Pub Date : 2025-01-30DOI: 10.1016/j.watres.2025.123220
Chuanjin Lin , Bin Dong , Zuxin Xu
Iron and organic carbon (OC) biogeochemical cycling is highly correlated, and dissolved organic matter (DOM), a highly reactive component of soil and water environments, is the main OC source. However, the micro-mechanism of the molecular fractionation of DOM, the spatial OC distribution on iron (oxyhydr)oxides, and how these factors further affect their redox properties remain to be fully understood. Therefore, this study investigated the DOM adsorption properties of iron (oxyhydr)oxides with different crystallinities at the molecular level through the Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and transmission electron microscopy/electron energy loss spectroscopy (TEM–EELS) analyses of the liquid-solid phases. Owing to the limited number of adsorption sites, OC sequestration on goethite and hematite surfaces generally followed an “onion” model, in the order of preference of aromatic, aliphatic, and carboxylic acid-rich compounds. Combined with dielectric electrochemical tests and charge differential density calculations, the results revealed that the complexation effect produced by iron ions increased the electron-accepting capacity (EAC) of the DOM remaining in the aqueous solution. In contrast, molecular selective adsorption and oxidative polymerization significantly enhanced the EAC of DOM adsorbed on the surface fraction of iron (oxyhydr)oxides. These findings help elucidate the mechanism of OC sequestration by iron (oxyhydr)oxides. The increased EAC may affect various biogeochemical processes, such as methane production and microbial Fe(III) reduction, facilitating the prediction of OC cycling in natural environments.
{"title":"Microscopic mechanism of organic carbon sequestration and redox properties influenced by iron (Oxyhydr)oxides","authors":"Chuanjin Lin , Bin Dong , Zuxin Xu","doi":"10.1016/j.watres.2025.123220","DOIUrl":"10.1016/j.watres.2025.123220","url":null,"abstract":"<div><div>Iron and organic carbon (OC) biogeochemical cycling is highly correlated, and dissolved organic matter (DOM), a highly reactive component of soil and water environments, is the main OC source. However, the micro-mechanism of the molecular fractionation of DOM, the spatial OC distribution on iron (oxyhydr)oxides, and how these factors further affect their redox properties remain to be fully understood. Therefore, this study investigated the DOM adsorption properties of iron (oxyhydr)oxides with different crystallinities at the molecular level through the Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and transmission electron microscopy/electron energy loss spectroscopy (TEM–EELS) analyses of the liquid-solid phases. Owing to the limited number of adsorption sites, OC sequestration on goethite and hematite surfaces generally followed an “onion” model, in the order of preference of aromatic, aliphatic, and carboxylic acid-rich compounds. Combined with dielectric electrochemical tests and charge differential density calculations, the results revealed that the complexation effect produced by iron ions increased the electron-accepting capacity (EAC) of the DOM remaining in the aqueous solution. In contrast, molecular selective adsorption and oxidative polymerization significantly enhanced the EAC of DOM adsorbed on the surface fraction of iron (oxyhydr)oxides. These findings help elucidate the mechanism of OC sequestration by iron (oxyhydr)oxides. The increased EAC may affect various biogeochemical processes, such as methane production and microbial Fe(III) reduction, facilitating the prediction of OC cycling in natural environments.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123220"},"PeriodicalIF":11.4,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072195","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}
Pub Date : 2025-01-30DOI: 10.1016/j.watres.2025.123221
Ivan V. Krickov , Sergey N. Vorobyev , Larisa G. Kolesnichenko , Yuri Kolesnichenko , Dmitri Zinchenko , Liudmila S. Shirokova , Oleg S. Pokrovsky
<div><div>Riverine export fluxes of organic carbon (OC), major and trace elements remain at the forefront of environmental research in Arctic and subarctic regions, due mostly to high sensitivity of river hydrochemical parameters to climate warming and, at the same time, global importance of OC, nutrients and toxicants delivered by rivers to the Arctic Ocean. In contrast to reliable information on export fluxes of carbon and metals from the mainland to the Arctic Ocean by large and mid-size Arctic rivers, the majority of these studies quantify either dissolved (< 0.45 µm) or particulate suspended matter (PSM) fluxes, without mechanistic analyses of element speciation in most labile, low molecular weight (LMW) or colloidal form. Here we assessed colloidal versus LMW (< 3 kDa) and suspended (> 0.45 µm) export of OC, major and trace elements in a large Siberian river (Ob) and its smaller tributaries, situated within a boreal taiga / wetland zone. The main differences between Ob and its small tributaries are (i) higher dissolved OC and dissolved and particulate Fe concentrations in tributaries, due to input from surrounding bogs, (ii) much higher PSM load (clays) in the large river (Ob) compared to smaller tributaries; and (iii) strong underground water input for the Ob River, especially during baseflow, which is less pronounced for its tributaries. These major environmental factors were largely responsible for specific features of colloidal vs particulate export for the Ob River and its tributaries.