Fluorotelomer alcohols (FTOHs) are the most well-known precursors of perfluoroalkyl carboxylic acids (PFCAs), but limited information is available on their occurrence and fate in municipal wastewater treatment plants (WWTPs). The occurrence of FTOHs was investigated in influent, secondary effluent, and sludge of 12 municipal WWTPs in nine cities of China. FTOHs were detected in all WWTPs, and 8:2 FTOH was the predominant congener, with concentrations of 2.10–11.0 ng/L, 3.05–12.4 ng/L, and 0.36–1.91 ng/g dry weight in the influent, secondary effluent, and sludge, respectively. Relatively high proportions of long-chain FTOHs (C10–16) were mainly detected in sludge samples. The mass balance of FTOHs and PFCAs in one of the WWTPs with an anaerobic-anoxic-oxic process was further explored. The decrease of mass loads was observed for 4:2 FTOH (mass change percentage: 21 ± 3.3%), 8:2 FTOH (22 ± 1.5%), and 10:2 FTOH (29 ± 7.3%) through aerobic treatment, while the increase of mass loads was observed for 12 PFCAs from 18 ± 16% (perfluorononanoic acid) to 165 ± 15% (perfluorobutyric acid)), suggesting the potential biotransformation of FTOHs to PFCAs in the aerobic unit. This work provides the first report on the occurrence of FTOHs in sludge samples of municipal WWTPs and their mass balance and highlights a new emission route to environment via WWTPs.

The occurrence of antibiotic-resistant bacteria and antibiotic resistance genes (ARGs) has been intensively investigated for wastewater treatment systems treating single class of antibiotic in recent years. However, the impacts of alternately occurring antibiotics in antibiotic production wastewater on the behavior of ARGs in biological treatment systems were not well understood yet. Herein, techniques including high-capacity quantitative PCR and quantitative PCR (qPCR) were used to investigate the behavior of ARGs in an anaerobic–aerobic full-scale system. The system alternately treated three kinds of antibiotic production wastewater including ribostamycin, spiramycin and paromomycin, which referred to stages 1, 2 and 3. The aminoglycoside ARGs (52.1–79.3%) determined using high-capacity quantitative PCR were the most abundant species in all sludge samples of the three stages. The total relative abundances of macrolide–lincosamide–streptogramin (MLS) resistance genes and aminoglycoside resistance genes measured using qPCR were significantly higher (P < 0.05) in aerobic sludge than in sewage sludge. However, the comparison of ARGs acquired from three alternate stages revealed that MLS genes and the aminoglycoside ARGs did not vary significantly (P > 0.05) in both aerobic and anaerobic sludge samples. In aerobic sludge, one acetyltransferase gene (aacA4) and the other three nucleotidyltransferase genes (aadB, aadA and aadE) exhibited positive correlations with intI1 (r2 = 0.83–0.94; P < 0.05), implying the significance of horizontal transfer in their proliferation. These results and facts will be helpful to understand the abundance and distribution of ARGs from antibiotic production wastewater treatment systems.

•PAM over 2 × 107 Da was reduced to less than one-third of its original size after biological treatment.•Both aerobic and anaerobic treatment were effective in the hydrolysis of large molecular weight PAM.•Thermophilic anaerobic treatment was more efficient in degrading PAM.High molecular weight partially hydrolyzed polyacrylamide (PAM) can be bio-hydrolyzed on the amide side group, however, solid evidence regarding the biological cleavage of its main carbon chain backbone is limited. In this study, viscometry, flow field-flow fractionation multi-angle light scattering (FFF-MALS), and attenuated total reflectance-Fourier transform infrared (ATR-FTIR) analysis were used to investigate the biodegradability of PAM with a nominal molecular weight of 2 × 107 Da (Da) in two suspended aerobic (25 and 40 °C) and two upflow anaerobic blanket reactors (35 and 55 °C) operated for 470 d under a hydraulic residence time (HRT) of 2 d. Both anaerobic and aerobic biological treatment reduced the viscosity from 2.02 cp in the influent to 1.45–1.60 cp, and reduced the molecular weight of PAM using FFF-MALS from 2.17 × 107 Da to less than one-third its original size. The removals of both the amide group and carbon chain backbone in the PAM molecule were further supported by the FTIR analysis. In comparison with the other conditions, thermophilic anaerobic treatment exhibited higher efficiency for PAM biodegradation. Batch test excluded the influence of temperature on the molecular weight of PAM over the range 25–55 °C, suggesting that cleavage of the main carbon chain backbone was attributed to biological degradation. Our results suggested that high molecular weight PAM was biodegradable, but mineralization did not occur.Download high-res image (310KB)Download full-size image

