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Effect of the type and concentration of multivalent cations on the durability of polymeric media for degrading quorum sensing signaling molecules in membrane bioreactors 多价阳离子的类型和浓度对膜生物反应器中降解法定人数感应信号分子的聚合物介质耐久性的影响
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-12 DOI: 10.1016/j.watres.2025.123637
Hosung Lee , Sojin Min , Dowon Chae , Chanyoung Kim , Hyun-Suk Oh , Kibaek Lee , Jaewoo Lee , Kwang-Ho Choo , Chung-Hak Lee , Pyung-Kyu Park
Quorum quenching (QQ) techniques have been applied to membrane bioreactors (MBRs) to inhibit biofouling in the form of polymeric media entrapping QQ bacteria, called QQ media. However, concerns about the durability of QQ media during long-term operation have been raised. To address this, the degree of cross-linking in QQ media was enhanced by either increasing the Ca²⁺ concentration in the 1st cross-linking solution or changing the type of multivalent metal cation in the 2nd cross-linking solution. The QQ beads fabricated under these conditions were compared to those of previously developed conditions in terms of physical durability and biological QQ efficiency. The improved QQ beads demonstrated greater durability, as confirmed by measurements of hardness, swelling ratio, and alginate leakage. In addition, they showed higher QQ efficiency, which was verified through bioassay and analysis of internal microorganisms. The results indicated optimal performance when the 1st cross-linking solution had 16 % w/v CaCl2, or when the 2nd cross-linking solution contained Al3+ as the metal cation, with 0.1 M Al2(SO4)3. Finally, the lifespan of the improved QQ beads was estimated using an experimentally derived formula, suggesting that the lifespan of 16 % w/v CaCl2 and 0.1 M Al2(SO4)3 QQ beads indicated an increase by factors of 2.71 and 3.35, respectively, when compared with the conventional QQ beads.
定量淬灭(QQ)技术已被应用于膜生物反应器(MBR),以夹带 QQ 细菌的聚合物介质(称为 QQ 介质)的形式抑制生物污垢。然而,人们对 QQ 介质在长期运行过程中的耐用性表示担忧。为了解决这个问题,通过增加第一交联溶液中 Ca²⁺ 的浓度或改变第二交联溶液中多价金属阳离子的类型,提高了 QQ 介质的交联度。将在这些条件下制造的 QQ 珠与之前开发的条件下制造的 QQ 珠在物理耐久性和生物 QQ 效率方面进行了比较。通过测量硬度、膨胀率和藻酸盐渗漏,证实改进后的 QQ 珠具有更高的耐用性。此外,它们还显示出更高的 QQ 效率,这一点通过生物测定和内部微生物分析得到了验证。结果表明,当第一种交联溶液含有 16% w/v CaCl2,或第二种交联溶液含有 Al3+ 作为金属阳离子(0.1 M Al2(SO4)3)时,QQ 的性能最佳。最后,利用实验得出的公式估算了改进型 QQ 珠的寿命,结果表明与传统 QQ 珠相比,16% w/v CaCl2 和 0.1 M Al2(SO4)3 QQ 珠的寿命分别增加了 2.71 和 3.35 倍。
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引用次数: 0
Integrating oxidation and reduction processes in electrochemical wastewater treatment for contaminant removal with byproduct control
IF 12.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123632
Kaichao Yang, He Zhen
Electrochemical technologies offer a promising approach for recalcitrant contaminants removal, but toxic halogenated byproducts from the treatment pose a critical challenge. Herein, an integrated electrochemical oxidation (EO) and reduction (ER) process was developed for both contaminant removal and byproduct control. The anodic EO achieved > 90% contaminant removal and generated > 0.6 μM THM4 and > 0.8 μM HAA5 when treating a saline wastewater. A trace amount of Br- led to the production of reactive bromine species and the brominated byproducts. Carbonates made EO more compound-specific by scavenging halogen radicals to CO3- and reduced the THM4 and HAA5 formation by 16% and 31%, respectively. The cathodic ER removed > 80% of THM4 and > 50% of HAA5 through direct reduction and H*-mediated indirect reduction pathways with the final concentrations of ∼ 0.1 μM THM4 and ∼ 0.4 μM HAA5. HAAs could achieve complete dehalogenation via ER and form the non-halogenated products. Throughout the treatment of the integrated process, phenolic contaminant was completely removed by the anodic EO with the kobs > 0.045 min-1, and the formed halogenated byproducts were subsequently removed by the cathodic ER to meet the national and global standards, with a total energy consumption of ∼ 4.5 kWh m-3. The results of this study would encourage the further exploration of enhanced electrochemical wastewater treatment with minimized byproduct residues.
