ABSTRACT
Visible light-driven intimately coupled photocatalysis and biodegradation (VDICPB) is an efficient technology for removing recalcitrant contaminants, but the degradation pathway on 17ß-estradiol 3-Sulfate (E2-3S) is still not clear. In this study, VDICPB based on N-doped TiO2 as a photocatalyst was established to investigate the removal and transformation of E2-3S in synthetic wastewater. VDICPB showed a satisfactory removal efficiency of 97.8 ± 0.4 %, which was much higher than that of independent photocatalysis (84.0 ± 2.2 %) or biodegradation system (71.4 ± 1.8 %). Steroid C/D-rings of E2-3S was broken in VDICPB since the transformation process reached terminal central pathway. Primary metabolites did not accumulate in VDICPB, resulting in a low expression of functional genes. E2-3S was mainly removed by cooperative interaction of photocatalysis and co-metabolism of biofilm. Photocatalysis led to deconjugation and microbes acted to mineralization. This study provides technical reference and theoretical support for the removal of new pollutants.
Subject(s)
Biodegradation, Environmental , Light , Catalysis , Water Pollutants, Chemical/metabolism , Titanium/chemistry , Estradiol/metabolism , Wastewater/chemistry , Estrogens/metabolism , Biofilms , Water Purification/methodsABSTRACT
As the key stage for purifying wastewater, elimination of emerging contaminants (ECs) is found to be fairly low in wastewater treatment plants (WWTPs). However, less knowledge is obtained regarding the transformation pathways between various chemical structures of ECs under different treatment processes. This study unveiled the transformation pathways of ECs with different structures in 15 WWTPs distributed across China by simplified network analysis (SNA) we proposed. After treatment, the molecular weight of the whole component of wastewater decreased and the hydrophilicity increased. There are significant differences in the structure of eliminated, consistent and formed pollutants. Amino acids, peptides, and analogues (AAPAs) were detected most frequently and most removable. Benzenoids were refractory. Triazoles were often produced. The high-frequency reactions in different WWTPs were similar, (de)methylation and dehydration occurred most frequently. Different biological treatment processes performed similarly, while some advanced treatment processes differed, such as a significant increase of -13.976 (2HO reaction) paired mass distances (PMDs) in the chlorine alone process. Further, the common structural transformation was uncovered. 4 anti-hypertensive drugs, including irbesartan, valsartan, olmesartan, and losartan, were identified, along with 22 transformation products (TPs) of them. OH2 and H2O PMDs occurred most frequently and in 80.81 % of the parent-transformation product pairs, the intensity of the product was higher than parent in effluents, whose risk should be considered in future assessment activity. Together our results provide a macrography perspective on the transformation processes of ECs in WWTPs. In the future, selectively adopting wastewater treatment technology according to structures is conductive for eliminating recalcitrant ECs in WWTPs.
Subject(s)
Water Pollutants, Chemical , Water Purification , Wastewater , Water Pollutants, Chemical/chemistry , Irbesartan/analysis , Losartan/analysisABSTRACT
Understanding the reaction mechanism of dissolved organic matter (DOM) during wastewater biotreatment is crucial for optimal DOM control. Here, we develop a directed paired mass distance (dPMD) method that constructs a molecular network displaying the reaction pathways of DOM. It couples direction inference and PMD analysis to extract the substrate-product relationships and delta masses of potentially paired reactants directly from sequential mass spectrometry data without formula assignment. Using this method, we analyze the influent and effluent samples from the bioprocesses of 12 wastewater treatment plants (WWTPs) and build a dPMD network to characterize the core reactome of DOM. The network shows that the first step of the transformation triggers reaction cascades that diversify the DOM, but the highly overlapped subsequent reaction pathways result in similar effluent DOM compositions across WWTPs despite varied influents. Mass changes exhibit consistent gain/loss preferences (e.g., +3.995 and -16.031) but different occurrences across WWTPs. Combined with genome-centric metatranscriptomics, we reveal the associations among dPMDs, enzymes, and microbes. Most enzymes are involved in oxygenation, (de)hydrogenation, demethylation, and hydration-related reactions but with different target substrates and expressed by various taxa, as exemplified by Proteobacteria, Actinobacteria, and Nitrospirae. Therefore, a functionally diverse community is pivotal for advanced DOM degradation.
