One-step fabrication of novel MIL-53(Fe, Al) for synergistic adsorption-photocatalytic degradation of tetracycline

Abstract

Bimetallic MOFs (MIL-53 (Fe, Al)) were successfully fabricated via a facile one-step solvothermal method for the removal of tetracycline (TC) from aqueous solutions. Tetracycline adsorption and photocatalytic experiments indicate that the optimum bimetallic synthetic molar ratio is 3:2 (40%MIL-53(Fe, Al)). The adsorption data are well fitted by the Freundlich model and pseudo-second-order adsorption kinetics. 40%MIL-53(Fe, Al) has an adsorption capacity of up to 402.033 mg/g. After the dark adsorption phase, 10 mg of 40%MIL-53(Fe, Al) can remove 94.33% of the tetracycline in a 70 mL aqueous solution (20 mg/L) under 50 min irradiation, while only 71.39% and 81.82% of the tetracycline are removed by MIL-53(Fe) and MIL-53(Al) under the same conditions. In addition, 40%MIL-53(Fe, Al) exhibits a significant adsorption-photocatalytic synergy (under direct irradiation without a dark adsorption phase), in which the pseudo-first-order kinetic constant increases by a factor of 3.11. Quenching experiments and ESR characterization indicate that ·O2−, ·OH, and h+ are the main active species in the photocatalytic process. Meanwhile, 40%MIL-53(Fe, Al) demonstrates good stability, with a tetracycline removal rate that still reaches 83.70% after 4 cycles. These results suggest that the prepared 40%MIL-53(Fe, Al) catalyst is a novel adsorption-photocatalytic material that can be used for the efficient treatment of tetracycline.