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The present study for the first time reports the occurrence, distribution, ecological and resistance risks of antibiotics in the surface water of freshwater finfish and brackish water shellfish aquaculture in Bangladesh. Among the nine targets, seven antibiotics were detected in finfish aquaculture, whereas four in shellfish aquaculture. The concentrations (ranges) and overall detection frequency of sulfamethoxazole (SMX) (nd-20.02 ng L−1 and 73%), trimethoprim (TMP) (nd-41.67 ng L−1 and 60%), tylosin (TYL) (nd-39.34 ng L−1 and 60%), sulfadiazine (SDZ) (nd-17.97 ng L−1 and 53%), sulfamethazine (SMT) (nd-11.71 ng L−1 and 33%), sulfamethizole (SMZ) (nd-10.81 ng L−1 and 40%) and penicillin G (PC_G) (nd-7.83 ng L−1, 7%) were found in finfish aquaculture. In case of shellfish aquaculture, the concentrations (ranges) and overall detection frequency were for SMX (nd-16.77 ng L−1 and 67%), TMP (nd-11.39 ng L−1 and 20%), TYL (nd-0.16 ng L−1 and 20%) and erythromycin-H2O (ERY-H2O) (nd-3.91 ng L−1 and 20%). The present findings revealed that finfish aquaculture is more contaminated with the higher numbers and concentrations of antibiotics. The preliminary ecological and resistance risks assessment showed that the calculated risk quotients (RQs) were lower than one (RQs

In China, a considerable part of industrial wastewater effluents are discharged into the municipal wastewater treatment plants (WWTPs) after pretreatment in their own wastewater treatment plants. Even though the industrial effluents meet the professional emission standards, many micro-pollutants still remained, and they could be resistant in the municipal WWTPs with conventional activated sludge process. Pigment wastewater was chosen in this study, and the acute toxicity reduction and identification of the pigment-contaminated wastewater treated by the conventional anaerobic-anoxic-oxic (A/A/O) process were evaluated. Results indicated that the raw pigment-contaminated wastewater was acutely toxic to Photobacterium phosphoreum (P. phosphoreum), Daphnia magna (D. magna) and Danio rerio (D. rerio). The acute toxicity was decreased in some degree after A/A/O treatment, but the final effluent still exhibited acute toxicity to D. magna and D. rerio with the toxic units (TU) of 1.1 and 2.0, respectively. Chemical analyses showed the presence of various refractory and toxic nitrogen-containing polycyclic and heterocyclic compounds in the pigment-contaminated wastewater. Toxicity identification by combining chemical analyses and correlation analysis showed that N-containing refractory organic toxicants were the main toxicity source for the pigment-contaminated wastewater, and several toxicants showed significant correlation with P. phosphoreum and D. magna. This study indicated that the A/A/O process was not efficient for pigment-contaminated wastewater treatment, and it was irradiative for technology improvement in the WWTPs receiving pretreated industrial wastewater effluents.

Perfluoroalkyl acids (PFAAs) and their precursors have been used in various consumer products. However, limited information regarding their occurrence and concentration levels in products is available. In this study, we investigated 18 PFAAs and 14 PFAA precursors in various categories of consumer products purchased in Japan. Relatively high total concentrations of PFAAs and their precursors were found in sprays for fabrics and textiles (

Organochlorine pesticides (OCPs) are subject to the Stockholm Convention on POPs and have been banned or restricted globally. In Ghana, concerns of illicit applications of some OCPs have been raised in recent times. Applying polyurethane foam (PUF) disk passive air samplers (PAS), the levels of OCPs in the atmosphere and their spatial resolution were investigated. It was the first nationwide coverage of OCPs monitoring in Ghana. ∑DDTs and endusulfans constituted the highest burden of atmospheric OCPs in Ghana, at average concentrations of 156±36 and 153±28 pg m(-3), respectively. Mirex had the lowest concentration (0.2±0.01 pg m(-3)). From the chemical signatures of the various OCPs, we deduced that DDT, endosulfans and heptachlor were freshly applied at certain sites, which were all agricultural sites. The OCPs were spatially resolved as a function of the types of crops cultivated in different areas, legacy issues and recent applications.