Subject(s)
Dissolved Organic Matter , Water Purification , Wastewater , BacteriaABSTRACT
The application of deep learning (DL) models for screening environmental estrogens (EEs) for the sound management of chemicals has garnered significant attention. However, the currently available DL model for screening EEs lacks both a transparent decision-making process and effective applicability domain (AD) characterization, making the reliability of its prediction results uncertain and limiting its practical applications. To address this issue, a graph neural network (GNN) model was developed to screen EEs, achieving accuracy rates of 88.9% and 92.5% on the internal and external test sets, respectively. The decision-making process of the GNN model was explored through the network-like similarity graphs (NSGs) based on the model features (FT). We discovered that the accuracy of the predictions is dependent on the feature distribution of compounds in NSGs. An AD characterization method called ADFT was proposed, which excludes predictions falling outside of the model's prediction range, leading to a 15% improvement in the F1 score of the GNN model. The GNN model with the AD method may serve as an efficient tool for screening EEs, identifying 800 potential EEs in the Inventory of Existing Chemical Substances of China. Additionally, this study offers new insights into comprehending the decision-making process of DL models.
Subject(s)
Estrogens , Neural Networks, Computer , Reproducibility of Results , China , UncertaintyABSTRACT
Wastewater treatment plants (WWTPs) are the major sources of contaminants discharged into downstream water bodies. Profiling the contaminants in effluent of WWTPs is crucial to assess the potential eco-risks toward downstream organisms. To this end, this study investigated the contaminants in effluent of 10 WWTPs locating in 10 cities of Yangtze River delta region of China by suspected screening analysis. Further, the persistence, bioaccumulation, toxicity (PBT) and the characteristics sub-structures of PBT-like chemicals were analyzed. Totally, 704 chemicals including 155 chemical products, 31 food additives, 52 natural substances, 112 personal care products, 123 pesticides, 192 pharmaceuticals, 17 hormones and 22 others were found. The results of PBT analysis suggested that 42 chemicals (5.97% among the detected chemicals in WWTPs) were with PBT property. Among them, 31 contaminants were not reported previously. 9 characteristics sub-structures (N-methyleneisobutylamine, 1-naphthaldehyde, 2,3,3-trimethylcyclohexene, cyclohexanol, N-sec-butyl-n-propylamine, (5E)-2,6-dimethylocta-1,5-diene, 2-ethylphenol, pentadecane and 6-methoxyhexane) were found for PBT-like chemicals. The sub-structures of highly linear alkyl partially explained the significantly higher PBT score for personal care products. Present study provides fundamental information on PBT properties of contaminants in effluent of WWTPs, which will benefit to prioritize contaminants with high concerns in effluent of WWTPs.
ABSTRACT
Advanced oxidation processes based on radicals and/or non-radical catalysis are emerging as promising technologies for eliminating pharmaceuticals (PhACs) from wastewater. However, the respective contributions of different removal pathways (radicals or non-radical) for PhAC degradation still lacks quantitative investigation. Zero-valent iron and carbon nanotubes are frequently used to generate both radicals and non-radical species via the activation of persulfate (Fe0/SWCNT/PDS). Herein, the removal kinetics of 1 µM PhACs are depicted, and the corresponding synergistic mechanism of the Fe0/SWCNT/PDS process is discussed. Coupled removal pathways showed the higher degradation of PhACs than the individual pathways. Radicals quenching studies combined with electron spin resonance characterisation suggested that the radical-based removal pathway tends to attack electron-deficient organics, whereas its counterpart is more likely to work on electron-rich organics. From the perspectives of the contribution rate, the redox cycles of conjugated Fe species play a more important role in the generation of radicals than free Fe species, and the faster electron transfer in the conductive bridge offered by SWCNT is responsible for the effective corrosion of Fe0 and the decomposition of PDS. Six real wastewater samples were used to prove the generality of the above removal contribution, regardless of the wastewater samples, and the results suggested that identical attack patterns were obtained in all real wastewater samples, although coexistence matrix slightly suppressed PhAC removal. This work provides a deeper insight into the high-performance working mechanism on synergistic interactions and contaminant removal in a combined catalysis system.
