Integrating chemical analysis and bioanalysis to evaluate the contribution of wastewater effluent on the micropollutant burden in small streams

Surface waters can contain a range of micropollutants from point sources, such as wastewater effluent, and diffuse sources, such as agriculture. Characterizing the source of micropollutants is important for reducing their burden and thus mitigating adverse effects on aquatic ecosystems. In this study, chemical analysis and bioanalysis were applied to assess the micropollutant burden during low flow conditions upstream and downstream of three wastewater treatment plants (VVWTPs) discharging into small streams in the Swiss Plateau. The upstream sites had no input of wastewater effluent, allowing a direct comparison of the observed effects with and without the contribution of wastewater. Four hundred and five chemicals were analyzed, while the applied bioassays included activation of the aryl hydrocarbon receptor, activation of the androgen receptor, activation of the estrogen receptor, photosystem II inhibition, acetylcholinesterase inhibition and adaptive stress responses for oxidative stress, genotoxicity and inflammation, as well as assays indicative of estrogenic activity and developmental toxicity in zebrafish embryos. Chemical analysis and bioanalysis showed higher chemical concentrations and effects for the effluent samples, with the lowest chemical concentrations and effects in most assays for the upstream sites. Mixture toxicity modeling was applied to assess the contribution of detected chemicals to the observed effect. For most bioassays, very little of the observed effects could be explained by the detected chemicals, with the exception of photosystem II inhibition, where herbicides explained the majority of the effect. This emphasizes the importance of combining bioanalysis with chemical analysis to provide a more complete picture of the micropollutant burden. While the wastewater effluents had a significant contribution to micropollutant burden downstream, both chemical analysis and bioanalysis showed a relevant contribution of diffuse sources from upstream during low flow conditions, suggesting that upgrading WWTPs will not completely reduce the micropollutant burden, but further source control measures will be required. (C) 2016 Elsevier B.V. All rights reserved.

Elimination of micropollutants in wastewater treatment plants: Ozonation or activated carbon? Conclusions of a one-year pilot project

David Andrew Barry, Nathalie Chèvre Rossi, Luiz Felippe De Alencastro, Anoys Magnet, Jonas Margot, Luca Rossi

Many organic micropollutants present in wastewater, such as pharmaceuticals and pesticides, are poorly removed in conventional wastewater treatment plants (WWTP). To reduce the release of these substances into the aquatic environment, advanced treatments are necessary. Two advanced treatments were tested in pilot systems over more than one year at the municipal WWTP of Lausanne, Switzerland. The first pilot involves the ozonation of the effluent to oxidize organic substances. It is followed by sand filtration (SF) to remove the readily biodegradable reaction products. The second pilot consists of a powdered activated carbon (PAC) addition into the effluent to sorb micropollutants. It is followed either by a membrane filtration (ultrafiltration) or a sand filtration to separate the PAC from the treated water. A selection of 58 potentially problematic substances (pharmaceuticals, pesticides, endocrine disruptors) were regularly measured at different stages of treatment by ultra performance liquid chromatography coupled to a tandem mass spectrometer, and a large battery of ecotoxicological tests (16 in vitro and 9 in vivo assays with different organisms) were performed to evaluate the toxicity of the effluents. The results showed that most compounds were removed over 80% with an average ozone dose of about 5.5 mgO3/l or a PAC dose between 10 and 20 mg/l. Only some single compounds, such as X-ray contrast media, were only partially eliminated in both cases. A clear reduction in toxicity was also observed after the two treatments in most of the cases. These two processes (ozonation and PAC addition) are therefore effective to reduce the release of micropollutants into surface waters. Ozonation-SF and PAC-SF proved to be feasible in terms of implementation and operation at large-scale in WWTP, for relatively similar investment and operation costs (about 0.1 to 0.15 € per m3 treated based on local costs). Each technique has its advantages and disadvantages. Therefore the method selection should be made case by case for each WWTP depending on the local constraints (e.g. space, security, energy costs, existing treatment processes, sludge disposal process, need for disinfection, etc.), the quality and the quantity of incoming water and the desired output water quality

2011

Elimination of micropollutants in wastewater treatment plants : Ozonation or activated carbon? Conclusions of a one-year pilot project

David Andrew Barry, Luiz Felippe De Alencastro, Anoys Magnet, Jonas Margot, Luca Rossi