</div><div>Annual export fluxes normalized to the watershed area (yields) were similar for most elements in dissolved (< 0.45 µm) fraction between the Ob and the tributaries, exempting Fe, Mn, Co and Zn which were higher in tributaries essentially due to input from wetlands. Export of Mo, V, W and U was higher in the Ob River due to pronounced groundwater influence. Colloidal (3 kDa – 0.45 µm) yields were also generally higher in the tributary compared to Ob, except for those soluble elements of groundwater input (Sr, Mo, W, U). The particulate suspended (> 0.45 µm) yield of all elements, except Mn, was much higher in the Ob River when compared to its smaller tributaries. Overall, elemental fluxes of small wetland-draining tributaries of the Ob River can be considered analogous to the small rivers of the permafrost-free portion of the Arctic coast. Such small rivers are more sensitive to processes occurring at the watershed level, hence being an efficient potential sentinel for environmental changes. Fluxes in large Arctic coast rivers are more conservative and are strongly controlled by the effects of PSM interaction with river water at high flow and groundwater loading at base flow. Global significance of our findings is that elemental dissolved (< 0.45 µm) yields of small Artic rivers draining coastal wetlands and boreal forests can be adequately (within a factor of 2 to 3, comparable to inter-annul variations and uncertainties) appro
{"title":"Export fluxes of dissolved, colloidal and particulate organic carbon, major and trace elements from the Ob River and its tributaries across seasons","authors":"Ivan V. Krickov , Sergey N. Vorobyev , Larisa G. Kolesnichenko , Yuri Kolesnichenko , Dmitri Zinchenko , Liudmila S. Shirokova , Oleg S. Pokrovsky","doi":"10.1016/j.watres.2025.123221","DOIUrl":"10.1016/j.watres.2025.123221","url":null,"abstract":"<div><div>Riverine export fluxes of organic carbon (OC), major and trace elements remain at the forefront of environmental research in Arctic and subarctic regions, due mostly to high sensitivity of river hydrochemical parameters to climate warming and, at the same time, global importance of OC, nutrients and toxicants delivered by rivers to the Arctic Ocean. In contrast to reliable information on export fluxes of carbon and metals from the mainland to the Arctic Ocean by large and mid-size Arctic rivers, the majority of these studies quantify either dissolved (< 0.45 µm) or particulate suspended matter (PSM) fluxes, without mechanistic analyses of element speciation in most labile, low molecular weight (LMW) or colloidal form. Here we assessed colloidal versus LMW (< 3 kDa) and suspended (> 0.45 µm) export of OC, major and trace elements in a large Siberian river (Ob) and its smaller tributaries, situated within a boreal taiga / wetland zone. The main differences between Ob and its small tributaries are (i) higher dissolved OC and dissolved and particulate Fe concentrations in tributaries, due to input from surrounding bogs, (ii) much higher PSM load (clays) in the large river (Ob) compared to smaller tributaries; and (iii) strong underground water input for the Ob River, especially during baseflow, which is less pronounced for its tributaries. These major environmental factors were largely responsible for specific features of colloidal vs particulate export for the Ob River and its tributaries.</div><div>Annual export fluxes normalized to the watershed area (yields) were similar for most elements in dissolved (< 0.45 µm) fraction between the Ob and the tributaries, exempting Fe, Mn, Co and Zn which were higher in tributaries essentially due to input from wetlands. Export of Mo, V, W and U was higher in the Ob River due to pronounced groundwater influence. Colloidal (3 kDa – 0.45 µm) yields were also generally higher in the tributary compared to Ob, except for those soluble elements of groundwater input (Sr, Mo, W, U). The particulate suspended (> 0.45 µm) yield of all elements, except Mn, was much higher in the Ob River when compared to its smaller tributaries. Overall, elemental fluxes of small wetland-draining tributaries of the Ob River can be considered analogous to the small rivers of the permafrost-free portion of the Arctic coast. Such small rivers are more sensitive to processes occurring at the watershed level, hence being an efficient potential sentinel for environmental changes. Fluxes in large Arctic coast rivers are more conservative and are strongly controlled by the effects of PSM interaction with river water at high flow and groundwater loading at base flow. Global significance of our findings is that elemental dissolved (< 0.45 µm) yields of small Artic rivers draining coastal wetlands and boreal forests can be adequately (within a factor of 2 to 3, comparable to inter-annul variations and uncertainties) appro","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123221"},"PeriodicalIF":11.4,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-30DOI: 10.1016/j.watres.2025.123230
Amanda Darling , Benjamin Davis , Thomas Byrne , Madeline Deck , Gabriel Maldonado Rivera , Sarah Price , Amber Amaral-Torres , Clayton Markham , Raul Gonzalez , Peter Vikesland , Leigh-Anne Krometis , Amy Pruden , Alasdair Cohen
As wastewater-based surveillance (WBS) is increasingly used to track community-level disease trends, it is important to understand how pathogen signals can be altered by phenomena that occur within sewersheds such as inflow and infiltration (I&I). Our objectives were to characterize I&I across a rural sewershed and assess potential impacts on viral (rotavirus, norovirus GII, and SARS-CoV-2), fecal indicator (HF183, the hCYTB484 gene specific to the human mitochondrial genome, and crAssphage), and antimicrobial resistance (intI1, blaCTX−M-1) targets. In a small town in Virginia (USA), we collected 107 wastewater samples at monthly intervals over a 12-month period (2022–2023) at the wastewater treatment plant (WWTP) influent and 11 up-sewer sites. Viral, fecal indicator, and antimicrobial resistance targets were enumerated using ddPCR. Physicochemical proxies for organics and nutrient levels in sewage (chemical oxygen demand (COD), total suspended solids (TSS), and NH3(aq)) and genetic markers of anthropogenic impact were used to characterize