You-Sheng Liu

Comprehensive Evaluation of Antibiotics Emission and Fate in the River Basins of China: Source Analysis, Multimedia Modeling, and Linkage to Bacterial Resistance

Antibiotics are widely used in humans and animals, but there is a big concern about their negative impacts on ecosystem and human health after use. So far there is a lack of information on emission inventory and environmental fate of antibiotics in China. We studied national consumption, emissions, and multimedia fate of 36 frequently detected antibiotics in China by market survey, data analysis, and level III fugacity modeling tools. Based on our survey, the total usage for the 36 chemicals was 92700 tons in 2013, an estimated 54000 tons of the antibiotics was excreted by human and animals, and eventually 53800 tons of them entered into the receiving environment following various wastewater treatments. The fugacity model successfully predicted environmental concentrations (PECs) in all 58 river basins of China, which are comparable to the reported measured environmental concentrations (MECs) available in some basins. The bacterial resistance rates in the hospitals and aquatic environments were found to be related to the PECs and antibiotic usages, especially for those antibiotics used in the most recent period. This is the first comprehensive study which demonstrates an alarming usage and emission of various antibiotics in China.

Occurrence and risks of triclosan and triclocarban in the Pearl River system, South China: from source to the receiving environment.

We investigated two commonly used antimicrobial agents triclosan (TCS) and triclocarban (TCC) in the Pearl River system in China (i.e., Liuxi, Zhujiang and Shijing Rivers) and four sewage effluents during dry and wet seasons. The median values for TCS and TCC were the highest in the surface water and sediments of the Shijing River, followed by the Zhujiang River and Liuxi River. Screening level risk assessment using the risk quotient (RQ) method showed that TCS and TCC in surface water posed median risks in the Zhujiang and Liuxi Rivers (RQs: 0.28-0.62 for TCS, and 0.15-0.80 for TCC) and high risks in the Shijing River (RQs: 5.15-9.55 for TCS, and 3.32-5.83 for TCC). Higher risks (RQs: 3.63-28.47 for TCS, and 3.13-24.54 for TCC) were found in the sediments than in surface water of the Pearl River system. The four sewage effluents and Shijing River as well as other urban streams in Guangzhou metropolitan area were identified as the sources of the two compounds in the main river Zhujiang River. The mass inventories of TCS and TCC in the Pearl River system indicate that the sediments are not only an important sink but also a potential source for the two compounds in surface water.

Occurrence and a screening-level risk assessment of human pharmaceuticals in the Pearl River system, South China.

Ten nonsteroidal antiinflammatory drugs (NSAIDs), two blood lipid regulators (BLRs), and two antiepileptic drugs (AEDs) were analyzed in the Pearl River system in China (i.e., Liuxi, Zhujiang, and Shijing Rivers) and four sewage effluents during the dry and wet seasons, and the environmental risks they posed were assessed. Eight pharmaceuticals were detected in the rivers and effluents, including five NSAIDs (salicylic acid, ibuprofen, diclofenac, mefenamic acid, and naproxen), two BLRs (clofibric acid and gemfibrozil), and one AED (carbamazepine). The median concentrations for the eight pharmaceuticals ranged from 11.2 to 102 ng/L. Seasonal variations were not obvious for most pharmaceuticals in the three rivers, except for salicylic acid and clofibric acid in the Zhujiang River, and diclofenac in the Zhujiang and Shijing Rivers. However, spatially considerable variations in the concentrations were observed for the eight pharmaceuticals in all three rivers. For most of the pharmaceuticals, the effluents from the four wastewater treatment plants and Shijing River water were found to be the major discharge sources for the Zhujiang River, but with additional discharge sources from some small urban streams in the wet season. Diclofenac in the Shijing River was the only pharmaceutical that had a risk quotient (RQ) >1, indicating a high risk to aquatic organisms in the river. Although higher RQs were calculated for the mixture of the pharmaceuticals in each river, the risk rating remained the same for the three rivers with the RQ being >1 only in Shijing River.