{"title":"Integrating oxidation and reduction processes in electrochemical wastewater treatment for contaminant removal with byproduct control","authors":"Kaichao Yang, He Zhen","doi":"10.1016/j.watres.2025.123632","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123632","url":null,"abstract":"Electrochemical technologies offer a promising approach for recalcitrant contaminants removal, but toxic halogenated byproducts from the treatment pose a critical challenge. Herein, an integrated electrochemical oxidation (EO) and reduction (ER) process was developed for both contaminant removal and byproduct control. The anodic EO achieved &gt; 90% contaminant removal and generated &gt; 0.6 μM THM4 and &gt; 0.8 μM HAA5 when treating a saline wastewater. A trace amount of Br<sup>-</sup> led to the production of reactive bromine species and the brominated byproducts. Carbonates made EO more compound-specific by scavenging halogen radicals to CO<sub>3</sub>•<sup>-</sup> and reduced the THM4 and HAA5 formation by 16% and 31%, respectively. The cathodic ER removed &gt; 80% of THM4 and &gt; 50% of HAA5 through direct reduction and H*-mediated indirect reduction pathways with the final concentrations of ∼ 0.1 μM THM4 and ∼ 0.4 μM HAA5. HAAs could achieve complete dehalogenation via ER and form the non-halogenated products. Throughout the treatment of the integrated process, phenolic contaminant was completely removed by the anodic EO with the <em>k</em><sub>obs</sub> &gt; 0.045 min<sup>-1</sup>, and the formed halogenated byproducts were subsequently removed by the cathodic ER to meet the national and global standards, with a total energy consumption of ∼ 4.5 kWh m<sup>-3</sup>. The results of this study would encourage the further exploration of enhanced electrochemical wastewater treatment with minimized byproduct residues.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"43 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Visible-light-switched radical/non-radical bichannel degradation mechanism via round-the-clock synergistic CDs-BiO1-xCl/PS system
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123623
Wenjie Liu , Yinghe Zhang , Qian Lei , Ziwen Yang , Zhiyang Li , Aziz Ur Rahim Bacha , Wenbiao Jin , Lei Yang
In order to achieve efficient degradation of organic pollutants (OPs) and to avoid interference from co-existing anions and natural organic matter, a synergistic CDs-BiO1-xCl/PS system is designed, which is capable of functioning under both dark and visible-light-controlled conditions, enabling round-the-clock operation. A novel nano photocatalyst CDs-BiO1-xCl was constructed by modifying the surface oxygen vacancy (Ov) rich bismuth oxychloride (BiO1-xCl) with carbon quantum dots (CDs). The key role of the edge carbon atoms (C) of CDs in CDs-BiO1-xCl photocatalyst for PS (persulfate) activation was revealed. Electron paramagnetic resonance spectroscopy, In-situ Raman, quenching experiments and density functional theory (DFT) analysis indicated that the C-edge atoms in the photocatalyst acted as an electron donor which facilitated the complexes formation with PS under dark conditions, and the complexes participated in organic pollutants degradation via electron transfer (non-free radical) pathways subsequently. The system cleverly utilizes the “on-off” of light to achieve the controlled triggering of free radical and non-free radical pathways for PS activation. Upon light irradiation, photogenerated carriers migrate toward CDs, promoting further decomposition of its surface complexes to produce sulfate radicals (·SO4-). Hence, this optimized light-controlled synergistic system showed complete removal of BPA (10 mg/L) in the presence of 2 mM PS within 15 min via free radical and non-free radical pathways. The visible-light-driven system did not produce any toxic byproducts and showed excellent stability under various reaction conditions. Therefore, the round-the-clock and photo-switching-regulated high-efficiency CDs-BiO1-xCl/PS system demonstrates promising application prospects for removing organic pollutants in complex water bodies.
