Synergistic effects of trace sulfadiazine and corrosion scales on disinfection by-product formation in bulk water of cast iron pipe.

The effects of trace sulfadiazine (SDZ) and cast-iron corrosion scales on the disinfection by-product (DBP) formation in drinking water distribution systems (DWDSs) were investigated. The results show that under the synergistic effect of trace SDZ (10 µg/L) and magnetite (Fe3O4), higher DBP concentration occurred in the bulk water with the transmission and distribution of the drinking water. Microbial metabolism-related substances, one of the important DBP precursors, increased under the SDZ/Fe3O4 condition. It was found that Fe3O4 induced a faster microbial extracellular electron transport (EET) pathway, resulting in a higher microbial regrowth activity. On the other hand, the rate of chlorine consumption was quite high, and the enhanced microbial EET based on Fe3O4 eliminated the need for microorganisms to secrete excessive extracellular polymeric substances (EPS). More importantly, EPS could be continuously secreted due to the higher microbial activity. Finally, high reactivity between EPS and chlorine disinfectant resulted in the continuous formation of DBPs, higher chlorine consumption, and lower EPS content. Therefore, more attention should be paid to the trace antibiotics polluted water sources and cast-iron corrosion scale composition in the future. This study reveals the synergistic effects of trace antibiotics and corrosion scales on the DBP formation in DWDSs, which has important theoretical significance for the DBP control of tap water.

Synergetic effects of catalyst-surface dual-electric centers and microbes for efficient removal of ciprofloxacin in water.

Antibiotics and antibiotic resistance genes (ARGs) are still a problem in biological treatment. Herein, we propose a synergetic strategy between microbes and dual-electric centers catalysts (CCN/Cu-Al2O3/ceramsite) for Ciprofloxacin (CIP)-contained (5 mg/L) water treatment in an up-flow biological filter. CIP was cleaved into small molecules by the catalyst, bringing a 57.6% removal and reducing 10.5% ARG. The characterization results verified that a Cu-π electrostatic force occurs on the catalyst surface, forming electron-rich areas around Cu and electron-poor areas at the carbon-doped g-C3N4 (CCN) aromatic ring. Thus, the electrons of adsorbed CIP were delocalized and then captured by the adsorbed extracellular polymeric substance at the electron-rich areas. Therefore, the synergetic process weakened the stress of CIP on bacteria and reduced ARG accumulation. It also enriched more electro-active bacteria on the surface of CCN/Cu-Al2O3/ceramsite, promoting the expression of extracellular electron transfer-related genes and reconstructing the energy metabolism mode. This result provides an opportunity for refractory antibiotic treatment in the biological process.

Self-purification of actual wastewater via microbial-synergy driving of catalyst-surface microelectronic field: A pilot-scale study.

High energy consumption is impedimental for eliminating refractory organics in wastewater by current technologies. Herein, we develop an efficient self-purification process for actual non-biodegradable dyeing wastewater at pilot scale, using N-doped graphene-like (CN) complexed Cu-Al2O3 supported Al2O3 ceramics (HCLL-S8-M) fixed-bed reactor without additional input. About 36% chemical oxygen demand removal was achieved within 20 min empty bed retention time and maintained stability for almost one year. The HCLL-S8-M structure feature and its interface on microbial community structure, functions, and metabolic pathways were analyzed by density-functional theory calculation, X-ray photoelectron spectroscopy, multiomics analysis of metagenome, macrotranscriptome and macroproteome. On the surface of HCLL-S8-M, a strong microelectronic field (MEF) was formed by the electron-rich/poor area due to Cu-π interaction from the complexation between phenolic hydroxy of CN and Cu species, driving the electrons of the adsorbed dye pollutants to the microorganisms through extracellular polymeric substance and the direct transfer of extracellular electrons, causing their degradation into CO2 and intermediates, which was degraded partly via intracellular metabolism. The lower energy feeding for the microbiome produced less adenosine triphosphate, resulting in little sludge throughout reaction. The MEF from electronic polarization is greatly potential to develop low-energy wastewater treatment technology.

Trace Iron as single-electron shuttle for interdependent activation of peroxydisulfate and HSO3-/O2 enables accelerated generation of radicals.

