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

被引：77

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

来源：

JOURNAL OF HAZARDOUS MATERIALS | 2023年 / 441卷

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.

引用

页数：11

共 56 条

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