Simple semi-theoretical models were developed to estimate the performance of three different kinds of advanced oxidation processes (AOPs) in the degradation of pharmaceuticals. The AOPs included the photo-Fenton process as an example of a liquid-liquid reaction, the TiO2 photocatalytic oxidation process as a solid-liquid reaction, and the combined ozone and hydrogen peroxide oxidation process as a gas-liquid reaction; the effects of the aqueous matrices (CESs: co-existing substances) of actual wastewater on the removal of pharmaceuticals (carbamazepine and diclofenac) was taken into account. By comparing the characteristic parameters of the models, obtained from the experiments using pure water and actual wastewater, the effects of CESs on the respective removal mechanisms could be separately and quantitatively evaluated. As a general tendency, the AOPs proceeded less effectively (were inhibited) in the matrices containing CESs, as observed with the use of a lower initial concentration of pharmaceuticals. The inhibition mechanisms differed for the three types of AOPs. In the photo-Fenton process, the Fenton reaction was improved by the incorporation of CESs, while the photo-reduction reaction was significantly inhibited. In the TiO2 photocatalytic oxidation process, competition between the pharmaceuticals and CESs for adsorption on the catalyst surface was a less significant inhibitory factor than the scavenger effects of the CESs. The combined ozone and hydrogen peroxide oxidation process was most strongly inhibited by CESs among the AOPs investigated in this study.

To efficiently reduce perfluorinated compound (PFC) pollution, it is important to have an understanding of PFC sources and their contribution to the pollution. In this study, source identification of diffuse water pollution by PFCs was conducted using a GIS-based approach. Major components of the source identification were collection of the monitoring data and preparation of the corresponding geographic information that was extracted from a constructed GIS database. The spatially distributed pollution factors were then explored by multiple linear regression analysis, after which they were visually expressed using GIS. Among the 35 PFC homologues measured in a survey of the Tokyo Bay basin, 18 homologues were analyzed. Pollution by perfluorooctane sulfonate (PFOS) was explained well by the percentage of arterial traffic area in the basin, and the 84% variance of the measured PFOS concentration was explained by two geographic variables, arterial traffic area and population. Source apportionment between point and nonpoint sources was conducted based on the results of the analysis. The contribution of PFOS from nonpoint sources was comparable to that from point sources in several major rivers flowing into Tokyo Bay. Source identification and apportionment using the GIS-based approach was shown to be effective, especially for ubiquitous types of pollution, such as PFC pollution.

Worldwide environmental pollution by perfluorinated compounds (PFCs) has been reported. PFCs have also been reported to have nonpoint sources (NPSs). A fixed-point hourly monitoring in the river was conducted during a storm event using an automatic sampler to estimate the impact of the first-flush of PFCs from NPS in this study. Perfluorocarboxylates (PFCAs) and perfluoroalkyl sulfonates (PFASs) with different chain lengths were monitored. The concentrations of short- to medium-chain-length PFCAs such as PFHpA, PFOA and PFNA, and PFASs such as PFBS, PFPeS, PFHxS, PFHpS and PFOS showed no marked increase with the storm-runoff event. However, in contrast to this, concentrations of long-chain-length PFCAs such as PFDA and PFUnA increased markedly. The concentrations of PFDA and PFUnA increased 3.4 (1.5–5.0 ng L−1)- and 2.0 (3.3–6.7 ng L−1)-fold, respectively. This study demonstrates that large loads of long-chain-length PFCAs are discharged to the Hayabuchi River during the first-flush after the rain event.

Products containing perfluorinated compounds (PFCs) have been widely used during the last 50 years. As a result, worldwide environmental pollution by PFCs has been reported. The sources of PFC pollution in the aquatic environment have been poorly understood. In this study, river water and sewage treatment plant (STP) effluent were sampled along the stretch of the Tsurumi River and also at a fixed station in the river. The concentrations of perfluorooctanesulfonate (PFOS), perfluorohexanoic acid (PFHxA), perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA) and perfluorodecanoic acid (PFDA) were measured. With an increase in river flow rate, it was observed that the PFC concentrations in the river water at fixed station were remained the same or increased for PFOS (179.9 ± 34.4–179.6 ± 69.5 ng l −1 ), PFHxA (5.5 ± 0.8–9.0 ± 2.6 ng l −1 ), PFHpA (3.1 ± 0.3–4.4 ± 1.0 ng l −1 ), and PFOA (15.9 ± 0.3–13.4 ± 2.5 ng l −1 ) whereas the concentration of PFNA (38.0 ± 3.3–15.4 ± 3.0 ng l −1 ) and PFDA (3.9 ± 0.3–2.1 ± 0.3 ng l −1 ) were decreased. On the other hand, the loads of every PFC increased with an increase in river flow rate. The loads of PFCs in rain runoff were estimated to be 2–11 times greater than those in STP effluents that are discharged into the river. These results indicate the existence of a PFC nonpoint source (NPS) and its impact to the total PFC load of river is significant.