Subject(s)
Nanotubes, Carbon , Water Pollutants, Chemical , Wastewater , Water Pollutants, Chemical/analysis , Iron , Oxidation-Reduction , Pharmaceutical PreparationsABSTRACT
Biotransformation of emerging contaminants (ECs) is of importance in various natural and engineered systems to eliminate the adverse effects of ECs toward organisms. In wastewater, structurally similar ECs may transform through similar reactions triggered by common enzymes. However, the transformation pattern for them was scarcely studied. To fill the research gaps, five sulfonamides were chosen as the targeted ECs with similar structure to explore the transformation pattern in wastewater biological treatment experiments at lab scale. Through molecular networking based nontarget screening, 45 transformation products (TPs) of sulfonamides were identified and 14 of them were newly found. On the basis, five specific transformation patterns were summarized for sulfonamides by transformation pathways comparing, reaction frequency analyzing and dominant TPs comparing. Results suggested that pterin-chelation and formylation (dominant transformation pathway) and acetylation, methylation and deamination reactions were commonly occurred for sulfonamides in wastewater. Among them, the role of formylation as the dominant transformation pathway for sulfonamides transformed in wastewater was firstly reported in present study. Subsequent frontier molecular orbital calculation suggested the active site of amino (N1H2-) may contribute the specific transformation pattern of sulfonamides. Present study reveals the specific transformation pattern of sulfonamides from the aspect of TPs and transformation pathways. In the future, knowledge on the specific transformation pattern can be used to regulate and enhance the removal of a class of ECs with similar structure rather than just one of ECs.
Subject(s)
Wastewater , Water Pollutants, Chemical , Sulfonamides , Sulfanilamide , Biotransformation , Water Pollutants, Chemical/chemistryABSTRACT
Removal of pharmaceuticals is essential in wastewater treatment systems due to their release and accumulation in the environment, which are raising issues for the environment and human health. A mathematical model could be used to predict pharmaceuticals removal under various operational parameters and assess the contributions of different removal pathways to pharmaceuticals removal. Here an ASM-PhACs model was established to describe pharmaceuticals removal including diclofenac (DCF), erythromycin (ERY), gemfibrozil (GEM) and carbamazepine (CBZ) removal in activated sludge system. The pharmaceuticals removal processes linked to co-metabolic biodegradation through the growth of ammonia oxidizing bacteria (AOB), metabolic biodegradation through AOB, metabolic biodegradation through heterotrophic bacteria (HB) and sludge adsorption were incorporated into activated sludge model (ASM1) framework. The kinetic equations were established for each pharmaceuticals removal process. To provide the experimental data for model calibration and validation, two sets of batch tests were designed and conducted in the laboratory scale using SBR technology. According to the batch test data and results of sensitivity analysis, the newly added parameters and some original default parameters affecting pharmaceuticals removal processes were screened and calibrated. The model could accurately simulate all the dynamics of chemical oxygen demand, nitrogen and pharmaceuticals under various conditions. To explore the effect of operational parameters on pharmaceuticals removal efficiency, the wide range of operational parameters was analyzed during model simulation. According to the simulation results, both influent NH4+-N concentration and DO were found to be the significant parameters that impact the removal of DCF, ERY and GEM. AOB biodegradation played an important role in DCF, ERY and GEM removal. The developed model framework helps to investigate the removal mechanisms and key influencing factors of pharmaceuticals removal, thus providing guidelines for reactor design, operation and optimization aiming at pharmaceuticals removal.