•Oxytetracycline and its antibacterial potency were removed by enhanced hydrolysis.•Anaerobic treatment of oxytetracyline wastewater was improved by enhanced hydrolysis.•The generation of ARGs were significantly reduced after enhanced hydrolysis.The presence of high concentration antibiotics in wastewater can disturb the stability of biological wastewater treatment systems and promote generation of antibiotic resistance genes (ARGs) during the treatment. To solve this problem, a pilot system consisting of enhanced hydrolysis pretreatment and an up-flow anaerobic sludge bed (UASB) reactor in succession was constructed for treating oxytetracycline production wastewater, and the performance was evaluated in a pharmaceutical factory in comparison with a full-scale anaerobic system operated in parallel. After enhanced hydrolysis under conditions of pH 7 and 85 °C for 6 h, oxytetracycline production wastewater with an influent chemical oxygen demand (COD) of 11,086 ± 602 mg L−1 was directly introduced into the pilot UASB reactor. With the effective removal of oxytetracycline and its antibacterial potency (from 874 mg L−1 to less than 0.61 mg L−1 and from 900 mg L−1 to less than 0.84 mg L−1, respectively) by the enhanced hydrolysis pretreatment, an average COD removal rate of 83.2%, 78.5% and 68.9% was achieved at an organic loading rate of 3.3, 4.8 and 5.9 kg COD m−3 d−1, respectively. At the same time, the relative abundances of the total tetracycline (tet) genes and a mobile element (Class 1 integron (intI1)) in anaerobic sludge on day 96 were one order of magnitude lower than those in inoculated sludge on day 0 (P < 0.01). The reduction of ARGs was further demonstrated by metagenomic sequencing. By comparison, the full-scale anaerobic system treating oxytetracycline production wastewater with an influent COD of 3720 ± 128 mg L−1 after dilution exhibited a COD removal of 51 ± 4% at an organic loading rate (OLR) 1.2 ± 0.2 kg m−3 d−1, and a total tet gene abundance in sludge was five times higher than the pilot-scale system (P < 0.01). The above result demonstrated that enhanced hydrolysis as a pretreatment method could enable efficient anaerobic treatment of oxytetracycline production wastewater containing high concentrations of oxytetracycline with significantly lower generation of ARGs.Download high-res image (228KB)Download full-size image