The generation of reactive oxygen species generally requires initiators in various environmental remediation processes, which necessitates high dosage of activators and downstream treatment for eliminating the accumulation of deactivated catalysts. Herein, a coupled process was constructed using trace iron for simultaneously activating HSO3-/O2 system and peroxydisulfate (PDS) oxidation system, where the iron ions (2 mg/L) transferred single-electron from the former system to the latter due to the moderate redox potential (Fe3+/Fe2+, +0.77 V) between the potentials of SO3·-/HSO3- (+0.63 V) and PDS/SO4·- (+2.01 V). Hence, the phenol degradation quickly occurred at a first-order kinetic constant of k1=0.223 min-1 due to the accelerated generation of sulfate radical (SO4·-) and hydroxyl radical (·OH) in the process. The k1 value was almost 6-fold of that in the deoxygenated condition (0.040 min-1). Density function theory reveals that the single electron shuttle spatially separates the electron-donating activation of HSO3- and electron-accepting activation of PDS, while avoiding the "mutual-annihilation" of HSO3- and S2O82- via direct two-electron transfer. Finally, utilizing the in-situ generated electron-shuttle (dissolved iron from cast iron pipe), the HSO3-/PDS reagent could efficiently inactivate the chlorine-resistant pathogens and inhibits biofilm regrowth inside the distribution systems at regular intervals or infectious disease outbreak in a neighborhood.

[Synergistic Control of Nitrogenous Disinfection By-products and Opportunistic Pathogens in Drinking Water by Iron-Modified Quartz Sand Filtration].

The main function of quartz sand in drinking water treatment has been to remove turbidity, while the microbial effect of its solid-liquid interface has been ignored. In order to solve the limitations of control of the disinfection by-products (DBPs) and opportunistic pathogens (OPs) in common quartz sand, the common quartz sand was modified to iron sand. The maximum DBPs formation potential of typical nitrogenous disinfection by-products (N-DBPs) and carbonaceous disinfection by-products was determined using gas chromatography-ECD. Compared with those of sand, the inhibition effects of halonitromethanes, haloacetamides, and haloacetonitriles by the Fe-sand were increased by 51.51%, 43.66%, and 90.6%, respectively. In addition, the gene copy numbers of Hartmanella vermiformis, Legionella spp., Mycobacterium spp., M. avium, and Naegleria spp. were detected via quantitative qPCR, and the results indicated that the Fe-sand did have a similar significant inhibitory effect on OPs. The Fe-sand had limited ability to enhance the removal of NOM. However, the Fe-sand effectively inhibited the continuous contribution of biofilm to N-DBPs and opportunistic pathogens. The distribution of biofilms on the surface of the Fe-sand filter media was uniform, not likely to fall off, and more stable; however, the suspended biofilms in the effluent were more difficult to aggregate. In addition, the α-helix of the secondary structure in the extracellular protein disappeared in the effluent of the Fe-sand. Therefore, the whole suspended biofilm was easily penetrated by chlorine. The Fe-sand solid-liquid interface did significantly change the microbial community structure and suspended biofilm characteristics, which provides a new concept to ensure the safety of drinking water quality and plays a good theoretical supporting role in the improvement and transformation of the existing process in drinking water treatment plants.

Contribution of extracellular polymeric substances and microbial community on the safety of drinking water quality: By mean of Cu/activated carbon biofiltration.

Change in water quality was investigated with laboratory-scale ozone-biological activated carbon filters using copper-modified granular activated carbon (Cu/GAC) and unmodified granular activated carbon (GAC). In the first seven days of the experimental period, Cu/GAC removed organic matter more efficiently owing to its enhanced adsorption capacity. As the running time increased, the amount of disinfection by-products (DBPs), dissolved organic carbon, and extracellular polymeric substances (EPS) increased sharply in the effluent of the Cu/GAC filter (CCW). More importantly, the EPS suspended in the CCW exhibited weaker flocculating efficiency and hydrophobicity, causing more active chemical reactions between chlorine and EPS substances. The copper species significantly limited the microbial biomass (0.01 nmol/L adenosine triphosphate) but stimulated the secretion of significant amounts of EPS by microorganisms for self-protection. Furthermore, the microbial community in the bulk water was successfully shaped by Cu/GAC, resulting in a continuous supply of EPS-derived DBP precursors and a sharp rise in chlorine consumption in the downstream drinking water distribution. Therefore, use of modified GAC materials, similar to Cu/GAC, as carrier materials for biological activated carbon (BAC) treatment remains controversial, despite enhanced pollutant adsorption capacity. This is the first study to reveal the mechanism of BAC-modified materials for water quality stability. The study potentially contributes to a comprehensive understanding of the effects of biofilm transformation and microbial community succession on drinking water quality. These results showed that tap water safety risks could be reduced by improving BAC pretreatment in drinking water treatment plants.

