College of Chemistry, Jilin University, Changchun 130012, China
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
University of Science and Technology of China, Hefei 230026, China
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Fe2-N-C was prepared by encapsulating nonacarbonyldiiron (Fe2(CO)9) into zeolitic imidazolate framework-8 (ZIF-8) by in situ synthesis. Studies have shown that the catalyst can efficiently catalyze the degradation of dyes and organic pollutants by activating peroxymonosulfate (PMS). The results show that the catalytic degradation activity of Fe2-N-C is twice that of Fe1-N-C and Fe3-N-C due to its unique Fe2N6 coordination structure, which fulfilled the complete degradation of rhodamine B (RhB), bisphenol A (BPA), and 2,4-dichlorophenol (2,4-DP) within 2 min. Electron paramagnetic resonance (EPR) and radical quenching experiments confirmed that 1O2 and Fe(IV) generated by PMS activation were the key active species.
Abstract
Atomically dispersed catalysts have been widely studied due to their high catalytic activity and atom utilization. Single-atom catalysts have achieved breakthrough progress in the degradation of emerging organic contaminants (EOCs) by activating peroxymonosulfate (PMS). However, the construction of atomically dispersed catalysts with diatomic/multiatomic metal active sites by activating PMS to degrade pollutants is still seldom reported, despite the unique merits of atom-pair in synergistic electronic modulation and breaking stubborn restriction of scaling relations on catalytic activity. We have synthesized Fe1-N-C, Fe2-N-C, and Fe3-N-C catalysts with monoatomic iron, diatomic iron, and triatomic iron active center, respectively. The results show that the catalytic degradation activity of Fe2-N-C is twice that of Fe1-N-C and Fe3-N-C due to its unique Fe2N6 coordination structure, which fulfilled the complete degradation of rhodamine B (RhB), bisphenol A (BPA), and 2,4-dichlorophenol (2,4-DP) within 2 min. Electron paramagnetic resonance (EPR) and radical quenching experiments confirmed that the reaction was a non-radical reaction on the catalyst surface. And singlet oxygen and Fe(IV) are the key active species.
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