Discovering Novel Organophosphorus Compounds in Wastewater Treatment Plant Effluents through Suspect Screening and Nontarget Analysis.

Limited knowledge on the structure of emerging organophosphorus compounds (OPCs) hampers our comprehensive understanding of their environmental occurrence and potential risks. Through suspect and nontarget screening, combining data-dependent acquisition, data-independent acquisition, and parallel reaction monitoring modes, we identified 60 OPCs (17 traditional and 43 emerging compounds) in effluents of 14 wastewater treatment plants (WWTPs) in Beijing and Qinghai, China. These OPCs comprise 26 organophosphate triesters, 17 organophosphate diesters, 6 organophosphonates, 7 organothiophosphate esters, and 4 other OPCs. Notably, 14 suspect OPCs were newly identified in WWTP effluents, and 16 nontarget OPCs were newly discovered in environmental matrices. Specifically, the cyclic phosphonate, (5-ethyl-2-methyl-1,3,2-dioxaphosphorinan-5-yl)methyl dimethyl phosphonate P-oxide (PMMMPn), consistently appeared in all WWTP effluents, with semiquantitative concentrations ranging from 44.4 to 282 ng/L. Its analogue, di-PMMMPn, presented in 93% of wastewater samples. Compositional differences between the WWTP effluents of two cities were mainly attributed to emerging OPCs. Hazard and ecological risk assessment underscored the substantial contribution of chlorinated organophosphate esters and organothiophosphate esters to overall risks of OPCs in WWTP effluents. This study provides the most comprehensive OPC profiles in WWTP effluents to date, highlighting the need for further research on their occurrence, fate, and risks, particularly for chlorinated OPCs.

Suspect and Nontarget Screening Reveal the Underestimated Risks of Antibiotic Transformation Products in Wastewater Treatment Plant Effluents.

Antibiotics are anthropogenic contaminants with a global presence and of deep concern in aquatic environments, while less is known about the occurrence and risks of their transformation products (TPs). Herein, we developed a comprehensive suspect and nontarget screening workflow based on high-resolution mass spectrometry to identify unknown antibiotic TPs in wastewater treatment plant effluents. We identified 211 compounds (35 parent antibiotics and 176 TPs) at confidence levels of ≥3 and 107 TPs originated from macrolides. TPs were quantified by 17 TPs standards and semiquantified by the predicted response factors and accounted for 55.6-95.1% (76.7% on average) of the total concentrations of parents and TPs. 22.2%, 63.1%, and 18.8% of the identified TPs were estimated to be more persistent, mobile, and toxic than their parent antibiotics, respectively. Further ecological risk assessment based on concentrations and toxicity to aquatic organisms revealed that the cumulative risks of TPs were generally higher than those of parents. Despite the newly formed N-oxide TPs, the tertiary treatment process (mainly ozonation) could decrease the averaged 20.3% of concentrations and 36.2% of the risks of antibiotic-related compounds. This study highlights the necessity to include antibiotic TPs in environmental scrutiny and risk assessment of antibiotics in different aquatic environments.

Wastewater treatment plant effluents exert different impacts on antibiotic resistome in water and sediment of the receiving river: Metagenomic analysis and risk assessment.

Wastewater treatment plants (WWTPs) are considered as hotspots for the spread of antibiotic resistome into the environment. However, the differential contributions of WWTPs to the antibiotic resistome in the receiving river water and sediment are poorly understood. Here, based on metagenomic analysis, we found that the WWTP effluents significantly elevated the diversities and abundances of antibiotic resistance genes (ARGs) and mobile genetic elements (MGEs) in the receiving river water from the Qinghai-Tibet Plateau, but showed less interference with the antibiotic resistome in sediment. Estimated by SourceTracker, WWTPs contributed 60.691.8% of ARGs in downstream river water, much higher than those for sediment (7.7568.0%). A holistic comparison of ARG risks based on analysis of ARG combination, mobility risk, ARG hosts and ARG-carrying pathogens further revealed the great impacts of WWTP effluents on downstream river water rather than sediment. Among various MGEs, tnpA exhibited the greatest potential for the dissemination of ARGs, and displayed highest co-occurrence frequency with multiple ARGs. P. aeruginosa, E. cloacae, and E. coli were identified as the critical-priority pathogens of ARG hosts. This study demonstrated the much greater impacts of WWTP effluents on the downstream water compared with sediment, which is significant for developing effective strategies to mitigate ARG risks.

