Photo-oxidation of Micro- and Nanoplastics: Physical, Chemical, and Biological Effects in Environments.

Micro- and nanoplastics (MNPs) are attracting increasing attention due to their persistence and potential ecological risks. This review critically summarizes the effects of photo-oxidation on the physical, chemical, and biological behaviors of MNPs in aquatic and terrestrial environments. The core of this paper explores how photo-oxidation-induced surface property changes in MNPs affect their adsorption toward contaminants, the stability and mobility of MNPs in water and porous media, as well as the transport of pollutants such as organic pollutants (OPs) and heavy metals (HMs). It then reviews the photochemical processes of MNPs with coexisting constituents, highlighting critical factors affecting the photo-oxidation of MNPs, and the contribution of MNPs to the phototransformation of other contaminants. The distinct biological effects and mechanism of aged MNPs are pointed out, in terms of the toxicity to aquatic organisms, biofilm formation, planktonic microbial growth, and soil and sediment microbial community and function. Furthermore, the research gaps and perspectives are put forward, regarding the underlying interaction mechanisms of MNPs with coexisting natural constituents and pollutants under photo-oxidation conditions, the combined effects of photo-oxidation and natural constituents on the fate of MNPs, and the microbiological effect of photoaged MNPs, especially the biotransformation of pollutants.

Appearance of Recalcitrant Dissolved Black Carbon and Dissolved Organic Sulfur in River Waters Following Wildfire Events.

Increasing wildfire frequency, a consequence of global climate change, releases incomplete combustion byproducts such as aquatic pyrogenic dissolved organic matter (DOM) and black carbon (DBC) into waters, posing a threat to water security. In August 2022, a series of severe wildfires occurred in Chongqing, China. Samples from seven locations along the Yangtze and Jialing Rivers revealed DBC, quantified by the benzene poly(carboxylic acid) (BPCA) method, comprising 9.5-19.2% of dissolved organic carbon (DOC). High concentrations of BPCA-DBC with significant polycondensation were detected near wildfire areas, likely due to atmospheric deposition driven by wind. Furthermore, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) revealed that wildfires were associated with an increase in condensed aromatics, proteins, and unsaturated hydrocarbons, along with a decrease in lignins. The condensed aromatics primarily consisted of dissolved black nitrogen (DBN), contributing to abundant high-nitrogen-containing compounds in locations highly affected by wildfires. Meanwhile, wildfires potentially induced the input of recalcitrant sulfur-containing protein-like compounds, characterized by high oxidation, aliphatic nature, saturation, and low aromaticity. Overall, this study revealed the appearance of recalcitrant DBC and dissolved organic sulfur in river waters following wildfire events, offering novel insights into the potential impacts of wildfires on water quality and environmental biogeochemistry.

Dissolved Black Carbon Facilitates the Photodegradation of Microplastics via Molecular Weight-Dependent Generation of Reactive Intermediates.

Photodegradation of microplastics (MPs) induced by sunlight plays a crucial role in determining their transport, fate, and impacts in aquatic environments. Dissolved black carbon (DBC), originating from pyrolyzed carbon, can potentially mediate the photodegradation of MPs owing to its potent photosensitization capacity. This study examined the impact of pyrolyzed wood derived DBC (5 mg C/L) on the photodegradation of polystyrene (PS) MPs in aquatic solutions under UV radiation. It revealed that the photodegradation of PS MPs primarily occurred at the benzene ring rather than the aliphatic segments due to the fast attack of hydroxyl radical (•OH) and singlet oxygen (1O2) on the benzene ring. The photosensitivity of DBC accelerated the degradation of PS MPs, primarily attributed to the increased production of •OH, 1O2, and triplet-excited state DBC (3DBC*). Notably, DBC-mediated photodegradation was related to its molecular weight (MW) and chemical properties. Low MW DBC (<3 kDa) containing more carbonyl groups generated more •OH and 1O2, accelerating the photodegradation of MPs. Nevertheless, higher aromatic phenols in high MW DBC (>30 kDa) scavenged •OH and generated more O2•-, inhibiting the photodegradation of MPs. Overall, this study offered valuable insights into UV-induced photodegradation of MPs and highlighted potential impacts of DBC on the transformation of MPs.

Human health risk assessment framework for new water resource recovery-based bio-composite materials.