{"title":"Visible-light-switched radical/non-radical bichannel degradation mechanism via round-the-clock synergistic CDs-BiO1-xCl/PS system","authors":"Wenjie Liu ,&nbsp;Yinghe Zhang ,&nbsp;Qian Lei ,&nbsp;Ziwen Yang ,&nbsp;Zhiyang Li ,&nbsp;Aziz Ur Rahim Bacha ,&nbsp;Wenbiao Jin ,&nbsp;Lei Yang","doi":"10.1016/j.watres.2025.123623","DOIUrl":"10.1016/j.watres.2025.123623","url":null,"abstract":"<div><div>In order to achieve efficient degradation of organic pollutants (OPs) and to avoid interference from co-existing anions and natural organic matter, a synergistic CDs-BiO<sub>1-x</sub>Cl/PS system is designed, which is capable of functioning under both dark and visible-light-controlled conditions, enabling round-the-clock operation. A novel nano photocatalyst CDs-BiO<sub>1-x</sub>Cl was constructed by modifying the surface oxygen vacancy (O<sub>v</sub>) rich bismuth oxychloride (BiO<sub>1-x</sub>Cl) with carbon quantum dots (CDs). The key role of the edge carbon atoms (C) of CDs in CDs-BiO<sub>1-x</sub>Cl photocatalyst for PS (persulfate) activation was revealed. Electron paramagnetic resonance spectroscopy, <em>In-situ</em> Raman, quenching experiments and density functional theory (DFT) analysis indicated that the C-edge atoms in the photocatalyst acted as an electron donor which facilitated the complexes formation with PS under dark conditions, and the complexes participated in organic pollutants degradation via electron transfer (non-free radical) pathways subsequently. The system cleverly utilizes the “on-off” of light to achieve the controlled triggering of free radical and non-free radical pathways for PS activation. Upon light irradiation, photogenerated carriers migrate toward CDs, promoting further decomposition of its surface complexes to produce sulfate radicals (·SO<sub>4</sub><sup>-</sup>). Hence, this optimized light-controlled synergistic system showed complete removal of BPA (10 mg/L) in the presence of 2 mM PS within 15 min via free radical and non-free radical pathways. The visible-light-driven system did not produce any toxic byproducts and showed excellent stability under various reaction conditions. Therefore, the round-the-clock and photo-switching-regulated high-efficiency CDs-BiO<sub>1-x</sub>Cl/PS system demonstrates promising application prospects for removing organic pollutants in complex water bodies.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123623"},"PeriodicalIF":11.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Theoretical framework for modeling flocculation in cohesive sediments with variable yield strength
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123593
Keivan Kaveh , Andreas Malcherek
While several models have been developed to describe the temporal evolution of flocs, many assume constant yield strength, which limits their applicability under different flow and sediment conditions. This study aims to improve existing flocculation models by introducing a more accurate parameterization of the floc yield strength, a critical factor in the breakup process. Building on previous work on variable yield strength, a new theoretical formulation for the yield strength of cohesive sediments is derived based on inter-particle bonding within a floc and under more realistic physical assumptions. The proposed model challenges the earlier conceptions, which suggested a direct correlation between floc size and yield strength. This formulation is integrated into a flocculation model based on a constant fractal dimension and validated with experimental data on the temporal evolution of floc size. The study also derives equations for equilibrium floc size and yield strength and demonstrates accurate predictive capabilities. Comparisons with the previous model of Son and Hsu (2009) show significant improvements in capturing the dynamic behavior of floc growth, especially during the transient phase. The results indicate that the proposed model is more consistent with measured floc sizes in several case studies and suggest that the proposed model provides a more robust understanding of floc formation processes.
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引用次数: 0
Removal of PFAS and pharmaceuticals from municipal wastewater using a novel β-cyclodextrin adsorbent over distinct contact times
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123631
Emma F. Shapiro , Zhi-Wei Lin , Edwin Saavedra Cifuentes , Francisco J. Barajas-Rodriguez , Rosa Gwinn , William R. Dichtel , Aaron I. Packman
Conventional adsorbents applied in wastewater treatment are ineffective at removing trace organic contaminants (TrOCs), including per and poly-fluoroalkyl substances (PFAS) and pharmaceuticals. Cross-linked β-cyclodextrin (β-CD) polymer adsorbents have demonstrated efficient removal of TrOCs and exhibit rapid kinetics and high adsorption capacity in wastewater. We evaluate the removal of a mixture of contaminants from wastewater by a styrene functionalized β-CD adsorbent (StyDex) through rapid small-scale column tests (RSSCTs). We found the kinetics observed in batch adsorption tests are maintained in RSSCTs. However, batch sorption kinetic constants did not match column breakthrough kinetics, due to an inability to describe complex flow-through behaviors. We correlated both batch kinetic constants and treatable bed volumes with hydrophobicity of target compounds, where PFOA and PFHxS had the highest affinity for StyDex in batch tests and the latest breakthroughs in RSSCTs. Breakthrough curves of five of the seven TrOCs were not affected by change in contact time. Conversely, decreasing the contact time led to earlier breakthrough of contaminants with the highest sorption affinity to StyDex: longer chained and sulfonated PFAS compounds. These effects were isolated in two-component competitive sorption experiments between PFOA and PFBA, and we observed the same preferential sorption of hydrophobic compounds identified in the multi-component mixture. Additionally, competitive adsorption-desorption increased with increasing contact times. We discuss how these findings are crucial for scale-up and large-scale testing of novel sorbents.
