SIPIBEL observatory: Data on usual pollutants (solids, organic matter, nutrients, ions) and micropollutants (pharmaceuticals, surfactants, metals), biological and ecotoxicity indicators in hospital and urban wastewater, in treated effluent and sludge from wastewater treatment plant, and in surface and groundwater.

The Bellecombe pilot site - SIPIBEL - was created in 2010 in order to study the characterisation, treatability and impacts of hospital effluents in an urban wastewater treatment plant. This pilot site is composed of: i) the Alpes Léman hospital (CHAL), opened in February 2012, ii) the Bellecombe wastewater treatment plant, with two separate treatment lines allowing to fully separate the hospital wastewater and the urban wastewater, and iii) the Arve River as the receiving water body and a tributary of the Rhône River and the Geneva aquifer. The database includes in total 48 439 values measured on 961 samples (raw and treated hospital and urban wastewater, activated sludge in aeration tanks, dried sludge after dewatering, river and groundwater, and a few additional campaigns in aerobic and anaerobic sewers) with 44 455 physico-chemistry values (including 15 pharmaceuticals and 14 related transformation products, biocides compounds, metals, organic micropollutants), 2 193 bioassay values (ecotoxicity), 1 679 microbiology values (including microorganisms and antibioresistance indicators) and 112 hydrobiology values.

Ecotoxicological risk assessment of contaminants of emerging concern identified by "suspect screening" from urban wastewater treatment plant effluents at a territorial scale.

Urban wastewater treatment plants (WWTP) are a major vector of highly ecotoxic contaminants of emerging concern (CECs) for urban and sub-urban streams. Ecotoxicological risk assessments (ERAs) provide essential information to public environmental authorities. Nevertheless, ERAs are mainly performed at very local scale (one or few WWTPs) and on pre-selected list of CECs. To cope with these limits, the present study aims to develop a territorial-scale ERA on CECs previously identified by a "suspect screening" analytical approach (LC-QToF-MS) and quantified in the effluents of 10 WWTPs of a highly urbanized territory during three periods of the year. Among CECs, this work focused on pharmaceutical residue and pesticides. ERA was conducted following two complementary methods: (1) a single substance approach, based on the calculation for each CEC of risk quotients (RQs) by the ratio of Predicted Environmental Concentration (PEC) and Predicted No Effect Concentration (PNEC), and (2) mixture risk assessment ("cocktail effect") based on a concentration addition model (CA), summing individual RQs. Chemical results led to an ERA for 41 CEC (37 pharmaceuticals and 4 pesticides) detected in treated effluents. Single substance ERA identified 19 CECs implicated in at least one significant risk for streams, with significant risks for DEET, diclofenac, lidocaine, atenolol, terbutryn, atorvastatin, methocarbamol, and venlafaxine (RQs reaching 39.84, 62.10, 125.58, 179.11, 348.24, 509.27, 1509.71 and 3097.37, respectively). Mixture ERA allowed the identification of a risk (RQmix > 1) for 9 of the 10 WWTPs studied. It was also remarked that CECs leading individually to a negligible risk could imply a significant risk in a mixture. Finally, the territorial ERA showed a diversity of risk situations, with the highest concerns for 3 WWTPs: the 2 biggest of the territory discharging into a large French river, the Rhône, and for the smallest WWTP that releases into a small intermittent stream.

Ecotoxicity and antibiotic resistance of wastewater during transport in an urban sewage network.

Urban wastewater (UWW) management usually entails biological and physicochemical monitoring due to its potential impact on the quality of the receiving environment. A major component of a sewage system is the pipe network leading the water to the treatment plant. Up to now, few studies have been conducted on the diverse phenomena that may affect the characteristics of the water during its transportation. In this study, ecotoxicity and potential antibiotic resistance were used in a global method to assess the change of UWW quality in a sewage system and determine if sewer pipes can act as a bioreactor spread. Three bioassays were conducted to assess the ecotoxicity of the samples and the concentration and relative abundance of two classes of integrons (as a proxy for antibiotic resistance) were measured. The results of the bioassay battery do not show a pattern, despite the fact that differences were noticeable between upstream and downstream samples. Antibiotic resistance appeared to decrease during transport in the pipe as the concentration and relative abundance of integrons decreased during several campaigns. This result should be confirmed in other sewer networks but already provides useful information for the management of urban sewage system.