In this study, we determined the detailed PCB congener patterns in flue gases from eight incinerators and four commercial PCB formulations (Kanechlors). About 160 PCB peaks were identified in samples using a DB-5 column and HRGC/HRMS. The concentration of incinerator stack emission gas ranged from 0.02 to 44 ng WHO-TEQ/N m3. The ratios of dioxin-like PCBs in the total PCB concentration were from 3.4% to 25.7% and from 0.63% to 9.1% in stack emission gases and Kanechlor samples, respectively. The PCB congener profiles of Kanechlor samples were similar to those of previous studies. To determine characteristic congeners in flue gas and Kanechlor samples, principal component analysis (PCA) of the data was conducted using STATISTICA for Windows 5.0J (StatSoft, Inc.). As a result, we obtained four principal components (PCs) and accounted for 74% of the total variance. PC 1 was interpreted combustion, PC 2 and PC 3 were interpreted the difference in the number of substituted chlorines and, PC 4 could not be determined. Moreover, we obtained three groups according to the PCB congeners pattern among samples by PCA. These specific congeners that represent characteristics of each class were identified. These data will be useful for the source analysis of PCBs in the environment.

We used a Lake Suwa version of Comprehensive Aquatic Systems Model (CASM_SUWA) to demonstrate the risk estimation of 10 different chemicals and examined the applicability and reliability of the model in ecological risk assessment by qualitatively and quantitatively comparing with the results of studies on multiple species using mesocosm tests. The qualitative comparison of the model results with those of the reported mesocosm tests indicated that some evidence observed in mesocosm studies supported the indirect effects predicted from simulation using the model. The comparison of the concentration levels at which 20% biomass reduction (BR20) in the most sensitive population estimated from the model with the no-observed effect concentration values derived from multiple species mesocosm tests (MS-NOEC) suggested that both data were related to each other and the model can be used to help in the determination of an ecological acceptable level of chemicals in aquatic environments. The analysis of the potential of indirect effects of a chemical for fish population indicated that the magnitude of the potential of indirect effects was quantified based on the ratio of BR50 to LC50 for fish population.

The overall atmospheric behavior of PCDDs/PCDFs in the Kanto region, Japan, was simulated by a one-compartment box model. For each homologue the relative significance and temperature dependences of dry deposition, wet deposition, degradation, and advection in both gas and particulate phases were examined and compared. The results of the model calculation suggested that the rates for dry deposition are comparable to those for wet deposition, and the rates for advection are comparable to those for bulk (dry + wet) depositions in the Kanto region. On the other hand, the rates of degradation for PCDDs/PCDFs in the atmosphere in the Kanto region would be negligible. The emission rates and the bulk deposition fluxes in the entire Kanto region estimated by the model calculation based on observed air concentrations were 0.084–0.90 kg-TEQ/month and 0.045–0.43 kg-TEQ/month, respectively. These estimated emission rates and bulk deposition fluxes were slightly higher than the estimated emission rate based on observed emission concentrations and the estimated bulk deposition fluxes based on observed deposition fluxes collected on water deposition surface, respectively. This study showed the model calculation can be available for understanding of the overall atmospheric behavior, verification of the source inventory, and estimation of deposition flux on the actual environment including various deposition surfaces.