Animal production predominantly contributes to antibiotic profiles in the Yangtze River.

Human-induced antibiotic pollution in the world's large rivers poses significant risk to riverine ecosystems, water quality, and human health. This study identified geophysical and socioeconomic factors driving antibiotic pollution in the Yangtze River by quantifying 83 target antibiotics in water and sediment samples collected in its 6300-km-long reach, followed by source apportionment and statistical modeling. Total antibiotic concentrations ranged between 2.05-111 ng/L in water samples and 0.57-57.9 ng/g in sediment samples, contributed predominantly by veterinary antibiotics, sulfonamides and tetracyclines, respectively. Antibiotic compositions were clustered according to three landform regions (plateau, mountain-basin-foothill, and plains), resulting from varying animal production practices (cattle, sheep, pig, poultry, and aquaculture) in the sub-basins. Population density, animal production, total nitrogen concentration, and river water temperature are directly associated with antibiotic concentrations in the water samples. This study revealed that the species and production of food animals are key determinants of the geographic distribution pattern of antibiotics in the Yangtze River. Therefore, effective strategies to mitigate antibiotic pollution in the Yangtze River should include proper management of antibiotic use and waste treatment in animal production.

Insights into the driving factors of vertical distribution of antibiotic resistance genes in long-term fertilized soils.

The prevalence of antibiotic resistance genes (ARGs) in soils has aroused wide attention. However, the influence of long-term fertilization on the distribution of ARGs in different soil layers and its dominant drivers remain largely unknown. In this study, a total of 203 ARGs were analyzed in greenhouse vegetable soils (0-100 cm from a 13-year field experiment applied with different fertilizers (control, chemical fertilizer, organic manure, and mixed fertilizer). Compared with unfertilized and chemically fertilized soils, manure application significantly increased the abundance and alpha diversity of soil ARGs, where the assembly of ARG communities was strongly driven by stochastic processes. The distribution of ARGs was significantly driven by manure application within 60 cm, while it was insignificantly changed in soil below 60 cm under different fertilization regimes. The inter-correlations of ARGs with mobile genetic elements (MGEs) and microbiota were strengthened in manured soil, indicating manure application posed a higher risk for ARGs diffusion in subsurface soil. Bacteria abundance and MGEs directly influenced ARG abundance and composition, whereas soil depth and manure application indirectly influenced ARG abundance and composition by affecting antibiotics. These results strengthen our understanding of the long-term anthropogenic influence on the vertical distribution of soil ARGs and highlight the ecological risk of ARGs in subsurface soil induced by long-term manure application.

Single and combined genotoxicity of metals and fluoroquinolones to zebrafish embryos at environmentally relevant concentrations.

Fluoroquinolones (FQs) are known to have genotoxicity to aquatic organisms. However, their genotoxicity mechanisms, individually and in combination with heavy metals, are poorly understood. Here, we investigated the single and joint genotoxicity of FQs, ciprofloxacin (CIP) and enrofloxacin (ENR), and metals (Cd and Cu) at environmentally relevant concentrations (0.2 µM) to zebrafish embryos. We found that FQs or/and metals induced genotoxicity (i.e., DNA damage and cell apoptosis) to zebrafish embryos. Compared with their single exposure, the combined exposure of FQs and metals elicited less ROS overproduction but higher genotoxicity, suggesting other toxicity mechanisms may also act in addition to oxidation stress. The upregulation of nucleic acid metabolites and the dysregulation of proteins confirmed the occurrence of DNA damage and apoptosis, and further revealed the inhibition of DNA repair by Cd and binding of DNA or DNA topoisomerase by FQs. This study deepens the knowledge on the responses of zebrafish embryos to exposure of multiple pollutants, and highlights the genotoxicity of FQs and heavy metals to aquatic organisms.