I&I across the sewershed. Overall, precipitation was negatively associated (Spearman test; ρ < 0; p < 0.01) with physicochemical markers (TSS, COD, K, PO43−-P, NH3(aq)) in the WWTP influent. We observed the highest concentrations of human fecal markers and a measure anthropogenic pollution and antibiotic resistance (intI1) in up-sewer sites with limited I&I. However, median viral gene copy concentrations were highest at the WWTP, compared to 100 % (n = 11), 90 % (n = 10), and 55 % (n = 6) of up-sewer sites for rotavirus, norovirus GII, and SARS-CoV-2, respectively. After adjusting for covariates (Ba, COD, dissolved oxygen, groundwater depth, precipitation, sampling date) using generalized linear models, moderate to high I&I was associated with statistically significant reductions in log10-transformed rotavirus and norovirus GII concentrations across the sewershed (coefficients = -0.7 and -0.9, p < 0.001, n = 95), though not for SARS-CoV-2 (coefficient = -0.2, p = 0.181, n = 95). Overall, we found that while I&I can diminish biomarker signals throughout a sewershed, including at the WWTP influent, I&I impacts vary depending on the target, and pathogen biomarker signals were, on average, higher and less variable over time at the WWTP compared to most up-sewer sites. As far as we are aware, this is the first study to assess in situ I&I impacts on multiple WBS targets. Taken together, our findings highlight challenges and tradeoffs associated with different sampling strategies for different WBS targets in heavily I&I impacted systems.
{"title":"Subsewershed analyses of the impacts of inflow and infiltration on viral pathogens and antibiotic resistance markers across a rural sewer system","authors":"Amanda Darling , Benjamin Davis , Thomas Byrne , Madeline Deck , Gabriel Maldonado Rivera , Sarah Price , Amber Amaral-Torres , Clayton Markham , Raul Gonzalez , Peter Vikesland , Leigh-Anne Krometis , Amy Pruden , Alasdair Cohen","doi":"10.1016/j.watres.2025.123230","DOIUrl":"10.1016/j.watres.2025.123230","url":null,"abstract":"<div><div>As wastewater-based surveillance (WBS) is increasingly used to track community-level disease trends, it is important to understand how pathogen signals can be altered by phenomena that occur within sewersheds such as inflow and infiltration (I&I). Our objectives were to characterize I&I across a rural sewershed and assess potential impacts on viral (rotavirus, norovirus GII, and SARS-CoV-2), fecal indicator (HF183, the hCYTB484 gene specific to the human mitochondrial genome, and crAssphage), and antimicrobial resistance (<em>int</em>I1, <em>bla</em><sub>CTX</sub><sub>−</sub><sub>M-1</sub>) targets. In a small town in Virginia (USA), we collected 107 wastewater samples at monthly intervals over a 12-month period (2022–2023) at the wastewater treatment plant (WWTP) influent and 11 up-sewer sites. Viral, fecal indicator, and antimicrobial resistance targets were enumerated using ddPCR. Physicochemical proxies for organics and nutrient levels in sewage (chemical oxygen demand (COD), total suspended solids (TSS), and NH<sub>3</sub>(aq)) and genetic markers of anthropogenic impact were used to characterize I&I across the sewershed. Overall, precipitation was negatively associated (Spearman test; ρ < 0; <em>p</em> < 0.01) with physicochemical markers (TSS, COD, K, PO<sub>4</sub><sup>3−</sup>-P, NH<sub>3</sub>(aq)) in the WWTP influent. We observed the highest concentrations of human fecal markers and a measure anthropogenic pollution and antibiotic resistance (<em>int</em>I1) in up-sewer sites with limited I&I. However, median viral gene copy concentrations were highest at the WWTP, compared to 100 % (<em>n</em> = 11), 90 % (<em>n</em> = 10), and 55 % (<em>n</em> = 6) of up-sewer sites for rotavirus, norovirus GII, and SARS-CoV-2, respectively. After adjusting for covariates (Ba, COD, dissolved oxygen, groundwater depth, precipitation, sampling date) using generalized linear models, moderate to high I&I was associated with statistically significant reductions in log<sub>10</sub>-transformed rotavirus and norovirus GII concentrations across the sewershed (coefficients = -0.7 and -0.9, <em>p</em> < 0.001, <em>n</em> = 95), though not for SARS-CoV-2 (coefficient = -0.2, <em>p</em> = 0.181, <em>n</em> = 95). Overall, we found that while I&I can diminish biomarker signals throughout a sewershed, including at the WWTP influent, I&I impacts vary depending on the target, and pathogen biomarker signals were, on average, higher and less variable over time at the WWTP compared to most up-sewer sites. As far as we are aware, this is the first study to assess <em>in situ</em> I&I impacts on multiple WBS targets. Taken together, our findings highlight challenges and tradeoffs associated with different sampling strategies for different WBS targets in heavily I&I impacted systems.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"276 ","pages":"Article 123230"},"PeriodicalIF":11.4,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072196","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}
Pub Date : 2025-01-29DOI: 10.1016/j.watres.2025.123219
Wei Liu , Tao Lin , Xiaoshu Yan