Blood of adult and juvenile black and turkey vultures in the Savannah River Site of South Carolina, USA was analyzed for the presence of 2,3,7,8-chlorine substituted polychlorinated dibenzo- p -dioxins (2,3,7,8-PCDDs), dibenzofurans (2,3,7,8-PCDFs), -dioxin-like and -di- ortho polychlorinated biphenyls. Concentration ranges of 2,3,7,8-PCDD/DFs in blood of black and turkey vultures were 14.2–34.6 and 8.7–56.2 pg/ml wet wt., respectively. Dioxin-like PCBs were in the ranges of 815–4627 and 753–3611 pg/ml wet wt. respectively, in black and turkey vultures. Considerable concentrations of two congeners of di- ortho PCBs were noticed in the ranges of 1415–10 325 and 663–7500 pg/ml respectively, in black and turkey vultures. Comparatively, greater toxic equivalency (TEQ) were observed in blood of turkey vultures with the ranges of 3.2–20, whereas black vulture contained 1.8–8.4 pg TEQ/ml wet wt. basis. The species-specific accumulation profiles of PCDD/DFs and dioxin-like PCBs may reflect the different feeding habits, ecology, metabolic capacity and migratory movements of these two scavenging species.

Livers of birds collected from Japan and Korea (n ¼ 83) were analyzed to determine the concentrations of perfluorooctanesulfonate (PFOS), perfluorooctanesulfonamide (FOSA), perfluorooctanoic acid (PFOA) and perfluorohexanesulfonate (PFHS). PFOS was found in the livers of 95% of the birds analyzed at concentrations greater than the limit of quantitation (LOQ) of 10 ng/g, wet weight. The greatest concentration of PFOS of 650 ng/g, wet weight, was found in the liver of a common cormorant from the Sagami River in Kanagawa Prefecture. Concentrations of PFOS in bird livers from Japan and Korea were within the ranges of values reported for those from the United States and certain European countries. PFOA and PFHS were found in 5–10% of the samples analyzed. The greatest concentrations of PFOA and PFHS in bird livers were 21 and 34 ng/g, wet weight, respectively. FOSA was found in all the samples (n ¼ 10) of cormorants collected from the Sagami River in Japan. The greatest concentration of FOSA in cormorant liver was 215 ng/g, wet weight. There was no significant correlation between the concentrations of PFOS and FOSA in cormorants collected from the Sagami River. These results suggested that the distribution of FOSA is localized. No ageor gender-specific differences in fluorochemical concentrations could be discerned in birds. 2002 Elsevier Science Ltd. All rights reserved.

One bottle of Yusho rice oil was obtained from a Yusho family in 1998. The levels of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs) in the causal oil were investigated with two different approaches and the individual concentrations of all the 17 2,3,7,8-substituted PCDD/F and 14 coplanar PCB (Co-PCB) congeners were elucidated for the first time. The concentrations of PCDDs and PCDFs were found to be 0.60 and 8.8 ppm, respectively. For PCBs, more than 130 PCB peaks were observed and a total concentration of 850 ppm including 170 ppm of Co-PCBs was obtained. The toxic equivalents (TEQs) of PCDDs, PCDFs, and Co-PCBs were calculated to be 17, 470, and 120 ppb, respectively. The relative contribution of these classes to the total TEQ in Yusho oil is 3%, 77%, and 20%, respectively, indicating that PCDFs play a major role in the toxicity of Yusho oil. Furthermore, it was confirmed that 2,3,4,7,8-penta-CDF contributes 58% to the total TEQ, supporting the view that this compound is the principal causal agent in Yusho poisoning. It is noteworthy that the most toxic 2.3,7,8-tetra-CDD was newly discovered, although it contributes only 0.1% to the total TEQ. Based on our data, the smallest TEQ intake during the latent period was estimated to be 0.067 mg for Yusho patients. This value is about 60% of that previously reported, suggesting a lower minimum threshold level for the development of the toxic symptoms of Yusho.

The atmospheric bulk (dry and wet) deposition of dioxins was investigated at four locations (Tokyo, Yokohama, Tsukuba, and Tanzawa) in the Kanto region (in Japan) over one year using a stainless-steel pot. Annual average polychlorinated dibenzo-p-dioxins/polychlorinated dibenzofurans (PCDD/PCDF) deposition fluxes were estimated to be from 450 to 1300 ng/m2/yr, and the annual average TEQ fluxes from 5.7 to 17 ng-TEQ/m2/yr at the four locations. The PCDD/PCDF deposition flux was higher in winter than in summer. The deposition flux could be related to ambient temperature, particularly for less chlorinated PCDDs/PCDFs, while the deposition flux is not necessarily related to the amount of precipitation. The PCDD/PCDF deposition flux increased as the particle deposition flux increased, for the winter samples. Based on the ratio of the PCDD/PCDF deposition fluxes to the particle deposition fluxes, the contribution of the reentrainment of soil particles to the TEQ of PCDD/PCDF deposition was considered to be negligible in this region. Based on the air concentrations monitored near our deposition sampling points by the municipalities, the ratio of the annual deposition flux to the annual average air concentration was roughly estimated to be 0.082 cm/s. The range of deposition flux in the Kanto region was estimated to be from 1.5 to 31 (median: 9.8) ng-TEQ/m2/yr based on the range of air concentration data measured by the municipalities. The total annual deposition flux in the entire Kanto region was estimated to range from 50 to 900 g-TEQ/yr (median 320 g-TEQ/yr). This estimated flux was of the same order as the sum of estimated emissions from municipal solid waste incinerators and industrial waste incinerators in the Kanto region. The contributions of dioxin-like PCBs in Yokohama, Tsukuba, and Tanzawa depositions were less than 10% of the total TEQ; however, in Tokyo it was almost equal to or more than 50%.

