Chang-Gui Pan

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.

Excretion masses and environmental occurrence of antibiotics in typical swine and dairy cattle farms in China

This paper evaluated the excretion masses and environmental occurrence of 11 classes of 50 antibiotics in six typical swine and dairy cattle farms in southern China. Animal feeds, wastewater and solid manure samples as well as environmental samples (soil, stream and well water) were collected in December 2010 from these farms. Twenty eight antibiotics, including tetracyclines, bacitracin, lincomycin, sulfonamides, fluoroquinolones, ceftiofur, trimethoprim, macrolides, and florfenicol, were detected in the feeds, animal wastes and receiving environments. The normalized daily excretion masses per swine and cattle were estimated to be 18.2mg/day/swine and 4.24 mg/day/cattle. Chlortetracycline (11.6 mg/day/swine), bacitracin (3.81 mg/day/swine), lincomycin (1.19 mg/day/swine) and tetracycline (1.04 mg/day/swine) were the main contributors to the normalized daily excretion masses of antibiotics per swine, while chlortetracycline (3.66 mg/day/cattle) contributed 86% of the normalized daily excretion masses of antibiotics per cattle. Based on the survey of feeds and animal wastes from the swine farms and interview with the farmers, antibiotics excreted by swine were mainly originated from the feeds, while antibiotics excreted by dairy cattle were mainly from the injection route. If we assume that the swine and cattle in China excrete the same masses of antibiotics as the selected livestock farms, the total excretion mass by swine and cattle per annum in China could reach 3,080,000 kg/year and 164,000 kg/year. Various antibiotics such as sulfonamides, tetracyclines, fluroquinolones, macrolides, trimethoprim, lincomycin and florfenicol were detected in well water, stream and field soil, suggesting that livestock farms could be an important pollution source of various antibiotics to the receiving environments.

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.

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.

Emission estimation and multimedia fate modeling of seven steroids at the river basin scale in China.

Steroids are excreted from humans and animals and discharged with wastewaters into the environment, resulting in potential adverse effects on organisms. Based on the excretion rates from different groups of humans and animals, the emissions of seven steroids (estrone (E1), 17β-estradiol (E2), estriol (E3), testosterone (T), androsterone (A), progesterone (P), and cortisol (C)) were comprehensively estimated in 58 river basins of whole China, and their multimedia fate was simulated by using a level III fugacity multimedia model. The results showed that higher emission densities for the steroids were found in the river basins of east China than in west China. This distribution was found to be generally similar to the distribution of Gross Domestic Product (GDP) across China. E3, A, and P displayed higher emission densities than the other steroids in most of the river basins. The total excretion of steroids by humans and animals in China was estimated to be 3069 t/yr. The excretion of steroids from animals was two times larger than that from humans. After various treatments, the total emission of steroids was reduced to 2486 t/yr, of which more than 80% was discharged into the water compartment. The predicted concentrations in water were within an order of magnitude of the measured concentrations available in the literature. Owing to wastewater irrigation, more steroid mass loadings in agricultural soil were found in the basins of Haihe River and Huaihe River in comparison with the other river basins. To the best of our knowledge, this is the first report on the emissions and multimedia fate of seven steroids in the river basins of China.

Bioaccumulation and risk assessment of per- and polyfluoroalkyl substances in wild freshwater fish from rivers in the Pearl River Delta region, South China.

Per- and polyfluoroalkyl substances (PFASs) are used in various industries, which results in their ubiquitous occurrence in the environment. This study determined the concentrations of eighteen PFASs in muscle and liver of nine wild freshwater fish species collected from rivers in the Pearl River Delta (PRD) region, South China, and assessed their bioaccumulation and potential health risks to local people. The results showed that eight and twelve PFASs were detected in the fish muscle and liver samples, respectively. Perfluorooctane sulfonate (PFOS) was found to be the predominant PFAS both in muscle and liver with its highest concentrations of 79ng/g wet weight (ww) in muscle and 1500ng/g ww in liver, followed by Perfluoroundecanoic acid (PFUnDA) and Perfluorotridecanoic acid (PFTrDA) with trace concentrations. The mean PFOS concentrations in fish muscle and liver tissues of the nine collected species ranged from 0.40ng/g in mud carp to 25ng/g in snakehead, and from 5.6ng/g in mud carp to 1100ng/g in snakehead, respectively. Significant positive correlations were found among PFASs both in water and fish, indicating a similar pollution source for these PFASs. In tilapia samples, PFOS concentrations showed an increasing trend with increasing length and weight, but no significant difference between genders. Bioaccumulation factors (logBAF) in fish for the PFASs were in the range from 2.1 to 5.0. The calculated hazard ratios (HR) of PFOS for all fishes were in the range of 0.05-2.8, with four out of nine species (tilapia, chub, leather catfish and snakehead) having their HR values more than 1.0. The results suggest that frequent consumption of these four fish species may pose health risks to local population.