•Biotransformation of N and S- containing pollutants deteriorated at pH > 8.0.•pH and NH4+–N partially shaped variation in microbial community functional genes.•Abundance of functional genes linked with biotransformation of N- and S- pollutants.•Bulkholderia, Actinomycetes, Pseudomonas and Thiobacillus were key functional taxa.•Aromatic dioxygenases were most abundant organic pollutant removal genes.Although coking wastewater is generally considered to contain high concentration of nitrogen- and sulfur-containing pollutants, the biotransformation processes of these compounds have not been well understood. Herein, a high throughput functional gene array (GeoChip 5.0) in combination with Illumina MiSeq sequencing of the 16S rRNA gene were used to identify microbial functional traits and their role in biotransformation of nitrogen- and sulfur-containing compounds in a bench-scale aerobic coking wastewater treatment system operated for 488 days. Biotransformation of nitrogen and sulfur-containing pollutants deteriorated when pH of the bioreactor was increased to >8.0, and the microbial community functional structure was significantly associated with pH (Mantels test, P < 0.05). The release of ammonia nitrogen and sulfate was correlated with both the taxonomic and functional microbial community structure (P < 0.05). Considering the abundance and correlation with the release of ammonia nitrogen and sulfate, aromatic dioxygenases (e.g. xylXY, nagG), nitrilases (e.g. nhh, nitrilase), dibenzothiophene oxidase (DbtAc), and thiocyanate hydrolase (scnABC) were important functional genes for biotransformation of nitrogen- and sulfur-containing pollutants. Functional characterization of taxa and network analysis suggested that Burkholderiales, Actinomycetales, Rhizobiales, Pseudomonadales, and Hydrogenophiliales (Thiobacillus) were key functional taxa. Variance partitioning analysis showed that pH and influent ammonia nitrogen jointly explained 25.9% and 35.5% of variation in organic pollutant degrading genes and microbial community structure, respectively. This study revealed a linkage between microbial community functional structure and the likely biotransformation of nitrogen- and sulfur-containing pollutants, along with a suitable range of pH (7.0–7.5) for stability of the biological system treating coking wastewater.Download high-res image (491KB)Download full-size image

To evaluate the potential effects of antibiotics on ammonia-oxidizing microbes, multiple tools including quantitative PCR (qPCR), 454-pyrosequencing, and a high-throughput functional gene array (GeoChip) were used to reveal the distribution of ammonia-oxidizing archaea (AOA) and archaeal amoA (Arch-amoA) genes in three wastewater treatment systems receiving spiramycin or oxytetracycline production wastewaters. The qPCR results revealed that the copy number ratios of Arch-amoA to ammonia-oxidizing bacteria (AOB) amoA genes were the highest in the spiramycin full-scale (5.30) and pilot-scale systems (1.49 × 10–1), followed by the oxytetracycline system (4.90 × 10–4), with no Arch-amoA genes detected in the control systems treating sewage or inosine production wastewater. The pyrosequencing result showed that the relative abundance of AOA affiliated with Thaumarchaeota accounted for 78.5–99.6% of total archaea in the two spiramycin systems, which was in accordance with the qPCR results. Mantel test based on GeoChip data showed that Arch-amoA gene signal intensity correlated with the presence of spiramycin (P < 0.05). Antibiotics explained 25.8% of variations in amoA functional gene structures by variance partitioning analysis. This study revealed the selection of AOA in the presence of high concentrations of spiramycin in activated sludge systems.

While antibiotic pollution has attracted considerable attention due to its potential in promoting the dissemination of antibiotic resistance genes in the environment, the antibiotic activity of their related substances has been neglected, which may underestimate the environmental impacts of antibiotic wastewater discharge. In this study, a real-time quantitative approach was established to evaluate the residual antibacterial potency of antibiotics and related substances in antibiotic production wastewater (APW) by comparing the growth of a standard bacterial strain (Staphylococcus aureus) in tested water samples with a standard reference substance (e.g. oxytetracycline). Antibiotic equivalent quantity (EQ) was used to express antibacterial potency, which made it possible to assess the contribution of each compound to the antibiotic activity in APW. The real-time quantitative method showed better repeatability (Relative Standard Deviation, RSD 1.08%) compared with the conventional fixed growth time method (RSD 5.62–11.29%). And its quantification limits ranged from 0.20 to 24.00 μg L−1, depending on the antibiotic. We applied the developed method to analyze the residual potency of water samples from four APW treatment systems, and confirmed a significant contribution from antibiotic transformation products to potent antibacterial activity. Specifically, neospiramycin, a major transformation product of spiramycin, was found to contribute 13.15–22.89% of residual potency in spiramycin production wastewater. In addition, some unknown related substances with antimicrobial activity were indicated in the effluent. This developed approach will be effective for the management of antibacterial potency discharge from antibiotic wastewater and other waste streams.