The profile and amount of dioxin impurity in agrochemicals were studied through detailed analysis of historic Japanese formulations. The chemicals analyzed include pentachlorophenol (PCP), 2,4,6-trichlorophenyl-4'-nitrophenyl ether (chloronitrofen, CNP), 2,4-dichlorophenyl-4'-nitrophenyl ether (nitrofen, NIP), tetrachloro-iso-phthalonitrile (chlorothalonil, TPN), 2-methyl-4-chloro-phenoxyacetic acid (MCP) and 2,4-dichlorophenoxyacetic acid (2,4-D). Among the six, two herbicides, PCP and CNP, produced during the 1960s and 1970s, contained very high concentrations of PCDD/DFs and TEQ. Others contained relatively low concentrations of PCDD/DFs. Dioxin-like PCB concentrations in all chemicals studied were low and their contributions to TEQ were negligible. The total dioxin emissions from the use of agrochemicals in Japan during the past 40 years (1955-1995) were estimated to be about a few hundred thousand kg of PCDD/DFs and 250 kg of WHO-TEQ from PCP and 190 x 10(3) kg of PCDD/DFs and 440 kg of WHO-TEQ from CNP. The major dioxin congeners present in PCP formulations were highly chlorinated PCDD/DFs that can be formed by the coupling of PCP and/or 2,3,4,6-tetrachlorophenol, and those in the CNP formulations were tetra- to hexa-chlorinated PCDD/DFs that can be formed from 2,4,6-trichlorophenol and/or 2,3,4,6-tetrachlorophenol.

Hexabromocyclododecane (HBCD) and its lower brominated derivatives were measured in both surface water and sediment samples from three Japanese rivers; Tsurumi River, Yodo River, and Kuzuryu River. The concentration level of ∑HBCD (sum of α-, β-, and γ-HBCD) was in the order of Kuzuryu > Yodo > Tsurumi Rivers, reflective of the different emission sources for each basin. The highest ∑HBCD concentration (7800 ng g−1 dw) was detected in the sediment sample from the Kuzuryu River that receives effluents from textile industries, which use HBCD in flame retardant finishes. A different diastereomeric pattern of α-, β-, and γ-HBCD of each river was investigated, indicating the level of HBCD in these rivers is directly influenced by emission source. Enantiomer fractions of HBCDs in water and sediment samples were also determined. Racemic mixtures were observed in the water samples, whereas enantiomeric enrichment of (−) γ-HBCD and (+) α-HBCD was observed in the sediment samples. Some lower brominated HBCD derivatives such as pentabromocyclododecenes were detected in both the water and sediment samples, and their concentration ranged from below the detection limit to 15 ng L−1 and 20 ng g−1 dw, respectively.

The transformations of chloronitrobenzenes (CNBs) in anaerobic estuarine sediment were examined. The sediment had been preexposed to various anthropogenic chemicals from the surrounding industries. The sulfate content of the interstitial and overlaying waters was approximately 20 mmole/1 indicating that the sediment was sulfidogenic. All the CNBs tested transformed without any lag period. The kinetic data followed a first-order reaction mechanism with rate constants ranging from 0.216 to 0.866 day −1 or half-lives from 0.8 to 3.2 days. The intermediates detected in the experiment indicated that the reduction of the nitro group was the first stage in the transformation of chloronitro aromatic compounds, resulting in the formation of corresponding chloroanilines (CAs). The CAs further transformed via ortho and para dechlorination pathways.

