Structure-activity relationship in periodate activation by Fe-MOFs:Why MIL-101(Fe)outperforms other MIL-series in antibiotic degradationOA
Antibiotics are emerging pollutants that pose significant risks to environmental and human health.Periodate(PI)-based advanced oxidation processes have shown promise for their effective degradation.In this study,we systematically investigate the structure-activity relationship of four representative Fe-based metal-organic frameworks(Fe-MOFs)-MIL-101(Fe),MIL-88B(Fe),MIL-88A(Fe),and MIL-53(Fe)-as PI activators for tetracycline(TC)degradation.Among them,MIL-101(Fe)exhibited the highest catalytic performance,owing to its unique Fe3O-OH nodes and mesoporous architecture.The MIL-101(Fe)/PI system achieved 93.3%TC degradation and 55.9%mineralization rate within 60 min.Mechanistic studies combining scavenger quenching,sulfoxide probe transformation,X-ray photoelectron spectroscopy,and X-ray absorption fine structure confirmed the generation of multiple reactive oxygen species,and high-valent Fe(IV)]O and O_(2)^(·-)played major roles in the tetracycline degradation process.Density functional theory calculations further revealed that MIL-101(Fe)and MIL-88B(Fe)effectively interact with PI to form Fe(Ⅲ)-superoxide(Fe(Ⅲ)-O-O^(·-)),a key intermediate in Fe(IV)]O generation.In contrast,the adsorption energy of MIL-53(Fe)and MIL-88A(Fe)was relatively weak,with fewer binding sites,resulting in poor performance.The synergy between Fe(Ⅲ)-O-O^(·-)formation and the pore accessibility of MIL-101(Fe)accounted for its superior catalytic efficiency.This work not only clarifies the structural factors governing PI activation in Fe-MOFs,but also proposes a mechanistically informed strategy for designing high-performance catalysts for antibiotic degradation.
Ning Liu;Jingwen Xu;Yixuan Zhai;Ziyi Zhang;Yi Dang;Yusong Cao;Zhe Li;Wenyuan Huang;Xiaodong Zhang;Liang Tang
School of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaDepartment of Chemistry,King''s College London,London,WC2R 2LS,UK The Francis Crick Institute,London,NW11AT,UKDepartment of Chemistry,University of Manchester,Manchester,M139PL,UKSchool of Environment and Architecture,University of Shanghai for Science and Technology,Shanghai,200093,ChinaKey Laboratory of Organic Compound Pollution Control Engineering(MOE),School of Environmental and Chemical Engineering,Shanghai University,Shanghai,200444,China
资源环境
PeriodateAdvanced oxidation processesFe-MOFsAntibiotic degradationFe(Ⅲ)-Superoxide
《Green Energy & Environment》 2026 (2)
P.578-590,13
National Natural Science Foundation of China(Nos.42177405,42377359,12075152)Energy Science and Technology discipline under the Shanghai Class IV Peak Disciplinary Development Program for the financial support.W.Y.Huang thanks the China Scholarship Council(CSC)for funding.
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