{"title":"Removal of PFAS and pharmaceuticals from municipal wastewater using a novel β-cyclodextrin adsorbent over distinct contact times","authors":"Emma F. Shapiro ,&nbsp;Zhi-Wei Lin ,&nbsp;Edwin Saavedra Cifuentes ,&nbsp;Francisco J. Barajas-Rodriguez ,&nbsp;Rosa Gwinn ,&nbsp;William R. Dichtel ,&nbsp;Aaron I. Packman","doi":"10.1016/j.watres.2025.123631","DOIUrl":"10.1016/j.watres.2025.123631","url":null,"abstract":"<div><div>Conventional adsorbents applied in wastewater treatment are ineffective at removing trace organic contaminants (TrOCs), including per and poly-fluoroalkyl substances (PFAS) and pharmaceuticals. Cross-linked β-cyclodextrin (β-CD) polymer adsorbents have demonstrated efficient removal of TrOCs and exhibit rapid kinetics and high adsorption capacity in wastewater. We evaluate the removal of a mixture of contaminants from wastewater by a styrene functionalized β-CD adsorbent (StyDex) through rapid small-scale column tests (RSSCTs). We found the kinetics observed in batch adsorption tests are maintained in RSSCTs. However, batch sorption kinetic constants did not match column breakthrough kinetics, due to an inability to describe complex flow-through behaviors. We correlated both batch kinetic constants and treatable bed volumes with hydrophobicity of target compounds, where PFOA and PFHxS had the highest affinity for StyDex in batch tests and the latest breakthroughs in RSSCTs. Breakthrough curves of five of the seven TrOCs were not affected by change in contact time. Conversely, decreasing the contact time led to earlier breakthrough of contaminants with the highest sorption affinity to StyDex: longer chained and sulfonated PFAS compounds. These effects were isolated in two-component competitive sorption experiments between PFOA and PFBA, and we observed the same preferential sorption of hydrophobic compounds identified in the multi-component mixture. Additionally, competitive adsorption-desorption increased with increasing contact times. We discuss how these findings are crucial for scale-up and large-scale testing of novel sorbents.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123631"},"PeriodicalIF":11.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rubber-derived chemicals in urban sewer networks and receiving waters: Fingerprints, driving factors and ecological impacts
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123629
Shaopeng Xu , Kai Zhang , Jia-Yong Lao , Qi Wang , Yan Jiang , Chen Li , Jun Kin Kwok , Guodong Cao , Chong Chen , Yue Deng , Kenneth M.Y. Leung
Rubber-derived chemicals (RDCs), which include rubber additives (RAs) and their transformation products (TPs), can be released into aquatic environments when rubber products, such as vehicle tires, are in use or discarded. However, RDCs and associated ecological risks have not been thoroughly investigated inside urban sewer networks and their receiving water bodies. To address these issues, we investigated the RDCs in Hong Kong's municipal sewer networks, including sewage and stormwater, as well as their receiving waters, such as rivers and coastal water. Among 45 target RDCs, the vulcanizing agents and corrosion inhibitors were found to be predominant in the water samples, accounting for 26–66 % and 29–72 % of total concentrations of 45 RDCs (∑45RDC), respectively, while antioxidants and their TPs presented in smaller quantities, accounting for 0.21–26 % and 0–15 % of ∑45RDC, respectively. Ten RAs from five classes were additionally identified by suspect screening. An estimated mass load of ∑45RDC amounting to 1690 kg/month is discharged into the coastal marine environment of Hong Kong, with sewage effluent being the primary source. Population density and vehicle-related factors (e.g., traffic load) were the major drivers shaping the spatial distribution of RDCs in surface water. Based on the ecological risk assessment outcomes, 16 out of 45 RDCs exhibited medium to high risks, and lists of candidate contaminants for various water bodies were proposed to support future risk management in water quality. These findings suggest that RDCs in stormwater and rivers should be carefully monitored, and management strategies should be developed to mitigate their risks.