Integration of target, suspect, and nontarget screening with risk modeling for per- and polyfluoroalkyl substances prioritization in surface waters.

Though thousands of per- and polyfluoroalkyl substances (PFAS) have been on the global market, most research focused on only a small fraction, potentially resulting in underestimated environmental risks. Here, we used complementary target, suspect, and nontarget screening for quantifying and identifying the target and nontarget PFAS, respectively, and developed a risk model considering their specific properties to prioritize the PFAS in surface waters. Thirty-three PFAS were identified in surface water in the Chaobai river, Beijing. The suspect and nontarget screening by Orbitrap displayed a sensitivity of > 77%, indicating its good performance in identifying the PFAS in samples. We used triple quadrupole (QqQ) under multiple-reaction monitoring for quantifying PFAS with authentic standards due to its potentially high sensitivity. To quantify the nontarget PFAS without authentic standards, we trained a random forest regression model which presented the differences up to only 2.7 times between measured and predicted response factors (RFs). The maximum/minimum RF in each PFAS class was as high as 1.2-10.0 in Orbitrap and 1.7-22.3 in QqQ. A risk-based prioritization approach was developed to rank the identified PFAS, and four PFAS (i.e., perfluorooctanoic acid, hydrogenated perfluorohexanoic acid, bistriflimide, 6:2 fluorotelomer carboxylic acid) were flagged with high priority (risk index > 0.1) for remediation and management. Our study highlighted the importance of a quantification strategy during environmental scrutiny of PFAS, especially for nontarget PFAS without standards.

Antibiotic profiles and their relationships with multitrophic aquatic communities in an urban river.

Antibiotics have garnered worldwide attention due to their omnipresence and detrimental effects on aquatic organisms, yet their potential relationships with multitrophic aquatic communities in natural rivers remain largely unknown. Here, we examined 107 antibiotics in water and sediment from an urban river in Chengdu, Sichuan province (China). The bacterial, algal, macroinvertebrates, and fish communities were synchronously measured based on the environmental DNA (eDNA) metabarcoding approach, and their relationships with antibiotics were further investigated. The results showed that the total antibiotic concentrations ranged from 1.12 to 377 ng/L and from 7.95 to 145 ng/g in water and sediment, respectively. Significant seasonal variations in the concentrations and compositions of antibiotics in water were observed. eDNA metabarcoding revealed great compositional variations of bacterial, algal, macroinvertebrates, and fish communities along the river, and antibiotics had significant negative relationships with the community diversities of aquatic organisms (p < 0.05) except for fish. Meanwhile, significant negative correlations were observed between antibiotic concentrations and the relative abundances of essential metabolism pathways of bacteria, e.g., energy metabolism (p < 0.05), carbohydrate metabolism (p < 0.05), and lipid metabolism (p < 0.01). Moreover, antibiotics demonstrated greater effects on the function of bacterial community compared with environmental variables. The findings highlight the significance of eDNA metabarcoding approach in revealing the relationships between aquatic communities and antibiotics, and call for further studies on the effects of antibiotics on multitrophic aquatic communities in natural waters.

Black carbon and humic acid alleviate the toxicity of antibiotics to a cyanobacterium Synechocystis sp.

Natural organic matters (NOMs), omnipresent in natural water, challenge the toxicity assessment of pollutants to aquatic organisms due to their complex interactions with chemicals and organisms. Here, we investigated the combined toxicity of one solid NOM (black carbon, BC) or one soluble NOM (humic acid, HA) with antibiotics, roxithromycin (RTM) or gatifloxacin (GAT), to the cyanobacterium Synechocystis sp.. The NOMs alleviated the toxicity of RTM and GAT to Synechocystis sp., and BC had greater alleviation effects than HA due to its stronger adsorption to antibiotics. Antibiotics disturbed the photosynthesis of Synechocystis sp. significantly, which were also mitigated by BC and HA. Proteomic analysis showed that BC up-regulated the pathway of ribosome and photosynthetic antenna protein. GAT down-regulated the pathways of ABC transporter and oxidative phosphorylation. RTM interfered the pathway of porphyrin and chlorophyll metabolism. Furthermore, the addition of BC reduced the number of differentially expressed proteins caused by antibiotics, corroborating its mitigation effects on the toxicity of antibiotics. The disturbance of HA on the pathway of ABC transporters inhibited the internalization of RTM, thus decreasing its toxicity. This study underscores the significance of NOMs in mediating the toxicity of organic pollutants to aquatic organisms in natural waters.