Subject(s)
Sewage , Water Pollutants, Chemical , Humans , Sewage/microbiology , Water Pollutants, Chemical/analysis , Biodegradation, Environmental , Heterotrophic Processes , Diclofenac/metabolism , Pharmaceutical Preparations , Waste Disposal, Fluid/methods , BioreactorsABSTRACT
Citalopram (CIT) and sertraline (SER) are highly consumed antidepressants worldwide and have been extensively detected in wastewater. Due to the incomplete mineralization, transformation products (TPs) of them can be detected in wastewater. Comparing with parent compounds, knowledge on TPs are limited. To fill these research gaps, lab-scale batch experiments, WWTPs sampling and in silico toxicity prediction were implemented to investigate the structure, occurrence and toxicity of TPs. Based on molecular networking nontarget strategy, 13 TPs of CIT and 12 TPs of SER were tentatively identified. Among them, 4 TPs from CIT and 5 TPs from SER were newly found in present study. TPs identification results compared with results obtained from previous nontarget strategies demonstrated that the excellent performances for molecular networking strategy on candidate TPs prioritizing and new TPs finding, especially for low abundance TPs. Further, transformation pathways for CIT and SER in wastewater were proposed. Newly identified TPs provided insights on defluorination, formylation and methylation for CIT and dehydrogenation, N-malonylation and N-acetoxylation for SER transformed in wastewater. Nitrile hydrolysis and N-succinylation were found to be the dominant transformation pathways for CIT and SER in wastewater, respectively. WWTPs sampling results shown the concentrations of SER and CIT ranged from 0.46 to 28.66 ng/L and 17.16 to 58.36 ng/L. In addition, 7 TPs of CIT and 2 TPs of SER found in lab-scale wastewater samples were found in WWTPs. In silico results suggested 2 TPs of CIT may be more toxic than CIT toward all three trophic levels organisms. Present study provides new insights into the transformation processes of CIT and SER in wastewater. In addition, the necessity of paying more attention on TPs was further highlighted from the aspects of toxicity for TPs of CIT and SER in effluent of WWTPs.
Subject(s)
Wastewater , Water Pollutants, Chemical , Sertraline , Citalopram/chemistry , Water Pollutants, Chemical/chemistryABSTRACT
Artificial sweeteners discharged into aquatic environments have raised concern because of their ubiquitous occurrence and potential biological effect. And some of them, such as sucralose (SUC) and acesulfame (ACE), have been identified as emerging contaminants. Wastewater treatment plants (WWTPs) are considered as important sources and sinks of artificial sweeteners discharged into the environment. In this study, the occurrence and removal of four representative artificial sweeteners in 12 WWTPs located in different provinces of China were investigated. The results showed that artificial sweeteners were detected widely in the investigated WWTPs. The median concentrations of the four target artificial sweeteners were detected in influents at levels of 0.03-3.85 µg L-1 and decreased in the order of SUC > ACE > aspartame (APM) > neotame (NTM). Additionally, the per capita mass loads of total artificial sweeteners in the WWTPs could be affected by the location of the WWTPs and were higher in southern cities than in northern cities. It was also found that there was a distinct linear correlation between the per capita mass load of ACE in influents and population density. During the treatment of WWTPs, the overall removal efficiency of artificial sweeteners ranged from -116% to 99.1%. Among the target artificial sweeteners, SUC and ACE might have potential risk to aquatic environments based on the calculation of the risk quotient. Thus, advanced treatment processes were carried to further remove SUC and ACE to reduce their long-term cumulative effect. Overall, UV/H2O2 and UV/PDS showed a better effect than granular activated carbon (GAC) adsorption in the removal of artificial sweeteners. The reaction constants of ACE by UV/H2O2 and UV/PDS were higher than those of SUC, which is related to molar extinction coefficients. Meanwhile, the adsorption ability of GAC adsorption for SUC was better than that of ACE, which is in correlation with the octanol-water partition coefficient. By comparison of removal efficiency, UV/PDS was considered as the most suitable advanced treatment process to remove ACE and SUC.