Ecotoxicological risk assessment of micropollutants from treated urban wastewater effluents for watercourses at a territorial scale: Application and comparison of two approaches.

In most cases, urban Wastewater Treatment Plants (WWTP) only partially abate pollutants occurring in the influent. Treated effluents can thus contain a complex mixture of ecotoxic pollutants, such as heavy metals, detergents, disinfectants, plasticizers, pharmaceuticals residues or pesticides. In this context, Ecotoxicological Risk Assessment (ERA) provide essential decision-making tools to public authorities for establishing environmental policies and conducting territorial planning. The present work aims to develop a territorial-scale ERA methodology using two complementary approaches based on a Risk Quotient (RQ) calculation: (1) the first, based on the risk linked to each individual pollutant (single substances ERA); (2) the second, considering all pollutants present, and the "cocktail effect" (mixture ERA). This research was performed at 33 urban WWTPs of in a highly urbanized part of France (Lyon area). Initial minimum, median and maximum pollutant concentrations in treated effluents were obtained from a literature review of physico-chemical analysis studies, to reconstitute "typical" effluents. The classical approach (single substances ERA) identified the riskiest substances (e.g. endocrine disruptors, as the Estrone with RQ up to 593.75), and showed the risks for each WWTP. The mixture ERA approach revealed new risks, which were not highlighted in the classical ERA approach, thus increasing the number of WWTPs identified as at risk. This study shows the importance of accounting for the cocktail effect, which is not considered in current regulatory decisions. Finally, this methodology allowed us to identify the riskiest situations (often medium sized WWTPs, releasing into small streams), that could worsen in the context of climate change.

Past and recent state of sediment contamination by persistent organic pollutants (POPs) in the Rhône River: Overview of ecotoxicological implications.

Twenty-one sediment samples were taken from five dated sediment cores collected along the Rhône River from 2008 to 2011. A total of 17 polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), 7 polychlorinated biphenyls (PCBs), 8 polybrominated diphenyl ethers (PBDEs), 3 polybrominated biphenyls (PBBs), 3 hexabromocyclododecanes (HBCD) and 31 organochlorine pesticides (OCPs) were investigated to provide information on deposition dynamics in time and space, but also regarding the ecotoxicological risks associated with these contaminants. Median concentrations of total PBDEs are nine times lower than the levels of total PCBs along the entire studied stretch of the Rhône River. The results show that total PBDEs concentrations range from 0.06 to 239 µg·kg-1 DW with a median value of 3.81 µg·kg-1 DW and a maximum concentration measured in the years 2000s. These maximum concentrations are identical to those measured for total PCBs at the end of the 1990s, but show a different pattern of distribution. Abnormal dichlorodiphenyltrichloroethane (DDT) levels were also detected in the downstream section of the river, with a peak concentration of 147.5 µg·kg-1 DW measured at the GEC site from 2005 onwards. Analyses of the enantiomeric fractions reveal a fresh input resulting from a technical formulation. Sediments from the core sampled at the most downstream site (GEC) are found to be highly toxic to organisms living nearby, particularly because of the total PCDD/Fs, DDE and DDT levels. In addition, based on available sediment quality guidelines, there may be a potential bioaccumulation risk for humans not only for these three compounds of concern but also for total PCBs and 7 out of the 8 analysed PBDEs.

Spatial and temporal dynamics of sediment ecotoxicity in urban stormwater retention basins: Methodological approach and application to a pilot site close to Lyon in France.

To characterize the spatio-temporal variation of sediment ecotoxicity in a retention/detention basin, a monitoring program using the Heterocypris incongruens bioassay was carried out for 72 months (5 years) on a field basin close to Lyon in France. Results showed that the variation of ecotoxicity is relatively small from one location of the basin to another, apart from sediment sampling collected in an open-air chamber located in basin supposed to collect gross pollutants and hydrocarbons. Regarding the temporal variation of ecotoxicity, the bioassays also showed a slight variation between 6 and 72 months. On the contrary, they highlighted the high ecotoxicity of the "fresh" sediments collected during rain events using sediment traps. Additional investigations are needed to understand the period of inflexion of ecotoxicity, occurring between 24 h and 6 months. These results can be used by practitioners of urban facilities and networks to improve maintenance strategies of retention/detention basins.

The SIPIBEL project: treatment of hospital and urban wastewater in a conventional urban wastewater treatment plant.

