In situ synthesis of oxygen-doped carbon quantum dots embedded in MIL-53(Fe) for efficient degradation of oxytetracycline.

Introducing carbon quantum dots (CQDs) into photocatalysts is believed to boost the charge transfer rate and reduce charge complexation. Doping heteroatoms such as N, S, or P enable CQDs to have an uplifting electron transfer capability. However, the application of oxygen-doped CQDs to improve the performance of photocatalysts has rarely been reported. Herein, a type of carbon-oxygen quantum dots (COQDs) was in situ embedded into MIL-53(Fe) to aid peroxydisulfate (PDS)-activated degradation of oxytetracycline (OTC) under visible light irradiation. The successful embedding of COQDs was confirmed by XRD, FT-IR, XPS, SEM, and TEM techniques. Photoelectrochemical testing confirmed its better performance. The prepared COQDs1/MIL-53(Fe) showed 88.2% decomposition efficiency of OTC in 60 min, which was 1.45 times higher than that of pure MIL-53(Fe). In addition, the performance of the material was tested at different pH, OTC concentrations, catalyst dosing, and PDS dosing. It was also subjected to cyclic testing to check stability. Moreover, free radical trapping experiments and electron paramagnetic resonance were conducted to explore the possible OTC deterioration mechanism. Our work provides a new idea for the development of MOFs for water treatment and remediation.

Removal of oxytetracycline from water by S-doped MIL-53(Fe): Synergistic effect of surface adsorption and persulfate activation.

In this study, a novel catalyst based on MIL-53(Fe) was synthesized and modified through sublimed sulfur (S-MIL-53(Fe)) to induce a synergistic effect of surface adsorption and persulfate activation. The S-doped modification not only increased the surface area but also accelerated the electron transfer process of the iron cycle. The performance of the newly synthesized S-MIL-53(Fe) adsorptive catalyst was evaluated by chemical adsorption and peroxydisulfate (PDS) activated removal of an emerging pollutants, oxytetracycline (OTC). The S-MIL-53(Fe) adsorptive catalyst was able to adsorb 61.7% of OTC after 120 min, and the removal efficiency reached 84.8% within 5 min after PDS dosing. The boosting effect of sulfur on the system was confirmed by characterization analysis and experimental testing. Even after 7 cycles, the removal efficiency of S-MIL-53(Fe) (69.0%) for OTC remained superior to that of pure MIL-53(Fe) (25.1%). Additionally, the adsorption kinetics and adsorption isotherm model of the material were investigated. The possible OTC degrading process was proposed based on radical quenching and electron paramagnetic resonance (EPR). This study provides a feasible way to fabricate an S-doped MIL-53(Fe) adsorptive catalyst for the remediation of antibiotics-containing wastewater.