A new type of bio-composite material is being produced from water-recovered resources such as cellulose fibres from wastewater, calcite from the drinking water softening process, and grass and reed from waterboard sites. These raw materials may be contaminated with pathogens and chemicals such as Escherichia coli, heavy metals, and resin compounds. A novel risk assessment framework is proposed here, addressing human health risks during the production of new bio-composite materials. The developed framework consists of a combination of existing risk assessment methods and is based on three main steps: hazard identification, qualitative risk mapping, and quantitative risk assessment. The HAZOP and Event Tree Analysis methodologies were used for hazard identification and risk mapping stages. Then, human health risks were quantitatively assessed using quantitative chemical risk assessment, evaluating cancer and non-cancer risk, and quantitative microbial risk assessment. The deterministic and the stochastic approaches were performed for this purpose. The contamination of raw materials may pose human health concerns, resulting in cancer risk above the threshold. Microbial risk is also above the safety threshold. Additional analysis would be significant as future research to better assess the microbial risk in biocomposite production. The framework has been effectively used for chemical and microbial risk assessment.

Assessing the Mass Concentration of Microplastics and Nanoplastics in Wastewater Treatment Plants by Pyrolysis Gas Chromatography-Mass Spectrometry.

The level of microplastics (MPs) in wastewater treatment plants (WWTPs) has been well evaluated by the particle number, while the mass concentration of MPs and especially nanoplastics (NPs) remains unclear. In this study, pyrolysis gas chromatography-mass spectrometry was used to determine the mass concentrations of MPs and NPs with different size ranges (0.01-1, 1-50, and 50-1000 µm) across the whole treatment schemes in two WWTPs. The mass concentrations of total MPs and NPs decreased from 26.23 and 11.28 µg/L in the influent to 1.75 and 0.71 µg/L in the effluent, with removal rates of 93.3 and 93.7% in plants A and B, respectively. The proportions of NPs (0.01-1 µm) were 12.0-17.9 and 5.6-19.5% in plants A and B, respectively, and the removal efficiency of NPs was lower than that of MPs (>1 µm). Based on annual wastewater effluent discharge, it is estimated that about 0.321 and 0.052 tons of MPs and NPs were released into the river each year. Overall, this study investigated the mass concentration of MPs and NPs with a wide size range of 0.01-1000 µm in wastewater, which provided valuable information regarding the pollution level and distribution characteristics of MPs, especially NPs, in WWTPs.

Identification and Quantification of Nanoplastics in Surface Water and Groundwater by Pyrolysis Gas Chromatography-Mass Spectrometry.

Nanoplastics (NPs) are currently considered an environmental pollutant of concern, but the actual extent of NP pollution in environmental water bodies remains unclear and there is not enough quantitative data to conduct proper risk assessments. In this study, a pretreatment method combining ultrafiltration (UF, 100 kDa) with hydrogen peroxide digestion and subsequent detection with pyrolysis gas chromatography-mass spectrometry (Py-GC/MS) was developed and used to identify and quantify six selected NPs in surface water (SW) and groundwater (GW), including poly(vinylchloride) (PVC), poly(methyl methacrylate) (PMMA), polypropylene (PP), polystyrene (PS), polyethylene (PE), and poly(ethylene terephthalate) (PET). The results show that the proposed method could detect NPs in environmental water samples. Nearly all selected NPs could be detected in the surface water at all locations, while PVC, PMMA, PS, and PET NPs were frequently below the detection limit in the groundwater. PP (32.9-69.9%) and PE (21.3-44.3%) NPs were the dominant components in both surface water and groundwater, although there were significant differences in the pollution levels attributed to the filtration efficiency of riverbank, with total mass concentrations of 0.283-0.793 µg/L (SW) and 0.021-0.203 µg/L (GW). Overall, this study quantified the NPs in complex aquatic environments for the first time, filling in gaps in our knowledge about NP pollution levels and providing a useful methodology and important reference data for future research.

Life Cycle Environmental Impacts of Wastewater-Derived Phosphorus Products: An Agricultural End-User Perspective.