Antibiotic resistome and its driving factors in an urban river in northern China.

Urban rivers dynamically interfered by anthropogenic activities are considered as a vital reservoir of antibiotic resistance genes (ARGs). Here, a total of 198 ARGs and 12 mobile genetic elements (MGEs) were profiled in water and sediment from the Chaobai river, Beijing. The total abundances of ARGs (1.01 × 106-4.58 × 108 copies/L in water and 2.92 × 106-3.34 × 109 copies/g in sediment), which were dominated by beta-lactamase genes, exhibited significant seasonal variations (p < 0.05). Significant linear correlations between the total abundances of ARGs and MGEs were observed in both water and sediment (p < 0.01). Variance partitioning analysis disclosed that environmental variables (i.e., water temperature (WT), dissolved oxygen (DO), nutrients, metals, etc.) and antibiotics were the main contributors to the variations of ARGs and MGEs, and explained 55-80 % and 27-67 % of the total variations in ARGs and MGEs, respectively. The partial least-squares path model revealed the ARG abundances in water and sediment were affected by environmental variables and antibiotics both directly and indirectly but by MGEs directly. Moreover, random forest algorithm explored that WT, Ni, DO, Co, and polyether and macrolide antibiotics were the main drivers (>10 %) of ARGs dissemination in water, whereas the transposase genes of Tp614, tnpA, and IS613 were the main drivers of ARGs dissemination in both water and sediment. This study provides a comprehensive understanding of the driving factors for the ARGs dissemination in an urban river, which is of great significance for risk management of antibiotic resistome.

Decipher the molecular descriptors and mechanisms controlling sulfonamide adsorption onto mesoporous carbon: Density functional theory calculation and partial least-squares path modeling.

Mesoporous carbons (MCs) exhibit excellent removal efficiencies to various organic chemicals. However, how the properties of chemicals influence the adsorption mechanisms and further determine their adsorption onto MCs are poorly understood. We investigated the adsorption of 22 sulfonamides (SAs) onto four MCs, and further uncovered the major molecular descriptors and adsorption mechanisms influencing the adsorption by density functional theory (DFT) and partial least-squares path modeling (PLS-PM). The results revealed that the excess molar refraction (E), McGowan's molar volume (V), energy of the highest occupied molecular orbital (EHOMO), hardness (H), and most positive net charge on carbon atom (Qc+) were identified as the indirect factors affecting the distribution coefficient (logKD), by influencing the BE(π-π), BE(H), and logKow. BE(π-π) and logKow displayed significant direct impacts on logKD (p < 0.05), while BE(H) showed insignificant direct influences on logKD (p > 0.05). The PLS-PM results indicate the main driving forces for SAs adsorption including π-π interactions, hydrophobic effects, and hydrogen bonding. This study provides a new perspective on revealing the adsorption mechanisms, and the identified factors can be used to develop the quantitative model to further predict the adsorption of SAs onto MCs.

Occurrence, source apportionment, and pollution assessment of per- and polyfluoroalkyl substances in a river across rural and urban areas.