Hospital wastewater (HWW) receives increasing attention because of its specific composition and higher concentrations of some micropollutants. Better knowledge of HWW is needed in order to improve management strategies and to ensure the preservation of wastewater treatment efficiency and freshwater ecosystems. This context pushed forward the development of a pilot study site named Site Pilote de Bellecombe (SIPIBEL), which collects and treats HWW separately from urban wastewater, applying the same conventional treatment process. This particular configuration offers the opportunity for various scientific investigations. It enables to compare hospital and urban wastewater, the efficiency of the two parallel treatment lines, and the composition of the resulting hospital and urban treated effluents, as well as the evaluation of their effects on the environment. The study site takes into account environmental, economic, and social issues and promotes scientific and technical multidisciplinary actions. ᅟ.

Ecotoxicity and antibiotic resistance of a mixture of hospital and urban sewage in a wastewater treatment plant.

Hospital and urban effluents are a source of diverse pollutants such as organic compounds, heavy metals, detergents, disinfectants, pharmaceuticals, and microorganisms resistant to antibiotics. Usually, these two types of effluent are mixed in the sewage network, but a pilot site in France now allows studying them separately or mixed to understand more about their characteristics and the phenomena that occur following their mixing. In this study, their ecotoxicity (Daphnia magna mobility, Pseudokirchneriella subcapitata growth, Brachionus calyciflorus reproduction, and SOS Chromotest) and antibiotic resistance (integron quantification) were assessed during mixing and treatment steps. The main results of this study are (i) the ecotoxicity and antibiotic resistance potentials of hospital wastewater are higher than in urban wastewater and (ii) mixing two different effluents does not lead to global synergistic or antagonistic effects on ecotoxicity and antibiotic resistance potential. The global additivity effect observed in this case must be confirmed by other studies on hospital and urban effluents on other sites to improve knowledge relating to this source of pollution and its management.

Identification, assessment and prioritization of ecotoxicological risks on the scale of a territory: Application to WWTP discharges in a geographical area located in northeast Lyon, France.

The ecotoxicological risk assessment methodologies developed up to now mainly focus on local pollution and do not incorporate an evaluation and prioritization of the different risk situations present in the same territory. This article presents the different phases of formulating an innovative methodology developed to fill this gap, and its application to all the 18 WasteWater Treatment Plants (WWTP) of a geographical area located northeast of Lyon, France. The aim was also take into account emerging pollutants that are very often "forgotten" in ecotoxicological risk assessments. The results of the study show the extreme diversity of the ecotoxicity of the pollutants present in discharges, with "minimum" PNEC values in the region of a millionth of a microgram (10-6 µg/l) and "maximum" PNEC values in the region of several tens of micrograms. They also show very considerable diversity of the flows of the receiving watercourses in the territory concerned (from several m3/s to 600 m3/s). The Risk Quotients (RQ) resulting from these 2 datasets, calculated for each WWTP and for each of the 10 pollutants most implicated in ecotoxicological risks (Diclofenac, Amoxicillin, Trimethoprim, Roxithromycin, 17ß-estradiol, 17α-Ethynylestradiol, Estrone, Nonylphenol, Octylphenol, Nickel, et NH4+), vary from 0.000002 to 187.7 when using the median concentration values of these pollutants, and from 0.000007 to 3750 when using their maximum concentration values. Globally, they show that: (1) the risks are higher for small streams that receive WWTP discharges of average size, (2) the risks are low to very low for discharges into watercourses with high flow rates.

Identification and assessment of ecotoxicological hazards attributable to pollutants in urban wet weather discharges.

Urbanization has led to considerable pressure on urban/suburban aquatic ecosystems. Urban Wet Weather Discharges (UWWD) during rainfall events are a major source of pollutants leached onto and into urban surfaces and sewers, which in turn affect aquatic ecosystems. We assessed the ecotoxicity of the different compounds identified in UWWD and identified the hazard represented by each of them. To this end, hazard quotient (HQ) values were calculated for each compound detected in UWWD based on their predicted no effect concentration (PNEC) values and their maximum measured effluent concentrations (MECmax) found in the dissolved part of UWWD. For the 207 compounds identified in UWWD, sufficient data existed for 165 of them to calculate their PNEC. The ecotoxicity of these compounds varied greatly. Pesticides represented a high proportion of the wide variety of hazardous compounds whose HQ values were calculated (94 HQ values), and they were among the most hazardous pollutants (HQ > 1000) transported by stormwater. The hazard of combined sewer overflows (CSO) was linked mainly to heavy metals and pharmaceutical compounds. Consequently, the monitoring of these pollutants should be a priority in the future. The hazard level of certain pollutants could have been underestimated due to their adsorption onto particles, leading to their low concentration in the dissolved phase of UWWD. Hence, an in-depth study of these pollutants will be required to clarify their effects on aquatic organisms.

