Role of bipyridyl in enhancing ferrate oxidation toward micropollutants.

Enhancing Fe(VI) oxidation ability by generating high-valent iron-oxo species (Fe(IV)/Fe(V)) has attracted continuous interest. This work for the first time reports the efficient activation of Fe(VI) by a well-known aza-aromatic chelating agent 2,2'-bipyridyl (BPY) for micropollutant degradation. The presence of BPY increased the degradation constants of six model compounds (i.e., sulfamethoxazole (SMX), diclofenac (DCF), atenolol (ATL), flumequine (FLU), 4-chlorophenol (4-CP), carbamazepine (CBZ)) with Fe(VI) by 2 - 6 folds compared to those by Fe(VI) alone at pH 8.0. Lines of evidence indicated the dominant role of Fe(IV)/Fe(V) intermediates. Density functional theory calculations suggested that the binding of Fe(III) to one or two BPY molecules initiated the oxidation of Fe(III) to Fe(IV) by Fe(VI), while Fe(VI) was reduced to Fe(V). The increased exposures of Fe(IV)/Fe(V) were experimentally verified by the pre-generated Fe(III) complex with BPY and using methyl phenyl sulfoxide as the probe compound. The presence of chloride and bicarbonate slightly affected model compound degradation by Fe(VI) in the presence of BPY, while a negative effect of humic acid was obtained under the same conditions. This work demonstrates the potential of N-donor heterocyclic ligand to activate Fe(VI) for micropollutant degradation, which is instructive for the Fe(VI)-based oxidation processes.

Simulated sunlight/periodate-triggered formation of toxic halogenated bisphenols in highly saline water.

Periodate (PI)-based oxidation using the activators, such as metal ions and light irradiation, has emerged as a feasible treatment strategy for the effective remediation of contaminated water and wastewater. Given the pervasive nature of PI residues and solar exposure during application, the role of solar light in remediating the challenging highly saline water matrices needs to be elucidated. In this study, bisphenol A (BPA) was selected as the targeted micropollutant, which can be efficiently eliminated by the simulated sunlight (SSL)/PI system in the presence of high-level Cl- (up to 846.0 mM) at pH 7.0. The presence of different background constituents of water, such as halides, nitrate, and dissolved organic matter, had no effect, or even accelerated BPA abatement. Particularly, the ubiquitous Br- or I- appreciably enhanced the BPA transformation efficiency, which may be ascribed to the generation of high-selective reactive HOBr or HOI. The in silico predictions suggested that the transformation products generated by halide-mediated SSL/PI systems via halogen substitutions showed greater persistence, bioaccumulation, and aquatic toxicity than BPA itself. These findings highlighted a widespread phenomenon during PI-based oxidative treatment of highly saline water, which needs special attention under solar light illumination.

Sustainable lithium extraction enabled by responsive metal-organic frameworks with ion-sieving adsorption effects.

Metal-organic frameworks (MOFs) are superior ion adsorbents for selectively capturing toxic ions from water. Nevertheless, they have rarely been reported to have lithium selectivity over divalent cations due to the well-known flexibility of MOF framework and the similar physiochemical properties of Li+ and Mg2+. Herein, we report an ion-sieving adsorption approach to design sunlight-regenerable lithium adsorbents by subnanoporous MOFs for efficient lithium extraction. By integrating the ion-sieving agent of MOFs with light-responsive adsorption sites of polyspiropyran (PSP), the ion-sieving adsorption behaviors of PSP-MOFs with 6.0, 8.5, and 10.0 Å windows are inversely proportional to their pore size. The synthesized PSP-UiO-66 with a narrowest window size of 6.0 Å shows high LiCl adsorption capacity up to 10.17 mmol g-1 and good Li+/Mg2+ selectivity of 5.8 to 29 in synthetic brines with Mg/Li ratio of 1 to 0.1. It could be quickly regenerated by sunlight irradiation in 6 min with excellent cycling performance of 99% after five cycles. This work sheds light on designing selective adsorbents using responsive subnanoporous materials for environmentally friendly and energy-efficient ion separation and purification.

Fe(IV)/Fe(V)-mediated polyferric sulfate/periodate system: A novel coagulant/oxidant strategy in promoting micropollutant abatement.