The widespread use of ceramic membranes in wastewater recycling is still hampered by membrane fouling problems. Frequent chemical cleaning increases operating and maintenance costs. This work proposes ozone micro-nano-bubble (O3-MNB) backwash as a new backwashing method to control the ceramic membrane fouling. Activated carbon filter backwash water (ACFBW) was used as feed water for the ceramic membrane and the effect of O3-MNB backwash was compared with tap water backwash, air-micro-nano-bubble (Air-MNB) backwash and ozone water backwash. The results of the flux tests showed that the irreversible fouling resistance (RFi) for the O3-MNB backwash was only 4.8 %, 10.0 % and 23.3 % of the RFi for the tap water backwash, Air-MNB backwash and O3 water backwash, respectively. The results of the SEM and CLSM analyses demonstrated that the combination of ozone with MNB for backwashing was an effective method for the removal of viable cells and majority of proteins and polysaccharides from the surface of the ceramic membrane. However, the application of ozone also led to the release of microbial DNA, which increased its binding to Al₂O₃ on the ceramic membrane. Furthermore, the increased ozone concentration transported by the MNB could promote the generation of a large number of hydroxyl radicals (•OH) due to the effect of Al₂O₃, which potentially enhanced the oxidation of macromolecular contaminants in the pores. At the same time, the electrostatic repulsion and hydrophobic action provided by the MNB improved the efficacy of peeling off the filter cake layer when cleaning the membrane pores. Consequently, this study demonstrated the effectiveness of O3-MNB backwash in the long-term operation of ceramic membranes and provided insights into the fundamental mechanism by which this process controlled the membrane fouling.
{"title":"Ceramic membrane fouling caused by recycling biological activated carbon filter backwash water: Effective backwash with ozone micro-nano bubbles","authors":"Wei Liu , Tao Lin , Xiaoshu Yan","doi":"10.1016/j.watres.2025.123219","DOIUrl":"10.1016/j.watres.2025.123219","url":null,"abstract":"<div><div>The widespread use of ceramic membranes in wastewater recycling is still hampered by membrane fouling problems. Frequent chemical cleaning increases operating and maintenance costs. This work proposes ozone micro-nano-bubble (O<sub>3</sub>-MNB) backwash as a new backwashing method to control the ceramic membrane fouling. Activated carbon filter backwash water (ACFBW) was used as feed water for the ceramic membrane and the effect of O<sub>3</sub>-MNB backwash was compared with tap water backwash, air-micro-nano-bubble (Air-MNB) backwash and ozone water backwash. The results of the flux tests showed that the irreversible fouling resistance (R<sub>Fi</sub>) for the O<sub>3</sub>-MNB backwash was only 4.8 %, 10.0 % and 23.3 % of the R<sub>Fi</sub> for the tap water backwash, Air-MNB backwash and O<sub>3</sub> water backwash, respectively. The results of the SEM and CLSM analyses demonstrated that the combination of ozone with MNB for backwashing was an effective method for the removal of viable cells and majority of proteins and polysaccharides from the surface of the ceramic membrane. However, the application of ozone also led to the release of microbial DNA, which increased its binding to Al₂O₃ on the ceramic membrane. Furthermore, the increased ozone concentration transported by the MNB could promote the generation of a large number of hydroxyl radicals (•OH) due to the effect of Al₂O₃, which potentially enhanced the oxidation of macromolecular contaminants in the pores. At the same time, the electrostatic repulsion and hydrophobic action provided by the MNB improved the efficacy of peeling off the filter cake layer when cleaning the membrane pores. Consequently, this study demonstrated the effectiveness of O<sub>3</sub>-MNB backwash in the long-term operation of ceramic membranes and provided insights into the fundamental mechanism by which this process controlled the membrane fouling.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123219"},"PeriodicalIF":11.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055424","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}
Pub Date : 2025-01-29DOI: 10.1016/j.watres.2025.123217
Chaoyang Li , Alberto Tiraferri , Peng Tang , Jun Ma , Baicang Liu
Unconventional oil and gas (UOG) extraction techniques typically involve the production of large volumes of so-called flowback and produced water (FPW), a site-specific wastewater stream characterized by complex organic and inorganic composition. Sustainable and cost-effective management of FPW, as well as mitigation of its environmental risks and impacts, represents substantial challenges for governments, industries, and societies worldwide. Among various treatment technologies, biological processes have gained interest due to their low installation and operational costs. However, the interaction of FPW's complex composition with microorganisms poses challenging scientific and engineering questions. This review examines the water quality characteristics and sources of FPW from twelve UOG extraction sites in China and North America, revealing strong spatio-temporal heterogeneity of organic, inorganic, and microbial components across different reservoirs. The complex and variable water quality, large wastewater volumes, and high treatment demands have driven the exploration of biological treatments for FPW. This work systematically reviews and analyzes the operating conditions, treatment efficiency, and technical applicability of suspended sludge reactors, attached sludge reactors, mixed systems, and resource/energy recovery systems. Developing skid-mounted equipment based on suspended sludge reactors to handle variations in wastewater quantity and innovating the form of attached sludge reactors, especially in enriching salt-tolerant microbes for in-situ FPW treatment, are deemed essential. The dominant microorganisms playing a key role in the biological treatment are also discussed, with focus on two different inoculation sources (activated sludge and FPW). Roseovarius from FPW and Pseudomonas from activated sludge have strong adaptability to different reactors. The review further underscores the need to integrate biological treatments with complementary technologies. Finally, it advocates for the establishment of robust and scalable biological treatments through research in three main directions: (i) exploring microbial resources in original FPW; (ii) using omics technologies to elucidate microbial function and species interaction; (iii) pre-designing environmental and operational conditions to optimize treatment efficiency.