Subject(s)
Water Pollutants, Chemical , Water Purification , Sweetening Agents/analysis , Wastewater , Hydrogen Peroxide , Water Pollutants, Chemical/analysis , China , Water Purification/methodsABSTRACT
Progesterone (P4) and norgestrel (NGT) are two steroid progestogens that can pose adverse effects on aquatic organisms at ng/L levels. Despite increasing concern on their occurrence and removal in wastewater, their fate in the wastewater treatment process has not been well documented. This study identified the transformation products (TPs) of P4 and NGT in anaerobic/anoxic/oxic (A/A/O) process. Potential functional genes involved in biotransformation of P4 and NGT were explored. The elimination or formation behavior of P4, NGT and convinced TPs along various units of A/A/O process was revealed through the mass flow. Results showed that 12 and 13 TPs were identified in the P4 and NGT groups respectively, wherein 10 identical TPs and C-19 structures transformation pathways were observed in both groups. Six genes were found that may be involved in dehydrogenation and isomerization reactions in the pathways. Mass flow indicated that P4 and NGT were mainly eliminated in anaerobic and anoxic units, while convinced TPs mainly formed in anaerobic and anoxic units and were then eliminated in aerobic unit. Further, the ecological risks of the effluent should not be ignored as residual compounds including P4 or NGT and their TPs in the effluent still posed adverse effects on zebrafish transcript levels.
Subject(s)
Norgestrel , Water Pollutants, Chemical , Animals , Progesterone/metabolism , Zebrafish/metabolism , Anaerobiosis , Water Pollutants, Chemical/analysis , Wastewater/chemistry , Biotransformation , Waste Disposal, Fluid/methodsABSTRACT
In this study, the spatiotemporal variation in the occurrence of 19 endocrine-disrupting chemicals (EDCs) spanning four seasons in wastewater treatment plants (WWTPs) located in 17 Chinese cities was investigated. Removal efficiencies for selected EDCs in 17 WWTPs over four seasons were analyzed. Contributions of conventional and advanced process segments to the removal efficiency of EDCs were explored, which compared the removal efficacies of a variety of secondary and advanced processes for EDCs. Results showed that EDCs were extensively detected in WWTPs, with bisphenol A (BPA), dehydroepiandrosterone (DHRD), androstenedione (ADD), and pregnanediol (PD) being dominant in excess sludge and wastewater. Seasonally, the greatest seasonal differences were observed in the influent, with the concentrations of 12 EDCs varying significantly between seasons. Spatially, concentrations of BPA, DHRD, testosterone (TTR), and estriol (E3) in the influent significantly varied between the northern and southern WWTPs. Fourteen EDCs were removed steadily among the four seasons, while most EDCs had considerable removal differences between WWTPs. Contribution of the conventional process segment to the removal of individual EDCs was higher than that of the advanced process segment in WWTPs. Quantitative meta-analysis indicated that the anaerobic-anoxic-anaerobic (AAO) process in the various secondary processes had the highest removal of the target EDCs. Mass balance analysis further suggested that biodegradation in the aerobic tank of the AAO process was the major pathway for most EDCs removal. This study systematically depicts the spatiotemporal distribution of EDCs in WWTPs located across China and deepens the comprehension of EDCs removal in Chinese WWTPs from a treatment process perspective.