Effects of cast iron pipe corrosion on nitrogenous disinfection by-products formation in drinking water distribution systems via interaction among iron particles, biofilms, and chlorine.

The effects of cast iron pipe corrosion on nitrogenous disinfection by-products formation (N-DBPs) in drinking water distribution systems (DWDSs) were investigated. The results verified that in the effluent of corroded DWDSs simulated by annular reactors with corroded cast iron coupons, typical N-DBPs, including haloacetamides, halonitromethanes, and haloacetonitriles, increased significantly compared with the influent of DWDSs. In addition, more dissolved organic carbon, adenosine triphosphate, and iron particles were simultaneously detected in the bulk water of corroded DWDSs, thereby indicating that abundant iron particles acted as a "protective umbrella" for microorganisms. Under the condition of corroded DWDSs, the extracellular polymeric substances gradually exhibited distinct characteristics, including a higher content and lower flocculation efficiency, thereby resulting in a large supply of N-DBPs precursors. Corroded cast iron pipes, equivalent to a unique microbial interface, induced completely distinct microbial community structures and metabolic functions in DWDSs, thereby enhancing the formation of N-DBPs. This is the first study to successfully reveal the interactions among iron particles, biofilms, and chlorine in DWDSs, which may help to fully understand the biofilm transformation and microbial community succession in DWDSs.

Destruction of microbial stability in drinking water distribution systems by trace phosphorus polluted water source.

The effects of trace phosphate concentrations (0, 0.3 and 0.6 mg/L) in water source were investigated on microbial stability of the drinking water distribution systems (DWDSs). Obviously, the results verified that in the effluent of DWDSs simulated by annular reactors (ARs), the total microbial biomass and the absolute concentration of opportunistic pathogens such as Legionella pneumophila, Mycobacterium avium, and Hartmanella vermiformis increased significantly with phosphate concentration increasing. Based on X-ray powder diffractometer and zeta potentials measurement, trace phosphate did change physicochemical properties of corrosion products, hence promoting microbes escape from corrosion products to bulk water to a certain extent. Stimulated by chlorine disinfectant and phosphate, the extracellular polymeric substances (EPS) from the suspended biofilms of AR-0.6 gradually exhibited superior characteristics including higher content, flocculating efficiency, hydrophobicity and tightness degree, contributing to formation of large-scale suspended biofilms with strong chlorine-resistance ability. However, the disinfection by-products concentration in DWDSs barely changed due to the balance of EPS precursors contribution and biodegradation effect, covering up the microbiological water quality risk. Therefore, more attention should be paid to the trace phosphorus polluted water source though its concentration was much lower than wastewater. This is the first study successfully revealing the influence mechanism of trace phosphate on microbial stability in DWDSs, which may help to fully understand the biofilms transformation and microbial community succession in DWDSs.

Enhancing inhibition of disinfection byproducts formation and opportunistic pathogens growth during drinking water distribution by Fe2O3/Coconut shell activated carbon.

