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