The vertical distribution patterns of the transofmration products of tri-n-butyltin (TBT) in sediment cores collected from 6 sites in Ise Bay, Japan indicated that TBT was transformed by two pathways: methylation and debutylation. Anaerobic incubation of sediment spiked with TBT showed that the methylation was mainly supported by sulfate reducing activity and debutylation was mainly supported by nitrate reducing activity. These results showed that contribution of the two transformation reactions of TBT varied according to the dominant microbial activities in the sediment. The two types of vertical distribution of butyltins observed in the sediment cores appear to be the result of different dominant microbial activity in the sediment.

The relation between dechlorination activities of 1,2,4-trichlorobenzene and anaerobic microbial activity were studied in the sediment collected at three sites in Ise Bay in Japan. The degradation rate of spiked 1,2,4-trichlorobenzene (3nmol ml−1) ranged from 15 to 35 pmol day−1 ml−1 wet sediment and about 1 3 to 1 2 of degraded the trichlorobenzene was recovered as dechlorinated products. Among the dichlorobenzenes, the 1,2-isomer had the highest and 1,3-isomer had the lowest production rate. Comparing the three sampling sites, the trichlorobenzene degradation and dichlorobenzenes production rates were related to the sulfate reducing activity for the unit number of sulfate reducing bacteria. Production rates of dichlorobenzenes were completely inhibited by adding molybdate (20 mM), nitrate (60 mM), and formaldehyde solution (4 %). These results indicated that dechlorination activity in the Ise Bay sediment was supported by sulfate reduction activity in the sediment, and not supported by any other anaerobic microbial activity.

In this study, we analyzed over 30 types of PFCs, including precursors in both the dissolved phase and particle solid phase, in 50 samples of river water collected from throughout the Tokyo Bay basin. PFCs were detected in suspended solids (SSs) at levels ranging from −1 (0.11–2470 ng g −1 dry weight). The concentrations of PFCs in the SS were one to two order(s) of magnitude lower than those of PFCs in the dissolved phase. Relatively high levels of PFCs (total of 35 PFCs) in SS were observed in urbanized areas. The concentration of PFCAs, including PFOA and PFNA, were significantly correlated with the geographic index as artificial area ( R 2 of the linear regression curve in a double logarithmic plot: 0.09–0.55). Conversely, PFOS and FOSA were significantly correlated with the arterial traffic area ( R 2 in a double logarithmic plot: 0.29–0.55). Those spatial trends were similar to the trends in dissolved PFCs. We estimated the loading amount of PFCs into Tokyo Bay from six main rivers and found that more than 90% of the total PFCs reached Tokyo Bay in the dissolved phase. However, 40.0–83.5% of the long chain PFCAs (C12–C15), were transported as particle sorbed PFCs. Rain runoff events might increase the loading amount of PFCs in SS. Overall, the results presented herein indicate that greater attention should be given to PFCs, especially for longer chain PFCs in SS in addition to dissolved PFCs.

Identification of pollution sources and estimation of their contribution to dioxin pollution are important for taking better countermeasures against such sources. The information based on seventeen 2,3,7,8-chlorine-substituted congeners and 10 homologues is usually not sufficient for source identification. The usefulness of detailed congener-specific information of tetra- to octachlorinated polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans was examined by principal component analysis and compared with conventional dioxin information. It was revealed that congener-specific information was far more effective for source identification than conventional information. For source apportioning, it was shown that multiple regression analysis with detailed source congener profiles could be carried out successfully when calculations were performed for individual homologues. This was because of the large variation in homologue composition in source dioxin profiles in addition to the difference in environmental behavior among the homologues. The newly proposed methods for statistical analysis were applied to the estimation of dioxin mass balance in Tokyo Bay basin. It was found that Tokyo Bay sediment core contained dioxins from three major sources: combustion, pentachlorophenol (PCP), and chloronitrophen (CNP). PCP and CNP contained large amounts of dioxin as impurity and were used extensively as paddy field herbicides in Japan in the past. The total dioxin load from the two herbicides to the basin during the past 45 years (1951-1995) was estimated to be five times larger than that from combustion source in terms of toxic equivalents (WHO-TEQ). However, in the surface sediment of the bay, the contribution from the herbicides was nearly equal to that from combustion. The herbicide contribution peaked during the 1960s and 1970s and gradually decreased thereafter.