Advertisement

Environmental Science and Pollution Research

, Volume 24, Issue 36, pp 28102–28120 | Cite as

Polybrominated diphenyl ethers (PBDEs) in background air around the Aegean: implications for phase partitioning and size distribution

  • Athanasios BesisEmail author
  • Gerhard Lammel
  • Petr Kukučka
  • Constantini Samara
  • Aysun Sofuoglu
  • Yetkin Dumanoglu
  • Kostas Eleftheriadis
  • Giorgos Kouvarakis
  • Sait C. Sofuoglu
  • Vassiliki Vassilatou
  • Dimitra Voutsa
Research Article

Abstract

The occurrence and atmospheric behavior of tri- to deca-polybrominated diphenyl ethers (PBDEs) were investigated during a 2-week campaign concurrently conducted in July 2012 at four background sites around the Aegean Sea. The study focused on the gas/particle (G/P) partitioning at three sites (Ag. Paraskevi/central Greece/suburban, Finokalia/southern Greece/remote coastal, and Urla/Turkey/rural coastal) and on the size distribution at two sites (Neochorouda/northern Greece/rural inland and Finokalia/southern Greece/remote coastal). The lowest mean total (G + P) concentrations of ∑7PBDE (BDE-28, BDE-47, BDE-66, BDE-99, BDE-100, BDE-153, BDE-154) and BDE-209 (0.81 and 0.95 pg m−3, respectively) were found at the remote site Finokalia. Partitioning coefficients, K P, were calculated, and their linear relationships with ambient temperature and the physicochemical properties of the analyzed PBDE congeners, i.e., the subcooled liquid pressure (P L°) and the octanol-air partition coefficient (K OA), were investigated. The equilibrium adsorption (P L°-based) and absorption (K OA-based) models, as well as a steady-state absorption model including an equilibrium and a non-equilibrium term, both being functions of log K OA, were used to predict the fraction Φ of PBDEs associated with the particle phase. The steady-state model proved to be superior to predict G/P partitioning of BDE-209. The distribution of particle-bound PBDEs across size fractions < 0.95, 0.95–1.5, 1.5–3.0, 3.0–7.2, and > 7.2 μm indicated a positive correlation between the mass median aerodynamic diameter and log P L° for the less brominated congeners, whereas a negative correlation was observed for the high brominated congeners. The potential source regions of PBDEs were acknowledged as a combination of long-range transport with short-distance sources.

Keywords

Absorption/adsorption models Gas/particle partitioning Long-range transport Aerosol mass size distribution 

Notes

Acknowledgements

We thank John Manousis (Region of Central Macedonia) and John Douros (AUTH) for meteorological data and data analysis; John Manousis, Jiři Kohoutek, Christos Efstathiou, and Roman Prokeš (MU) for on-site support; Petra Pribylová and Lenka Vanková (MU) and Mustafa Odabasi (DEU) for chemical analyses and laboratory support; and Pourya Shahpoury (MPI) for discussion.

Funding information

This research was supported by the Granting Agency of the Czech Republic (project No. 312334), the Czech Ministry of Education, Youth, and Sports (LO1214 and LM2015051), the Izmir Institute of Technology Scientific Research Foundation (2013İYTE14), and the European Union FP7 (No. 262254 ACTRIS).

Supplementary material

11356_2017_285_MOESM1_ESM.pdf (380 kb)
ESM 1 (PDF 379 kb).