Many organic micropollutants present in wastewater, such as pharmaceuticals and pesticides, are poorly removed in conventional wastewater treatment plants (WWTP). To reduce the release of these substances into the aquatic environment, advanced treatments are necessary and may be soon mandatory in Switzerland. Two advanced treatments were tested in pilot systems over more than one year at the municipal WWTP of Lausanne, Switzerland. The first pilot involves the ozonation of the effluent to oxidize organic substances. It is followed by a sand filtration (SF) to remove the readily biodegradable reaction products. The second pilot consists of a powdered activated carbon (PAC) addition into the effluent to sorb micropollutants. It is followed either by a membrane filtration (ultrafiltration) or a sand filtration to separate the PAC from the treated water. A selection of 58 potentially problematic substances (pharmaceuticals, pesticides, endocrine disruptors) were regularly measured at different stages of treatment by ultra performance liquid chromatography coupled to a tandem mass spectrometer, and a large battery of ecotoxicological tests (16 in vitro and 9 in vivo assays with different organisms) were performed to evaluate the toxicity of the effluents. The results showed that most compounds were removed over 80% with an average ozone dose of about 5.5 mgO3/l or a PAC dose between 10 and 20 mg/l. Only some single compounds, such as X-ray contrast media, were only partially eliminated in both cases. A clear reduction in toxicity was also observed after the two treatments in most of the cases. These two processes (ozonation and PAC addition) are therefore effective to reduce the release of micropollutants into surface waters. Ozonation-SF and PAC-SF proved to be feasible in terms of implementation and operation at large-scale in WWTP, for relatively similar investment and operation costs (about 0.1 to 0.15 € per m3 treated based on local costs). Each technique has its advantages and disadvantages. Therefore the method selection should be made case by case for each WWTP depending on the local constraints (e.g. space, security, energy costs, existing treatment processes, sludge disposal process, need for disinfection, etc.), the quality and the quantity of incoming water and the desired output water quality.

2011

Origines et flux de biocides et de filtres UV dans les stations d'épuration des eaux usées

Cécile Plagellat

Adverse effects on the environment have become a matter of increasing concern considering the increase of industrialization and of the amount of commercialized chemicals. At present, approximately 100'000 substances are on the market, 3000 are sold at high volumes. In Europe, 200 to 300 new substances are authorized every year (in Switzerland, approximately 50). Contamination is induced by consumption of numerous products frequently applied by private or professional users. Persistence and ecotoxicity of certain organic compounds contained in these products might have impacts on the quality of our environment. Knowledge on potential sources of these substances is the first step in order to limit their release. The project developed within the present PhD thesis aims at determining the sources of certain compounds by applying material flux analysis on the basis of sewage sludge. Presently, a large number of anthropogenic organic compounds originating from private households, craft industry, industry and stormwater is disposed of into the collector system and ends up in sewage sludge. Carbendazim, diuron, Irgarol 1051®, octhilinone, permethrin, tributyltin (TBT) and triphenyltin (TPT) comprise numerous applications as biocides and pesticides whilst methylbenzylidene camphor (4-MBC), octyl methoxy cinnamate (OMC), octocrylene (OC) and octyl triazone (OT) are used as UV-screens (type UVB) in a large number of cosmetic products. Their toxic effects on non-target organisms and their potential for bioaccumulation give rise to environmental concern. These substances are used as ingredients in products of daily use and are disposed of into wastewater. Due to their physico-chemical properties they are more or less lipophilic and are likely to persist in sewage sludge. On the basis of the analysis of sewage sludge samples from well characterized sites (catchments and wastewater treatment plants, WWTPs) it is possible to determine the sources (private households, craft industry, industry and stormwater). The first step of this study was the development of analytical methods which allow for quantification of these compounds in sewage sludge. Due to their different physico-chemical properties, four different methods were required. These methods have recovery rates ranging between 75 and 106 % and limits of detection in the order of μg/kg dry matter. The analysis of sludge from 12 sites obtained within 2 sampling periods show that most of the substances are present in all samples. Mean concentrations were 6,8 μg/kg dm (dry matter) for carbendazim, 9,5 μg/ kg d.m. for diuron, 98,1 μg/kg d.m. for permethrin, 148 μg/kg d.m. for TBT, 1777 μg/kg d.m.for 4-MBC, 110 μg/kg d.m. for OMC, 4834 μg/kg d.m. for OC and 5517 μg/kg d.m. for OT. Octhilinone was not detected whilst Irgarol 1051® and TPT were found in 7 and 11 samples, respectively. The transfer of these compounds from wastewater into sludge is an important parameter for material flux analysis on the basis of sewage sludge. A study on the fate of carbendazime and permethrin during wastewater treatment has been carried out on two WWTPs. Whilst removal of permethrin was high (>94%) up to 70% of carbendazime present in sewage were found in treatment plant effluents. Adsorption is an important process for removal of permethrin. However, only 4 to 15 % of the load in wastewater was transferred to sewage sludge. Carbendazim is mainly associated to the aqueous phase and thus, a very small quantity ends up in sludge (approximately 1%). Therefore, the loads found in sewage sludge are more or less representative for consumption of the compounds in the catchments according to their physico-chemical properties. Additionally, it has been shown that the part of permethrine ending up in sludge depends on the treatment techniques of the WWTPs. Thus, for comparison of the pollutant loads in sewage sludge between different sites their fate in the WWTPs has to be known. The loads per inhabitant of the three well characterized types of sites have been calculated in order to determine the sources of the substances. Type A comprises sites with a separate sewer system and a catchment where mainly private households are present. Type B has a combined sewer system collecting sewage from private households, craft industry and stormwater whilst type C comprises a combined sewer system which includes effluents from private households and industry as well as stormwater. The results are as follows: Stromwater is considered as main source of carbendazim in wastewater whilst diuron originates mainly from stormwater and from industrial effluents. Private households contribute significantly to the loads of permethrine and TBT in sewage. For UV-screens the loads from private households are also important but stormwater and industrial effluents are likely to be potential sources as well. A difference in consumption between rural (type A) and more urban sites (type B and C) is possible which might hamper a proper estimate of the sources of UV-screens.