The purpose of this study was to find a better enzyme extraction reagent for the SOS/umu test to replace the conventional one (the combination of sodium dodecyl sulfate (SDS) and Z-buffer), which has the disadvantage of denaturing β-galactosidase leading to decreased measurement sensitivity. By adopting a microplate system, the performance of the umu test using BugBuster Master Mix, a commercially available enzyme extraction reagent, was compared with that using the conventional reagent for detecting the genotoxicity of known mutagens as well as environmental samples. BugBuster Master Mix was found to increase the detection sensitivities of the selected genotoxins and environmental water samples, due to the fact that it doesn’t denature β-galactosidase. The result of this study showed that BugBuster Master Mix could be a better enzyme extraction reagent for umu test.

Ten yeast strains acquired from different sources and capable of utilizing vegetable oil or related compounds (fatty acid or oleic acid) as sole carbon sources were inoculated into a sequencing batch reactor (SBR) for the treatment of high-strength vegetable oil-containing wastewater. The SBR system stably removed >89% of chemical oxygen demand (COD) and >99% of oil when fed with wastewater containing 15 g/L COD and 10 g/L oil in average. Denaturing gradient gel electrophoresis of polymerase chain reaction-amplified 26S rRNA genes showed that among the ten yeast strains, only Candida lipolytica, Candida tropicalis, and Candida halophila were dominant in the system. To elucidate the major factors affecting the selection of yeast strains in the SBR system, the three dominant strains were compared with two non-dominant strains in terms of COD removal performance, biomass yield, cell settleability, cell flocculation ability, cell emulsification ability, and surface hydrophobicity. Results showed that hydrophobicity and emulsification ability of yeast cells were the two most important factors determining the selection of yeast strains in the treatment of high-strength oil-containing wastewater.

The mechanism of arsenate (As(V)) adsorption on an Fe–Ce bimetal (hydrous) oxide (Fe–Ce) was investigated using complementary analysis techniques including extended X-ray absorption fine structure (EXAFS) and surface complexation modeling. The As K-edge EXAFS spectra showed that the second peak of Fe–Ce after As(V) adsorption was the As–Fe shell, which supported the finding that As(V) adsorption occurred mainly at the Fe surface active sites. Two As–Fe distances of 3.30 Å and 3.55 Å were observed from the EXAFS spectra of As(V) adsorbed samples at three pH levels (5.0, 7.6, and 9.0) and two initial surface loadings of 70 and 130 mg/g, which indicated that monodentate mononuclear and bidentate binuclear As surface complexes coexisted. When compared with the reported dominant species of bidentate binuclear complex for As existing on iron (hydro)oxides, the existence of Ce atoms in the bimetal oxide and the high surface loading were the likely reasons for the existence of the monodentate complex. A Charge Distribution-Multi-site Sites Complexation (CD-MUSIC) model showed that protonated monodentate (MH) and deprotonated bidentate (B) complexes preferred to exist on the Fe–Ce surface in a high surface loading range (Γ = 5.11–14.4 μmol/m2). The MH complex was shown to be dominant at pH < 8. Based on the results from EXAFS analysis and the CD-MUSIC model, the adsorptive behavior of As(V) on Fe–Ce with high surface loadings was satisfactorily interpreted and understood.

Most nonylphenol ethoxylate (NPEO)-degrading isolates have been assigned to γ-Proteobacteria, which is different from the results acquired by using molecular ecological techniques. To better understand the environmental fate of NPEOs, bacterial isolation strategy characterized by the use of gellan gum as a gelling reagent and a low concentration of target carbon source were used to isolate phylogenetically diverse NPEO-degrading bacteria from activated sludge, and the biotransformation pathways of the isolates were investigated. Eight NPEO-degrading isolates with high diversity were acquired, which were distributed among seven different genera: Pseudomonas, Sphingomonas, Sphingobium, Cupriavidus, Ralstonia, Achromobacter and Staphylococcus. The latter five genera have never been reported to be able to degrade NPEOs. Three biotransformation pathways of NPEOs were observed in the eight stains. Six strains belonging to α, β and γ classes of Proteobacteria and Firmicutes phylum degraded NPEOs by initially shortening the EO chain and then oxidizing the terminal alcohol of the shortened NPEOs to the corresponding nonylphenoxy carboxylates (NPECs), which could explain most of the reported observations for the degradation of NPEOs in environment. An isolate (NP42a) belonging to the genus Sphingomonas degraded NPEOs through a non-oxidative pathway, with nonylphenol monoethoxylate (NP1EO) as the dominant product. Another isolate (NP47a) belonging to the genus Ralstonia degraded NPEOs by oxidizing the EO chain directly without the formation of short chain products.