Recovering phosphorus from wastewater in more concentrated forms has potential to sustainably recirculate phosphorus from cities to agriculture. The environmental sustainability of wastewater-based phosphorus recovery processes or wastewater-derived phosphorus products can be evaluated using life cycle assessment (LCA). Many LCA studies used a process perspective to account for the impacts of integrating phosphorus recovery processes at wastewater treatment plants, while some used a product perspective to assess the impacts of producing wastewater-derived phosphorus products. We demonstrated the application of an end-user perspective by assessing life cycle environmental impacts of substituting half of the conventional phosphorus rock-based fertilizers used in three crop production systems with wastewater-derived phosphorus products from six recovery pathways (RPs). The consequential LCA results show that the substitution reduces global warming potential, eutrophication potential, ecotoxicity potential, and acidification potential of the assessed crop production systems in most RPs and scenarios. The end-user perspective introduced in this study can (i) complement with the process perspective and the product perspective to give a more holistic picture of environmental impacts along the "circular economy value chains" of wastewater-based resource recovery, (ii) enable systemwide assessment of wide uptake of wastewater-derived products, and (iii) draw attention to understanding the long-term environmental impacts of using wastewater-derived products.

Changes in biofilm composition and microbial water quality in drinking water distribution systems by temperature increase induced through thermal energy recovery.

Drinking water distribution systems (DWDSs) have been thoroughly studied, but the concept of thermal energy recovery from DWDSs is very new and has been conceptualized in the past few years. Cold recovery results in a temperature increase of the drinking water. Its effects on drinking water quality and biofilm development are unclear. Hence, we studied both bulk water and biofilm phases for 232 days in two parallel pilot scale distribution systems with two temperature settings after cold recovery, 25 °C and 30 °C, and compared these with a reference pilot system without cold recovery. In all three pilot distributions systems (DSs) our results showed an initial increase in biomass (ATP) in the biofilm phase, along with occurrence of primary colonizers (Betaproteobacteriales) and subsequently a decrease in biomass and an increasing relative abundance of other microbial groups (amoeba resisting groups; Xanthobacteraceae, Legionellales), including those responsible for EPS formation in biofilms (Sphingomonadaceae). The timeline for biofilm microbial development was different for the three pilot DSs: the higher the temperature, the faster the development took place. With respect to the water phase within the three pilot DSs, major microbial contributions came from the feed water (17-100%) and unkown sources (2-80%). Random contributions of biofilm (0-70%) were seen between day 7-77. During this time period six-fold higher ATP concentration (7-11 ng/l) and two-fold higher numbers of high nucleic acid cells (5.20-5.80 × 104 cells/ml) were also observed in the effluent water from all three pilot DSs, compared to the feed water. At the end of the experimental period the microbial composition of effluent water from three pilot DSs revealed no differences, except the presence of a biofilm related microbial group (Sphingomonadaceae), within all three DSs compared to the feed water. In the biofilm phase higher temperatures initiated the growth of primary colonizing bacteria but this did not lead to differences in microbial diversity and composition at the end of the experimental period. Hence, we propose that the microbiological water quality of DWDSs with cold recovery should be monitored more frequently during the first 2-3 months of operation.

Model development for evidence-based prioritisation of policy action on emerging chemical and microbial drinking water risks.

While the burden of disease from well-studied drinking water contaminants is declining, risks from emerging chemical and microbial contaminants arise because of social, technological, demographic and climatological developments. At present, emerging chemical and microbial drinking water contaminants are not assessed in a systematic way, but reactively and incidence based. Furthermore, they are assessed separately despite similar pollution sources. As a result, risks might be addressed ineffectively. Integrated risk assessment approaches are thus needed that elucidate the uncertainties in the risk evaluation of emerging drinking water contaminants, while considering risk assessors' values. This study therefore aimed to (1) construct an assessment hierarchy for the integrated evaluation of the potential risks from emerging chemical and microbial contaminants in drinking water and (2) develop a decision support tool, based on the agreed assessment hierarchy, to quantify (uncertain) risk scores. A multi-actor approach was used to construct the assessment hierarchy, involving chemical and microbial risk assessors, drinking water experts and members of responsible authorities. The concept of value-focused thinking was applied to guide the problem-structuring and model-building process. The development of the decision support tool was done using Decisi-o-rama, an open-source Python library. With the developed decision support tool (uncertain) risk scores can be calculated for emerging chemical and microbial drinking water contaminants, which can be used for the evidence-based prioritisation of actions on emerging chemical and microbial drinking water risks. The decision support tool improves existing prioritisation approaches as it combines uncertain indicator levels with a multi-stakeholder approach and integrated the risk assessment of chemical and microbial contaminants. By applying the concept of value-focused thinking, this study addressed difficulties in evidence-based decision-making related to emerging drinking water contaminants. Suggestions to improve the model were made to guide future research in assisting policy makers to effectively protect public health from emerging drinking water risks.