A posteriori assessment of ecotoxicological risks linked to building a hospital.

Hospital wastewater (HWW) contain a large number of chemical pollutants such as disinfectants, surfactants, and pharmaceutical residues. A part of these pollutants is not eliminated by traditional urban wastewater treatment plants (WWTP), leading to a risk for the aquatic ecosystems receiving these effluents. In order to assess this risk, we formulated a specific methodology based on the ecotoxicological characterisation of the hospital wastewater using a battery of three chronic bioassays (Pseudokirchneriella subcapitata, Heterocypris incongruens and Brachionus calyciflorus). We used it for the posteriori risk assessment of a hospital recently built in south-east France, and we studied the evolution of this risk during two years. We also used it to assess the decrease of the ecotoxicological risk after treatment of the effluent in a specific line of the local WWTP. Lastly, we compared these results with the risk assessment made before the building of the hospital in the context of a priori risk assessment. The results obtained showed an important evolution of the risk overtime, according to the hospital activities and the river flows, and a real decrease of the risk after treatment in the dedicated line. They also showed that the a priori assessment of ecotoxicological risks, made previously, was overstated, mainly because of the application of the precautionary principle.

Respective contributions of diet and medium to the bioaccumulation of pharmaceutical compounds in the first levels of an aquatic trophic web.

Nowadays, pharmaceuticals (PCs) are ubiquitous in aquatic ecosystems. It is known that these compounds have ecotoxic effects on aquatic organisms at low concentrations. Moreover, some of them can bioaccumulate inside organisms or trophic webs exposed at environmental concentrations and amplify ecotoxic impacts. PCs can bioaccumulate in two ways: exposure to a medium (e.g., respiration, diffusion, etc.) and/or through the dietary route. Here, we try to assess the respective contributions of these two forms of contamination of the first two levels of an aquatic trophic web. We exposed Daphnia magna for 5 days to 0, 5, and 50 µg/L (15)N-tamoxifen and then fed them with control and contaminated diets. We used an isotopic method to measure the tamoxifen content inside the daphnids after several minutes' exposure and every day before and after feeding. We found that tamoxifen is very bioaccumulative inside daphnids (BCF up to 12,000) and that the dietary route has a significant impact on contamination by tamoxifen (BAF up to 22,000), especially at low concentrations in medium.

Bioconcentration of (15)N-tamoxifen at environmental concentration in liver, gonad and muscle of Danio rerio.

Pharmaceutical compounds (PCs) are ubiquitous in aquatic ecosystems. In addition to the direct ecotoxicological risk presented by certain PCs, others can accumulate inside organisms and along trophic webs, subsequently contaminating whole ecosystems. We studied the bioconcentration of a bioaccumulative PC already found several times in the environment: tamoxifen. To this end, we exposed Danio rerio for 21d to (15)N-tamoxifen concentrations ranging from 0.1 to 10µg/L and used an analytic method based on stable isotopes to evaluate the tamoxifen content in these organisms. The evolution of the (15)N/(14)N ratio was thus measured in liver, muscle and gonads of exposed fish compared to control fish. We succeeded in quantifying (15)N-tamoxifen bioconcentrations at all the exposure concentrations tested. The highest bioconcentration factors of tamoxifen measured were 14,920 in muscle, 73,800 in liver and 85,600 in gonads of fish after 21d exposure at a nominal concentration of 10µg/L. However, these bioconcentration factors have to be considered as maximal values (BCFMAX). Indeed, despite its proven stability, tamoxifen can be potentially partially degraded during experiments. We now need to refine these results by using a direct analytic method (i.e. LC-MS/MS).

Quantitative and qualitative assessment of the impact of climate change on a combined sewer overflow and its receiving water body.

