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

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INTRODUCTION 1.3 Physico-chemical properties Ionic and neutral PFCs, PBDEs and musk fragrances have considerably different physicochemical properties that determine their partitioning behaviour in the environment. In general, those properties are determined by their functional groups within the molecule as well as carbon-fluorine chain lengths (PFCs) or bromine content (PBDEs). Physico-chemical constants of substances investigated in this study are presented in table 4. The vapour pressures of PFSAs and PFCAs are generally low (Rayne and Forest 2009). In contrast, vapour pressures of neutral PFCs are more than 1000 times higher than those of ionic PFCs (Hekster et al. 2002; Rayne and Forest 2009). Vapour pressures of PBDEs are directly linked to the bromine content of the congener. Each additional bromine substitution causes a decline of vapour pressures by factors of 6-9 (Wong et al. 2001). Musk fragrances have comparable vapour pressures as FASEs. Therefore, neutral PFCs, BDE28 and BDE47 as well as musk fragrances are likely being transported as gaseous compounds in the atmosphere. Ionic PFCs and higher-brominated BDE congeners are not primarily expected in the gas phase, but atmospheric transport may still be possible if compounds adsorb to particles. The water solubilities of ionic PFCs are several orders of magnitude higher than those of neutral PFCs. Solubility decreases with increasing chain length of the both neutral and ionic PFCs (Rayne and Forest 2009). In contrast, musk fragrances are fairly well soluble in water. It is assumed that PBDEs are not predominantly transported via the water phase, whereas musk fragrances are more likely entering aqueous media (Rimkus 1999; Wania and Dugani 2003). Ionic PFCs are predominantly dissolved in the aqueous phase and/or bound to particles (especially long-chained PFSAs) (Rayne and Forest 2009). Polycyclic musk fragrances and FTOHs have relatively high Henry’s law constants that exceed those of PBDEs and nitro musks. For PBDEs, the tendency to volatilize from the water phase is influenced by the degree of bromination (Wong et al. 2001). In contrast to FTOHs, ionic PFCs have lower Henry constants (OECD 2002). Overall, it can be concluded that particularly FTOHs and polycyclic musk fragrances may volatilize from the aqueous phase to the atmosphere, whereas PBDEs and ionic PFCs rather partition to the water phases. It has been reported that KOA values for PBDEs, FTOHs, FASAs and FASEs are increasing with decreasing of temperatures (Harner and Shoeib 2002; Thuens et al. 2008; Dreyer et al. 2009a). Particularly highly brominated congeners are expected in the particle phase (Harner and Shoeib 2002). For musk fragrances KOA values have not yet been reported. However, 10
INTRODUCTION several studies observed those compounds predominantly in the gas phase (Peck and Hornbuckle 2004; Xie et al. 2007). A substance is bioaccumulative with a log KOW value greater than 5 (UNEP 2010). On the basis of this criterion, almost all substances of this study are assumed to be bioaccumulative. Due to the amphipilic character of ionic PFCs it is not possible to determine their KOW. However, their potential of bioaccumulation has been demonstrated (Conder et al. 2008). Table 4: Physico-chemical properties of semi-volatile and volatile PFCs, PBDEs and musk fragrances analysed in this study. MW: molecular weight, MP: melting point, VP: vapor pressure, KOW: octanol-water partition coefficient, KOA: octanol-air partition coefficient, SW: water solubility, kH: Henry’s law constant. Analyte MW (g mol -1 ) MP (°C) VP at 25 °C (Pa) log KOW at 25 °C log KOA at 25 °C SW (mg L -1 ) kH (Pa m 3 mol -1 ) Per- and polyfluorinated compounds (PFCs) 4:2 FTOH 264 - 252 1 3.28 2 4.57 4 974 5 174 1 6:2 FTOH 364 - 145.2 1 4.7 2 4.84 4 18.8 5 240 1 8:2 FTOH 464 - 45.9 1 6.14 2 5.58 4 0.194 23 650 1 10:2 FTOH 564 - 13.27 1 7.57 2 5.71 4 0.006 5 - 12:2 FTOH 664 - - - 6.2 4 - - 6:2 FTA 418 - - - 4.4 3 - - 8:2 FTA 518 - - - 5.2 3 - - 10:2 FTA 618 - - - 5.7 3 - - Me2FOSA 527 - - - - - - EtFOSA 527 - - - 6.6 3 - - MeFBSA 313 - - - - - - MeFOSA 513 - - - 6.3 3 - - PFOSA 499 - - - - - - EtFOSA 527 - 2.38 1 - - - - MeFOSE 557 - 0.33 1 - 6.4 3 - - MeFBSE 357 - - - - - - EtFOSE 571 - 0.19 1 - 6.7 3 - - Polybrominated Diphenyl Ethers (PBDEs) BDE28 407 64-64.5 6 0.0016 7 5.94 8 9.5 13 0.07 6 4.83 11 BDE47 486 78.75 9 0.00025 7 6.81 8 10.53 13 0.0146 10 0.85 11 BDE99 565 92.3 12 0.000018 7 7.32 8 11.31 13 0.009 6 0.6 11 BDE100 565 97 9 0.00005 7 7.24 8 11.31 13 0.00786 10 0.24 11 BDE153 644 160-163 6 0.0000058 7 7.9 8 11.82 13 0.001 6 0.26 11 BDE154 644 142 9 0.0000034 6 7.82 8 11.92 13 0.001 6 0.08 11 BDE183 722 171-173 6 0.0000066 (21 °C) 16 8.27 8 11.96 13 0.0005 16 0.0074 6 BDE209 960 300-310 14 0.0000046 (21 °C) 14 8.7 15 15.27 22
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 20 and 21: INTRODUCTION 175 chemicals classifi
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 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
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Page 68 and 69: STUDY 1: LANDFILLS AS SOURCES Table
Page 70 and 71: STUDY 1: LANDFILLS AS SOURCES 52 c
Page 74 and 75: 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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