{"title":"Current status, potential assessment, and future directions of biological treatments of unconventional oil and gas wastewater","authors":"Chaoyang Li , Alberto Tiraferri , Peng Tang , Jun Ma , Baicang Liu","doi":"10.1016/j.watres.2025.123217","DOIUrl":"10.1016/j.watres.2025.123217","url":null,"abstract":"<div><div>Unconventional oil and gas (UOG) extraction techniques typically involve the production of large volumes of so-called flowback and produced water (FPW), a site-specific wastewater stream characterized by complex organic and inorganic composition. Sustainable and cost-effective management of FPW, as well as mitigation of its environmental risks and impacts, represents substantial challenges for governments, industries, and societies worldwide. Among various treatment technologies, biological processes have gained interest due to their low installation and operational costs. However, the interaction of FPW's complex composition with microorganisms poses challenging scientific and engineering questions. This review examines the water quality characteristics and sources of FPW from twelve UOG extraction sites in China and North America, revealing strong spatio-temporal heterogeneity of organic, inorganic, and microbial components across different reservoirs. The complex and variable water quality, large wastewater volumes, and high treatment demands have driven the exploration of biological treatments for FPW. This work systematically reviews and analyzes the operating conditions, treatment efficiency, and technical applicability of suspended sludge reactors, attached sludge reactors, mixed systems, and resource/energy recovery systems. Developing skid-mounted equipment based on suspended sludge reactors to handle variations in wastewater quantity and innovating the form of attached sludge reactors, especially in enriching salt-tolerant microbes for in-situ FPW treatment, are deemed essential. The dominant microorganisms playing a key role in the biological treatment are also discussed, with focus on two different inoculation sources (activated sludge and FPW). <em>Roseovarius</em> from FPW and <em>Pseudomonas</em> from activated sludge have strong adaptability to different reactors. The review further underscores the need to integrate biological treatments with complementary technologies. Finally, it advocates for the establishment of robust and scalable biological treatments through research in three main directions: (i) exploring microbial resources in original FPW; (ii) using omics technologies to elucidate microbial function and species interaction; (iii) pre-designing environmental and operational conditions to optimize treatment efficiency.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123217"},"PeriodicalIF":11.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055423","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}
Pub Date : 2025-01-28DOI: 10.1016/j.watres.2025.123218
Haibo Wang , Min Wang , Yukang Li , Xinyuan Yang , Xueci Xing , Baoyou Shi
The interaction between water and pipe surfaces can deteriorate drinking water quality, thus threatening public health. However, uncertainties remain in the release mechanism of phthalates acid esters (PAEs) from plastic pipes and their effects on drinking water quality. Our study indicated that PAEs released from polyvinyl chloride (PVC) pipes was higher than polyethylene (PE) pipes. Chlorine disinfection increased the released PAEs concentration in effluents of PE-Cl2 and PVCCl2 pipes to 6.60∼7.87 μg/L and 7.45∼8.88 μg/L, respectively. PAEs release varied the CHO and tannins numbers in dissolved organic matter (DOM), increasing the cytotoxicity of water. Although chorine disinfection reduced the abundance of pathogenic bacteria, it upregulated the relative abundance of bacterial metabolic pathways related to human disease, such as drug resistance: antimicrobial and cancer: overview. In addition, various biofilm bacterial community compositions affected the interactions between bacteria and pipe surfaces, and the roughness of pipe surfaces increased after biofilm formation. The hydrophilicity of pipe surfaces also increased due to biofilm formation and chlorine disinfection. After five months of running, higher hydrophilicity of PVC pipe surface was observed than that of PE pipes, especially after chlorine disinfection, consequently enhancing PAEs release. In conclusion, chlorine disinfection accelerated PAEs release from plastic pipes by increasing the hydrophilicity of pipe surfaces, resulting in higher cytotoxicity and microbial risk of drinking water, especially in PVCCl2 pipes. This study revealed the influence of chlorine disinfection on PAEs release and its potential risk to public health, which provided insightful visions for the future drinking water security monitoring.