The effects of biological activated carbon treatment using Fe2O3 modified coconut shell-based activated carbon (Fe/CAC) were investigated on the occurrence of opportunistic pathogens (OPs) and formation of disinfection by-products (DBPs) in simulated drinking water distribution systems (DWDSs) with unmodified CAC as a reference. In the effluent of annular reactor (AR) with Fe/CAC, the OPs growth and DBPs formation were inhibited greatly. Based on the differential pulse voltammetry and dehydrogenase activity tests, it was verified that extracellular electron transfer was enhanced in the attached biofilms of Fe/CAC, hence improving the microbial metabolic activity and biological removal of organic matter especially DBPs precursors. Meanwhile, the extracellular polymeric substances (EPS) on the surface of Fe/CAC exhibited stronger viscosity, higher flocculating efficiency and better mechanical stability, avoiding bacteria or small-scale biofilms falling off into the water. Consequently, the microbial biomass and EPS substances amount decreased markedly in the effluent of Fe/CAC filter. More importantly, Fe/CAC did significantly enhance the shaping role on microbial community of downstream DWDSs, continuously excluding OPs advantage and inhibiting EPS production. The weakening of EPS in DWDSs resulted in decrease of microbial chlorine-resistance ability and EPS-derived DBPs precursors supply. Therefore, the deterioration of water quality in DWDSs was inhibited greatly, sustainably maintaining the safety of tap water. Our findings indicated that optimizing biological activated carbon treatment by interface modification is a promising method for improving water quality in DWDSs.

Efficient removal of disinfection by-products precursors and inhibition of bacterial detachment by strong interaction of EPS with coconut shell activated carbon in ozone/biofiltration.

The change of water quality was investigated in pilot-scale ozone-biological activated carbon (O3-BAC) filters using an emerging coconut shell-based granular activated carbon (CAC) or traditional granular activated carbon (GAC), respectively. More dissolved organic carbon (DOC) and disinfection by-products (DBPs) precursors were removed, meanwhile, less microbes, less metabolites and smaller microbial clusters were detected in the effluent of CAC compared with GAC. Sequentially, lower DBPs formation and higher disinfection efficiency were achieved in drinking water distribution systems (DWDSs). Furthermore, it was observed that extracellular electron transfer was enhanced in the attached biofilms of CAC, hence improving the microbial metabolic activity and biological removal of DOC. The results were attributed to the strong interaction of extracellular polymeric substances (EPS) with highly graphitized CAC. In addition, CAC resulted in totally different EPS in attached biofilms with superior characteristics including stronger viscosity, higher flocculating efficiency, mechanical stability and numerous binding sites for bacterial cells. Consequently, a wide range of compact interconnected biofilms formed on the surface of CAC and exhibited certain binding effect for microbial flocs and metabolites. Therefore, CAC resulted in higher microbial metabolic activity and lower release of microbes and metabolites, which was beneficial to maintain water quality safety in downstream DWDSs.

Effect of sequential UV/free chlorine disinfection on opportunistic pathogens and microbial community structure in simulated drinking water distribution systems.

Drinking water distribution systems (DWDS) may be a "Trojan Horse" for some waterborne diseases caused by opportunistic pathogens (OPs). In this study, two simulated DWDS inoculated with groundwater were treated with chlorine (Cl2) and ultraviolet/chlorine (UV/Cl2) respectively to compare their effects on the OPs distributed in four different phases (bulk water, biofilms, corrosion products, and loose deposits) of DWDS. 16S rRNA genes sequencing and qPCR were used to profile microbial community and quantify target genes of OPs, respectively. Results showed that UV/Cl2 was more effective than single Cl2 to control the regrowth of OPs in the water with the same residual chlorine concentration. However, the OPs inhabiting the biofilms, corrosion products, and loose deposits seemed to be tolerant to UV/Cl2 and Cl2, demonstrating that OPs residing in these phases were resistant to the disinfection processes. Some significant microbial correlations between OPs and Acanthamoeba were found by Spearman correlative analysis (p < 0.05), demonstrating that the ecological interactions may exist in the DWDS. 16S rRNA genes sequencing of water samples revealed a significant different microbial community structure between UV/Cl2 and Cl2. This study may give some implications for controlling the OPs in the DWDS disinfected with UV/Cl2.

Response of microorganisms in biofilm to sulfadiazine and ciprofloxacin in drinking water distribution systems.