Low-Carbon Urban Water Systems: Opportunities beyond Water and Wastewater Utilities?

The provision of urban water and wastewater services contributes to greenhouse gas (GHG) emissions. Urban water supply and wastewater utilities can potentially achieve low-carbon or carbon-neutral operation through many "utility opportunities". Outside the jurisdiction of water utilities, many water-related "wider opportunities" can also contribute to GHG emissions abatement for cities. This study aims to explore the GHG emissions abatement potential, cost effectiveness, and enabling factors of implementing wider opportunities in cities. Using Amsterdam as a case study, we developed a marginal abatement cost curve to compare the abatement potential and cost effectiveness of both utility and wider opportunities. The results show that many wider opportunities related to thermal energy, water end use, and life cycle are cost-effective with significant abatement potential, compared to utility opportunities. This case study and emerging worldwide examples show that the water industry has a role to play to support wider water-related opportunities in cities. This vision can be supported by developing mechanisms to credit utilities for wider opportunity initiatives, building inter- and intrasectoral partnerships for utilities, accounting for scope 3 emissions of utilities, and being open to extend utilities' role beyond water and wastewater services providers.

Thermal energy recovery from chlorinated drinking water distribution systems: Effect on chlorine and microbial water and biofilm characteristics.

Thermal energy recovery from drinking water has a high potential in the application of sustainable building and industrial cooling. However, drinking water and biofilm microbial qualities should be concerned because the elevated water temperature after cold recovery may influence the microbial activities in water and biofilm phases in drinking water distribution systems (DWDSs). In this study, the effect of cold recovery on microbial qualities was investigated in a chlorinated DWDS. The chlorine decay was slight (1.1%-15.5%) due to a short contact time (~60 s) and was not affected by the cold recovery (p > 0.05). The concentrations of cellular ATP and intact cell numbers in the bulk water were partially inactivated by the residual chlorine, with the removal rates of 10.1%-16.2% and 22.4%-29.4%, respectively. The chlorine inactivation was probably promoted by heat exchangers but was not further enhanced by higher temperatures. The higher water temperature (25 °C) enhanced the growth of biofilm biomass on pipelines. Principle coordination analysis (PCoA) showed that the biofilms on the stainless steel plates of HEs and the plastic pipe inner surfaces had totally different community compositions. Elevated temperatures favored the growth of Pseudomonas spp. and Legionella spp. in the biofilm after cold recovery. The community functional predictions revealed more abundances of five human diseases (e.g. Staphylococcis aureus infection) and beta-lactam resistance pathways in the biofilms at higher temperature. Compared with a previous study with a non-chlorinated DWDS, chlorine dramatically reduced the biofilm biomass growth but raised the relative abundances of the chlorine-resistant genera (i.e. Pseudomonas and Sphingomonas) in bacterial communities.

An exploration of disinfection by-products formation and governing factors in chlorinated swimming pool water.

This paper investigates disinfection by-products (DBPs) formation and their relationship with governing factors in chlorinated swimming pools. The study compares concentrations of DBPs with WHO guidelines for drinking water quality recommended to screen swimming pool water quality. The statistical analysis is based on a global database of 188 swimming pools accumulated from 42 peer-reviewed journal publications from 16 countries. The mean and standard deviation of dichloroacetic acid and trichloroacetic acid were estimated as 282 ± 437 and 326 ± 517 µg L-1, respectively, which most often surpassed the WHO guidelines. Similarly, more than half of the examined pools had higher values of chloral hydrate (102 ± 128 µg L-1). The concentration of total chloramines (650 ± 490 µg L-1) was well above the WHO guidelines in all reported cases. Nevertheless, the reported values remained below the guidelines for most of the studied pools in the case of total trihalomethanes (134 ± 160 µg L-1), dichloroacetonitrile (12 ± 12 µg L-1) and dibromoacetonitrile (8 ± 11 µg L-1). Total organic carbon, free residual chlorine, temperature, pH, total nitrogen and bromide ions play a pivotal role in DBPs formation processes. Therefore, proper management of these governing factors could significantly reduce DBPs formation, thereby, contributing towards a healthy swimming pool environment.