Strategic modulation of the advanced oxidation processes for the selective oxidation of micropollutants has attracted accumulating attention in water decontamination. This study first reported the combination of the coagulant polyferric sulfate (PFS) and oxidant periodate (PI) to accomplish synergistic abatement of the antibiotic sulfamethoxazole (SMX). The oxidizing performance of SMX by this system was almost unaffected by coexisting water constituents, indicating the great promise of selective oxidation. Different from the current hydroxyl radicals (•OH)-mediated coagulant/oxidant systems (e.g., PFS/H2O2 and PFS/ozone), the dominance of high-valent Fe(IV)/Fe(V) intermediates was unambiguously verified in the PFS/PI treatment. The PFS colloids before and after the oxidation were characterized and the iron speciation was analyzed. The transformation of monomeric iron configurations (Fe(a)) to oligomeric iron configurations (Fe(b)) could maintain the homeostasis of surface-bound Fe(III) and Fe(II). The interaction mechanisms included the production of reactive species and dynamic reaction equilibrium for micropollutant degradation. Finally, the transformation pathways of SMX and carbamazepine (CMZ) in the PFS/PI system were postulated. Overall, this study provided a novel coagulant/oxidant strategy to achieve selective and sustainable water purification.

Environmental fate and risk evolution of calcium channel blockers from chlorine-based disinfection to sunlit surface waters.

Organic micropollutants present in disinfected wastewater and discharged to sunlit surface waters may be transformed by multiple processes, such as chlorination due to the presence of chlorine residuals, solar irradiation as well as solar-irradiated chlorine residues. This study reports, for the first time, the multi-scenario degradation kinetics, transformation products, and risk evolution of calcium channel blockers (CCBs), a class of emerging pharmaceutical contaminants with worldwide prevalence in natural waters and wastewater. It was found that the chlorination of the studied CCBs (amlodipine (AML) and verapamil (VER)) was dominated by the reaction of HOCl with their neutral species, with second-order rate constants of 6.15×104 M-1 s-1 (AML) and 7.93×103 M-1 s-1 (VER) at pH 5.0-11.0. Bromination is much faster than chlorination, with the measured kapp,HOBr values of 2.94×105 M-1 s-1 and 6.58×103 M-1 s-1 for AML and VER, respectively, at pH 7.0. Furthermore, both CCBs would undergo photolytic attenuations with hydroxyl and carbonate radicals as the dominant reactive species in water. Notably, free chlorine mainly contributed to their abatement during the solar/chlorine treatment. Additionally, the halogen addition on the aromatic ring was observed during chlorination and bromination of the two CCBs. Cyclization was observed under solar irradiation only, while the aromatic ring was opened in the solar/chlorine system. Some products generated by the three transformation processes exhibited non-negligible risks of high biodegradation recalcitrance and toxicity, potentially threatening the aquatic environment and public health. Overall, this study elucidated the environmental fate of typical CCBs under different transformation processes to better understand the resulting ecological risks in these environmental scenarios.

Rapid sand filtration for <10 µm-sized microplastic removal in tap water treatment: Efficiency and adsorption mechanisms.

The omnipresence of microplastics (MPs) in potable water has become a major concern due to their potential disruptive effect on human health. Therefore, the effective removal of MPs in drinking water is essential for life preservation. In this study, tap water containing microplastic <10 µm in size was treated using constructed pilot-scale rapid sand filtration (RSF) system to investigate the removal efficiency and the mechanisms involved. The results show that the RSF provides significant capacity for the removal and immobilization of MPs < 10 µm diameter (achieving 98 %). Results showed that silicate sand reacted with MPs through a cooperative assembly process, which mainly involved interception, trapping, entanglement, and adsorption. The MPs were quantified by Flow cytometry instrument. A kinetics study underlined the pivotal role of physio-chemisorption in the removal process. MP particles smaller than absorbents, saturation of adsorbents, and reactor hydrodynamics were identified as limiting factors, which were alleviated by backwashing. Backwashing promoted the desorption of up to 97 % MPs, conducive for adsorbent active site regeneration. These findings revealed the critical role of RSF and the importance of backwashing in removing MPs. Understanding the mechanisms involved in removing microplastics from drinking water is crucial in developing more efficient strategies to eliminate them.

Degradation of methotrexate by unactivated and solar-activated peroxymonosulfate in water: Moiety-specific reaction kinetics and transformation product-associated risks.