Projections from the Canadian Regional Climate Model (CRCM) for the southern part of the province of Québec, Canada, suggest an increase in extreme precipitation events for the 2050 horizon (2041-2070). The main goal of this study consisted in a quantitative and qualitative assessment of the impact of the 20 % increase in rainfall intensity that led, in the summer of 2013, to overflows in the "Rolland-Therrien" combined sewer system in the city of Longueuil, Canada. The PCSWMM 2013 model was used to assess the sensitivity of this overflow under current (2013) and future (2050) climate conditions. The simulated quantitative variables (peak flow, Q(CSO), and volume discharged, VD) served as the basis for deriving ecotoxicological risk indices and event fluxes (EFs) transported to the St. Lawrence (SL) River. Results highlighted 15 to 500% increases in VD and 13 to 148% increases in Q(CSO) by 2050 (compared to 2013), based on eight rainfall events measured from May to October. These results show that (i) the relationships between precipitation and combined sewer overflow variables are not linear and (ii) the design criteria for current hydraulic infrastructure must be revised to account for the impact of climate change (CC) arising from changes in precipitation regimes. EFs discharged into the SL River will be 2.24 times larger in the future than they are now (2013) due to large VDs resulting from CC. This will, in turn, lead to excessive inputs of total suspended solids (TSSs) and tracers for numerous urban pollutants (organic matter and nutrients, metals) into the receiving water body. Ecotoxicological risk indices will increase by more than 100% by 2050 compared to 2013. Given that substantial VDs are at play, and although CC scenarios have many sources of uncertainty, strategies to adapt this drainage network to the effects of CC will have to be developed.

Tamoxifen ecotoxicity and resulting risks for aquatic ecosystems.

Tamoxifen, a drug used to treat cancer, is regularly found in hydrosystems at concentrations of several hundred ng L(-1). To characterize its ecotoxicity, we implemented a battery of bioassays on organisms belonging to 3 different trophic levels: Pseudokirchneriella subcapitata, Chlorella vulgaris and Chlamydomonas reinhardtii, for primary producers, Daphnia magna (immobilization, grazing and reproduction) for primary consumers, and Danio rerio for secondary consumers (embryotoxicity test). In view of the results obtained and the ecotoxicity values of tamoxifen available in the literature, we established a PNEC (Predictive No Effect Concentration) equal to 81 ng L(-1) for continental water. This PNEC allowed us to calculate Risk Quotients (RQ) for 4 continental hydrosystems in 4 different countries in which measures of tamoxifen had already been performed on surface waters. In two of the situations studied, RQs were higher than 1, reaching a maximum of 2.6. These results show the need to deepen the characterization of ecotoxicological risks linked to the discharge of tamoxifen in surface waters. In addition, we propose applying this approach to other drug residues detected in the environment.

Experimental assessment of the bioconcentration of (15)N-tamoxifen in Pseudokirchneriella subcapitata.

Nowadays, pharmaceutical compounds (PC) are ubiquitous in aquatic ecosystems. In addition to direct ecotoxicity, the bioconcentration of PC in organisms is a phenomenon which could have an impact on the whole ecosystem. In order to study this phenomenon, we exposed unicellular algae (Pseudokirchneriella subcapitata) to (15)N-tamoxifen, an anticancer drug labelled with a stable nitrogen isotope used as a tracer. By measuring (15)N enrichment over time, we were able to measure the increase of tamoxifen content in algae. This enrichment was measured by an elemental analyser coupled with an isotopic ratio mass spectrometer (EA-IRMS). Algal cells were exposed for 7d to 3 concentrations of tamoxifen: 1, 10 and 100µgL(-1). Our result shows a high bioconcentration in algae from the first minutes of contact. The highest bioconcentration factor measured is around 26500. We also observe that bioconcentration is not linked to the exposure concentration. This study is the first to use stable isotopes in order to monitor PCs in aquatic organisms such as algae. The use of stable isotopes in ecotoxicology offers interesting perspectives in the field of contaminant transfer in organisms and along the trophic web.

Assessment of the ecotoxicological risk of combined sewer overflows for an aquatic system using a coupled "substance and bioassay" approach.