橡胶衍生化学品(RDCs)包括橡胶添加剂(RAs)及其转化产物(TPs),当橡胶制品(如汽车轮胎)被使用或丢弃时,会释放到水生环境中。然而,目前尚未对城市下水道网络及其受纳水体中的 RDC 及其相关生态风险进行深入研究。为了解决这些问题,我们调查了香港市政污水网络中的 RDC(包括污水和雨水)及其受纳水体(如河流和沿岸水域)。在 45 种目标 RDCs 中,我们发现硫化剂和缓蚀剂在水样中占主导地位,分别占 45 种 RDCs 总浓度(∑45RDC)的 26-66% 和 29-72%,而抗氧化剂及其 TPs 的含量较少,分别占∑45RDC 的 0.21-26% 和 0-15%。通过可疑筛选,还发现了来自五个类别的十种 RA。估计每月排入香港沿岸海洋环境的∑45RDC 总量为 1690 千克,主要来源是污水。人口密度和车辆相关因素(如交通负荷)是影响地表水中 RDC 空间分布的主要驱动因素。根据生态风险评估结果,45 种 RDC 中有 16 种表现出中高风险,并提出了各种水体的候选污染物清单,以支持未来的水质风险管理。这些研究结果表明,应仔细监测雨水和河流中的 RDCs,并制定管理策略以降低其风险。
{"title":"Rubber-derived chemicals in urban sewer networks and receiving waters: Fingerprints, driving factors and ecological impacts","authors":"Shaopeng Xu ,&nbsp;Kai Zhang ,&nbsp;Jia-Yong Lao ,&nbsp;Qi Wang ,&nbsp;Yan Jiang ,&nbsp;Chen Li ,&nbsp;Jun Kin Kwok ,&nbsp;Guodong Cao ,&nbsp;Chong Chen ,&nbsp;Yue Deng ,&nbsp;Kenneth M.Y. Leung","doi":"10.1016/j.watres.2025.123629","DOIUrl":"10.1016/j.watres.2025.123629","url":null,"abstract":"<div><div>Rubber-derived chemicals (RDCs), which include rubber additives (RAs) and their transformation products (TPs), can be released into aquatic environments when rubber products, such as vehicle tires, are in use or discarded. However, RDCs and associated ecological risks have not been thoroughly investigated inside urban sewer networks and their receiving water bodies. To address these issues, we investigated the RDCs in Hong Kong's municipal sewer networks, including sewage and stormwater, as well as their receiving waters, such as rivers and coastal water. Among 45 target RDCs, the vulcanizing agents and corrosion inhibitors were found to be predominant in the water samples, accounting for 26–66 % and 29–72 % of total concentrations of 45 RDCs (∑<sub>45</sub>RDC), respectively, while antioxidants and their TPs presented in smaller quantities, accounting for 0.21–26 % and 0–15 % of ∑<sub>45</sub>RDC, respectively. Ten RAs from five classes were additionally identified by suspect screening. An estimated mass load of ∑<sub>45</sub>RDC amounting to 1690 kg/month is discharged into the coastal marine environment of Hong Kong, with sewage effluent being the primary source. Population density and vehicle-related factors (e.g., traffic load) were the major drivers shaping the spatial distribution of RDCs in surface water. Based on the ecological risk assessment outcomes, 16 out of 45 RDCs exhibited medium to high risks, and lists of candidate contaminants for various water bodies were proposed to support future risk management in water quality. These findings suggest that RDCs in stormwater and rivers should be carefully monitored, and management strategies should be developed to mitigate their risks.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123629"},"PeriodicalIF":11.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Binding interaction between chlorine and powder activated carbon driving nonradical oxidation toward diclofenac abatement: surface-bound complexes generating on diverse sites performing diverse duties
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-11 DOI: 10.1016/j.watres.2025.123620
Liang Chen , Xin Cheng , Guijing Chen , Ying Wang , Xin Chen , Chunyan Yang , Wen Liu , Gretchen Kalonji , Jun Ma , Baicang Liu
Photolysis of chlorine by UV irradiation is commonly used as an advanced oxidation process for the abatement of micropollutants, but suffers from the energy-extensive consumption and potential risk, e.g., formation of disinfection byproduct and use of fragile mercury-containing lamps. This study demonstrates powder activated carbon (PAC) catalysis-mediated chlorine activation to significantly promote the degradation of diclofenac (DCF), a representative emerging contaminant, via nonradical oxidation pathways, thus reconsidering the interaction between PAC and chlorine in depth which are widely applied in actual water treatment. The chlorine/PAC process produces reactive metastable surface-bound complexes, i.e., PAC-HOCl*, via the cleavage of O–Cl bond in chlorine and formation of C–Cl by interfacial binding interaction, to regulate the charge distribution and electron density configuration. Carbonyl groups and structural defects of PAC are determined as the active sites via functional group derivatization and defect engineering for PAC modification, and performed diverse duties in the chlorine activation, producing PAC-C=O-HOCl* and PAC-D-HOCl*, responsible for the oxidation ability improvement and electron transfer acceleration, respectively. Of particular significance is that the chlorine/PAC process performs high efficiencies in the degradation of diverse micropollutants and is scarcely affected by water matrices, exhibiting a high potential of practical application for the decontamination of emerging micropollutants without the requirement of external energy input.