Forty-three novel and legacy per- and polyfluoroalkyl substances (PFASs) in water and sediments from the Chaobai River (Beijing) were quantified. The total PFASs concentrations varied from 0.04 to 31.3 ng/L in water with significant spatial but insignificant seasonal variations, and changed from 0.03 to 4.29 ng/g in sediment with insignificant spatial but significant seasonal variations. The PFASs concentrations in water from the upstream across the rural area reflected the background level due to the extremely low concentration and very few detected PFASs. The consumer products and metal plating/textile were the predominant pollution sources of PFASs in winter and summer, respectively, for both water and sediment samples. Integrating the determined baseline value, the distribution of PFASs concentrations, and the ecological risks of PFASs, three criteria were proposed, which divide the PFASs concentrations in water into four pollution levels, i.e., insignificant, low, medium, and high. According to the suggested criteria, 96.4% of the PFASs levels in upstream was insignificant pollution, which decreased to 50.4% in downstream and 50.8% in reservoirs. The PFASs in China's and world's surface waters demonstrated similar pollution patterns, with PFOA, PFOS, and PFHxA being the top 3 polluted PFASs. This study makes a small step forward the development of water quality standard for PFASs, which is of great importance for pollution control and risk management of PFASs.

Sediments alleviate the inhibition effects of antibiotics on denitrification: Functional gene, microbial community, and antibiotic resistance gene analysis.

Both antibiotics and sediments can affect the denitrification in aquatic systems. However, little is known how antibiotics influence the denitrification in the presence of sediments. Here, the effects of antibiotics (sulfamethoxazole, tetracycline and ofloxacin) on denitrification in the absence and presence of sediments were investigated. The influencing mechanisms were revealed by quantifying the denitrification functional genes (DNGs), 16S-seq of bacteria, and antibiotic resistance genes (ARGs). The results showed that the presence of antibiotics inhibited NO3-N reduction by decreasing the abundances of narG, nirK, nosZ, total DNGs, and denitrifying bacteria. However, the inhibition effect was alleviated by sediments, which promoted the growth of bacteria and decreased the selective pressure of antibiotics as the vector of bacteria and antibiotics, thus increasing the abundances of denitrifying bacteria and all the DNGs. Partial least-squares path model disclosed that antibiotics had negative effects on bacteria, ARGs and DNGs, while sediments had negative effects on ARGs but positive effects on bacteria and DNGs. The network analysis further revealed the close relation of the genera Bacillus, Acinetobacter, and Enterobacter with the ARGs and DNGs. The findings are helpful to understand the denitrification in antibiotic-polluted natural waters.

Comparison and prioritization of antibiotics in a reservoir and its inflow rivers of Beijing, China.

The occurrence of antibiotics in drinking water resources, like reservoirs, is of considerable concern due to their potential risks to ecosystem, human health, and antimicrobial resistance development. Here, we quantified 83 antibiotics in water and sediments of wet and dry seasons from the Miyun reservoir and its inflow rivers in Beijing, China. Twenty-four antibiotics were detected in water with concentrations of ND-11.6 ng/L and 19 antibiotics were observed in sediments with concentrations of ND-6.50 ng/g. Sulfonamides (SAs) were the dominated antibiotics in water in two seasons. SAs and quinolones (QNs) in wet season and macrolides (MLs) and QNs in dry season predominated in sediments. The reservoir and inflow rivers showed significant differences in antibiotic concentrations and compositions in water and sediments. As an important input source of reservoir, the river water showed significantly higher total antibiotic concentrations than those in the reservoir. In contrast, the reservoir sediments are the sink of antibiotics, and had higher total antibiotic concentrations compared with rivers. A prioritization approach based on the overall risk scores and detection frequencies of antibiotics was developed, and 3 (sulfaguanidine, anhydroerythromycin, and sulfamethoxazole) and 5 (doxycycline, sulfadiazine, clarithromycin, roxithromycin, and flumequine) antibiotics with high and moderate priority, respectively, were screened. The study provides a comprehensive insight of antibiotics in the Miyun Reservoir and its inflow rivers, and is significant for future monitoring and pollution mitigation of antibiotics.

Occurrence and risks of antibiotics in an urban river in northeastern Tibetan Plateau.

