95% with RSD < 5%. Furthermore, as a new removal sorbent, the removal reproducibility of MCNTs@ZIF-67 for TBBPA was favorable and stable, with only a 6.0% decrease after 6 cycles.
Keywords: Carbon nanotubes; Magnetic separation; Metal organic frameworks; Pollutant removal; Tetrabromobisphenol A.