Anticancer drugs have raised worldwide concern owing to their ubiquitous occurrence and ecological risks, necessitating the development of efficient removal strategies in water and wastewater treatment. Although peroxymonosulfate (PMS) is known to be a promising chemical in water decontamination, limited information is available regarding the removal efficiency of anticancer drugs by PMS and solar/PMS systems. This study first reports the moiety-specific reaction kinetics and mechanisms of methotrexate (MTX), an anticancer drug with widespread attention, by PMS (unactivated) and solar-activated PMS in water. It was found that MTX abatement by the direct PMS oxidation followed second-order kinetics, and the pH-dependent rate constants increased from 0.4 M-1 s-1 (pH 5.0) to 1.3 M-1 s-1 (pH 8.0), with a slight decrease to 1.1 M-1 s-1 at pH 9.0. The presence of chloride and bromide exerted no obvious influence on the removal of MTX by PMS. Furthermore, the chemical reactivity of MTX and its seven substructures with different reactive species was evaluated, and the degradation contributions of the reactive species involved were quantitatively analyzed in the solar/PMS system. The product analysis suggested similar reaction pathways of MTX by PMS and solar/PMS systems. The persistence, bioaccumulation, and toxicity of the transformation products were investigated, indicating treatment-driven risks. Notably, MTX can be removed efficiently from both municipal and hospital wastewater effluents by the solar/PMS system, suggesting its great potential in wastewater treatment applications. Overall, this study systematically evaluated the elimination of MTX by the unactivated PMS and solar/PMS treatment processes in water. The obtained findings may have implications for the mechanistic understanding and development of PMS-based processes for the degradation of such micropollutants in wastewater.

Elucidating sulfate radical-induced oxidizing mechanisms of solid-phase pharmaceuticals: Comparison with liquid-phase reactions.

As a class of organic micropollutants of global concern, pharmaceuticals have prevalent distributions in the aqueous environment (e.g., groundwater and surface water) and solid matrices (e.g., soil, sediments, and dried sludge). Their contamination levels have been further aggravated by the annually increased production of expired drugs as emerging harmful wastes worldwide. Sulfate radicals (SO4•-)-based oxidation has attracted increasing attention for abating pharmaceuticals in the environment, whereas the transformation mechanisms of solid-phase pharmaceuticals remain unknown thus far. This investigation presented for the first time that SO4•-, individually produced by mechanical force-activated and heat-activated persulfate treatments, could effectively oxidize three model pharmaceuticals (i.e., methotrexate, sitagliptin, and salbutamol) in both solid and liquid phases. The high-resolution mass spectrometric analysis suggested their distinct transformation products formed by different phases of SO4•- oxidation. Accordingly, the SO4•--mediated mechanistic differences between the solid-phase and liquid-phase pharmaceuticals were proposed. It is noteworthy that the products from both systems were predicted with the remaining persistence, bioaccumulation, and multi-endpoint toxicity. Therefore, some post-treatment strategies need to be considered during practical applications of SO4•--based technologies in remediating different phases of micropollutants. This work has environmental implications for understanding the comparative transformation mechanisms of pharmaceuticals by SO4•- oxidation in remediating the contaminated solid and aqueous matrices.

Solar/periodate-triggered rapid inactivation of Microcystis aeruginosa by interrupting the Calvin-Benson cycle.

Frequent outbreak of cyanobacteria is a serious problem for drinking water treatment. The microcystins released from Microcystis aeruginosa (M. aeruginosa) could cause irreversible damage to human health. Catalyst-free solar/periodate (PI) system has recently presented great potential for bacterial inactivation, whereas the application potential and underlying mechanisms of the effective M. aeruginosa control remain unclear. Our work delineated the key role of ROS that inactivating/harmless disposing M. aeruginosa in the simulated sunlight (SSL)/PI system. Singlet oxygen may specifically cause DNA damage but maintain membrane integrity, preventing the risk of microcystins leakage. The SSL/PI 300 µM system could also effectively inhibit M. aeruginosa recovery for >7 days and completely degrade microcystin-LR (50.0 µg/L) within 30 min. Non-targeted metabolomic analysis suggested that the SSL/PI system inactivated M. aeruginosa mainly by interrupting the Calvin-Benson cycle, which damaged the metabolic flux of glycolysis and its downstream pathways such as the oxidative PPP pathway and glutathione metabolism. Furthermore, the activated PI system exhibited an even better algal inhibition under natural sunlight irradiation, evidenced by the seriously damaged cell membrane of M. aeruginosa. Overall, this study reported the comprehensive mechanisms of algal control and application potentials of solar/PI systems. The findings facilitated the development of emerging algicidal technology and its application in controlling environmental harmful algae.