Effects of sulfadiazine and ciprofloxacin on microorganisms in biofilm of drinking water distribution systems (DWDSs) were studied. The results verified that the increases of 16S rRNA for total bacteria and bacterial genus Hyphomicrobium were related to the promotion of antibiotic resistance genes (ARGs) and class 1 integrons (int1) in DWDSs with sulfadiazine and ciprofloxacin. Moreover, the bacteria showed higher enzymatic activities in DWDSs with sulfadiazine and ciprofloxacin, which resulted in more production of extracellular polymeric substances (EPS). The higher contents of EPS proteins and secondary structure ß-sheet promoted bacterial aggregation and adsorption onto surface of pipelines to form biofilm. EPS can serve as a barrier for the microorganisms in biofilm. Therefore, the biofilm bacterial communities shifted and the 16S rRNA for total bacteria increased in DWDSs with antibiotics, which also drove the ARGs promotion. Furthermore, the two antibiotics exhibited stronger combined effects than that caused by sulfadiazine and ciprofloxacin alone.

O3-BAC-Cl2: A multi-barrier process controlling the regrowth of opportunistic waterborne pathogens in drinking water distribution systems.

Simulated drinking water distribution system (DWDS) treated with O3-BAC-Cl2 (ozone-biological activated carbon-chlorine) was constructed to study its effects on the regrowth of five typical opportunistic pathogens (OPs). It was found that O3-BAC-Cl2 could significantly reduce the regrowth of target OPs in the effluents of DWDS compared with Cl2 and O3-Cl2 with the same residual chlorine levels. However, the effect of O3-BAC-Cl2 on the average numbers of target OPs gene markers in the biofilms of DWDS was not apparent, suggesting that OPs in the biofilms of DWDS were tolerant to the upstream disinfection process. The quantification of target OPs in the BAC-filter column demonstrated that OPs decreased with the increase of depth, which was likely due to the organic nutrient gradient and microbial competition inside the BAC-filter. Increase in the ozone dose could further reduce the OPs at the bottom of the BAC-filter. Spearman correlation analysis demonstrated that some significant correlations existed between target microorganisms, suggesting potential microbial ecological relationships. Overall, our results demonstrated that the BAC-filter may act as a "battlefield" suppressing the OPs through microbial competition. O3-BAC-Cl2 could be an effective multi-barrier process to suppress the proliferation of OPs in the bulk water of DWDS. However, OPs protected by the biofilms of DWDS should receive further attention because OPs may be detached and released from the biofilms.

One-year survey of opportunistic premise plumbing pathogens and free-living amoebae in the tap-water of one northern city of China.

In this study, qPCR was used to quantify opportunistic premise plumbing pathogens (OPPPs) and free-living amoebae in 11 tap water samples collected over four seasons from a city in northern China. Results demonstrated that the average numbers of gene copies of Legionella spp. and Mycobacterium spp. were significantly higher than those of Aeromonas spp. (p < 0.05). Legionella spp. and Mycobacterium spp. were 100% (44/44) positively detected while P. aeruginosa and Aeromonas spp. were 79.54% (35/44) and 77.27% (34/44) positively detected. Legionella pneumophila was only detected in 4 samples (4/44), demonstrating its occasional occurrence. No Mycobacterium avium or Naegleria fowleri was detected in any of the samples. The average gene copy numbers of target OPPPs were the highest in summer, suggesting seasonal prevalence of OPPPs. Average gene copy numbers of OPPPs in the taps of low-use-frequency were higher than in taps of high-use-frequency, but the difference was not significant for some OPPPs (p > 0.05). Moderate negative correlations between the chlorine concentration and the gene copy numbers of OPPPs were observed by Spearman analysis (rs ranged from -0.311 to -0.710, p < 0.05). However, no significant correlations existed between OPPPs and AOC, BDOC, or turbidity. Moderate positive correlations were observed between the target microorganisms, especially for Acanthamoeba spp., through Spearman analysis (p < 0.05). Based on our studies, it is proposed that disinfectant concentration, season, taps with different-use frequency, OPPP species, and potential microbial correlations should be considered for control of OPPPs in tap water.

Electronic Structure Modulation of Graphitic Carbon Nitride by Oxygen Doping for Enhanced Catalytic Degradation of Organic Pollutants through Peroxymonosulfate Activation.