Decolorization of reactive brilliant red X-3B was studied by using an Fe–Ce oxide hydrate as the heterogeneous catalyst in the presence of H2O2 and UV. The decolorization rate was in the order of UV–Fe–Ce–H2O2 > UV–Fe3+–H2O2 > UV–H2O2 > UV–Fe–Ce ≥ Fe–Ce–H2O2 > Fe–Ce. Under the conditions of 34 mg l−1 H2O2, 0.500 g l−1 Fe–Ce, 36 W UV and pH 3.0, 100 mg l−1 X-3B could be decolorized at efficiency of more than 99% within 30 min. The maximum dissolved Fe during the reaction was 1 mg l−1. From the fact that the decolorization rate of the UV–Fe–Ce–H2O2 system was significantly higher than that of the UV–Fe3+–H2O2 system at Fe3+ = 1 mg l−1, it is clear that the Fe–Ce functioned mainly as an efficient heterogeneous catalyst. UV–vis, its second derivative spectra, and ion chromatography (IC) were employed to investigate the degradation pathway. Fast degradation after adsorption of X-3B is the dominant mechanism in the heterogeneous catalytic oxidation system. The first degradation step is the breaking down of azo and CN bonds, resulting in the formation of the aniline- and phenol-like compounds. Then, the breaking down of the triazine structure occurred together with the transformation of naphthalene rings to multi-substituted benzene, and the cutting off of sulphonic groups from the naphthalene rings. The last step includes further decomposition of the aniline structure and partial mineralization of X-3B.

Nonylphenol ethoxylate (NPEO)-degrading bacteria were isolated from activated sludge using an improved isolation method, and the corresponding degradation behaviours were investigated. Eight NPEO-degrading strains distributed in genera Pseudomonas, Sphingomonas, Sphingobium, Cupriavidus, Ralstonia, Achromobacter, and Staphylococcus were acquired. The latter five genera have never been reported for the degradation of NPEOs. Four degradation patterns were observed for the eight pure strains. In pattern A, NPEOs were converted to short-chain NPEOs and carboxylated products, while in pattern B, lower ethoxylated oligomers appeared. Nonylphenol monoethoxylate was the main product in pattern C, while in pattern D ethoxylated units was oxidized but not shortened. Pattern C and D have not yet been reported.

The purpose of this study was to reveal how activated sludge communities respond to influent quality and indigenous communities by treating two produced waters from different origins in a batch reactor in succession. The community shift and compositions were investigated using Polymerase Chain Reaction–denaturing gradient gel electrophoresis (PCR–DGGE) and further 16S ribosomal DNA (rDNA) clone library analysis. The abundance of targeted genes for polycyclic aromatic hydrocarbon (PAH) degradation, nahAc/phnAc and C12O/C23O, was tracked to define the metabolic ability of the in situ microbial community by Most Probable Number (MPN) PCR. The biosystem performed almost the same for treatment of both produced waters in terms of removals of chemical oxygen demand (COD) and PAHs. Sludge communities were closely associated with the respective influent bacterial communities (similarity > 60%), while one sludge clone library was dominated by the Betaproteobacteria (38%) and Bacteriodetes (30%) and the other was dominated by Gammaproteobacteria (52%). This suggested that different influent and water quality have an effect on sludge community compositions. In addition, the existence of catabolic genes in sludge was consistent with the potential for degradation of PAHs in the treatment of both produced waters.System performance is associated with abundance of catabolic genes by different community composition sourced by different influent.Download full-size image