Distribution, fate and risk assessment of antibiotics in sewage treatment plants in Hong Kong, South China.

Occurrence, removal, consumption and environmental risks of sixteen antibiotics were investigated in several sewage treatment plants (STPs) featuring different treatment levels in Hong Kong, China. Cefalexin, ofloxacin and erythromycin-H(2)O were predominant with concentrations of 1020-5640, 142-7900 and 243-4740 ng/L in influent, respectively; their mass loads were comparable to levels reported in urban regions in China and were at the high end of the range reported for western countries. The target antibiotics behaved differently depending on the treatment level employed at the STPs and relatively higher removal efficiencies (>70%) were observed for cefalexin, cefotaxime, amoxicillin, sulfamethoxazole and chloramphenicol during secondary treatment. ß-lactams were especially susceptible to removal via the activated sludge process while macrolides were recalcitrant (<20%) in the dissolved phase. Two fluoroquinolones, ofloxacin (4%) and norfloxacin (52%), differed greatly in their removal efficiencies, probably because of disparities in their pK(a) values which resulted in different sorption behaviour in sludge. Overall antibiotic consumption in Hong Kong was back-calculated based on influent mass flows and compared with available prescription and usage data. This model was verified by a good approximation of 82% and 141% to the predicted consumption of total ofloxacin, but a less accurate estimate was obtained for erythromycin usage. Risk assessment indicated that algae are susceptible to the environmental concentrations of amoxicillin as well as the mixture of the nine detected antibiotics in receiving surface waters.

Human blood monitoring program in Japan: contamination and bioaccumulation of persistent organochlorines in Japanese residents.

Concentrations of persistent organochlorines (OCs)-such as polychlorinated biphenyls (PCBs), 1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (DDT) and its metabolites (DDTs), hexachlorocyclohexane isomers (HCHs), chlordane compounds (CHLs), hexachlorobenzene, and tris(4-chlorophenyl)methane [TCPMe]-were determined in plasma samples from residents of three sub-metropolitan locations in Japan (Miyako, Saku, and Tottori) for the purpose of studying the geographic variation and specific accumulation of OCs. Residue concentrations of PCBs and DDTs were the highest in samples collected in Saku (400 and 370 ng/g lipid wt, respectively) whereas samples from Miyako contained greater CHL residues (70 ng/g lipid wt) than those from the other two locations. This contamination pattern reflects the historic use of OCs in each area. For the first time, tris (4-chlorophenyl) methane (TCPMe) concentrations were detected in most of the plasma sample analyzed. Concentrations of TCPMe which ranged from <0.1 to 8.1 ng/g lipid wt eight, were lower than those previouly reported in other human tissue. Larger geographic differences in OC accumulation were observed for PCBs and CHLs, whereas DDTs and HCHs exhibited little variability. PCB concentrations in samples from Saku residents were higher than those from residents of countries in the circumpolar Arctic region but lower than those reported for some populations in the United States and Western European countries. Interestingly, CHL residue concentrations in human blood from Japan are among the highest values reported for the countries examined, suggesting continued increased exposure to CHLs of the Japanese population. Time-trend analysis of CHLs in human blood samples from Miyako (Okinawa prefecture) showed that CHL residues have decreased substantially during the last decade, indicating the effect of the official ban of CHLs in 1986 in Japan. Isomer-specific analysis of PCBs revealed lower proportions of higher chlorinated congeners such as hepta- and octachlorobiphenyls in women than in men, suggesting the possibility of preferential elimination of higher chlorinated biphenyls in women. The difference in sex-dependent accumulation of OC compounds in healthy and ill persons was suggested. To our knowledge, this is the first report on the specific accumulation of persistent QCs, including TCPMe, in human blood samples from Japan.

Contamination by persistent organic pollutants in dumping sites of Asian developing countries: implication of emerging pollution sources.

