Constructing tunable coordinatively unsaturated sites in Fe-based metal-organic framework for effective degradation of pharmaceuticals in water: Performance and mechanism

被引:7
|
作者
Li, Yunyun [1 ,2 ]
Li, Xiang [1 ]
Wang, Bo [1 ]
机构
[1] Beijing Inst Technol, Sch Chem & Chem Engn, Adv Res Inst Multidisciplinary Sci, Beijing 100081, Peoples R China
[2] Yan An Univ, Shanxi Key Lab Chem React Engn, Coll Chem & Chem Engn, Yanan 716000, Shanxi, Peoples R China
基金
中国国家自然科学基金;
关键词
Micropollutants; Charge-transfer; Photocatalysis; Metal cluster; Lewis acid; PHOTO-FENTON; MIL-53(FE); EVOLUTION; OXIDATION; CATALYST;
D O I
10.1016/j.chemosphere.2022.136816
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Micropollutants are ubiquitously detected in the aqueous environment, which needs to be removed by novel materials effectively. Herein, we synthesized a photo-Fenton catalyst based on MIL-53 (Fe) to effectively degrade sulfadimidine, one of the micropollutants in water. Abundant Lewis acid active sites (54.26 mu mol/g) were successfully constructed within the metal cluster using FeCl3 center dot 6H(2)O, 1,4-benzene dicarboxylate, and modulators. This study reports a strategy by effectively constructing tunable Lewis acid active sites within the cavities in MIL53 (Fe) via a facile solvothermal reaction for sixteen micropollutants removal. The photo-Fenton degradation of sulfamethazine was completely removed (similar to 99%) within only 1 min with a small amount of hydrogen peroxide added. Both theoretical calculation and the experiment results prove that introducing the unsaturated coordinated/lewis acid sites can remarkably reduce the band gap energy and increase the charge-separation efficiency by changing the electron configuration with more distribution asymmetry of structures. The effective degradation of structurally diverse pharmaceuticals with environmentally relevant concentrations was studied by immobilizing MOF-catalyst into a PVDF support. This work advanced the development of effective approaches for emergency contaminants control.
引用
收藏
页数:11
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