Oxygen-doped graphitic carbon nitride (O-CN) was fabricated via a facile thermal polymerization method using urea and oxalic acid dihydrate as the graphitic carbon nitride precursor and oxygen source, respectively. Experimental and theoretical results revealed that oxygen doping preferentially occurred on the two-coordinated nitrogen positions, which create the formation of low and high electron density areas resulting in the electronic structure modulation of O-CN. As a result, the resultant O-CN exhibits enhanced catalytic activity and excellent long-term stability for peroxymonosulfate (PMS) activation toward the degradation of organic pollutants. The O-CN with modulated electronic structure enables PMS oxidation over the electron-deficient C atoms for the generation of singlet oxygen (1O2) and PMS reduction around the electron-rich O dopants for the formation of hydroxyl radical (•OH) and sulfate radical (SO4•-), in which 1O2 is the major reactive oxygen species, contributing to the selective reactivity of the O-CN/PMS system. Our findings not only propose a novel PMS activation mechanism in terms of simultaneous PMS oxidation and reduction for the production of nonradical and radical species but also provide a valuable insight for the development of efficient metal-free catalysts through nonmetal doping toward the persulfate-based environmental cleanup.

Effects of O3/Cl2 disinfection on corrosion and opportunistic pathogens growth in drinking water distribution systems.

The effects of O3/Cl2 disinfection on corrosion and the growth of opportunistic pathogens in drinking water distribution systems were studied using annular reactors (ARs). The corrosion process and most probable number (MPN) analysis indicated that the higher content of iron-oxidizing bacteria and iron-reducing bacteria in biofilms of the AR treated with O3/Cl2 induced higher Fe3O4 formation in corrosion scales. These corrosion scales became more stable than the ones that formed in the AR treated with Cl2 alone. O3/Cl2 disinfection inhibited corrosion and iron release efficiently by changing the content of corrosion-related bacteria. Moreover, ozone disinfection inactivated or damaged the opportunistic pathogens due to its strong oxidizing properties. The damaged bacteria resulting from initial ozone treatment were inactivated by the subsequent chlorine disinfection. Compared with the AR treated with Cl2 alone, the opportunistic pathogens M. avium and L. pneumophila were not detectable in effluents of the AR treated with O3/Cl2, and decreased to (4.60±0.14) and (3.09±0.12) log10 (gene copies/g corrosion scales) in biofilms, respectively. The amoeba counts were also lower in the AR treated with O3/Cl2. Therefore, O3/Cl2 disinfection can effectively control opportunistic pathogens in effluents and biofilms of an AR used as a model for a drinking water distribution system.

A human cell panel for evaluating safe application of nano-ZrO2/polymer composite in water remediation.

Nanomaterials, such as ZrO2 nanoparticles (ZrO2 NPs), are very effective in water remediation. However, the safety issues related to nanoparticle release and toxicity to humans remain to be resolved. Here we evaluated the cytotoxicity of ZrO2 NPs and their adducts with pollutants using a human cell panel containing stomach, intestine, liver and kidney cells. We found that different pollutants or ZrO2NP/pollutant adducts targeted cells from different organs, suggesting the necessity of a cell panel to model oral exposures. The cooperation of ZrO2 NPs and pollutants was quite complex, consisting of synergistic, antagonistic, or additive effects. For example, ZrO2 NPs enhanced the cytotoxicity of Pb2+ in GES-1 cells and of Pb2+, Cd2+ in FHC cells, while alleviating the toxicity of Pb2+ and As (III) in HepG2 and Hek293 cells. Our results also indicated that even concentrations of pollutants that meet the national standard, the ZrO2 NPs concentration should be kept below 17 µg/mL to avoid ZrO2 NP/pollutant adduct synergistic toxicity.

Characterization of bacterial community and iron corrosion in drinking water distribution systems with O3-biological activated carbon treatment.