In Asian developing countries, large amounts of municipal wastes are dumped daily in open dumping sites without proper management. This practice may cause several adverse environmental consequences and increased health risk to local communities. To elucidate contamination by persistent organic pollutants (POPs)--including dichloro-diphenyl-trichloroethane and its metabolites (DDTs), hexachlorocyclohexanes (HCHs), chlordanes, hexachlorobenzene (HCB), and polychlorinated biphenyls (PCBs)--in such dumping sites, soil samples were collected from open dumping sites and respective control sites in Cambodia, India, and Vietnam from 1999 through 2001. Our results demonstrated that DDTs, PCBs, and HCHs were dominant contaminants in the dumping sites. However, the contamination pattern was not consistent, showing higher HCHs in India than in Cambodia and Vietnam. Interestingly, in all of the countries, extremely higher levels of POPs were observed in the dumping sites compared with those in the respective control sites, suggesting significant amplification of POP contamination in the dumping sites of Asian developing countries. Mean concentrations of DDTs and PCBs were 350 and 140 ng/g dry weight, respectively, in the dumping sites of Cambodia and 26 and 210 ng/g, respectively, in India. These residue levels were hundreds to thousands times higher than those in general soils, implying possible risk to human health of the local communities, especially to the rag pickers, including children who work in these sites to collect recyclable materials. Composition of DDT compounds suggested their recent use in populated areas, which in turn might have caused increased levels of DDTs in the open dumping sites. In addition, composition of HCH isomers revealed their different use pattern in different countries.

Dioxins and related compounds in human breast milk collected around open dumping sites in Asian developing countries: bovine milk as a potential source.

In this study, concentrations of dioxins and related compounds (DRCs)--such as polychlorinated dibenzo- p-dioxins, polychlorinated dibenzofurans, and coplanar polychlorinated biphenyls--were found in human breast milk from women living near dumping sites of municipal waste and reference sites in India, Cambodia, Vietnam, and the Philippines during 1999 to 2000. DRCs were detected in all human breast milk samples analyzed, demonstrating that residents in these Asian developing countries have been exposed to these contaminants. In India, the concentrations of DRCs in human breast milk from women living near the investigated dumping site were notably higher than those from women living near reference sites and from women in other Asian developing countries. Toxic equivalent quantity (TEQ) levels of DRCs were comparable with or higher than those reported in the general populations of developed countries since 1990. In contrast, levels of these contaminants in human breast milk in women from Cambodia and Vietnam were not significantly different between milk from women living near the dumping and reference sites. These results indicate that significant pollution sources for DRCs are present in Indian dumping sites and that residents there have been exposed to relatively higher levels of these contaminants. TEQ levels in human breast milk from the dumping site in India tended to decrease with an increase in the number of previous deliveries by mothers, whereas no significant relationship was observed in Cambodia, Vietnam, or the Philippines. This suggests that mothers who have been exposed to relatively high levels of DRCs transfer greater amounts of these contaminants to the first infant than later ones through breast-feeding, which in turn implies that the first children of these mothers might be at higher risk from DRCs. When the residue levels of DRCs in bovine milk collected from the Indian dumping site and reference sites were examined, TEQ levels in bovine milk from the dumping site were higher than those from reference sites. This result suggests that bovine milk is a potential source of DRCs for residents living near the dumping site in India. To our knowledge, this is the first comprehensive study on exposure to DRCs of residents living in proximity to open dumping sites of municipal waste in Asian developing countries.

Risk to breeding success of fish-eating Ardeids due to persistent organic contaminants in Hong Kong: evidence from organochlorine compounds in eggs.

