Iron single-atom catalysts drive peroxymonosulfate activation for efficient degradation of extracellular antibiotic resistance genes through singlet oxygen-mediated DNA damage
文献类型: 外文期刊
作者: Zhang, Yunhong;Yu, Ping;Guo, Xujing;Wang, Lan;Wang, Wenguo;Deng, Liangwei;Zhang, Hongwei;He, Ting;Xiong, Zhaokun;Lai, Bo
作者机构:
关键词: Single-atom catalyst;Peroxymonosulfate;Singlet oxygen;Antibiotic resistance genes;DNA damage
期刊名称: CHEMICAL ENGINEERING JOURNAL
ISSN: 1385-8947
年卷期: 2025 年 525 卷
页码:
收录情况: SCIE(2025版) ; ; EI(2025版)
摘要: The misuse of antibiotics in the aquatic environment has triggered a serious contamination problem of extra-cellular antibiotic resistance genes (eARGs), posing significant threats to human health and ecological safety. This study developed an efficient treatment system based on an iron single-atom catalyst (Fe SACs) to activate peroxymonosulfate (PMS) for addressing this issue. The Fe SACs catalysts with Fe-N5 active sites were successfully synthesized through a soft-template method for polypyrrole hydrogel preparation, followed by an iron adsorption-pyrolysis-acid etching process. The Fe SACs/PMS system achieved a 3.76 logs removal of eARGs within 30 min under optimized conditions, demonstrating environmental applicability and broad-spectrum gene degradation capability. Its practical application, however, requires further optimization for complex real wastewater matrices where background components can diminish treatment effect. Mechanistic studies revealed that the Fe-N5 site activate PMS via electron transfer to generate singlet oxygen (1O2), which degrades plasmid DNA through a tripartite mechanism of structural destruction-functional inactivation-component mineralization: 1O2 disrupts DNA base and supercoiled structures, induces strand breakage to inactivate gene amplification functionality, and ultimately mineralizes eARGs into small molecules and inorganic ions. The system effectively suppresses environmental transmission of eARGs, providing a highly efficient and stable solution for controlling resistance gene pollution in aquatic environments, with significant implications for ecological and health protection.
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