{"title":"Binding interaction between chlorine and powder activated carbon driving nonradical oxidation toward diclofenac abatement: surface-bound complexes generating on diverse sites performing diverse duties","authors":"Liang Chen ,&nbsp;Xin Cheng ,&nbsp;Guijing Chen ,&nbsp;Ying Wang ,&nbsp;Xin Chen ,&nbsp;Chunyan Yang ,&nbsp;Wen Liu ,&nbsp;Gretchen Kalonji ,&nbsp;Jun Ma ,&nbsp;Baicang Liu","doi":"10.1016/j.watres.2025.123620","DOIUrl":"10.1016/j.watres.2025.123620","url":null,"abstract":"<div><div>Photolysis of chlorine by UV irradiation is commonly used as an advanced oxidation process for the abatement of micropollutants, but suffers from the energy-extensive consumption and potential risk, e.g., formation of disinfection byproduct and use of fragile mercury-containing lamps. This study demonstrates powder activated carbon (PAC) catalysis-mediated chlorine activation to significantly promote the degradation of diclofenac (DCF), a representative emerging contaminant, via nonradical oxidation pathways, thus reconsidering the interaction between PAC and chlorine in depth which are widely applied in actual water treatment. The chlorine/PAC process produces reactive metastable surface-bound complexes, i.e., PAC-HOCl*, via the cleavage of O–Cl bond in chlorine and formation of C–Cl by interfacial binding interaction, to regulate the charge distribution and electron density configuration. Carbonyl groups and structural defects of PAC are determined as the active sites via functional group derivatization and defect engineering for PAC modification, and performed diverse duties in the chlorine activation, producing PAC-C=O-HOCl* and PAC-D-HOCl*, responsible for the oxidation ability improvement and electron transfer acceleration, respectively. Of particular significance is that the chlorine/PAC process performs high efficiencies in the degradation of diverse micropollutants and is scarcely affected by water matrices, exhibiting a high potential of practical application for the decontamination of emerging micropollutants without the requirement of external energy input.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123620"},"PeriodicalIF":11.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Neglected role of virus-host interactions driving antibiotic resistance genes reduction in an urban river receiving treated wastewater
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-10 DOI: 10.1016/j.watres.2025.123627
Xiaojie Yan , Yuan Xin , Liying Zhu , Qihe Tang , Min Chen , Yuansong Wei , Junya Zhang , Hans Hermann Richnow
Treated wastewater from wastewater treatment plants (WWTPs) is a major contributor to the transfer of antibiotic resistance genes (ARGs) into urban rivers. However, the role of viral communities in this process remains poorly understood. This study focused on North Canal in Beijing, China, which receives over 80 % of its water from treated wastewater, to investigate the impact of viral communities on ARGs transfer. Results showed significant seasonal variation in the abundance and composition of ARGs, with 30 high-risk ARGs detected, accounting for 1.50 % ± 1.28 % of total ARGs. The assembly of ARGs in North Canal followed a stochastic process of homogenizing dispersal, with conjugative mobility playing a key role in horizontal gene transfer with Pseudomonas as primary host for HGT. The potential conjugative mobility of ARGs is significantly higher in wet season (69.4 % ± 17.3 %) compared to dry season (42.9 % ± 17.1 %), with conjugation frequencies ranging from 1.18 × 10–6 to 2.26 × 10–4. Viral species accumulation curves approaching saturation indicated the well captured viral diversity, and no phages carrying ARGs were found among 27,523 non-redundant viral operational taxonomic units. Most of the phages (89.2 % ± 3.8 %) were lytic in North Canal, which were observed to contribute to ARGs reduction by lysing their host bacteria, reflected by higher virus-host ratio and demonstrated by the phage lysis assays in treated wastewater and receiving river. We provided compelling evidence that phage-host interactions can reduce ARGs through host lysis, highlighting their potential role in mitigating ARG transmission in urban rivers receiving treated wastewater.
