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

IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Shayok Ghosh , Guanghan Zhang , Yiwei Chen , Jiangyong Hu
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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 (Cl2) 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/Cl2 exhibited stronger synergistic effects achieving an optimal synergy value of 4.02 log, 265/Cl2 displayed better degradation rates with the maximum degradation rate of 0.117 cm2/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. Cl2 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 Cl2 at 285 nm improved the performance of 285/Cl2 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 (SO4·‾), 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/Cl2 and 285/PS, HO· was the primary contributor, with minimal contributions from other radicals. Significant contributions from RCS and SO4·‾ radicals were observed for 285/Cl2 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.

Abstract Image

Abstract Image

应用基于紫外发光二极管(UV-LED)的高级氧化工艺(AOPs)降解抗生素耐药基因(ARGs)的功效
抗生素耐药基因(ARGs)在水生环境中的广泛传播已成为公共卫生关注的问题。本研究评估了基于UV-LED的高级氧化工艺(AOPs)的性能,例如同时应用UV-LED(265和285 nm)和氧化剂(氯和过硫酸盐)来降解ARGs。过硫酸盐(PS)处理体系对胞外ARGs (e-ARGs)的对数去除率低于氯(Cl2),在265 nm和285 nm处,PS的摩尔吸收系数分别比氯低13.66和66.4倍。285/Cl2具有较强的协同效应,最优协同值为4.02 log; 265/Cl2具有较好的降解速率,最大降解速率为0.117 cm2/mJ。265/PS的降解率是285/PS的1.2 ~ 2.2倍。265/PS的协同效应也比285/PS更显著,最优协同值为2.56。两种氧化剂在265 nm处的量子产率(Φ)比285 nm处高约1.1倍。Cl2在285 nm处的流通量比265 nm高约1.7倍,而过硫酸盐在265 nm处的流通量比285 nm高约2.93倍。因此,在285 nm处Cl2的较优的λ值提高了285/Cl2在285/PS上的性能。以硝基苯(NB)和乙醇(EtOH)为猝灭剂,对自由基的清除作用进行了研究。EtOH与羟基自由基(HO•)、活性氯种(RCS)和硫酸盐自由基(SO4•)反应迅速,而NB主要与HO•反应,与其他自由基反应性最小。自由基在不同AOPs中的作用随波长的不同而不同。对于265/Cl2和285/PS, HO•是主要的贡献者,其他自由基的贡献很小。285/Cl2和265/PS的RCS和SO4•自由基以及HO•的贡献显著。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磷酸糖主链的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作用减弱了AOPs对细胞内ARGs (i-ARGs)降解的协同作用。虽然AOPs对细胞外聚合物(EPS)有显著的降解作用,但EPS的缺失并没有增强对i-ARGs的降解。游离ARGs (f-ARGs)总浓度受膜损伤程度和e-ARG降解效果两个因素的相互作用影响。本研究提供了基于UV-LED的AOPs灭活各种形式arg的有效性和机制的详细见解,以及相关的挑战。了解相关的机制和挑战将有助于开发一种可持续和高效的基于UV-LED的AOP技术,用于从水和废水中去除ARGs。
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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