{"title":"Chlorination enhances the phthalates release and increases the cytotoxicity and bacterial functions related to human disease of drinking water in plastic pipes","authors":"Haibo Wang , Min Wang , Yukang Li , Xinyuan Yang , Xueci Xing , Baoyou Shi","doi":"10.1016/j.watres.2025.123218","DOIUrl":"10.1016/j.watres.2025.123218","url":null,"abstract":"<div><div>The interaction between water and pipe surfaces can deteriorate drinking water quality, thus threatening public health. However, uncertainties remain in the release mechanism of phthalates acid esters (PAEs) from plastic pipes and their effects on drinking water quality. Our study indicated that PAEs released from polyvinyl chloride (PVC) pipes was higher than polyethylene (PE) pipes. Chlorine disinfection increased the released PAEs concentration in effluents of PE-Cl<sub>2</sub> and PVC<img>Cl<sub>2</sub> pipes to 6.60∼7.87 μg/L and 7.45∼8.88 μg/L, respectively. PAEs release varied the CHO and tannins numbers in dissolved organic matter (DOM), increasing the cytotoxicity of water. Although chorine disinfection reduced the abundance of pathogenic bacteria, it upregulated the relative abundance of bacterial metabolic pathways related to human disease, such as drug resistance: antimicrobial and cancer: overview. In addition, various biofilm bacterial community compositions affected the interactions between bacteria and pipe surfaces, and the roughness of pipe surfaces increased after biofilm formation. The hydrophilicity of pipe surfaces also increased due to biofilm formation and chlorine disinfection. After five months of running, higher hydrophilicity of PVC pipe surface was observed than that of PE pipes, especially after chlorine disinfection, consequently enhancing PAEs release. In conclusion, chlorine disinfection accelerated PAEs release from plastic pipes by increasing the hydrophilicity of pipe surfaces, resulting in higher cytotoxicity and microbial risk of drinking water, especially in PVC<img>Cl<sub>2</sub> pipes. This study revealed the influence of chlorine disinfection on PAEs release and its potential risk to public health, which provided insightful visions for the future drinking water security monitoring.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"276 ","pages":"Article 123218"},"PeriodicalIF":11.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050221","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}
Pub Date : 2025-01-28DOI: 10.1016/j.watres.2025.123205
Hanlin Yan , Xiaoguang Liu , Yang Zong , Zhendong Lei , Qunbiao He , Zhenyu Zhao , Zhengwei Zhou , Guojie Ye , Chengsi Hou , Deli Wu
In situ synthesis and activation of peracetic acid (PAA) for water decontamination is a promising way to overcome the transport and storage problems in PAA applications. Here, an in situ electrochemical PAA synthesis and activation system is constructed using RuO2−Ti “active” electrode and graphite plate as the anode and the cathode, respectively. PAA is efficiently generated at the RuO2−Ti anode with a maximum real-time concentration of ∼1020 μM and a negligible precursor loss of 2.91 % after 180 min, and can be activated at the cathode to destruct a refractory pollutant (i.e., benzoic acid (BA)) with the rate constant of 0.22−0.28 h−1, even under the interference of co-existing anions. Multiple pieces of evidence, including differential electrochemical mass spectrometry, sulfoxide probing test, and electron paramagnetic resonance spectroscopy, indicate that the oxygen-atom-transferring oxidation of CH3COO− by a high-valent ruthenium-oxo intermediate (i.e., RuO3) in situ formed through the electrode reconfiguration between RuO2 and chem-sorbed HO• mainly accounts for PAA synthesis. Acetylperoxyl radical (CH3C(O)OO•) was evidenced as the dominant species for BA degradation. This study proposes an in situ strategy to electrochemically synthesize and activate PAA for selective water decontamination and enriches the understandings of the mechanism of “active” electrode in peroxide synthesis.
{"title":"Dynamic electrode reconfiguration promotes in situ electrochemical peracetic acid synthesis for selective water decontamination","authors":"Hanlin Yan , Xiaoguang Liu , Yang Zong , Zhendong Lei , Qunbiao He , Zhenyu Zhao , Zhengwei Zhou , Guojie Ye , Chengsi Hou , Deli Wu","doi":"10.1016/j.watres.2025.123205","DOIUrl":"10.1016/j.watres.2025.123205","url":null,"abstract":"<div><div><em>In situ</em> synthesis and activation of peracetic acid (PAA) for water decontamination is a promising way to overcome the transport and storage problems in PAA applications. Here, an <em>in situ</em> electrochemical PAA synthesis and activation system is constructed using RuO<sub>2</sub>−Ti “active” electrode and graphite plate as the anode and the cathode, respectively. PAA is efficiently generated at the RuO<sub>2</sub>−Ti anode with a maximum real-time concentration of ∼1020 μM and a negligible precursor loss of 2.91 % after 180 min, and can be activated at the cathode to destruct a refractory pollutant (i.e., benzoic acid (BA)) with the rate constant of 0.22−0.28 h<sup>−1</sup>, even under the interference of co-existing anions. Multiple pieces of evidence, including differential electrochemical mass spectrometry, sulfoxide probing test, and electron paramagnetic resonance spectroscopy, indicate that the oxygen-atom-transferring oxidation of CH<sub>3</sub>COO<sup>−</sup> by a high-valent ruthenium-oxo intermediate (i.e., RuO<sub>3</sub>) <em>in situ</em> formed through the electrode reconfiguration between RuO<sub>2</sub> and chem-sorbed HO<sup>•</sup> mainly accounts for PAA synthesis. Acetylperoxyl radical (CH<sub>3</sub>C(O)OO<sup>•</sup>) was evidenced as the dominant species for BA degradation. This study proposes an <em>in situ</em> strategy to electrochemically synthesize and activate PAA for selective water decontamination and enriches the understandings of the mechanism of “active” electrode in peroxide synthesis.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123205"},"PeriodicalIF":11.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050174","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}
Excitation emission matrix (EEM) of fluorescence intensity has been often used to characterize dissolved organic matter in the aquatic environment. On EEM, there is a peak (Peak X) around excitation (emission) wavelengths of 490 (520) nm that is detected only in municipal wastewater-related samples. Peak X has been reported in very few papers. We investigated the characteristics of substances associated with Peak X from various perspectives. Based on that information, we hypothesized that Peak X was derived from fluorescein. This hypothesis was supported by the results of several estimates in this study, and it was revealed for the first time that Peak X on EEM was derived from fluorescein contained in colored bath salts widely used in Japan. We used Peak X to quantify how effluent from a wastewater treatment plant (WWTP) was dispersed in the outfall area of the plant and to evaluate its impact on the water quality to the area. By using Peak X, it was shown that the influence of the WWTP effluent on the discharged area extended several hundred meters. In other words, it was quantitatively demonstrated that the effluent significantly contributed to the increase in nutrient concentrations and primary production. These findings are expected to be highly useful for the control of nutrient concentrations in river water using the WWTP effluent, which has been the focus of much attention in recent years.