There is a dearth of information on the occurrence and risks of antibiotics in the urban rivers from plateau areas. This study investigated 83 antibiotics in water and sediments of an urban river and effluents of sewage treatment plants (E-STPs) in Xining, Qinghai (northeastern Tibetan Plateau). Fifty-three antibiotics were detected, and the concentrations of individual antibiotics varied in the range of undetected (ND)-552 ng/L in water, ND-164 ng/g in sediments, and ND-3821 ng/L in E-STPs. Seasonal differences of antibiotic concentrations were significant for water samples (p < 0.05) but insignificant for sediments (p > 0.05). In urban area, E-STP is the main source of antibiotics in the river, while runoff from manured cropland contributes partially to antibiotics in the river in the suburban area. The antibiotic compositions in water were different from those in sediments, but were similar to those in E-STPs. Notably, because of strong solar radiation and long sunshine hours in the plateau area, low levels of quinolones, which are sensitive to photolysis, were observed in river water. Moreover, norfloxacin and enrofloxacin, observed in urban river from other regions of China, were not detected in the Huangshui River water. The occurrence of ofloxacin, erythromycin, roxithromycin, clarithromycin, and trimethoprim in E-STPs may induce a possible risk to antibiotic resistance evolution. Trimethoprim, anhydroerythromycin, sulfamethoxazole, sulfapyridine, and clindamycin in river water could pose low to medium risks to aquatic organisms. Further investigation on the occurrence and distribution of antibiotic resistance genes in the Huangshui River is urgently needed.

Enrichment of antibiotics in an inland lake water.

Inland water is very susceptible to the input of pollutants. However, little is known about the occurrence of antibiotics in inland lakes. In this study, a total of 83 target antibiotics were quantified in water and sediment samples collected from the Qinghai Lake, the largest inland lake of China located on the northeast of Qinghai-Tibet plateau, and its inflowing rivers. The results showed that 27 and 25 antibiotics were detected in water and sediments, respectively, with the summed concentrations (SUM) of 1.14-17.3 ng/L and 0.72-8.31 ng/g. Compared with the input rivers, significantly higher levels of sulfonamides (SAs), quinolones (QNs), polyethers (PEs), and SUM in water samples were observed in Qinghai Lake water. The average proportions of SAs (50.9-52.7%) and QNs (22.0-28.3%) in Qinghai Lake water nearly doubled compared to those in input rivers. An enrichment factor (EF) was proposed to reveal the enrichment degree of antibiotics in Qinghai Lake compared to its input river water. Sulfaguanidine (SGD), flumequine (FLU), and nalidixic acid (NDA) were enriched in Qinghai Lake up to several ten times based on the calculated EF values, due to their persistence in such a cold saline lake. Risk assessment showed that most antibiotics except anhydrochlortetracycline (ACTC) had insignificant risks to aquatic organisms and antibiotic resistance selection in Qinghai Lake water. This study was the first to reveal the enrichment of antibiotics in Qinghai Lake water, and suggests the urgent need to investigate the possible long-term enrichment and environmental risks of antibiotics in inland lakes.

Polyfluoroalkyl substances in Danjiangkou Reservoir, China: Occurrence, composition, and source appointment.

Legacy polyfluoroalkyl substances (PFASs) have been widely detected in various environmental matrices, which has caused great public concern. This study investigated the concentration, composition, partitioning, source apportionment, estimated daily intake (EDI), and ecological risks of 18 PFASs in water and sediments from Danjiangkou Reservoir. The total PFASs concentrations were 0.46-97.94 ng/L in water and 0.07-1.62 µg/kg in sediments. The total PFASs concentrations in water followed the order of spring > summer > winter > autumn (p < 0.05), and the PFAS compositions in water also varied among four seasons. However, no seasonal differences in the concentrations and compositions of PFASs were observed in sediments. The calculated logKoc values of perfluoroalkyl carboxylic acids (PFCAs) were dependent on carbon chain length, decreasing first from C6 to C8 and then increasing from C8 to C13 due to the combined effects of steric hindrance and hydrophobic interaction, while the logKoc values of C14 and C16 PFCAs were the lowest because of their very limited use. Principal component analysis-multiple linear regression analysis (PCA-MLRA) showed that food packaging/metal plating were the main sources of PFASs in spring, autumn, and winter, accounting for 64.8-81.9% and 50.5-76.9% of the total PFASs in water and sediments, respectively. However, in summer, 68.6% of total PFASs in water originated from leather/fabrics/textiles, and 70.0% of total PFASs in sediments were derived from textile treatment agents. The total EDI values through drinking water and dermal contact were 0.85, 0.69, 0.51, and 0.47 ng/kg bw/day for children (2-6, 7-12, and 13-17 years old) and adults, respectively, which were lower than the European Food Safety Authority's tolerable daily intake. However, the detected PFASs could pose low to medium ecological risks to daphnids and fish in spring. The study was significant for the development of effective strategies for controlling PFASs pollution in the Danjiangkou Reservoir.