Spatial and seasonal distribution of selected antibiotics in surface waters of the Pearl Rivers, China

The distribution and occurrence of 15 antibiotics in surface water of the Pearl River System (Liuxi River, Shijing River and Zhujiang River) and effluents of four wastewater treatment plants (WWTPs) were investigated in two sampling events representing wet season and dry season by using rapid resolution liquid chromatography–electrospray tandem mass spectrometry (RRLC-MS/MS) in positive ionization mode. Only eight antibiotics (sulfadiazine, sulfapyridine, sulfamethazine, sulfamethoxazole, trimethoprim, roxithromycin, erythromycin-H2O and norfloxacin) were detected in the water samples of the three rivers and the effluents. The detection frequencies and levels of antibiotics in the dry season were higher than those in the wet season. This could be attributed to the dilution effects in the wet season and relatively lower temperature in the dry season under which antibiotics could persist for a longer period. The levels of the detected antibiotics in different sites are generally in a decreasing order as follows: Shijing River ⩾WWTP effluent ⩾Zhujiang River ⩾ Liuxi River. Risk assessment based on the calculated risk quotients showed that only erythromycin-H2O and roxithromycin detected in the Pearl Rivers might have adverse effects on aquatic organisms.

Evaluation of triclosan and triclocarban at river basin scale using monitoring and modeling tools: implications for controlling of urban domestic sewage discharge.

Triclosan (TCS) and triclocarban (TCC) are two commonly used personal care products. They may enter into aquatic environments after consumption and pose potential risks to aquatic organisms. We investigated the occurrence and fate of TCS and TCC in five large rivers (the Liao River, Hai River, Yellow River, Zhujiang River and Dongjiang River) in China, and compared the monitoring data with the predicted results from Level III fugacity modeling. TCS and TCC were detected in the five large rivers with the detection frequencies of 100% or close to 100% in surface water and sediments of almost every river. TCS and TCC were found at concentrations of up to 478 ng/L and 338 ng/L in surface water, and up to 1329 ng/g and 2723 ng/g in sediments. Cluster analysis indicated that the sites with higher concentrations were usually located in or near urban area. Meanwhile, principal component analysis also suggested that the mass inventories of TCS and TCC in water and sediment were significantly influenced by the factors such as the total or untreated urban domestic sewage discharge at river basin scale. The concentrations and mass inventories from the fugacity modeling were found at the same order of magnitude with the measured values, suggesting that the fugacity modeling can provide a useful tool for evaluating the fate of TCS and TCC in riverine environments. Both monitoring and modeling results indicated that the majority of mass inventories of TCS and TCC were stored into sediment, which could be a potential pollution source for river water. The wide presence of TCS and TCC in these large rivers of China implies that better controlling of urban domestic sewage discharge is needed.

Biodegradation of three selected benzotriazoles under aerobic and anaerobic conditions

We examined the biodegradability of three benzotriazoles (benzotriazole: BT, 5-methylbenzotriazole: 5-TTri and 5-chlorobenzotriazole: CBT) under aerobic and anaerobic (nitrate, sulfate, and Fe (III) reducing) conditions. All three benzotriazoles were degraded by microorganisms under aerobic and anaerobic conditions. Both the biodegradation efficiency and biodegradation products were dependent on the predominant terminal electron-accepting condition. Among the redox conditions studied, the shortest biodegradation half lives for BT and 5-TTri were 114 days and 14 days, respectively, under aerobic condition. The shortest half-life for CBT was 26 days under Fe (III) reducing condition. The longest biodegradation half lives for BT and CBT were 315 days and 96 days, respectively, under sulfate reducing condition, while that of 5-TTri was 128 days under nitrate reducing condition. These results suggest that aerobic biodegradation is the dominant natural attenuation mechanism for BT and 5-TTri, while the most favorable process for CBT was anaerobic biodegradation. This study demonstrated that different predominant terminal electron-acceptors present in natural environment play a key role on the biodegradation of BT, 5-TTri and CBT, leading to specific biodegradability. This could have significant implications on in-situ biodegradation of the selected benzotriazoles in aerobic and anaerobic waters, soils and sediments.

Dissemination of antibiotic resistance genes in representative broiler feedlots environments: identification of indicator ARGs and correlations with environmental variables.