Subject(s)
Endocrine Disruptors , Water Pollutants, Chemical , Water Purification , China , Endocrine Disruptors/analysis , Environmental Monitoring/methods , Sewage/analysis , Waste Disposal, Fluid/methods , Wastewater/analysis , Water Pollutants, Chemical/analysis , Water Purification/methodsABSTRACT
Dissolved organic matter (DOM) mediates the microbial transformation of micropollutants, including norgestrel (NGT) in natural waters. However, little is known of the effect of complex and variable wastewater-derived DOM composition on NGT degradation during wastewater treatment. In this study, the relationship between the compositions of initial DOM and NGT removal efficiencies of 17 wastewater treatment plants (WWTPs) in spring and summer were analyzed. The different molecular composition of DOM was selected in the lab to further explore its effect on NGT degradation by activated sludge. Results indicated that the DOM composition was a substantial driver of NGT removal in WWTPs. The discrepancies in the initial DOM composition contributed to the differences in the kinetics of NGT degradation by activated sludge. The larger rapid decay phase rates of NGT are usually accompanied by a large proportion of labile substances in DOM. High-throughput sequencing and ultrahigh-resolution mass spectrometry were used to further analyze the evolution of bacterial communities and DOM molecular composition were combined with network analysis to reveal the intrinsic relationship that how DOM composition affected NGT degradation by regulating core microbes. Eighty-nine core OTUs were significantly associated with NGT degradation, and 73 occurred in the rapid decay phase, implying that NGT degradation was mainly regulated by the initial composition of DOM. Nine major transformation products were identified in different groups with widely varying concentrations or relative abundances of these transformation products. This work provides valuable insights into the effects of wastewater-derived DOM composition on NGT degradation by activated sludge and innovatively explores the influence mechanisms from the bacterial community and molecular characterization perspectives.
Subject(s)
Sewage , Wastewater , Bacteria , Dissolved Organic Matter , Norgestrel , Sewage/microbiologyABSTRACT
The characteristics of dissolved organic matter (DOM) can significantly affect the degradation of target compounds by the advanced oxidation processes. In this study, the effects of the different hydrophobicity/hydrophilicity fractions, molecular weight (MW) fractions, fluorescence components and molecular components of DOM extracted from municipal wastewater on the degradation of 4 pharmaceutically active compounds (PhACs), including carbamazepine, clofibric acid, atenolol and erythromycin by the UV/H2O2 process were investigated. The results showed that the degradation rate constants of 4 PhACs decreased dramatically in the presence of DOM. The linear regressions of 4 PhACs degradation as a function of specific fluorescence intensity (SFI) are exhibited during the degradation of 4 PhACs and the SFI may be used to evaluate effect of DOM on target compounds in wastewater. The hydrophobic acid (HPO-A) exhibited the strongest inhibitory effect on degradation of 4 PhACs during oxidation process. The small MW fractions of DOM significantly inhibited the degradation of 4 PhACs during oxidation process. Among three fluorescence components, hydrophobic humic-like substances may significantly inhibit the degradation of 4 PhACs during oxidation process. At the molecular level, the formulas may be derived from terrestrial sources. CHO compound may significantly inhibit the degradation of 4 PhACs during oxidation process on formula classes. The unsaturated hydrocarbons, carbohydrates and tannins compounds may significantly inhibit the effectiveness of the UV/H2O2 process on compound classes.