Formation of halogenated chloroxylenols through chlorination and their photochemical activity.

Trace organic contaminants usually go through multiple treatment units in a modern water treatment train. Structural modification triggered by pretreatment (e.g., prechlorination) may influence the further transformation and fate of contaminants in downstream units. However, knowledge on this aspect is still limited. In this contribution, we investigated the chlorination of chloroxylenol (PCMX), an antimicrobial agent extensively used during COVID-19 pandemic, and the photoreactivity of its halogenated derivatives. Results indicate that chlorination of PCMX mainly proceeded through electrophilic substitution to give chlorinated products, including Cl- and 2Cl-PCMX. The presence of bromide (Br-) resulted in brominated analogues. Owing to the bathochromic and "heavy atom" effects of halogen substituents, these products show increased light absorption and photoreactivity. Toxicity evaluation suggest that these halo-derivatives have higher persistence, bioaccumulation, and toxicity (PBT) than the parent PCMX. Results of this contribution advance our understanding of the transformation of PCMX during chlorination and the photochemical activity of its halogenated derivatives in subsequent UV disinfection process or sunlit surface waters.

Unveiling the treatment-driven secondary risks of pharmaceuticals: New lessons from calcium channel blocker transformation by multiple oxidants.

The worldwide detection of numerous pharmaceuticals and their transformation products (TPs) in different environmental matrices has gained considerable concern about their potential ecological hazards. Increasing evidence suggested that calcium channel blockers (CCBs) are ubiquitous pharmaceutical pollutants in natural waters. However, their TPs, reaction pathways, and secondary risks have been limitedly known during oxidative water treatment. This study systematically assessed the TP formation and transformation mechanisms of two typical CCBs (i.e., amlodipine, AML; verapamil, VER) oxidized by ferrate(VI), permanganate, and ozone, as well as the in silico prediction on the TPs' properties. The high-resolution mass spectrometer analysis suggested a total of 16 TPs of AML and 8 TPs of VER identified for these reaction systems. Transformation of AML mainly proceeded through hydroxylation of the aromatic ring, ether bond cleavage, NH2 substitution by a hydroxyl group, and H-abstraction, while VER was oxidized via hydroxylation/opening of the aromatic ring and cleavage of the CN bond. Notably, certain TPs of both CCBs were estimated with low biodegradation, multi-endpoint toxicity, and high persistence and bioaccumulation, suggesting their severe risks to aquatic ecosystems. This study has implications for understanding the environmental behaviors, fate, and secondary risks of the globally prevalent and concerned CCBs under oxidative water treatment scenarios.

Qualitative and quantitative analysis of the effects of drinking water disinfection processes on eukaryotic microorganisms: A meta-analysis.

The risk of eukaryotic microorganisms in drinking water treatment has not received sufficient attention. As the final step in ensuring drinking water quality, the effectiveness of disinfection in inactivating eukaryotic microorganisms remains to be qualitatively and quantitatively demonstrated. In this study, we conducted a meta-analysis using a mixed effects model and bootstrapping analysis to assess the effects of the disinfection process on eukaryotic microorganisms. The results revealed significant reduction of eukaryotic microorganisms in drinking water associated with the disinfection process. The estimated logarithmic reduction rates for chlorination, ozone, and UV disinfection were 1.74, 1.82 and 2.15 log, respectively, for all eukaryotic microorganisms. Analysis of relative abundance variation of eukaryotic microorganisms also indicated certain phyla and classes exhibited tolerance and competitive advantage during disinfection. This study provides qualitatively and quantitatively analysis on the influence of drinking water disinfection processes on eukaryotic microorganisms, and highlights the persistent risk of eukaryotic microbial contamination in drinking water even after disinfection, calling for further optimization of current conventional disinfection methods.

Ferrate(VI)/Periodate System: Synergistic and Rapid Oxidation of Micropollutants via Periodate/Iodate-Modulated Fe(IV)/Fe(V) Intermediates.