Decision support for water quality management of contaminants of emerging concern.

Water authorities and drinking water companies are challenged with the question if, where and how to abate contaminants of emerging concern in the urban water cycle. The most effective strategy under given conditions is often unclear to these stakeholders as it requires insight into several aspects of the contaminants such as sources, properties, and mitigation options. Furthermore the various parties in the urban water cycle are not always aware of each other's requirements and priorities. Processes to set priorities and come to agreements are lacking, hampering the articulation and implementation of possible solutions. To support decision makers with this task, a decision support system was developed to serve as a point of departure for getting the relevant stakeholders together and finding common ground. The decision support system was iteratively developed in stages. Stakeholders were interviewed and a decision support system prototype developed. Subsequently, this prototype was evaluated by the stakeholders and adjusted accordingly. The iterative process lead to a final system focused on the management of contaminants of emerging concern within the urban water cycle, from wastewater, surface water and groundwater to drinking water, that suggests mitigation methods beyond technical solutions. Possible wastewater and drinking water treatment techniques in combination with decentralised and non-technical methods were taken into account in an integrated way. The system contains background information on contaminants of emerging concern such as physical/chemical characteristics, toxicity and legislative frameworks, water cycle entrance pathways and a database with associated possible mitigation methods. Monitoring data can be uploaded to assess environmental and human health risks in a specific water system. The developed system was received with great interest by potential users, and implemented in an international water cycle network.

A bottom-up approach to estimate dry weather flow in minor sewer networks.

In order to evaluate the feasibility of installing decentralised installations for wastewater reuse in cities, information about flows at specific spots of a sewer is needed. However, measuring intermittent flows in partially filled conduits is a technical task which is sometimes difficult to accomplish. This paper describes a method to model intermittent discharges in small sewers by linking a stochastic model for wastewater discharge to a hydraulic model to predict the attenuation of the discharges and its impact on the arrival time to a defined spot. The method was validated in a case study. The model estimated adequately the wastewater discharges on working days.

Environmental risk assessment related to using resource recovery-based bio-composite materials in the aquatic environment with new laboratory leaching test data.

The concept of circular economy, aiming at increasing the sustainability of products and services in the water and other sectors, is gaining momentum worldwide. Driven by this concept, novel bio-composite materials produced by recovering resources from different parts of the water cycle are now manufactured in The Netherlands. The new materials are used for different products such as canal bank protection elements, as an alternative to similar elements made of hardwood. As much as these new materials are appealing from the sustainability point of view, they may leach toxic substances into the aquatic environment given some of their ingredients, e.g., cellulose recovered from wastewater treatment. Therefore, a methodology for the assessment of related environmental risks is needed and it does not exist currently. This paper addresses this knowledge gap by presenting a framework for this. The framework is based on European environmental risk assessment guidelines, and it includes four key steps: (i) hazard identification, (ii) dose-response modelling, (iii) exposure assessment and (iv) risk characterisation (i.e. assessment). As part of the first step, laboratory leaching tests were carried out to evaluate the potential release of specific chemical substances such as heavy metals and resin compounds into the aquatic environment. Laboratory test results were then used as input data to evaluate the risk of potential leaching from canal bank protection elements into surface water. A deterministic model was used first to identify the chemicals exceeding the guideline threshold. Subsequently, a stochastic model was applied to evaluate the environmental risks across a range of leachate concentrations and water velocities in the canal, thereby simulating a broader spectrum of possible situations. The risk analyses were conducted for four alternative bio-composite materials made of different ingredients, two different flow conditions (stagnant water and advective flow) in two types of canals (wide ditch and primary watercourse) and for two different water levels based on season conditions (summer and winter conditions). The results obtained from leaching tests identified Cu, Mn, Zn, styrene and furfuryl alcohol as potentially troublesome chemicals. In the case of stagnant water, the absence of a flow rate increases the residence time of the chemicals in the surface water, resulting in a higher PEC/PNEC (i.e. risk) value. However, under stagnant case conditions, environmental risks for all chemicals considered turned out to be below the safety threshold. In the advective case, the existence of a flow rate, even at low velocities simulating the conditions of 'almost no flow,' contributes to increased dilution, resulting in lower PEC/PNEC ratio values. The results presented here, even though representing real-case scenarios, are only indicative as these are based on laboratory leaching tests and a number of assumptions made. Additional field tests involving collecting and analysing water and sediment samples from the canal where the canal bank protection elements are located, over a prolonged period, are required to come up with more conclusive findings.

