Rational design of coordination environment of Fe-based metal-organic frameworks (Fe-MOFs) is still a challenge in achieving enhanced catalytic activity for Fenten-like advanced oxidation process. Here in, novel porous Fe-MOFs with modulated O-Fe-N coordination was developed by configurating amino terephthalic acid (H2ATA) and pyrazine-dicarboxylic acid (PzDC) (Fe-ATA/PzDC-7:3). PzDC ligands introduce pyridine-N sites to form O-Fe-N coordination with lower binding energy, which affect the local electronic environment of Fe-clusters in Fe-ATA, thus decreased its interfacial H2O2 activation barrier. O-Fe-N coordination also accelerate Fe(II)/Fe(III) cycling of Fe-clusters by triggering the reactive oxidant species mediated Fe(III) reduction. As such, Fe-ATA/PzDC-7:3/H2O2 system exhibited excellent degradation performance for typical antibiotic sulfamethoxazole (SMX), in which the steady-state concentration of hydroxyl radical (OH) was 1.6 times higher than that of unregulated Fe-ATA. Overall, this study highlights the role of O-Fe-N coordination and the electronic environment of Fe-clusters on regulating Fenton-like catalytic performance, and provides a platform for precise engineering of Fe-MOFs.
Pyrazine-based iron metal organic frameworks (Fe-MOFs) with modulated O-Fe-N coordination for enhanced hydroxyl radical generation in Fenton-like process.
Zongchen Li,Jian Lu,Tianyang Zhang,Ying Liu,Renjie Pan,Qi Fu,Xinru Liu,Shun Mao,Bin Xu
Published 2024 in Journal of Colloid and Interface Science
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- Publication year
2024
- Venue
Journal of Colloid and Interface Science
- Publication date
2024-06-01
- Fields of study
Medicine, Materials Science, Chemistry, Environmental Science
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Semantic Scholar, PubMed
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