The presence of organic micropollutants in water sources worldwide has created a need for the development of effective and selective oxidation methods in complex water matrices. This study is the first report of the combination of ferrate(VI) (Fe(VI)) and periodate (PI) for synergistic, rapid, and selective elimination of multiple micropollutants. This combined system was found to outperform other Fe(VI)/oxidant systems (e.g., H2O2, peroxydisulfate, and peroxymonosulfate) in rapid water decontamination. Scavenging, probing, and electron spin resonance experiments showed that high-valent Fe(IV)/Fe(V) intermediates, rather than hydroxyl radicals, superoxide radicals, singlet oxygen, and iodyl radicals, played a dominant role in the process. Further, the generation of Fe(IV)/Fe(V) was evidenced directly by the 57Fe Mössbauer spectroscopic test. Surprisingly, the reactivity of PI toward Fe(VI) is rather low (0.8223 M-1 s-1) at pH 8.0, implying that PI was not acting as an activator. Besides, as the only iodine sink of PI, iodate also played an enhanced role in micropollutant abatement by Fe(VI) oxidation. Further experiments proved that PI and/or iodate might function as the Fe(IV)/Fe(V) ligands, causing the utilization efficiency of Fe(IV)/Fe(V) intermediates for pollutant oxidation to outcompete their auto-decomposition. Finally, the oxidized products and plausible transformation pathways of three different micropollutants by single Fe(VI) and Fe(VI)/PI oxidation were characterized and elucidated. Overall, this study proposed a novel selective oxidation strategy (i.e., Fe(VI)/PI system) that could efficiently eliminate water micropollutants and clarified the unexpected interactions between PI/iodate and Fe(VI) for accelerated oxidation.

Oxidation of Pharmaceuticals by Ferrate(VI)-Amino Acid Systems: Enhancement by Proline.

The occurrence of micropollutants in water threatens public health and ecology. Removal of micropollutants such as pharmaceuticals by a green oxidant, ferrate(VI) (FeVIO42-, Fe(VI)) can be accomplished. However, electron-deficient pharmaceuticals, such as carbamazepine (CBZ) showed a low removal rate by Fe(VI). This work investigates the activation of Fe(VI) by adding nine amino acids (AA) of different functionalities to accelerate the removal of CBZ in water under mild alkaline conditions. Among the studied amino acids, proline, a cyclic AA, had the highest removal of CBZ. The accelerated effect of proline was ascribed by demonstrating the involvement of highly reactive intermediate Fe(V) species, generated by one-electron transfer by the reaction of Fe(VI) with proline (i.e., Fe(VI) + proline → Fe(V) + proline•). The degradation kinetics of CBZ by a Fe(VI)-proline system was interpreted by kinetic modeling of the reactions involved that estimated the rate of the reaction of Fe(V) with CBZ as (1.03 ± 0.21) × 106 M-1 s-1, which was several orders of magnitude greater than that of Fe(VI) of 2.25 M-1 s-1. Overall, natural compounds such as amino acids may be applied to increase the removal efficiency of recalcitrant micropollutants by Fe(VI).

Partial quaternization promoted metal-organic frameworks for efficient photocatalytic removal of chromium(VI).

A one-step strategy is applied to partially quaternize the ligand of UiO-66-NH2, and the resultant UiO-66-N(CH3)3+ showed greatly improved photocatalytic performance for Cr(VI) reduction, with the apparent reaction rate constant k increasing by 8.3 times. This strategy could be used to effectively promote the performance of other MOFs-NH2, demonstrating general applicability.

Microbiological risks increased by ammonia-oxidizing bacteria under global warming: The neglected issue in chloraminated drinking water distribution system.

A rising outbreak of waterborne diseases caused by global warming requires higher microbial stability in the drinking water distribution system (DWDS). Chloramine disinfection is gaining popularity in this context due to its good persistent stability and fewer disinfection byproducts. However, the microbiological risks may be significantly magnified by ammonia-oxidizing bacteria (AOB) in distribution systems during global warming, which is rarely noticed. Hence, this work mainly focuses on AOB to explore its impact on water quality biosafety in the context of global warming. Research indicates that global warming-induced high temperatures can directly or indirectly promote the growth of AOB, thus leading to nitrification. Further, its metabolites or cellular residues can be used as substrates for the growth of heterotrophic bacteria (e.g., waterborne pathogens). Thus, biofilm may be more persistent in the pipelines due to the presence of AOB. Breakpoint chlorination is usually applied to control such situations. However, switching between this strategy and chloramine disinfection would result in even more severe nitrification and other adverse effects. Based on the elevated microbiological risks in DWDS, the following aspects should be paid attention to in future research: (1) to understand the response of nitrifying bacteria to high temperatures and the possible association between AOB and pathogenic growth, (2) to reveal the mechanisms of AOB-mediated biofilm formation under high-temperature stress, and (3) to develop new technologies to prevent and control the occurrence of nitrification in drinking water distribution system.

