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不同 Fe-N 共掺杂生物炭活化过一硫酸盐同时去除抗生素耐药菌和抗生素耐药基因:吡啶-N 和 Fe-N 位点的关键作用。

Simultaneous elimination of antibiotic-resistant bacteria and antibiotic resistance genes by different Fe-N co-doped biochars activating peroxymonosulfate: The key role of pyridine-N and Fe-N sites.

机构信息

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

出版信息

J Colloid Interface Sci. 2024 Aug 15;668:12-24. doi: 10.1016/j.jcis.2024.04.082. Epub 2024 Apr 15.

DOI:10.1016/j.jcis.2024.04.082
PMID:38669989
Abstract

The coexistence of antibiotic resistance genes (ARGs) and antibiotic-resistant bacteria (ARB) in the environment poses a potential threat to public health. In our study, we have developed a novel advanced oxidation process for simultaneously removing ARGs and ARB by two types of iron and nitrogen-doped biochar derived from rice straw (FeN-RBC) and sludge (FeN-SBC). All viable ARB (approximately 10 CFU mL) was inactivated in the FeN-RBC/ peroxymonosulfate (PMS) system within 40 min and did not regrow after 48 h even in real water samples. Flow cytometry identified 96.7 % of dead cells in the FeN-RBC/PMS system, which verified the complete inactivation of ARB. Thorough disinfection of ARB was associated with the disruption of cell membranes and intracellular enzymes related to the antioxidant system. Whereas live bacteria (approximately 200 CFU mL) remained after FeN-SBC/PMS treatment. Intracellular and extracellular ARGs (tetA and tetB) were efficiently degraded in the FeN-RBC/PMS system. The production of active species, primarily •OH, SO and Fe (IV), as well as electron transfer, were essential to the effective disinfection of FeN-RBC/PMS. In comparison with FeN-SBC, the better catalytic performance of FeN-RBC was mainly ascribed to its higher amount of pyridine-N and Fe, and more reactive active sites (such as CO group and Fe-N sites). Density functional theory calculations indicated the greater adsorption energy and Bader charge, more stable Fe-O bond, more easily broken OO bond in FeN-RBC/PMS, which demonstrated the stronger electron transfer capacity between FeN-RBC and PMS. To encapsulate, our study provided an efficient and dependable method for the simultaneous elimination of ARGs and ARB in water.

摘要

抗生素耐药基因 (ARGs) 和抗生素耐药菌 (ARB) 在环境中的共存对公共健康构成了潜在威胁。在我们的研究中,我们开发了一种新型的高级氧化工艺,通过两种类型的铁和氮掺杂生物炭(来自稻草的 FeN-RBC 和来自污泥的 FeN-SBC)同时去除 ARGs 和 ARB。所有存活的 ARB(约 10 CFU mL)在 40 分钟内被 FeN-RBC/过一硫酸盐 (PMS) 系统灭活,并且在 48 小时后即使在实际水样中也不会再生。流式细胞术鉴定出 FeN-RBC/PMS 系统中 96.7%的死细胞,这验证了 ARB 的完全失活。ARB 的彻底消毒与破坏与抗氧化系统相关的细胞膜和细胞内酶有关。而在 FeN-SBC/PMS 处理后,仍有活细菌(约 200 CFU mL)存在。细胞内和细胞外的 ARGs(tetA 和 tetB)在 FeN-RBC/PMS 系统中得到有效降解。活性物质的产生,主要是 •OH、SO 和 Fe (IV),以及电子转移,是 FeN-RBC/PMS 有效消毒的关键。与 FeN-SBC 相比,FeN-RBC 更好的催化性能主要归因于其更高的吡啶-N 和 Fe 含量,以及更多的反应活性位点(如 CO 基团和 Fe-N 位点)。密度泛函理论计算表明,FeN-RBC/PMS 中 FeN-RBC 的吸附能和 Bader 电荷更大,Fe-O 键更稳定,OO 键更容易断裂,这表明 FeN-RBC 和 PMS 之间具有更强的电子转移能力。总之,我们的研究为水中同时消除 ARGs 和 ARB 提供了一种高效可靠的方法。

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