Livestock operations are known to harbor elevated levels of antibiotic resistance genes (ARGs) that may pose a threat to public health. Broiler feedlots may represent an important source of ARGs in the environment. However, the prevalence and dissemination mechanisms of various types of ARGs in the environment of broiler feedlots have not previously been identified. We examined the occurrence, abundance and variation of ARGs conferring resistance to chloramphenicols, sulfonamides and tetracyclines in the environments of two representative types of broiler feedlots (free range and indoor) by quantitative PCR, and assessed their dissemination mechanisms. The results showed the prevalence of various types of ARGs in the environmental samples of the broiler feedlots including manure/litter, soil, sediment, and water samples, with the first report of five chloramphenicol resistance genes (cmlA, floR, fexA, cfr, and fexB) in broiler feedlots. Overall, chloramphenicol resistance genes and sulfonamides sul genes were more abundant than tetracyclines tet genes. The ARG abundances in the samples from indoor boiler feedlots were generally different to the free range feedlots, suggesting the importance of feeding operations in ARG dissemination. Pearson correlation analysis showed significant correlations between ARGs and mobile genetic element genes (int1 and int2), and between the different classes of ARGs themselves, revealing the roles of horizontal gene transfer and coselection for ARG dissemination in the environment. Further regression analysis revealed that fexA, sul1 and tetW could be reliable indicator genes to surrogate anthropogenic sources of ARGs in boiler feedlots (correlations of fexA, sul1 and tetW to all ARGs: R = 0.95, 0.96 and 0.86, p < 0.01). Meanwhile, significant correlations were also identified between indicator ARGs and their corresponding antibiotics. In addition, some ARGs were significantly correlated with typical metals (e.g., Cu, Zn, and As with fexA, fexB, cfr, sul1, tetW, tetO, tetS: R = 0.52-0.71) and some environmental parameters (e.g., TOC, TN, TP, NH3-N with fexA, fexB, cfr, sul1, tetW, tetO, tetQ, tetS: R = 0.53-0.87) (p < 0.01). Further redundancy analysis demonstrated that the distribution and transportation of ARGs from the boiler feedlots to the receiving environments were correlated with environmental variables. The findings highlight the contribution of some chemicals such as antibiotics and metals to the development of ARGs in broiler feedlots environments; and the observed ARG dissemination mechanism in the broiler feedlots facilitates the development of effective mitigation measures.

Tissue-specific bioaccumulation of human and veterinary antibiotics in bile, plasma, liver and muscle tissues of wild fish from a highly urbanized region

We investigated the bioaccumulation of antibiotics in bile, plasma, liver and muscle tissues of wild fish from four rivers in the Pearl River Delta region. In total, 12 antibiotics were present in at least one type of fish tissues from nine wild fish species in the four rivers. The mean values of log bioaccumulation factors (log BAFs) for the detected antibiotics in fish bile, plasma, liver, and muscle tissues were at the range of 2.06-4.08, 1.85-3.47, 1.41-3.51, and 0.48-2.70, respectively. As the digestion tissues, fish bile, plasma, and liver showed strong bioaccumulation ability for some antibiotics, indicating a different bioaccumulation pattern from hydrophobic organic contaminants. Human health risk assessment based on potential fish consumption indicates that these antibiotics do not appear to pose an appreciable risk to human health. To the best of our knowledge, this is first report of bioaccumulation patterns of antibiotics in wild fish bile and plasma.

Discharge of swine wastes risks water quality and food safety: Antibiotics and antibiotic resistance genes from swine sources to the receiving environments.

Swine feedlots are widely considered as a potential hotspot for promoting the dissemination of antibiotic resistance genes (ARGs) in the environment. ARGs could enter the environment via discharge of animal wastes, thus resulting in contamination of soil, water, and food. We investigated the dissemination and diversification of 22 ARGs conferring resistance to sulfonamides, tetracyclines, chloramphenicols, and macrolides as well as the occurrence of 18 corresponding antibiotics from three swine feedlots to the receiving water, soil environments and vegetables. Most ARGs and antibiotics survived the on-farm waste treatment processes in the three swine farms. Elevated diversity of ARGs was observed in the receiving environments including river water and vegetable field soils when compared with respective controls. The variation of ARGs along the vertical soil profiles of vegetable fields indicated enrichment and migration of ARGs. Detection of various ARGs and antibiotic residues in vegetables fertilized by swine wastes could be of great concern to the general public. This research demonstrated the contribution of swine wastes to the occurrence and development of antibiotic resistance determinants in the receiving environments and potential risks to food safety and human health.

Contamination profiles of antibiotic resistance genes in the sediments at a catchment scale

The aim of this study was to investigate the contamination profiles of tetracycline, sulfonamide, and macrolide resistance genes, as well as integrons in sediments of Dongjiang River basin of South China by real time quantitative polymerase chain reaction. sul2 was the most abundant resistance gene, with the average concentration of 6.97×10(8) copies/g and 1.00×10(8) copies/g in the dry and wet seasons, respectively, followed by ermF, sul3, sul1, intI1, tetA, ermB, tetX, tetM, tetQ, tetO, tetW, tetS, ermC, and tetB. The abundance of intI2 gene was the lowest in the sediment samples. Significant correlations existed between the ARGs and sediment properties as well as metals (Cu and Zn) and corresponding antibiotic classes, suggesting that the contamination of ARGs is related to chemical pollution of the sediments in the river basin. Principal component analysis showed distinct groupings of the sampling sites, reflecting that human activities are the key player in the dissemination of ARGs in the catchment environment.