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Incorporating Fe-O cluster in Multivariate (MTV) metal-organic frameworks for promoting visible-light photo-Fenton degradation of micropollutants from water
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-06-09 , DOI: 10.1016/j.cej.2022.137446
Xiang Li , Yuli Yao , Bo Wang

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 m2/g ∼1389 m2/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 μg/g min. The modified material enhanced the visible-light absorption and facilitated the formation of reactive oxygen species (•OH, 1O2, and O2•-) 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.



中文翻译:

在多变量 (MTV) 金属有机框架中加入 Fe-O 簇以促进水中微污染物的可见光光芬顿降解

探索高效的多相光芬顿催化对于先进的水净化至关重要。本研究合成了一系列随着 Fe 含量增加的多元 (MTV) 金属有机骨架 MIL-100 (Sc 0.98, 0.95, 0.87, 0.75, 0.58, Fe 0.02, 0.05, 0.13, 0.25 0.42 ) 催化剂以有效降解微污染物。通过将 Fe-O 簇结合到框架中,磺胺甲基噻唑 (SMX) 的降解率比 MTV MIL-100 (Sc 0.58, Fe 0.42 ) 提高了 11.85 倍。永久性多孔结构和高表面积(1597 m 2 /g ∼1389 m 2/g) 促进了吸附过程。结果表明,喹诺酮类和抗炎组的初始吸附率极高,v 0 = 463.16 ∼ 407.15 μg/g·min。改性材料增强了对可见光的吸收并促进了活性氧(•OH、1 O 2和 O 2 •-) 在太阳光的照射下。应用了电子顺磁共振俘获技术和猝灭实验。详细提出了日光照射下活性氧形成的途径。使用 UPLC-Q-TOF-MS 鉴定和定量分析芳香族中间体。我们相信,这种在 MOF 中加入混合金属簇的策略为提高当前材料的性能提供了有用的指导。

更新日期:2022-06-10
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