Eggs of two Ardeid species, the Little Egret (Egretta garzetta) and the Black-crowned Night Heron (Nycticorax nycticorax), were collected from two egretries located in the New Territories of Hong Kong with one located near the internationally acclaimed wetland reserve, the Mai Po Marshes, and the other in a remote site (A Chau). The eggs were analysed for organochlorine (OC) compounds including the DDTs, PCBs, hexachlorocyclohexanes (HCHs) and the chlordanes (CHLs). All of the OCs under investigation were detected in the eggs of both species with significantly higher levels in the Little Egret (DDTs, 560-2200; PCBs, 270-1700; CHLs, 81-470 ng g(-1) wet weight) than the Night Heron (DDTs, 210-1200; PCBs, 85-600; CHLs 59-75 ng g(-1) wet weight). The DDTs consisted mainly of DDE with levels ranging from 85% to 95% of the total. The HCHs were at about the same levels in both species (8.4-30 ng g(-1) wet weight). All of the OCs had linear concentration probability distributions on a log-normal basis which were used to evaluate exposure associated with these compounds as part of a probabilistic risk analysis. A linear dose/response relationship for the percentage reduction in the survival of young associated with DDE in eggs was developed. This probabilistic relationship was used to establish the threshold level (1000 ng g(-1) wet weight) at which there was a significant level of reduction in the survival of young above zero and the variability in DDE concentrations at this effect level. Using a threshold level of 1000 ng g(-1), the calculated Risk Quotient (RQ) had a 12.4% probability of RQ exceeding unity with the Night Heron, and 40.9% with the Little Egret. These results indicate that the DDTs in eggs would be expected to be associated with adverse effects on the survival of young of both species, particularly the Little Egret.

Specific accumulation and elimination kinetics of tris(4-chlorophenyl)methane, tris(4-chlorophenyl)methanol, and other persistent organochlorines in humans from Japan.

We examined human adipose tissue, liver, and bile from humans in Japan to understand the contamination status, specific accumulation, and elimination of two newly identified environmental contaminants, tris(4-chlorophenyl)methane (TCPMe), tris(4-chlorophenyl)methanol (TCPMOH), and other persistent organochlorines such as polychlorinated biphenyls (PCBs), DDT and its metabolites (DDTs), hexachlorocyclohexane isomers (HCHs), hexachlorobenzene (HCB), and chlordane compounds (CHLs). TCPMe and TCPMOH concentrations in Japanese human adipose tissue were slightly higher than those reported previously, indicating widespread exposure to these compounds in humans. Elevated residues of PCBs and DDTs are found in adipose tissue and liver. Concentrations in bile strongly correlated with concentrations in adipose fat and liver, which may suggest an equilibration in adipose fat/bile and liver/bile and possible biliary excretion of persistent organochlorines in humans. Composition of the organochlorines accumulated further indicates a metabolic capacity in humans higher than that of marine mammals. We observed age-dependent accumulation for TCPMe, TCPMOH, and other organochlorines, but there were no significant gender differences. p,p'-DDE and TCPMe were estimated to have low biliary excretion rate. Elimination potential of persistent organochlorines may be related to their octanol-water partition coefficient. The relationship between excretion rate and octanol-water partition coefficient may be used to predict the biliary excretion potential of some other lipophilic organochlorines such as dioxins and dibenzofurans in humans. The presence of organochlorines in bile suggests that the hepatic excretory system plays a major role in the elimination of xenobiotics in humans. To our knowledge, this is the first study of accumulation and elimination of TCPMe and TCPMOH in humans.

Isomer-specific accumulation and toxic assessment of polychlorinated biphenyls, including coplanar congeners, in cetaceans from the North Pacific and Asian coastal waters.

To elucidate the global distribution and toxicological impacts of polychlorinated biphenyls (PCBs) on cetaceans, the present study determined the concentrations of individual PCB congeners, including toxic non-ortho (IUPAC Nos. 77, 126, 169) and mono-ortho (IUPAC Nos. 105, 118, 156) coplanar congeners, in the blubber of 10 species of adult male odontocetes collected from several locations in the North Pacific Ocean and along coastal waters of Japan, Hong Kong, the Philippines, and India during 1985-1997. Total PCB concentrations in cetaceans from temperate and cold waters were higher than those in cetaceans from tropical regions. Residue levels were found to be the highest in Fraser's dolphins collected off Kii Peninsula, Japan, and hump-backed dolphins from Hong Kong, reflecting serious marine pollution by PCBs in industrialized Asian countries. Penta- and hexa-chlorobiphenyls were the predominant PCB congeners, accounting for about 70% of the total PCBs. 2,3,7,8-Tetrachlorodibenzo-p-dioxin equivalents (TEQs) of non- and mono-ortho coplanar PCBs in the blubber of cetaceans ranged from 36 (in spinner dolphins from the Philippines) to 510 pg/g wet weight (in hump-backed dolphins from Hong Kong). Toxic evaluation of coplanar PCBs using the TEQ concept indicates an greater impact on cetaceans from mid-latitudes. Toxicity contribution of mono-ortho congener IUPAC 118 was prominent in species from high latitude oceans, such as the Bering Sea and the North Pacific, whereas non-ortho congener IUPAC 126 accounted for the highest contribution in cetaceans from lower latitude regions, such as the Philippines and India. The estimated TEQ concentrations in the blubber of some cetacean species, such as northern right whale dolphin and Pacific white-sided dolphin from the northern North Pacific, Dall's porpoise from the Japan Sea, striped dolphin off Sanriku and Fraser's dolphin off Kii Peninsula, Japan, hump-backed dolphin and finless porpoise from Hong Kong, exceeded the levels associated with immunosuppression in harbour seals.