A new approach to circularity assessment for a sustainable water sector: Accounting for environmental functional flows and losses.

Resource recovery solutions can reduce the water sector's resource use intensity. With many such solutions being proposed, an assessment method for effective decision-making is needed. The water sector predominantly deals with biogeochemical resources (e.g., nitrogen) that are different from technical resources (e.g., industrial coagulants) in three ways: (1) they move through the environment in natural cycles; (2) they fulfil different human and environmental functions; and (3) they are subject to substantial environmental losses. Whilst several circularity assessment methods exist for technical resources, biogeochemical resources have received less attention. To address this, a well-established material circularity indicator (MCI) method is modified. This is done by redefining the terms: restoration, regeneration, and linear flows to create a new circularity assessment approach. The new approach is demonstrated in a real-life case study involving treated wastewater (TW) fertigation. The new approach reveals that using the original MCI method underestimates the circularity of resource recovery solutions involving biogeochemical resources. This is because, in the original MCI method, only the flows that are reused/recycled for human functions can be considered circular, whereas, in the new approach, one also considers flows such as N2 emission and groundwater infiltration as circular flows. Even though these may not be reuse/recycle type flows, they still contribute towards future resource availability and, thus, towards sustainability. The modified assessment method shows that TW fertigation can significantly improve nitrogen and water circularity. However, careful planning of the fertigation schedule is essential since increasing fertigation frequency leads to lower water but higher nitrogen circularity. Additionally, collecting drainage water for reuse can improve nitrogen circularity. In conclusion, using the modified MCI approach, circularity can be assessed in a manner that is better aligned with sustainability.

The contribution of deeper layers in slow sand filters to pathogens removal.

Slow Sand Filtration is popular in drinking water treatment for the removal of a wide range of contaminants (e.g., particles, organic matter, and microorganisms). The Schmutzdecke in slow sand filters (SSFs) is known to be essential for pathogen removal, however, this layer is also responsible for increased head loss. Since the role of deeper layers in bacteria and virus removal is poorly understood, this research investigated the removal of E.coli WR1 and PhiX 174 at different depths of a full-scale SSF. Filter material from top (0-5 cm), middle (5-20 cm) and deep (20-35 cm) layers of an established filter was used in an innovative experimental set-up to differentiate physical-chemical and biological removal processes. In the analysis, we distinguished between removal by biological activity, biofilm and just sand. In addition, we modelled processes by a one-side kinetic model. The different layers contributed substantially to overall log removal of E.coli WR1 (1.4-1.7 log10) and PhiX 174 (0.4-0.6 log10). For E.coli WR1, biological activity caused major removal, followed by removal within biofilm and sand, whereas, removal of PhiX 174 mainly occurred within sand, followed by biofilm and biological activity. Narrow pore radii in the top layer obtained by micro-computed tomography scanner suggested enhanced retention of bacteria due to constrained transport. The retention rates of E.coli WR1 and PhiX 174 in top layer were four and five times higher than deeper layers, respectively (kret 1.09 min-1 vs 0.26 min-1 for E.coli WR1 and kret 0.32 min-1 vs of 0.06 min-1 for PhiX 174). While this higher rate was restricted to the Schmutzdecke alone (top 5 cm), the deeper layers extend to around 1 m in full-scale filters. Therefore, the contribution of deeper layers of established SSFs to the overall log removal of bacteria and viruses is much more substantial than the Schmutzdecke.

Effects of phosphate addition on the removal of disinfection by-product formation potentials by biological activated carbon filtration.