Contamination profiles of perfluoroalkyl substances in five typical rivers of the Pearl River Delta region, South China

A survey on contamination profiles of eighteen perfluoroalkyl substances (PFASs) was performed via high performance liquid chromatography-tandem mass spectrometry for surface water and sediments from five typical rivers of the Pearl River Delta region, South China in summer and winter in 2012. The total concentrations of the PFASs in the water phase of the five rivers ranged from 0.14 to 346.72 ng L(-1). The PFAS concentrations in the water phase were correlated positively to some selected water quality parameters such as chemical oxygen demand (COD) (0.7913) and conductivity (0.5642). The monitoring results for the water samples showed significant seasonal variations, while those for the sediment samples showed no obvious seasonal variations. Among the selected 18 PFASs, perfluorooctane sulfonic acid (PFOS) was the dominant PFAS compound both in water and sediment for two seasons with its maximum concentration of 320.5 ng L(-1) in water and 11.4 ng g(-1) dry weight (dw) in sediment, followed by perfluorooctanoic acid (PFOA) with its maximum concentration of 26.48 ng L(-1) in water and 0.99 ng g(-1) dw in sediment. PFOS and PFOA were found at relatively higher concentrations in the Shima River and Danshui River than in the other three rivers (Xizhijiang River, Dongjiang River and Shahe River). The principal component analysis for the PFASs concentrations in water and sediment separated the sampling sites into two groups: rural and agricultural area, and urban and industrial area, suggesting the PFASs in the riverine environment were mainly originated from industrial and urban activities in the region.

Occurrence and dissipation of three azole biocides climbazole, clotrimazole and miconazole in biosolid-amended soils.

This study investigated the occurrence and dissipation of three azole biocides climbazole, clotrimazole and miconazole in biosolid-amended soils of the three sites (Zhejiang, Hunan and Shandong) in China following three treatments (CK: control without biosolid application; T1: one biosolid application; T2: biosolid application every year). The results showed that climbazole, clotrimazole and miconazole were present in the biosolid and biosolid-amended soils, but absent in the control soils. In the soils treated with biosolids, the concentrations of climbazole, clotrimazole and miconazole were mostly lower in the Zhejiang soils than in the Shandong or Hunan soils, suggesting that these three biocides are more readily dissipated under the flooding condition. During the one year monitoring, the concentrations of climbazole, clotrimazole and miconazole in the biosolid-applied soils showed only slight variations. The dissipation half-lives for miconazole calculated under the field conditions of Shandong site were 440 days for T1 and the half-lives for clotrimazole were 365 days for T2. The results suggested the persistence of these three biocides in the soil environments.

Typical Azole Biocides in Biosolid-Amended Soils and Plants Following Biosolid Applications

Biosolid application on agricultural land may contaminate soils with various household chemicals and personal care products. This study investigated the occurrence and dissipation of typical azole biocides climbazole, clotrimazole, and miconazole in biosolid-amended soils as well as the uptake of these biocides by plants. The field trial includes two treatment groups: old groups with biosolid application at rates of 5, 10, 20, and 40 t/ha every year within 5 years, and new groups with only one biosolid application. The results showed that climbazole, clotrimazole, and miconazole were detected in biosolid-amended soils, but not detected in control soils. These biocides were not found in the crop plants collected from the trial plots. The dissipation half-lives for climbazole, clotrimazole, and miconazole under the field conditions were 175-179, 244, and 130-248 days, respectively. High biosolid application rates and repeated biosolid applications could lead to higher persistence of the biocides in the agricultural soils. An exposure model could effectively predict the residual concentrations of climbazole and miconazole in the biosolid-amended soils of the old treatments with different biosolid application rates. Thus, the field trial demonstrated high persistence of these three biocides in the soil environments.

Persistence of antibiotic resistance genes and bacterial community changes in drinking water treatment system: From drinking water source to tap water

As emerging contaminants, antibiotic resistance genes (ARGs) have become a public concern. This study aimed to investigate the occurrence and diversity of ARGs, and variation in the composition of bacterial communities in source water, drinking water treatment plants, and tap water in the Pearl River Delta region, South China. Various ARGs were present in the different types of water. Among the 27 target ARGs, floR and sul1 dominated in source water from three large rivers in the region. Pearson correlation analysis suggested that sul1, sul2, floR, and cmlA could be potential indicators for ARGs in water samples. The total abundance of the detected ARGs in tap water was much lower than that in source water. Sand filtration and sedimentation in drinking water treatment plants could effectively remove ARGs; in contrast, granular activated carbon filtration increased the abundance of ARGs. It was found that Pseudomonas may be involved in the proliferation and dissemination of ARGs in the studied drinking water treatment system. Bacteria and ARGs were still present in tap water after treatment, though they were significantly reduced. More research is needed to optimize the water treatment process for ARG removal.