期刊
CHEMICAL ENGINEERING JOURNAL
卷 446, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.137446
关键词
Isostructural; Degradation; Micropollutants; Visible-light; photo-Fenton
资金
- National Natural Science Foundation of China [21625102, 21971017, 21906007]
- National Key Research and Development Program of China [2020YFB1506300]
- Beijing Institute of Technology Research Fund Program
Exploring efficient heterogeneous photo-Fenton catalysis is crucial for advanced water purification. In this study, a series of multivariate metal-organic framework catalysts were synthesized, and by incorporating the Fe-O cluster into the framework, the degradation rate of SMX was significantly improved. The modified material enhanced visible-light absorption and facilitated the formation of reactive oxygen species, leading to further improvement in degradation efficiency.
Exploring efficient heterogeneous photo-Fenton catalysis is crucial for advanced water purification. In this study, a series of multivariate (MTV) metal-organic framework MIL-100 (Sc 0.98, 0.95, 0.87, 0.75, 0.58, Fe 0.02, 0.05, 0.13, 0.25 0.42) catalysts with increasing Fe contents were synthesized to effectively degrade micropollutants. By incorporating the Fe-O cluster into the framework, the degradation rate of sulfamethylthiazole (SMX) was improved 11.85 times over the MTV MIL-100 (Sc 0.58, Fe 0.42). The permanent porous structures and high surface areas (1597 m(2)/g - 1389 m(2) f/g) facilitated the adsorption processes. Results show that the initial adsorption rates for quinolone and anti-inflammatory groups were extremely high, with v0 = 463.16 - 407.15 mu g/g min. The modified material enhanced the visible-light absorption and facilitated the formation of reactive oxygen species (center dot OH, O-1(2), and O-2(center dot-)) under the irradiation of solar light. Electron paramagnetic resonance trapping technologies and quenching experiments were applied. The pathway for ROS formation under solar-light irradiation was proposed in detail. Aromatic intermediates were identified and quantitatively analyzed using UPLC-Q-TOF-MS. We believe that this strategy of incorporating mixed metal clusters in MOFs offers useful guidance to improve the performance of current materials.
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