Landfills and waste water treatment plants as sources of ... - GKSS

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INTRODUCTION 175 chemicals classified as flame retardants (WHO 1997). Besides inorganic and nitrogenbased flame retardants, there is a major group of halogenated flame retardants in use. Among halogenated flame retardants, brominated flame retardants (BFRs) are the most important ones. This is particularly because of high efficiency of bromine in trapping free radicals produced during combustion processes and the low decomposition temperatures, compared to other halogens such as fluorine. Furthermore, bromines bound to organic carbons are characterized by a long-lasting stability during lifetime of the products as well as sufficient compatibility to the target polymer. This suitability of bromine results in more than 75 different aliphatic and aromatic BFRs (Alaee et al. 2003). Among BFRs, polybrominated diphenyl ethers (PBDEs) are widely applied as flame retardants. Beside their favourable properties as flame retardants, PBDEs are reported to be persistent in the environment, have low water solubility as well as high lipohilicy and tend therefore to accumulate in biota and sediments (De Wit 2002). Since they are simply blended to the product to be protected, they have a strong potential of being released throughout the lifecycle. The chemical structures of PBDEs consist of diphenyl ether molecules containing 10 hydrogen atoms, which can be exchanged with bromine to varying degrees. This results in 209 possible congeners. Due to structural similarities to polychlorinated diphenyl ethers (PCBs), the same nomenclature is used as introduced by Ballschmiter and Zell (1980). The majority of PBDEs were produced in three commercial formulations: pentaBDE, octaBDE and decaBDE. These three formulations contain varying proportions of the respective PBDE congeners. PBDE congeners analysed in this study (table 2) were selected according to the three commercial formulations and their main ingredients as suggested by Law et al. (2006). Basically, musk is a naturally gland secretion of the male musk deer (Moschus moscherifus L.) that has been used as fragrance for centuries. Until the 19 th century musk fragrances were completely obtained from those natural sources. However, since the 1950s musk compounds are almost completely of artificial origin (Sommer 2004). They have been used in various personal care products and household commodities, such as deodorants, shampoos, perfumes, detergents and washing powders. After their use they are predominantly discharged into the sewage system and can finally reach aquatic ecosystems. Due to their high lipophilicy, musk fragrances tend to accumulate in aquatic biota (Rimkus 1999). In general, musk fragrances can be divided in three substance classes (aromatic nitro musks, polycyclic musks and macrocyclic musk fragrances) that exhibit a common flavour, the distinct musk flavour. Nitro musks are two or three-folded nitrated benzenes that comprise alkyl-, keto- or methoxy moieties (Sommer 2004). Compared to the nitro musks, polycyclic musk fragrances 2
INTRODUCTION are characterised by increased light and alkali resistance as well as the ability to adsorb to fabrics (Sommer 2004). The chemical structure of polycyclic musk fragrances consists of polycyclic properties in combination with several methyl groups and either an ether or a carbonyl oxygen. Due to these structures they are capable to form different stereoisomers which determine their odourous character. Macrocyclic musks contain at least 14 carbon atoms and are characterized by a ring structure. Due to high production costs their commercial importance is still limited. Therefore, this study focuses on the two main nitro musks, musk ketone (MK) and musk xylene (MX) as well as five polycyclic musks that are frequently used. Chemical structures are given table 3. Table 1: Per- and polyfluorinated compounds analysed in this study Analytes Acronym CAS-Nr. Chemical structure 4:2 fluorotelomer alcohol 6:2 fluorotelomer alcohol 8:2 fluorotelomer alcohol 10:2 fluorotelomer alcohol 12:2 fluorotelomer alcohol 6:2 fluorotelomer acrylate 8:2 fluorotelomer acrylate 10:2 fluorotelomer acrylate N-methylperfluorooctane sulfonamido ethanol N-methyl- perfluorobutane sulfonamido ethanol N-ethylperfluorooctane sulfonamido ethanol Fluorotelomer alcohols (FTOHs) 4:2 FTOH 2043-47-2 F 3C 6:2 FTOH 647-42-7 F 3 C 8:2 FTOH 678-39-7 F 3 C 10:2 FTOH 865-86-1 F 3 C 12:2 FTOH 3929-77-5 F 3 C Fluorotelomer acrylates (FTAs) CF2 CF2 CH2 CF2 CH2 OH CF2 CF2 CF2 CH2 CF2 CF2 CH2 OH CF2 CF2 CF2 CF2 CH2 CF2 CF2 CF2 CH2 OH CF2 CF2 CF2 CF2 CF2 CH2 CF2 CF2 CF2 CF2 CH2 OH CF2 CF2 CF2 CF2 CF2 CF2 CH2 CF2 CF2 CF2 CF2 CF2 CH2 OH 6:2 FTA 17527-29-6 F3C CH2 CF2 CF2CF2CF2CH2CH2O CF2 O C C H 8:2 FTA 27905-45-9 F3C CH2 CH O 2 CF2CF2CF2CF2CF2CH2CH2O CF2 C C H 10:2 FTA 17741-60-5 F3C CF2 CH2CF2CF2CF2CF2CF2CF2CH2CH2O CF2 O C C H Perfluoroalkyl sulfonamido ethanols (FASEs) MeFOSE 24448-09-7 MeFBSE 34454-97-2 EtFOSE 1691-99-2 CH 2 F3C O CF2 CF2 CF2 CF2 CF CH 2 CF2 CF2 S 2 N O CH3 CH3OH F3C O CF2 CF2 CF CH 2 S 2 N O CH3 CH3OH F3C O CF2 CF2 CF2 CF2 CF CH 2 CF2 CF2 S 2 N O CH2 CH3OH CH3 3