{"title":"Neglected role of virus-host interactions driving antibiotic resistance genes reduction in an urban river receiving treated wastewater","authors":"Xiaojie Yan ,&nbsp;Yuan Xin ,&nbsp;Liying Zhu ,&nbsp;Qihe Tang ,&nbsp;Min Chen ,&nbsp;Yuansong Wei ,&nbsp;Junya Zhang ,&nbsp;Hans Hermann Richnow","doi":"10.1016/j.watres.2025.123627","DOIUrl":"10.1016/j.watres.2025.123627","url":null,"abstract":"<div><div>Treated wastewater from wastewater treatment plants (WWTPs) is a major contributor to the transfer of antibiotic resistance genes (ARGs) into urban rivers. However, the role of viral communities in this process remains poorly understood. This study focused on North Canal in Beijing, China, which receives over 80 % of its water from treated wastewater, to investigate the impact of viral communities on ARGs transfer. Results showed significant seasonal variation in the abundance and composition of ARGs, with 30 high-risk ARGs detected, accounting for 1.50 % ± 1.28 % of total ARGs. The assembly of ARGs in North Canal followed a stochastic process of homogenizing dispersal, with conjugative mobility playing a key role in horizontal gene transfer with <em>Pseudomonas</em> as primary host for HGT. The potential conjugative mobility of ARGs is significantly higher in wet season (69.4 % ± 17.3 %) compared to dry season (42.9 % ± 17.1 %), with conjugation frequencies ranging from 1.18 × 10<sup>–6</sup> to 2.26 × 10<sup>–4</sup>. Viral species accumulation curves approaching saturation indicated the well captured viral diversity, and no phages carrying ARGs were found among 27,523 non-redundant viral operational taxonomic units. Most of the phages (89.2 % ± 3.8 %) were lytic in North Canal, which were observed to contribute to ARGs reduction by lysing their host bacteria, reflected by higher virus-host ratio and demonstrated by the phage lysis assays in treated wastewater and receiving river. We provided compelling evidence that phage-host interactions can reduce ARGs through host lysis, highlighting their potential role in mitigating ARG transmission in urban rivers receiving treated wastewater.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123627"},"PeriodicalIF":11.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fate variations of Per- and polyfluoroalkyl substances in diverse aquatic environments: An overlooked influence of hydrodynamics
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-10 DOI: 10.1016/j.watres.2025.123628
Liang Yu , Xiaodong Liu , Zulin Hua , Xiaolei Xing , Hongqin Xue
Per- and polyfluoroalkyl substances (PFASs) have become a significant global issue; nevertheless, information regarding the hydrodynamic effect on their catchment-scale fate remains lacking. Thus, this study investigated PFASs in water and paired sediment samples from diverse aquatic habitats within the Qinhuai River Basin (QRB), where high concentrations of PFASs are ubiquitous. Rarity score analysis reveals that PFASs were diffusely distributed across the QRB, yet specific sites were identified as emission hotspots. The sediment-water and suspended particulate matter-water partitioning coefficients of PFASs both exhibited significant correlations with chemical structures, ambient variables, land use, and flow velocity (p < 0.05). Flow velocity can promote the liberation of PFASs from particles into water, reducing their accumulation capacity; hence, the higher partitioning coefficients of PFASs were observed in relatively low-velocity aquatic systems, such as lakes, reservoirs, and ponds. A partial least-squares structural equation model was employed to further elucidate their effect pathways and magnitudes on partitioning coefficients. In addition, the primary sources of PFASs were identified, emphasizing their complexity. The ecological risks of PFASs were assessed, indicating priority PFAS species (long-chain PFCAs and HFPO-TA) for management and suggesting water as the preferable environmental medium for regulation. This is the first field investigation to quantify the significance of hydrodynamic influences on the catchment-scale fate of PFASs, improving our understanding of their distribution and behaviors from the perspective of environmental hydraulics.
