Cooperation of oxygen vacancy and FeIII/FeII sites in H2-reduced Fe-MIL-101 for enhanced Fenton-like degradation of organic pollutants

被引:65
作者
Bao, Chaosheng [1 ]
Wang, Hu [1 ]
Wang, Caiyun [1 ]
Zhang, Xiaohui [1 ]
Zhao, Xiaoliang [1 ]
Dong, Chung-Li [2 ]
Huang, Yu-Cheng [2 ]
Chen, Shuai [3 ]
Guo, Peng [4 ]
She, Xilin [1 ]
Sun, Yuanyuan [1 ]
Yang, Dongjiang [1 ]
机构
[1] Qingdao Univ, Inst Marine Biobased Mat, Shandong Collaborat Innovat Ctr Marine Biobased Fi, Sch Environm Sci & Engn,State Key Lab Biofibers &, Qingdao 266071, Peoples R China
[2] Tamkang Univ, Res Ctr X ray Sci, Dept Phys, Tamsui 25137, Taiwan
[3] Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Peoples R China
[4] China Univ Petr East China, Adv Chem Engn & Energy Mat Res Ctr, Qingdao 266580, Peoples R China
基金
中国国家自然科学基金;
关键词
Mixed valence; Oxygen vacancy; Heterogeneous Fenton -like reaction; Degradation; Fe-MIL-101; COORDINATIVELY UNSATURATED SITES; WATER; OXIDATION; ADSORPTION; FRAMEWORKS; CIPROFLOXACIN; EFFICIENCY; PRODUCTS; ACID;
D O I
10.1016/j.jhazmat.2022.129922
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Metal-organic frameworks (MOFs)-based Fenton-like catalysts with mixed-valence and oxygen vacancies (OVs) were designed by H2 reduction of Fe-MIL-101 to activate H2O2. The degradation efficiency of norfloxacin (NOR) by Fe-MIL-101 treated at 220 degrees C (Fe-MIL-101-H-220) (100 %) was significantly higher than that of original Fe -MIL-101 (51.1 %) and showed excellent degradation efficiency for other pollutants. Moreover, the Fe-MIL-101-H-220/H2O2 system exhibited superior degradation efficiency for NOR over a wide pH range and could maintain 93.6 % after 5 cycles. The high performance is assigned to the cooperation of OVs and FeIII/FeII sites.H2O2 could be rapidly activated to produce center dot OH at the FeII sites. Further, electron-rich OVs sites could increase the inter-action between adjacent FeIII sites and H2O2, benefitting the reduction of FeIII site to FeII site and accelerating FeIII/FeII cycle. This study provides a new strategy for the enhanced Fenton-like degradation of pollutants usingiron-based MOFs catalyst, and unveils the intrinsic origin of the superior activity of thermally reduced Fe-MIL -101 for H2O2 activation.
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页数:11
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