Page 1: ISSN 0344-9629 Landfills and waste
Page 4 and 5: Die Berichte der GKSS werden kosten
Page 6 and 7: Deponien und Kläranlagen als Quell
Page 8 and 9: TABLE OF CONTENTS VI 4.2.5 Extracti
Page 10 and 11: LIST OF FIGURES Figure 20: Proporti
Page 12 and 13: LIST OF TABLES Table S6: Table of r
Page 14 and 15: ABBREVIATIONS BDE47 2,2',4,4'-Tetra
Page 16 and 17: ABBREVIATIONS MW molecular weight M
Page 18 and 19: 2 INTRODUCTION
Page 22 and 23: INTRODUCTION Table 1 cont. Analytes
Page 24 and 25: INTRODUCTION Table 3: Polycyclic mu
Page 26 and 27: INTRODUCTION Mabury 2006). This inc
Page 28 and 29: INTRODUCTION 1.3 Physico-chemical p
Page 30 and 31: INTRODUCTION 1.4 Environmental conc
Page 32 and 33: INTRODUCTION Chen et al. 2007a; Har
Page 34 and 35: INTRODUCTION prevent xenobiotica fr
Page 36 and 37: INTRODUCTION al. 2009c) and being d
Page 38 and 39: INTRODUCTION Table 6: Selection of
Page 40 and 41: INTRODUCTION 1.5 Sources Sources of
Page 42 and 43: OBJECTIVES 2. Objectives In recent
Page 44 and 45: METHOD OPTIMISATION Simonich et al.
Page 46 and 47: METHOD OPTIMISATION used as carrier
Page 48 and 49: METHOD OPTIMISATION 3.3 Extraction
Page 50 and 51: METHOD OPTIMISATION 3.3 Results 3.3
Page 52 and 53: METHOD OPTIMISATION AHMI). For less
Page 54 and 55: METHOD OPTIMISATION 3.3.5 Extractio
Page 56 and 57: METHOD OPTIMISATION 3.4 Discussion
Page 58 and 59: METHOD OPTIMISATION partly due to h
Page 60 and 61: METHOD OPTIMISATION Figure 7: Final
Page 62 and 63: STUDY 1: LANDFILLS AS SOURCES volat
Page 64 and 65: STUDY 1: LANDFILLS AS SOURCES On ea
Page 66 and 67: STUDY 1: LANDFILLS AS SOURCES (Supe
Page 68 and 69: STUDY 1: LANDFILLS AS SOURCES Table
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STUDY 1: LANDFILLS AS SOURCES 52 c
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STUDY 1: LANDFILLS AS SOURCES 4.3.2
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STUDY 1: LANDFILLS AS SOURCES 4.5 D
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STUDY 1: LANDFILLS AS SOURCES conce
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STUDY 1: LANDFILLS AS SOURCES influ
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STUDY 2: WASTE WATER TREATMENT PLAN
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CONCLUSIONS AND OUTLOOK BDE183 were
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REFERENCES wastewater treatment/pol
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REFERENCES Capuano, F. Cavalchi, B.
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REFERENCES Dreyer, A. Temme, C. Stu
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REFERENCES Harada, K. Nakanishi, S.
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REFERENCES Kallenborn, R. Gatermann
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REFERENCES sexual development, and
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REFERENCES Oros, D. R. Hoover, D. R
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REFERENCES Rimkus, G. (1995): Nitro
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REFERENCES Smithwick, M. Mabury, S.
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REFERENCES USEPA (2006): 2010/2015
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REFERENCES Zhao, Y.-X. Qin, X.-F. L
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SUPPORTING INFORMATION Figure S3: H
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SUPPORTING INFORMATION Table S1: Ta
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SUPPORTING INFORMATION Table S2: Ma
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SUPPORTING INFORMATION Table S5: Ta
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SUPPORTING INFORMATION Table S7: Bl
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SUPPORTING INFORMATION Table S11: P
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SUPPORTING INFORMATION Figure S7: S
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SUPPORTING INFORMATION Figure S7 co
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SUPPORTING INFORMATION Table S16: T
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SUPPORTING INFORMATION Table S19: M
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ERKLÄRUNG DER SELBSTSTÄNDIGEN VER
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