{"title":"Identification of wastewater-specific peak on EEM and their application for detecting the effluent in the discharged area","authors":"Kazuhiro Komatsu , Takashi Onodera , Kenji Tsuchiya , Ayato Kohzu , Kazuaki Syutsubo","doi":"10.1016/j.watres.2025.123213","DOIUrl":"10.1016/j.watres.2025.123213","url":null,"abstract":"<div><div>Excitation emission matrix (EEM) of fluorescence intensity has been often used to characterize dissolved organic matter in the aquatic environment. On EEM, there is a peak (Peak X) around excitation (emission) wavelengths of 490 (520) nm that is detected only in municipal wastewater-related samples. Peak X has been reported in very few papers. We investigated the characteristics of substances associated with Peak X from various perspectives. Based on that information, we hypothesized that Peak X was derived from fluorescein. This hypothesis was supported by the results of several estimates in this study, and it was revealed for the first time that Peak X on EEM was derived from fluorescein contained in colored bath salts widely used in Japan. We used Peak X to quantify how effluent from a wastewater treatment plant (WWTP) was dispersed in the outfall area of the plant and to evaluate its impact on the water quality to the area. By using Peak X, it was shown that the influence of the WWTP effluent on the discharged area extended several hundred meters. In other words, it was quantitatively demonstrated that the effluent significantly contributed to the increase in nutrient concentrations and primary production. These findings are expected to be highly useful for the control of nutrient concentrations in river water using the WWTP effluent, which has been the focus of much attention in recent years.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123213"},"PeriodicalIF":11.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050222","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-28DOI: 10.1016/j.watres.2025.123211
Yiyuan Xing, Wenjie Li, Xiaojian Liao, Lu Wang, Bo Wang, Yongzhen Peng
The scarcity of rapidly biodegradable organics, which serve as essential electron donors for the partial denitrification (PD) process, significantly hinders the combined application of PD coupled with anammox (PDA) in municipal wastewater treatment plants. This study innovatively applied, for the first time, a step-feed strategy combined with the use of sludge fermentation liquid (SFL) as an external carbon source in an integrated fixed-film activated sludge (IFAS) system, successfully driving full nitrification and PDA to achieve advanced nitrogen removal from low C/N real municipal wastewater. Moreover, the associated nitrogen removal mechanism of this system was systematically analyzed. By employing second-step SFL feed as a supplementary carbon source, the nitrogen removal efficiency reached 92.26 ± 2.77 % and the effluent total inorganic nitrogen was 6.43 ± 2.23 mg/L, with anammox contributing approximately 70 % to total inorganic nitrogen removal. 16S rRNA gene sequencing and fluorescence in situ hybridization analysis unveiled the extensive cooperation and synergistic interactions among anammox bacteria, denitrifying bacteria, and nitrifying bacteria, with Candidatus Brocadia being highly enriched in biofilms with a relative abundance of 2.21 %. Metagenomic sequencing confirmed that the relative abundance of the narGHI gene was greater than that of the nirS gene, providing stable nitrite accumulation conditions for the anammox process. Overall, this study proposes an innovative synergistic treatment scheme that utilizes a step-feed full nitrification-PDA process driven by SFL to achieve advanced nitrogen removal in municipal wastewater treatment plants. This approach is characterized by low energy consumption, low operational costs and a high nitrogen removal efficiency.