Occurrence of Tris(4-chlorophenyl)methane, tris(4-chlorophenyl)methanol, and some other persistent organochlorines in Japanese human adipose tissue.

Tris(4-chlorophenyl)methane (TCPMe) and tris(4-chlorophenyl)methanol (TCPMOH) are among the most recently identified environmental contaminants. Despite their widespread contamination in the marine environment, human exposure to these compounds remains relatively unknown. We determined the concentrations of TCPMe, TCPMOH, and other persistent organochlorines such as polychlorinated biphenyls (PCBs), DDT and its metabolites, hexachlorocyclohexane isomers, hexachlorobenzene, and chlordane compounds (CHLs) in human adipose tissue from Japan. TCPMe and TCPMOH were detected in all of the adipose samples analyzed; the concentrations ranged from 2.5-21 and 1.1-18 ng/g lipid weight, respectively. Concentrations of TCPMe and TCPMOH in humans were less than those reported in marine mammals, suggesting the possibility of metabolism and elimination of these compounds by humans. Significant correlation between TCPMe and TCPMOH with concentrations of DDT and its metabolites in human adipose tissues suggested that exposure to DDT is the source of TCPMe and TCPMOH in humans. The age- and sex-dependent accumulation of TCPMe and TCPMOH as well as other organochlorines was less pronounced. Results for other organochlorines indicated that recent contamination status of PCBs in human samples from Japan was higher than that in developing countries, whereas DDT contamination is lower. Greater concentrations of CHLs in human adipose tissue from Japan than in those from other countries suggest that continuous monitoring of CHLs in humans in Japan is necessary. To our knowledge, this is the first study on the accumulation of TCPMe and TCPMOH in human adipose tissue.

Widespread contamination by tris(4-chlorophenyl)methane and tris(4-chlorophenyl)methanol in cetaceans from the North Pacific and Asian coastal waters.

For understanding global distribution, transport and behavior of tris(4-chlorophenyl)methane (TCPMe) and tris(4-chlorophenyl)methanol (TCPMOH), the two newly identified microcontaminants, the present study determined their concentrations and other persistent organochlorines (OCs) in the blubber of nine species of adult male cetaceans collected from various locations in the North Pacific Ocean and coastal waters of some Asian countries, during 1985-97. Concentrations of TCPMe and TCPMOH were found to be highest in northern right whale dolphins, which may be attributable to wide distribution of this species, including some heavily polluted areas such as coastal California. Elevated residue levels of TCPMe and TCPMOH were observed in both off-shore and coastal species, suggesting widespread contamination of these compounds in the marine environment. Higher contamination of TCPMe and TCPMOH was found in cetaceans from temperate and cold waters than those from tropical regions. The latitudinal distribution of TCPMe and TCPMOH in cetaceans from the North Pacific and Asian coastal waters was similar to that of DDTs, suggesting less transportable nature of TCPMe and TCPMOH in the marine environment. Data on the occurrence of TCPMe and TCPMOH further indicated high bioaccumulation potential of these compounds, which was comparable to DDTs. Relative concentrations of TCPMe/TCPMOH in cetaceans were apparently higher than those observed in seals, suggestive of lower metabolic capacity for these compounds in cetaceans than in pinnipeds, which is similar to classic contaminants like polychlorinated biphenyls and DDTs.