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Efficient non-radical Dominated activation of persulfate through magnetite nanoparticles for tetracycline oxidation in natural water systems: Mechanism Evaluation and DFT calculations
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2024-12-19 , DOI: 10.1016/j.ces.2024.121119 Jingyi Shang, Xudong Hu, Shuang Li, Xinhai Wang, Usman Farooq
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2024-12-19 , DOI: 10.1016/j.ces.2024.121119 Jingyi Shang, Xudong Hu, Shuang Li, Xinhai Wang, Usman Farooq
Antibiotic resistance has emerged in recent years, posing a threat to human health and the environment. There is promising evidence that Fe3O4 nanomaterials can act as catalysts for the breakdown of antibiotics in aqueous systems. Herein, Fe3O4 was synthesized using a hydrothermal technique, and its potential as a catalyst for tetracycline (TC) degradation in the persulfate (PS) system was explored. Highly crystalline (73.4 %) Fe3O4 possessed a prominent octahedral and tetrahedral structure. After testing different combinations of Fe3O4 dosage, PS concentration, pH, and temperature, the optimal conditions for removing about 86.7 % of the TC were 0.20 g/L Fe3O4, 8.0 mM PS, and pH around 8. In contrast to the more typically seen sulfate (SO4•−) and hydroxyl (OH•) radicals, quenching tests showed that the non-radical oxo-specie (1O2) predominated in TC degradation, which was also supported by density functional theory (DFT) calculations, when the O
O bond was stretched, the free energy barrier of OO bond break (transition state) was 1.2 eV, followed by a thermodynamically favorable process to produce 1O2. However, the reaction energy barrier (2.03 eV) for generating OH• and SO4•− on Fe3O4 (4 4 0) was higher, making it difficult to trigger the reaction. Furthermore, electron spin resonance (ESR) tests validated the prominence of the 1O2 species in TC degradation. The stability experiments showed that the TC degradation efficiency remained at over 56 % after three cycles. Finally, natural water systems using lake and river water demonstrated that the Fe3O4 catalyst was suitable for practical applications, with more than 70 % TC degradation. Based on these findings, Fe3O4 nanomaterials showed non-radical dominant activation of PS as a potential candidate in practical applications for the degradation of organic pollutants in water systems.
更新日期：2024-12-20
O bond was stretched, the free energy barrier of OO bond break (transition state) was 1.2 eV, followed by a thermodynamically favorable process to produce 1O2. However, the reaction energy barrier (2.03 eV) for generating OH• and SO4•− on Fe3O4 (4 4 0) was higher, making it difficult to trigger the reaction. Furthermore, electron spin resonance (ESR) tests validated the prominence of the 1O2 species in TC degradation. The stability experiments showed that the TC degradation efficiency remained at over 56 % after three cycles. Finally, natural water systems using lake and river water demonstrated that the Fe3O4 catalyst was suitable for practical applications, with more than 70 % TC degradation. Based on these findings, Fe3O4 nanomaterials showed non-radical dominant activation of PS as a potential candidate in practical applications for the degradation of organic pollutants in water systems.
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