Uncovering novel disinfection mechanisms of solar light/periodate system: The dominance of singlet oxygen and metabolomic insights.

Disinfection plays an essential role in waterborne pathogen control and disease prevention, especially during the COVID-19 pandemic. Catalyst-free solar light/periodate (PI) system has recently presented great potential in water disinfection, whereas the in-depth chemical and microbiological mechanisms for efficient bacterial inactivation remain unclear. Our work delineated firstly the critical role of singlet oxygen, instead of reported hydroxyl radicals and superoxide radicals, in dominating bacterial inactivation by the PI/simulated sunlight (SSL) system. Multi-evidence demonstrated the prominent disinfection performance of this system for Staphylococcus aureus in terms of culturability (> 6 logs CFU), cellular integrity, and metabolic activity. Particularly, the excellent intracellular DNA removal (> 95%) indicated that PI/SSL system may function as a selective disinfection strategy to diminish bacterial culturability without damaging the cell membrane. The PI/SSL system could also effectively inhibit bacterial regrowth for > 5 days and horizontal gene transfer between E. coli genera. Nontargeted metabolomic analysis suggested that PI/SSL system inactivated bacteria by triggering the accumulation of intracellular reactive oxygen species and the depletion of reduced glutathione. Additionally, the PI/SSL system could accomplish simultaneous micropollutant removal and bacterial inactivation, suggesting its versatility in water decontamination. Overall, this study deciphers more comprehensive antibacterial mechanisms of this environmentally friendly disinfection system, facilitating the technical development and application of the selective disinfection strategy in environmental pathogen control.

Promoting selective water decontamination via boosting activation of periodate by nanostructured Ru-supported Co3O4 catalysts.

The superior catalytic efficiency of ruthenium (Ru)-based nanocomposites in advanced oxidation processes for water decontamination has attracted accumulating attention worldwide. However, rather limited knowledge is currently available regarding their roles in activating periodate (PI), an emerging oxidant with versatile environmental applications. This study firstly delineated that Ru-supported Co3O4 (Ru/Co3O4), a typical Ru-based nanomaterial, can efficiently accomplish PI activation to eliminate multiple organic micropollutants and inactivate different pathogenic bacteria. Almost all eight micropollutants can be completely removed within 2 min of Ru/Co3O4-PI oxidation except sulfamethoxazole (SMX), which was degraded ∼70 % at 2 min with 100 % mineralization after 10 min. The excellent catalytic performance was independent of PI dosages, initial pH, and coexisting water constituents, demonstrating its prominent capability as a selective oxidation strategy. Diverse lines of evidence indicated the dominant role of single oxygen in the Ru/Co3O4-PI system, which triggered the generation of five transformation products of SMX with reduced environmental risks. Concurrently, PI was stoichiometrically converted to the eco-friendly IO3-. Additionally, Ru/Co3O4-PI system achieved 6-log inactivation of different pathogenic bacteria within 1 min, implying the feasibility of rapid water disinfection. Overall, this work demonstrated the excellent promise of Ru-based composites in PI activation for highly efficient and selective water decontamination.

Microbiological quality of roof tank water in an urban village in southeastern China.

Urban villages are unique residential neighborhoods in urban areas in China. Roof tanks are their main form of water supply, and water quality deterioration might occur in this system because of poor hygienic conditions and maintenance. In this study, water samples were seasonally collected from an urban village to investigate the influence of roof tanks as an additional water storage device on the variation in the microbial community structure and pathogenic gene markers. Water stagnation in the roof tank induced significant decreases in chlorine (p < 0.05), residual chlorine was as low as 0.02 mg/L in spring. Propidium monoazide (PMA)-qPCR revealed a one-magnitude higher level of total viable bacterial concentration in roof tank water samples (2.14 ± 1.81 × 105 gene copies/mL) than that in input water samples (3.57 ± 2.90 × 104 gene copies/mL, p < 0.05), especially in spring and summer. In addition, pathogenic fungi, Mycobacterium spp., and Legionella spp. were frequently detected in the roof tanks. Terminal users might be exposed to higher microbial risk induced by high abundance of Legionella gene marker. Spearman's rank correlation and redundancy analysis showed that residual chlorine was the driving force that promoted bacterial colonization and shaped the microbial community. It is worth noted that the sediment in the pipe will be agitated when the water supply is restored after the water outages, which can trigger an increase in turbidity and bacterial biomass. Overall, the findings provide practical suggestions for controlling microbiological health risks in roof tanks in urban villages.