In drinking water treatment plants (DWTPs), the widely used biological activated carbon filters (BACFs), as the last barrier before disinfection, can remove dissolved organic matter (DOM) known as precursors of disinfection by-products (DBPs). Whether phosphate addition can improve water purification and DBP control of BACFs is still controversial. This study investigated short-term and long-term effects of phosphate addition on controlling DBP formation potentials (FPs) by BACFs via column and batch experiments. The BAC columns presented good water purification performance: they removed around 50 % DOM, nearly all fulvic acid-likes and humic acid-likes as well as 5 %-70 % chlor(am)innated THM4, HAA9 and HAN4 FPs (except chloraminated THM4 FPs)， which was mainly contributed by aerobic bacteria not anoxic bacteria. Phosphate addition within 7-14 days further improved removals of DOM, aromatic organics, fluorescence fractions in DOM as well as HAA9 and HAN4 FPs (especially TCAA FP and TCAN FP) to different extent. However, this improvement did not last longer, and removals of DOM, aromatic organics, two fluorescence fractions (soluble microbial byproduct-likes and humic acid-likes) and DBP FPs decreased despite long-term phosphate addition. Oxic and anoxic batch experiments showed that the positive response of water purification to short-term phosphate addition was also mainly attributed to aerobic bacteria and not to anoxic bacteria. For example, the former decreased DOM and DBP FPs, while the latter increased protein- and tryptophan-like substances as well as chloraminated THM4 FPs. Phosphate addition resulted in EPS increase in anoxic reactors and decrease in oxic reactors. These results indicated that a high dissolved oxygen in BACFs may be helpful for water purification and DBP control. Overall, short-term phosphate addition into phosphorus-limited water is beneficial for BACFs to control DBPs while long-term addition has no effect. Therefore, an intermittent phosphate addition into BACFs is suggested to control DBPs in DWTPs.

Service-lines as major contributor to water quality deterioration at customer ends.

Biofilm detachment contributes to water quality deterioration. However, the contributions of biofilm detachment from different pipes have not been quantified or compared. Following the introduction of partial reverse osmosis (RO) in drinking water production, this study analyzed particles at customers' ends and tracked their origins to water distribution mains and service lines. For doing so, filter bags were installed in front of water meters to capture upstream detached particles, while biofilm from water main and service line were sampled by cutting pipe specimens. The results showed that elemental concentrations of the biofilm in mains were higher than those of service lines (54.3-268.5 vs. 27.1-44.4 µg/cm2), both dominated by Ca. Differently, filter bags were dominated by Fe/Mn (77.5-98.1%). After introducing RO, Ca significantly decreased in biofilms of mains but not service lines, but the released Fe/Mn rather than Ca arrived at customers' ends. The ATP concentrations of service lines were higher than mains, which decreased on mains but increased in service lines after introducing RO. For the core ASVs, 13/24 were shared by service lines (17), mains (21), and filter bags (17), which were assigned mainly to Nitrospira spp., Methylomagnum spp., Methylocytis spp., and IheB2-23 spp. According to source tracking results, service lines contributed more than mains to the particulate material collected by filter bags (57.6 ± 13.2% vs. 13.0 ± 11.6%). To the best of our knowledge, the present study provides the first evidence of service lines' direct and quantitative contributions to potential water quality deterioration at customers' ends. This highlights the need for the appropriate management of long-neglected service line pipes, e.g., regarding material selection, length optimization, and proper regulation.

Direct discharge of sewage to natural water through illicitly connected urban stormwater systems: An overlooked source of dissolved organic matter.

The illicit connection of sewage pipes to stormwater pipes commonly occurs in urban stormwater systems. This brings problems that sewage might be directly discharges into natural water and even drinking water sources without treatment, posing risks to ecological safety. Sewage contains various unknown dissolved organic matter (DOM), which could react with disinfectants and lead to the formation of carcinogenic disinfection byproducts (DBPs). Thus, understanding the impacts of illicit connections on downstream water quality is of significance. This study firstly investigated the characteristics of DOM using fluorescence spectroscopy and the formation of DBPs after chlorination in an urban stormwater drainage system in the case of illicit connections. The results found that the concentrations of dissolved organic carbon and dissolved organic nitrogen ranged from 2.6 to 14.9 mg/L and from 1.8 to 12.6 mg/L, respectively, with the highest levels occurring at the illicit connection points. Concerning DBP precursors, pipe illicit connections introduced considerable precursors of highly toxic haloacetaldehydes and haloacetonitriles into the stormwater pipes. Furthermore, illicit connections introduced more contents of tyrosine-like and tryptophan-like aromatic proteins, which may be related to foods, nutrients, personal care products, etc. in the untreated sewage. This indicated that the urban stormwater drainage system was a significant input source of DOM and DBP precursors to natural water. The results of this study are of great significance for protecting the security of water sources and promoting the sustainability of urban water environment.