Nearly zero peroxydisulfate consumption for persistent aqueous organic pollutants degradation via nonradical processes supported by in-situ sulfate radical regeneration in defective MIL-88B(Fe)

被引:43
|
作者
Li, Yu-Hang [1 ,2 ]
Wang, Chong-Chen [1 ,2 ]
Wang, Fei [1 ,2 ]
Liu, Wen [3 ]
Chen, Long [3 ]
Zhao, Chen [1 ,2 ]
Fu, Huifen [1 ,2 ]
Wang, Peng [1 ,2 ]
Duan, Xiaoguang [4 ]
机构
[1] Beijing Univ Civil Engn & Architecture, Sch Environm & Energy Engn, Beijing Key Lab Funct Mat Bldg Struct & Environm, Beijing 100044, Peoples R China
[2] Beijing Univ Civil Engn & Architecture, Beijing Energy Conservat & Sustainable Urban & Ru, Beijing 100044, Peoples R China
[3] Peking Univ, Coll Environm Sci & Engn, Minist Educ, Key Lab Water & Sediment Sci, Beijing 100871, Peoples R China
[4] Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
Defective MIL-88B(Fe); Persulfate regeneration; Nonradical Pathway; Persistent bisphenol A degradation; ENHANCED DEGRADATION; OXYGEN VACANCY; ACTIVATION; FRAMEWORK; PERSULFATE; OXIDATION;
D O I
10.1016/j.apcatb.2023.122699
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The porous defective MIL-88B(Fe) with abundant oxygen vacancies and Fe-N sites was fabricated to accomplish nearly zero peroxydisulfate (PDS) consumption for persistent bisphenol A (BPA) degradation via electron-transfer pathway (ETP). Interestingly, the generated sulfates during ETP were oxidized to yield the confined sulfate radicals and to accomplish the peroxydisulfate regeneration in the fine-tuned MIL-88B(Fe), which was verified by series experiments and DFT calculations. Further studies suggested that the optimal De-MIL-88B(Fe)-1.25 catalyst achieved the persistent nonradical reactions for BPA decomposition under visible light irradiation with both low input and low consumption of PDS. It was the first case to achieve nearly zero PDS consumption for emerging pollutants elimination, which provided new strategy to design and tune defective metal-organic frameworks for the purpose of reducing the stoichiometry between PDS and contaminants for nearly zero PDS consumption.
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页数:11
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