Subject(s)
Dissolved Organic Matter , Wastewater , Water Pollutants, Chemical , Hydrogen Peroxide , Wastewater/chemistry , Water Pollutants, Chemical/analysisABSTRACT
This study investigated the overall occurrence and spatiotemporal variation of 19 progestogens in 608 samples collected from 17 wastewater treatment plants (WWTPs) distributed across China during four seasons. The aqueous removal efficiencies of progestogens were calculated and the efficacies of process segments, secondary and advanced processes, and process units in the removal of progestogens were explored. The results indicated that progestogens were widely detected in investigating WWTPs, with the progesterone, dydrogesterone, dienogest, ethisterone, and norethindrone were always dominant in the influent, secondary effluent, final effluent, and excess sludge. Seasonally, the influent exhibited more variability than the other matrices, that 10 progestogens concentrations varied significantly during the four seasons. Spatially, the influent concentrations of progestogens were generally higher in northern WWTPs than that in southern WWTPs during spring and summer. Eight progestogens were stably removed by the WWTPs across seasons, and most progestogens varied considerably in removal in different WWTPs. The conventional process segment was the dominant contributor to progestogen removal. The anaerobic-anoxic-oxic process and a combined process consisting of densadeg and cloth media filter and ultraviolet disinfection showed the highest removal of progestogens among various secondary and advanced treatment processes, respectively. Mass balance analysis showed that most progestogens were effectively eliminated in the aerobic unit, with biodegradation being the primary removal pathway. This study presents the first picture of the spatiotemporal dynamics of the distribution of progestogens in WWTPs of China and provides valuable information for better understanding of the occurrence and removal of progestogens in WWTPs.
Subject(s)
Water Pollutants, Chemical , Water Purification , China , Environmental Monitoring , Progestins/analysis , Sewage , Waste Disposal, Fluid , Wastewater , Water Pollutants, Chemical/analysisABSTRACT
Advanced nitrogen removal of effluent discharged from secondary treatment systems can avoid eutrophication. However, the lack of biodegradable organics limits biodenitrification. Packed bed reactors filled with carriers with different micromagnetic field (MMF) strengths were used to perform tertiary denitrification. The results showed that MMF significantly improved the denitrification performance, especially at low C/N ratios. Total nitrogen (TN) removal was increased by 4.12% with 0.6 mT MMF when C/N = 4 and increased by 7.06% and 8.06% with 0.3 mT and 0.9 mT MMFs when C/N = 3, respectively. Zooglea, Flavobacterium, and Denitratisoma contributed to the advanced denitrification performance under MMF. In addition, 0.6 mT MMF enhanced nitrogen metabolism and ABC transporter protein and two-component system activities of microorganisms under C/N = 4; 0.3 mT and 0.9 mT MMFs increased nitrogen, carbohydrate, and amino acid metabolism and ABC transporter protein activities under C/N = 3. These findings indicate that MMF has great potential for advanced denitrification from secondary effluent.
Subject(s)
Carbon , Nitrogen , Bioreactors , Denitrification , Wastewater/analysisABSTRACT
This study aimed to explore whether the "window" effect of static magnetic field (SMF) on nitrous oxide (N2O) emission from the biological nitrogen removal process at low temperature existed and reveal its biological mechanism at the gene level. Four sequencing batch reactors (SBRs) with SMFs of 0, 10, 45, and 75 mT were operated continuously for 110 days at 10 °C and the lowest N2O-Gas cumulative emission (5.50 mg N/day) and N2O conversion rate (4.28 %) in 45 mT SMF-SBR verified the existence of the "window" effect. In 45 mT SMF-SBR, nearly all enzymatic activities related to N2O reduction and corresponding functional gene abundances improved significantly. Metagenomic high-throughput sequencing analysis revealed that Alicycliphilus denitricans, Paracoccus denitrificans, Rhodopseudomonas palustris, Pseudomonas stutzeri, and Dechloromonas aromatica, as species related to N2O reduction, could be separately enriched by applying suitable SMF intensity. Gene functions annotation based on KEGG and CAZy databases indicated that SMF not only accelerated the rate of free ammonia into ammonia-oxidizing bacteria and electrons delivered to the corresponding denitrification reductases, but also enhanced the degradation of complex organic matter into smaller molecules, and thus reducing the production of N2O via nitrifier denitrification and incomplete denitrification pathways at 10 °C. These findings provided a guideline and presented a blueprint of ecophysiology for the future application of magnetic field to the reduction of N2O emission in wastewater treatment plants in the cold region.