{"title":"Enhanced nitrogen removal from low C/N municipal wastewater in a step-feed integrated fixed-film activated sludge system: Synergizing anammox and partial denitrification with sludge fermentation liquid supplementation","authors":"Yiyuan Xing, Wenjie Li, Xiaojian Liao, Lu Wang, Bo Wang, Yongzhen Peng","doi":"10.1016/j.watres.2025.123211","DOIUrl":"10.1016/j.watres.2025.123211","url":null,"abstract":"<div><div>The scarcity of rapidly biodegradable organics, which serve as essential electron donors for the partial denitrification (PD) process, significantly hinders the combined application of PD coupled with anammox (PDA) in municipal wastewater treatment plants. This study innovatively applied, for the first time, a step-feed strategy combined with the use of sludge fermentation liquid (SFL) as an external carbon source in an integrated fixed-film activated sludge (IFAS) system, successfully driving full nitrification and PDA to achieve advanced nitrogen removal from low C/N real municipal wastewater. Moreover, the associated nitrogen removal mechanism of this system was systematically analyzed. By employing second-step SFL feed as a supplementary carbon source, the nitrogen removal efficiency reached 92.26 ± 2.77 % and the effluent total inorganic nitrogen was 6.43 ± 2.23 mg/L, with anammox contributing approximately 70 % to total inorganic nitrogen removal. 16S rRNA gene sequencing and fluorescence in situ hybridization analysis unveiled the extensive cooperation and synergistic interactions among anammox bacteria, denitrifying bacteria, and nitrifying bacteria, with <em>Candidatus</em> Brocadia being highly enriched in biofilms with a relative abundance of 2.21 %. Metagenomic sequencing confirmed that the relative abundance of the <em>narGHI</em> gene was greater than that of the <em>nirS</em> gene, providing stable nitrite accumulation conditions for the anammox process. Overall, this study proposes an innovative synergistic treatment scheme that utilizes a step-feed full nitrification-PDA process driven by SFL to achieve advanced nitrogen removal in municipal wastewater treatment plants. This approach is characterized by low energy consumption, low operational costs and a high nitrogen removal efficiency.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123211"},"PeriodicalIF":11.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050224","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}
Pub Date : 2025-01-28DOI: 10.1016/j.watres.2025.123215
Michael Attia , Frank T.-C. Tsai , Shuo Yang , Burke Minsley , Wade H. Kress
Coastal Louisiana is known for saltwater intrusion that threatens wetlands, aquifers, and rivers. However, the extent of saltwater intrusion is not well understood. This study develops an innovative framework with airborne electromagnetic (AEM) data to map chloride concentration distributions for wetlands in the Mississippi River deltaic plain and Chenier plain as well as for the Mississippi River Valley alluvial aquifer (MRVA) and Chicot aquifer. Moreover, the framework maps chloride concentrations along the Mississippi River and Atchafalaya River. Key components in the framework include the establishment of resistivity-to-chloride concentration transformation, 3D resistivity architecture building through geostatistics, and the employment of a lithologic model. The transformation functions correlate AEM resistivity data with porewater salinity measurements and groundwater and river chloride samples. The results show that AEM data reliably infers soil water chloride concentrations and correlates well with the distribution of various marsh types. AEM data reveals extensive saltwater presence at depth and near the coast, originating from salt domes and the Gulf of Mexico, respectively. The saltwater upconing pattern in the Chicot aquifer is likely due to excessive groundwater withdrawals. The AEM data also confirms a distinct tongue of saltwater intruding into the Atchafalaya Basin from the Gulf. The AEM data helps to identify faults that are obscured or eroded at the surface, which appear as leaky barriers in the subsurface where dramatic changes in chloride concentration are apparent. Finally, this study uses the AEM data to infer the presence of an extensive seawater wedge in the Mississippi River and Atchafalaya River.
{"title":"Airborne geophysical analysis to decipher salinization for coastal Louisiana","authors":"Michael Attia , Frank T.-C. Tsai , Shuo Yang , Burke Minsley , Wade H. Kress","doi":"10.1016/j.watres.2025.123215","DOIUrl":"10.1016/j.watres.2025.123215","url":null,"abstract":"<div><div>Coastal Louisiana is known for saltwater intrusion that threatens wetlands, aquifers, and rivers. However, the extent of saltwater intrusion is not well understood. This study develops an innovative framework with airborne electromagnetic (AEM) data to map chloride concentration distributions for wetlands in the Mississippi River deltaic plain and Chenier plain as well as for the Mississippi River Valley alluvial aquifer (MRVA) and Chicot aquifer. Moreover, the framework maps chloride concentrations along the Mississippi River and Atchafalaya River. Key components in the framework include the establishment of resistivity-to-chloride concentration transformation, 3D resistivity architecture building through geostatistics, and the employment of a lithologic model. The transformation functions correlate AEM resistivity data with porewater salinity measurements and groundwater and river chloride samples. The results show that AEM data reliably infers soil water chloride concentrations and correlates well with the distribution of various marsh types. AEM data reveals extensive saltwater presence at depth and near the coast, originating from salt domes and the Gulf of Mexico, respectively. The saltwater upconing pattern in the Chicot aquifer is likely due to excessive groundwater withdrawals. The AEM data also confirms a distinct tongue of saltwater intruding into the Atchafalaya Basin from the Gulf. The AEM data helps to identify faults that are obscured or eroded at the surface, which appear as leaky barriers in the subsurface where dramatic changes in chloride concentration are apparent. Finally, this study uses the AEM data to infer the presence of an extensive seawater wedge in the Mississippi River and Atchafalaya River.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"275 ","pages":"Article 123215"},"PeriodicalIF":11.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050173","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}
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