Bacterial community structure and iron corrosion were investigated for simulated drinking water distribution systems (DWDSs) composed of annular reactors incorporating three different treatments: ozone, biologically activated carbon and chlorination (O3-BAC-Cl2); ozone and chlorination (O3-Cl2); or chlorination alone (Cl2). The lowest corrosion rate and iron release, along with more Fe3O4 formation, occurred in DWDSs with O3-BAC-Cl2 compared to those without a BAC filter. It was verified that O3-BAC influenced the bacterial community greatly to promote the relative advantage of nitrate-reducing bacteria (NRB) in DWDSs. Moreover, the advantaged NRB induced active Fe(III) reduction coupled to Fe(II) oxidation, enhancing Fe3O4 formation and inhibiting corrosion. In addition, O3-BAC pretreatment could reduce high-molecular-weight fractions of dissolved organic carbon effectively to promote iron particle aggregation and inhibit further iron release. Our findings indicated that the O3-BAC treatment, besides removing organic pollutants in water, was also a good approach for controlling cast iron corrosion and iron release in DWDSs.

Effects of phosphate-enhanced ozone/biofiltration on formation of disinfection byproducts and occurrence of opportunistic pathogens in drinking water distribution systems.

The effects of ozone-biologically activated carbon (O3-BAC) treatment with various phosphate doses (0, 0.3 or 0.6 mg/L) were investigated on the formation of disinfection by-products (DBPs) and occurrence of opportunistic pathogens (OPs) in drinking water distribution systems (DWDSs) simulated by annular reactors (ARs). It was found that the lowest DBPs and the highest inactivation of OPs such as Mycobacterium spp., Mycobacterium avium, Aeromonas spp., Pseudomonas aeruginosa and Hartmanella vermiformis, occurred in the effluent of the AR with 0.6 mg/L phosphate addition. Based on the results of different characterization techniques, for the AR with 0.6 mg/L phosphate-enhanced O3-BAC treatment, dissolved organic carbon in the influent exhibited the lowest concentration and most stable fraction due to the improved biodegradation effect. Moreover, the total amount of suspended extracellular polymeric substances (EPS) in the bulk water of the AR decreased greatly, resulting in the lowest chlorine consumption and DBPs formation in the AR. In Fourier transform infrared spectra of the suspended EPS, the amide II band (1600-1500 cm-1) disappeared and the protein/polysaccharide ratio decreased remarkably, indicating the destruction of protein and a decrease in hydrophobicity. Moreover, ß-sheets and α-helices in the protein secondary structures were degraded while the random coils increased sharply as phosphate addition increased to 0.6 mg/L, inhibiting microbial aggregation and hence weakening the chlorine-resistance capability. Thus, most of the OPs in suspended biofilms were more easily inactivated by residual chlorine, resulting in the lowest OPs occurrence in the effluent of the AR. Our findings indicated that enhancing the efficiency of the BAC filter by adding phosphate is a promising method for improving water quality in DWDSs.

Sulfadiazine/ciprofloxacin promote opportunistic pathogens occurrence in bulk water of drinking water distribution systems.

Effects of sulfadiazine and ciprofloxacin on the occurrence of free-living and particle-associated opportunistic pathogens in bulk water of simulated drinking water distribution systems (DWDSs) were investigated. It was found that sulfadiazine and ciprofloxacin greatly promoted the occurrence of opportunistic pathogens including Pseudomonas aeruginosa, Legionella pneumophila, Mycobacterium avium and its broader genus Mycobacterium spp., as well as the amoebae Acanthamoeba spp. and Hartmanella vermiformis, in bulk water of DWDSs. Moreover, sulfadiazine and ciprofloxacin exhibited much stronger combined effects on the increase of these opportunistic pathogens. Based on the analysis of the antibiotic resistance genes (ARGs) and extracellular polymeric substances (EPS), it was verified that EPS production was increased by the antibiotic resistant bacteria arising from the effects of sulfadiazine/ciprofloxacin. The combined effects of sulfadiazine and ciprofloxacin induced the greatest increase of EPS production in DWDSs. Furthermore, the increased EPS with higher contents of proteins and secondary structure ß-sheet led to greater bacterial aggregation and adsorption. Meanwhile, large numbers of suspended particles were formed, increasing the chlorine-resistance capability, which was responsible for the enhancement of the particle-associated opportunistic pathogens in bulk water of DWDSs with sulfadiazine/ciprofloxacin. Therefore, sulfadiazine and ciprofloxacin promoted the occurrence of particle-associated opportunistic pathogens in bulk water of DWDSs due to the role of EPS produced by the bacteria with ARGs.