EPFL2004

Elimination of micropollutants in wastewater treatment plants: Ozonation or activated carbon? Conclusions of a one-year pilot project

David Andrew Barry, Nathalie Chèvre Rossi, Luiz Felippe De Alencastro, Anoys Magnet, Jonas Margot, Luca Rossi

2011

Elimination of micropollutants in wastewater treatment plants : Ozonation or activated carbon? Conclusions of a one-year pilot project

David Andrew Barry, Luiz Felippe De Alencastro, Anoys Magnet, Jonas Margot, Luca Rossi

Many organic micropollutants present in wastewater, such as pharmaceuticals and pesticides, are poorly removed in conventional wastewater treatment plants (WWTP). To reduce the release of these substances into the aquatic environment, advanced treatments are necessary and may be soon mandatory in Switzerland. Two advanced treatments were tested in pilot systems over more than one year at the municipal WWTP of Lausanne, Switzerland. The first pilot involves the ozonation of the effluent to oxidize organic substances. It is followed by a sand filtration (SF) to remove the readily biodegradable reaction products. The second pilot consists of a powdered activated carbon (PAC) addition into the effluent to sorb micropollutants. It is followed either by a membrane filtration (ultrafiltration) or a sand filtration to separate the PAC from the treated water. A selection of 58 potentially problematic substances (pharmaceuticals, pesticides, endocrine disruptors) were regularly measured at different stages of treatment by ultra performance liquid chromatography coupled to a tandem mass spectrometer, and a large battery of ecotoxicological tests (16 in vitro and 9 in vivo assays with different organisms) were performed to evaluate the toxicity of the effluents. The results showed that most compounds were removed over 80% with an average ozone dose of about 5.5 mgO3/l or a PAC dose between 10 and 20 mg/l. Only some single compounds, such as X-ray contrast media, were only partially eliminated in both cases. A clear reduction in toxicity was also observed after the two treatments in most of the cases. These two processes (ozonation and PAC addition) are therefore effective to reduce the release of micropollutants into surface waters. Ozonation-SF and PAC-SF proved to be feasible in terms of implementation and operation at large-scale in WWTP, for relatively similar investment and operation costs (about 0.1 to 0.15 € per m3 treated based on local costs). Each technique has its advantages and disadvantages. Therefore the method selection should be made case by case for each WWTP depending on the local constraints (e.g. space, security, energy costs, existing treatment processes, sludge disposal process, need for disinfection, etc.), the quality and the quantity of incoming water and the desired output water quality.

2011

Origines et flux de biocides et de filtres UV dans les stations d'épuration des eaux usées

Cécile Plagellat

EPFL2004