{"title":"Fate variations of Per- and polyfluoroalkyl substances in diverse aquatic environments: An overlooked influence of hydrodynamics","authors":"Liang Yu ,&nbsp;Xiaodong Liu ,&nbsp;Zulin Hua ,&nbsp;Xiaolei Xing ,&nbsp;Hongqin Xue","doi":"10.1016/j.watres.2025.123628","DOIUrl":"10.1016/j.watres.2025.123628","url":null,"abstract":"<div><div>Per- and polyfluoroalkyl substances (PFASs) have become a significant global issue; nevertheless, information regarding the hydrodynamic effect on their catchment-scale fate remains lacking. Thus, this study investigated PFASs in water and paired sediment samples from diverse aquatic habitats within the Qinhuai River Basin (QRB), where high concentrations of PFASs are ubiquitous. Rarity score analysis reveals that PFASs were diffusely distributed across the QRB, yet specific sites were identified as emission hotspots. The sediment-water and suspended particulate matter-water partitioning coefficients of PFASs both exhibited significant correlations with chemical structures, ambient variables, land use, and flow velocity (<em>p</em> &lt; 0.05). Flow velocity can promote the liberation of PFASs from particles into water, reducing their accumulation capacity; hence, the higher partitioning coefficients of PFASs were observed in relatively low-velocity aquatic systems, such as lakes, reservoirs, and ponds. A partial least-squares structural equation model was employed to further elucidate their effect pathways and magnitudes on partitioning coefficients. In addition, the primary sources of PFASs were identified, emphasizing their complexity. The ecological risks of PFASs were assessed, indicating priority PFAS species (long-chain PFCAs and HFPO-TA) for management and suggesting water as the preferable environmental medium for regulation. This is the first field investigation to quantify the significance of hydrodynamic influences on the catchment-scale fate of PFASs, improving our understanding of their distribution and behaviors from the perspective of environmental hydraulics.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"282 ","pages":"Article 123628"},"PeriodicalIF":11.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hydroxyl radicals produced from oxidation of ferrous sulfides promote mobilization of mercuric sulfide in soil–water system 硫化亚铁氧化产生的羟基自由基促进了土壤-水系统中硫化汞的迁移
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-04-10 DOI: 10.1016/j.watres.2025.123625
Dongrui Li , Hong Li , Xujun Liang , Qingliang Chen , Xu Bai , Lizhong Zhu , Yuxi Gao , Jiating Zhao
Mercuric sulfide nanoparticles (HgS-NPs) are recognized as a significant source of bioavailable mercury in paddy fields. The factors influencing the mobilization and bioavailability of HgS-NPs formed in flooded or drained paddy field-like systems are complicated and remain unexplored to date. Here, we show that ferrous sulfide (FeS) as an important mineral substance plays a crucial role in the dissolution and transformation of HgS-NPs in overlying water or during the drainage stage, as well as their bioavailability toward rice. Specifically, we found that oxidation of FeS significantly enhances the dissolution of HgS-NPs, with the degree of activation intensified with increasing FeS concentrations. This activation was further evidenced to be driven by the generation of hydroxyl radicals (•OH) during FeS oxidation, leading to the release of Hg(Ⅱ). The enhanced dissolution of HgS-NPs increases its bioavailability, as verified by the augmented accumulation of Hg in rice upon FeS oxidation. This study underscores the overlooked yet important role of FeS in affecting the fate of HgS-NPs and offers valuable insights for pollution control of Hg-contaminated paddy fields and wetlands.
{"title":"Hydroxyl radicals produced from oxidation of ferrous sulfides promote mobilization of mercuric sulfide in soil–water system","authors":"Dongrui Li ,&nbsp;Hong Li ,&nbsp;Xujun Liang ,&nbsp;Qingliang Chen ,&nbsp;Xu Bai ,&nbsp;Lizhong Zhu ,&nbsp;Yuxi Gao ,&nbsp;Jiating Zhao","doi":"10.1016/j.watres.2025.123625","DOIUrl":"10.1016/j.watres.2025.123625","url":null,"abstract":"<div><div>Mercuric sulfide nanoparticles (HgS-NPs) are recognized as a significant source of bioavailable mercury in paddy fields. The factors influencing the mobilization and bioavailability of HgS-NPs formed in flooded or drained paddy field-like systems are complicated and remain unexplored to date. Here, we show that ferrous sulfide (FeS) as an important mineral substance plays a crucial role in the dissolution and transformation of HgS-NPs in overlying water or during the drainage stage, as well as their bioavailability toward rice. Specifically, we found that oxidation of FeS significantly enhances the dissolution of HgS-NPs, with the degree of activation intensified with increasing FeS concentrations. This activation was further evidenced to be driven by the generation of hydroxyl radicals (•OH) during FeS oxidation, leading to the release of Hg(Ⅱ). The enhanced dissolution of HgS-NPs increases its bioavailability, as verified by the augmented accumulation of Hg in rice upon FeS oxidation. This study underscores the overlooked yet important role of FeS in affecting the fate of HgS-NPs and offers valuable insights for pollution control of Hg-contaminated paddy fields and wetlands.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"281 ","pages":"Article 123625"},"PeriodicalIF":11.4,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819569","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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