Occurrence and removal of antibiotics and antibiotic resistance genes in natural and constructed riverine wetlands in Beijing, China.

Simultaneous elimination of antibiotics and antibiotic resistance genes (ARGs) is rarely investigated in full-scale riverine wetlands. Here, we compared the occurrence, abundance, and removal of 60 antibiotics and 27 ARGs in natural (Yeya Lake (YL)) and constructed (Bai River (BR)) riverine wetlands in Beijing, China. The concentrations of antibiotics in YL wetland were ND-51.9 ng/L in water and ND-37.9 ng/g in sediments. Significantly higher concentrations were found in BR wetland (ND-546 ng/L in water and ND-118 ng/g in sediments), which locates at the downstream of a reclaimed water treatment plant. The abundances of ARGs in YL and BR wetlands were up to 5.33 × 105 and 8.41 × 105 copies/mL in water, and 1.60 × 107 and 4.67 × 108 copies/g in sediments, respectively. These results suggest that wastewater greatly contributes to the elevated abundance of antibiotics and ARGs in both water and sediments. Compared to summer, higher levels of antibiotics in water were found in winter due to the higher usage, slower attenuation and the limited dilution. But higher abundances of ARGs were found in summer than in winter, in accordance with the favored microbial growth at higher temperature as denoted by copies of 16S rRNA. Compared to BR wetland, YL wetland achieved better removal of antibiotics and ΣARGs, with average removal efficiencies of 70.0% and 87.5%. Antibiotics, ARGs and environmental factors showed strong correlations in water samples from YL wetland. However, in BR wetland that receives urban wastewater effluents, no correlation between antibiotics and ARGs was found although the distribution of antibiotics was affected by aquatic environmental factors. These results indicate that subinhibitory concentrations of antibiotics may stimulate the prevalence of ARGs in natural wetlands.

A duodecennial national synthesis of antibiotics in China's major rivers and seas (2005-2016).

The occurrence of 94 antibiotics in water and sediments from seven major rivers and four seas in China during 2005-2016 was reviewed. Twelve antibiotics were most frequently detected in both water and sediment samples, including 3 sulfonamides (SAs), 2 tetracyclines (TCs), 4 fluoroquinolones (FQs), and 3 macrolides (MLs). Their median concentrations were below 100ng/L and 100ng/g in river water and sediments, respectively. The highest median concentrations were found in water (1.30-176ng/L) and sediments (0.15-110ng/g) in the Hai River, due to its larger population density, higher consumption of antibiotics, and lower water flow. The concentrations of TCs and FQs were higher in the Pearl River sediments, due to their extensive use in aquaculture. The Yangtze River showed lower median concentrations of antibiotics in both water (1.33-17.3ng/L) and sediments (0.31-14.8ng/g), resulting from its larger catchment size, and higher precipitation and water flow. The Yellow River exhibited lower median concentrations of antibiotics in sediments (0.04-9.04ng/g), probably due to low organic matter content in sediments and high suspended particle content in water. Organic carbon normalized distribution coefficients (Koc) of antibiotics were positively correlated with the octanol/water partition coefficients (Kow) of antibiotics, and the correlation for MLs with a macrocyclic lactone ring was different from that of SAs, FQs, and TCs, likely due to their much larger molecular size. Among China's major rivers, the Hai River had the highest ecotoxicological risk from antibiotics to algae, invertebrate, fish, and plant.