Very few tools are available for assessing the impact of combined sewer overflows (CSOs) on receiving aquatic environments. The main goal of the study was to assess the ecotoxicological risk of CSOs for a surface aquatic ecosystem using a coupled "substance and bioassay" approach. Wastewater samples from the city of Longueuil, Canada CSO were collected for various rainfall events during one summer season and analyzed for a large panel of substances (n = 116). Four bioassays were also conducted on representative organisms of surface aquatic systems (Pimephales promelas, Ceriodaphnia dubia, Daphnia magna, and Oncorhynchus mykiss). The analytical data did not reveal any ecotoxicological risk for St. Lawrence River organisms, mainly due to strong effluent dilution. However, the substance approach showed that, because of their contribution to the ecotoxicological hazard posed by the effluent, total phosphorus (Ptot), aluminum (Al), total residual chlorine, chromium (Cr), copper (Cu), pyrene, ammonia (N-NH4 (+)), lead (Pb), and zinc (Zn) require more targeted monitoring. While chronic ecotoxicity tests revealed a potential impact of CSO discharges on P. promelas and C. dubia, acute toxicity tests did not show any effect on D. magna or O. mykiss, thus underscoring the importance of chronic toxicity tests as part of efforts aimed at characterizing effluent toxicity. Ultimately, the study leads to the conclusion that the coupled "substance and bioassay" approach is a reliable and robust method for assessing the ecotoxicological risk associated with complex discharges such as CSOs.

Health risk assessment linked to filling coastal quarries with treated dredged seaport sediments.

Dredged seaport sediments raise complex management problems since it is no longer possible to discharge them into the sea. Traditional waste treatments are poorly adapted for these materials in terms of absorbable volumes and cost. In this context, filling quarries with treated sediments appears interesting but its safety regarding human health must be demonstrated. To achieve this, a specific methodology for assessing health risks has been developed and tested on three seaport sediments. This methodology includes the development of a conceptual model of the global scenario studied and the definition of specific protocols for each of its major steps. The approach proposed includes in particular the use of metrological and experimental tools that are new in this context: (i) an experimental lysimeter for characterizing the deposit emissions, and (ii) a geological radar for identifying potential preferential pathways between the sediment deposit and the groundwater. The application of this approach on the three sediments tested for the scenario studied showed the absence of health risk associated with the consumption of groundwater for substances having a "threshold effect" (risk quotient <1), and an acceptable risk for substances having a "non-threshold effect", with the notable exception of arsenic (individual risk equal to 3.10(-6)).

Stormwater retention basin efficiency regarding micropollutant loads and ecotoxicity.

Retention basin efficiency in micropollutant removal has not been very well studied, in particular for pollutants highlighted by the European Water Framework Directive of 2000 such as pesticides, polybrominated diphenyl ethers (PBDEs) and alkylphenols. This study is based on in situ experiments carried out on a stormwater retention basin with the aim of estimating the basin efficiency in trapping and removing micropollutants from stormwater run-off from an industrial catchment drained by a separate sewer system. Along with stormwater, the basin receives some dry weather effluent flows, which are supposedly non-polluted. Ninety-four substances from five families (metals, polycyclic aromatic hydrocarbons (PAHs), PBDEs, alkylphenols and pesticides) were analyzed during 10 event campaigns in urban wet weather discharges at the inlet and outlet of the basin. The ecotoxicity of the samples was also tested. The results show high inter-event variability in both chemical and ecotoxic characteristics. They indicate good event efficiency concerning heavy metals and most PAHs. The studied pesticides, mainly found in the dissolved fraction, were not trapped. Particulate fraction study highlighted that settling is not the main process explaining micropollutant removal in a retention basin, as was noted for alkylphenols and PBDEs.

Historical records, sources, and spatial trends of PCBs along the Rhône River (France).

Despite bans on PCB use since 1975 (open systems) and 1987 (closed systems), concentrations of PCBs in riverine fish in France continue to exceed regulatory levels. We present historical records of PCB concentrations in sediment cores from eight sites on the Rhône River, from Lake Geneva to the Mediterranean Sea. Maximum PCB concentrations (sum of seven indicator PCBs) increase downstream, from 11.50 µg/kg at the most upstream site to 417.1 µg/kg at the most downstream site. At some sites peak concentrations occur in sediment deposited as recently as the 2000s. Hierarchical clustering (five clusters) identified differences in PCB congener profiles within and between sites. Exponential models fit to decadal time windows indicate that rapid reductions in concentrations during about 1990-2000 have slowed, and that it might be decades before target concentrations in sediment that correspond to regulatory thresholds in fish will be reached at some sites.