Cooperation of oxygen vacancy and FeIII/FeII sites in H2-reduced Fe-MIL-101 for enhanced Fenton-like degradation of organic pollutants
2023
Bao, Chaosheng | Wang, Hu | Wang, Caiyun | Zhang, Xiaohui | Zhao, Xiaoliang | Dong, Chung-Li | Huang, Yu-Cheng | Chen, Shuai | Guo, Peng | She, Xilin | Sun, Yuanyuan | Yang, Dongjiang
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 °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 •OH at the Feᴵᴵ sites. Further, electron-rich OVs sites could increase the interaction 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 using iron-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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