Subject(s)
Denitrification , Nitrous Oxide , Betaproteobacteria , Bioreactors , Magnetic Fields , Nitrification , Nitrogen , Nitrous Oxide/analysis , Rhodopseudomonas , Sewage , TemperatureABSTRACT
Understanding the degradation of dissolved organic matter (DOM) is vital for optimizing DOM control. However, the microbe-mediated DOM transformation during wastewater treatment remains poorly characterized. Here, microbes and DOM along full-scale biotreatment processes were simultaneously characterized using comparative genomics and high-resolution mass spectrometry-based reactomics. Biotreatments significantly increased DOM's aromaticity and unsaturation due to the overproduced lignin and polyphenol analogs. DOM was diversified by over five times in richness, with thousands of nitrogenous and sulfur-containing compounds generated through microbe-mediated oxidoreduction, functional group transfer, and C-N and C-S bond formation. Network analysis demonstrated microbial division of labor in DOM transformation. However, their roles were determined by their functional traits rather than taxa. Specifically, network and module hubs exhibited rapid growth potentials and broad substrate affinities but were deficient in xenobiotics-metabolism-associated genes. They were mainly correlated to liable DOM consumption and its transformation to recalcitrant compounds. In contrast, connectors and peripherals were potential degraders of recalcitrant DOM but slow in growth. They showed specialized associations with fewer DOM molecules and probably fed on metabolites of hub microbes. Thus, developing technologies (e.g., carriers) to selectively enrich peripheral degraders and consequently decouple the liable and recalcitrant DOM transformation processes may advance DOM removal.
Subject(s)
Water Purification , Genomics , Mass Spectrometry , Nitrogen , Oxidation-ReductionABSTRACT
Humic acid (HA) is the main component of organic matter in effluent from wastewater treatment. The effective removal of HA is significant. In this study, a novel catalyst was prepared using a transition metal oxide as the active component and Al2O3 as a granular carrier. The mechanism of catalytic ozonation of HA under neutral pH conditions and its efficiency were investigated. Under the chosen conditions (an ozone concentration of 2.2 mg/L, 50 mg/L HA solution, catalyst dosage of 5 g/L and initial pH of 6.49), the Cu/Ce-Al2O3 bimetallic catalyst led to 54.79% TOC removal rate after 30 min; the removal rate by ozone alone was only 20.49%. The characteristics of organic compounds determined by FT-IR and GC-MS showed that organic compounds were degraded significantly by the catalytic treatment. The addition of catalysts could effectively degrade toxic intermediates and reduce the acute toxicity produced by ozonation. Humic acid substances were largely removed and transformed into biodegradable intermediates. This study proposes a new and efficient ozonation catalyst for practical applications in advanced wastewater treatment.
ABSTRACT
Wastewater treatment plants (WWTPs) are the main sources of emerging contaminants (ECs) in aquatic environment. However, the standards for limiting emerging pollutants in effluent are extremely lacking. We investigated the occurrence and removal of emerging pollutants in 16 WWTPs in China using non-target analysis. 568 substances screened out were divided into 9 kinds including 167 pharmaceuticals, 113 natural substances, 85 pesticides, 86 endogenous substances, 64 chemical raw materials, 14 personal care products, 17 food additives, 6 hormones and 16 others. And they were divided into 5 fates. Pesticides and pharmaceutical compounds seemed to be the most notable categories, the kinds detected in each sample is the largest compared with other compounds. Besides, the average removal rate of pesticides and pharmaceuticals in all WWTPs were the lowest, at 9.54% and 23.77%, respectively. Priority pollutants were screened by considering distribution of pollutants with different fates. Pollutants with the same fate especially "consistent" in different WWTPs had attracted attention. 4 potential priority pollutants including metoprolol, carbamazepine, 10, 11-dihydro-10, 11-dihydroxycarbamazepine and irbesartan were proposed. And it was found that the 4 compounds, "consistent suspects" and "consistent non-targets" had similar rankings of removal rate in 16 WWTPs, which can reflect the performance of different WWTPs.