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通过应用基于紫外发光二极管(UV-LED)的高级氧化工艺(AOPs)降解抗生素抗性基因(ARGs)的效果。

The efficacies of degrading antibiotic resistance genes (ARGs) by applying UV light emitting diodes (UV-LEDs) based advanced oxidation processes (AOPs).

作者信息

Ghosh Shayok, Zhang Guanghan, Chen Yiwei, Hu Jiangyong

机构信息

Department of Civil & Environmental Engineering, National University of Singapore, 1 Engineering Drive 2, Singapore 117576, Singapore.

NUS Environmental Research Institute, National University of Singapore, #02-03, T-Lab Building 5A Engineering Drive 1 Singapore 117411, Singapore.

出版信息

Water Res. 2025 May 15;276:123197. doi: 10.1016/j.watres.2025.123197. Epub 2025 Jan 27.

Abstract

Widespread dissemination of antibiotic resistance genes (ARGs) in the aquatic environment has become a concern for public health. This study evaluated the performance of UV light emitting diodes (UV-LEDs) based advanced oxidation processes (AOPs) such as the simultaneous application of UV-LEDs (265 and 285 nm) and oxidants (chlorine and persulfate) to degrade ARGs. Persulfate (PS)-based treatment systems showed lower log-removals than chlorine (Cl) to degrade extracellular ARGs (e-ARGs), with the molar absorption coefficients (ɛ) for PS being 13.66 and 66.4 times lower than those for chlorine at 265 nm and 285 nm, respectively. While 285/Cl exhibited stronger synergistic effects achieving an optimal synergy value of 4.02 log, 265/Cl displayed better degradation rates with the maximum degradation rate of 0.117 cm/mJ. Degradation rates induced by 265/PS were 1.2 to 2.2 times higher than 285/PS across all applied concentrations of oxidants. 265/PS also demonstrated a more pronounced synergistic effect than 285/PS with an optimal synergy value of 2.56. Quantum yields (Φ) at 265 nm are ∼1.1 times higher than at 285 nm for both oxidants. Cl has ∼1.7 times higher ɛ-value at 285 nm than at 265 nm, while persulfate's ɛ-value is ∼2.93 times higher at 265 nm than at 285 nm. Thus, the better ɛ-value of Cl at 285 nm improved the performance of 285/Cl over 285/PS than 265 nm-based AOPs. Radical roles were investigated using scavenger studies with nitrobenzene (NB) and ethanol (EtOH) as quenchers. EtOH reacts quickly with hydroxyl radical (HO·), reactive chlorine species (RCS), and sulfate radical (SO·‾), while NB primarily reacts with HO· and shows minimal reactivity with other radicals. The involvement of radicals in different AOPs varied depending on the wavelength. For 265/Cl and 285/PS, HO· was the primary contributor, with minimal contributions from other radicals. Significant contributions from RCS and SO·‾ radicals were observed for 285/Cl and 265/PS, respectively, alongside HO·. Plasmid linearization was observed when the plasmid was subjected to AOPs, confirming the role of radicals in initiating the process of plasmid linearization through their interaction with the sugar-phosphate backbone. Scavenging of radicals by cellular components diminished the synergistic impact of AOPs on intracellular ARGs (i-ARGs) degradation. While AOPs demonstrated a notable degradation of extracellular polymeric substances (EPS), the absence of EPS didn't enhance the degradation of i-ARGs. The overall concentration of free ARGs (f-ARGs) was influenced by the interplay of two factors: the extent of membrane damage and the efficacy of e-ARG degradation. This study offers detailed insights into the effectiveness and mechanisms of UV-LED based AOPs for inactivating various forms of ARGs, as well as the associated challenges. Understanding the relevant mechanisms and challenges will assist in developing a sustainable and efficient UV-LED based AOP technology for removing ARGs from water and wastewater.

摘要

抗生素抗性基因(ARGs)在水环境中的广泛传播已成为公共卫生领域的一个关注点。本研究评估了基于紫外发光二极管(UV-LEDs)的高级氧化工艺(AOPs)的性能,例如同时应用UV-LEDs(265和285纳米)和氧化剂(氯和过硫酸盐)来降解ARGs。基于过硫酸盐(PS)的处理系统在降解细胞外ARGs(e-ARGs)方面的对数去除率低于氯(Cl),在265纳米和285纳米处,PS的摩尔吸收系数(ɛ)分别比氯低13.66倍和66.4倍。虽然285/Cl表现出更强的协同效应,达到了4.02对数的最佳协同值,但265/Cl显示出更好的降解速率,最大降解速率为0.117厘米/毫焦。在所有应用的氧化剂浓度下,265/PS诱导的降解速率比285/PS高1.2至2.2倍。265/PS也表现出比285/PS更显著的协同效应,最佳协同值为2.56。两种氧化剂在265纳米处的量子产率(Φ)比在285纳米处高约1.1倍。Cl在285纳米处的ɛ值比在265纳米处高约1.7倍,而过硫酸盐的ɛ值在265纳米处比在285纳米处高约2.93倍。因此,Cl在285纳米处更好的ɛ值使得285/Cl比基于265纳米的AOPs在性能上优于285/PS。使用硝基苯(NB)和乙醇(EtOH)作为淬灭剂的清除剂研究对自由基的作用进行了研究。EtOH能快速与羟基自由基(HO·)、活性氯物种(RCS)和硫酸根自由基(SO·‾)反应,而NB主要与HO·反应,与其他自由基的反应性最小。不同AOPs中自由基的参与情况因波长而异。对于265/Cl和285/PS,HO·是主要贡献者,其他自由基的贡献最小。对于285/Cl和265/PS,分别观察到RCS和SO·‾自由基的显著贡献,同时还有HO·。当质粒受到AOPs作用时观察到质粒线性化,证实了自由基通过与糖磷酸骨架相互作用在启动质粒线性化过程中的作用。细胞成分对自由基的清除减弱了AOPs对细胞内ARGs(i-ARGs)降解的协同影响。虽然AOPs对细胞外聚合物物质(EPS)有显著降解作用,但EPS的缺失并未增强i-ARGs的降解。游离ARGs(f-ARGs)的总体浓度受两个因素相互作用的影响:膜损伤程度和e-ARG降解效率。本研究详细深入地探讨了基于UV-LED的AOPs灭活各种形式ARGs的有效性和机制,以及相关挑战。了解相关机制和挑战将有助于开发一种可持续且高效的基于UV-LED的AOP技术,用于从水和废水中去除ARGs。

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