References

  1. Besis A, Botsaropoulou E, Voutsa D, Samara C (2015) Particle-size distribution of polybrominated diphenyl ethers (PBDEs) in the urban agglomeration of Thessaloniki, northern Greece. Atmos Environ 104:176–185.  https://doi.org/10.1016/j.atmosenv.2015.01.019 CrossRefGoogle Scholar
  2. Besis A, Samara C (2012) Polybrominated diphenyl ethers (PBDEs) in the indoor and outdoor environments—a review on occurrence and human exposure. Environ Pollut 169:217–229.  https://doi.org/10.1016/j.envpol.2012.04.009 CrossRefGoogle Scholar
  3. Besis A, Voutsa D, Samara C (2016) Atmospheric occurrence and gas-particle partitioning of PBDEs at industrial, urban and suburban sites of Thessaloniki, northern Greece: implications for human health. Environ Pollut 215:113–124.  https://doi.org/10.1016/j.envpol.2016.04.093 CrossRefGoogle Scholar
  4. Bezares-Cruz J, Jafvert CT, Hua I (2004) Solar photodecomposition of decabromodiphenyl ether: products and quantum yield. Environ Sci Technol 38:4149–4156.  https://doi.org/10.1021/es049608o CrossRefGoogle Scholar
  5. Cetin B, Odabasi M (2007a) Air–water exchange and dry deposition of polybrominated diphenyl ethers at a coastal site in Izmir Bay, Turkey. Environ Sci Technol 41:785–791.  https://doi.org/10.1021/es061368k CrossRefGoogle Scholar
  6. Cetin B, Odabasi M (2007b) Particle-phase dry deposition and air–soil gas-exchange of polybrominated diphenyl ethers (PBDEs) in Izmir, Turkey. Environ Sci Technol 41:4986–4992.  https://doi.org/10.1021/es070187v CrossRefGoogle Scholar
  7. Cetin B, Odabasi M (2008) Atmospheric concentrations and phase partitioning of polybrominated diphenyl ethers (PBDEs) in Izmir, Turkey. Chemosphere 71:1067–1078.  https://doi.org/10.1016/j.chemosphere.2007.10.052 CrossRefGoogle Scholar
  8. Cetin B, Odabasi M (2011) Polybrominated diphenyl ethers (PBDEs) in indoor and outdoor window organic films in Izmir, Turkey. J Hazard Mater 185:784–791.  https://doi.org/10.1016/j.jhazmat.2010.09.089 CrossRefGoogle Scholar
  9. Chao HR, Tsou TC, Huang HL, Chang-Chien GP (2011) Levels of breast milk PBDEs from southern taiwan and their potential impact on neurodevelopment. Pediatr Res 70:596–600.  https://doi.org/10.1203/PDR.0b013e3182320b9b CrossRefGoogle Scholar
  10. Chen LG et al (2006) Concentration levels, compositional profiles, and gas-particle partitioning of polybrominated diphenyl ethers in the atmosphere of an urban city in South China. Environ Sci Technol 40:1190–1196.  https://doi.org/10.1021/es052123v CrossRefGoogle Scholar
  11. Chrysikou LP, Samara CA (2009) Seasonal variation of the size distribution of urban particulate matter and associated organic pollutants in the ambient air. Atmos Environ 43:4557–4569.  https://doi.org/10.1016/j.atmosenv.2009.06.033 CrossRefGoogle Scholar
  12. Cincinelli A, Pieri F, Martellini T, Passaponti M, Del Bubba M, Del Vento S, Katsoyiannis AA (2014) Atmospheric occurrence and gas-particle partitioning of PBDEs in an industrialised and urban area of Florence, Italy. Aerosol Air Qual Res 14:1121–1130.  https://doi.org/10.4209/aaqr.2013.01.0021 Google Scholar
  13. Darnerud PO, Eriksen GS, Jóhannesson T, Larsen PB, Viluksela M (2001) Polybrominated diphenyl ethers: occurrence, dietary exposure, and toxicology. Environ Health Perspect 109:49–68CrossRefGoogle Scholar
  14. Dayan U, Ricaud P, Zbinden R, Dulac F (2017) Atmospheric pollution concentrations over the Eastern Mediterranean during summer—a review. Atmos Chem Phys Discuss 2017:1–65.  https://doi.org/10.5194/acp-2017-79 CrossRefGoogle Scholar
  15. de Wit CA, Herzke D, Vorkamp K (2010) Brominated flame retardants in the Arctic environment—trends and new candidates. Sci Total Environ 408:2885–2918.  https://doi.org/10.1016/j.scitotenv.2009.08.037 CrossRefGoogle Scholar
  16. Finizio A, Mackay D, Bidleman T, Harner T (1997) Octanol-air partition coefficient as a predictor of partitioning of semi-volatile organic chemicals to aerosols. Atmos Environ 31:2289–2296.  https://doi.org/10.1016/S1352-2310(97)00013-7 CrossRefGoogle Scholar
  17. Gevao B et al (2013) Seasonal variations in the atmospheric concentrations of polybrominated diphenyl ethers in Kuwait. Sci Total Environ 454–455:534–541.  https://doi.org/10.1016/j.scitotenv.2013.02.073 CrossRefGoogle Scholar
  18. Harner T, Bidleman TF (1998) Octanol-air partition coefficient for describing particle/gas partitioning of aromatic compounds in urban air. Environ Sci Technol 32:1494–1502.  https://doi.org/10.1021/es970890r CrossRefGoogle Scholar
  19. Harner T, Shoeib M (2002) Measurements of octanol–air partition coefficients (KOA) for polybrominated diphenyl ethers (PBDEs): predicting partitioning in the environment. J Chem Eng Data 47:228–232.  https://doi.org/10.1021/je010192t CrossRefGoogle Scholar
  20. Harner T, Shoeib M, Diamond M, Ikonomou M, Stern G (2006) Passive sampler derived air concentrations of PBDEs along an urban–rural transect: spatial and temporal trends. Chemosphere 64:262–267.  https://doi.org/10.1016/j.chemosphere.2005.12.018 CrossRefGoogle Scholar
  21. He W et al (2014) Atmospheric PBDEs at rural and urban sites in central China from 2010 to 2013: residual levels, potential sources and human exposure. Environ Pollut 192:232–243.  https://doi.org/10.1016/j.envpol.2014.03.014 CrossRefGoogle Scholar
  22. La Guardia MJ, Hale RC, Harvey E (2006) Detailed polybrominated diphenyl ether (PBDE) congener composition of the widely used penta-, octa-, and deca-PBDE technical flame-retardant mixtures. Environ Sci Technol 40:6247–6254.  https://doi.org/10.1021/es060630m CrossRefGoogle Scholar
  23. Lammel G et al (2015) Air and seawater pollution and air–sea gas exchange of persistent toxic substances in the Aegean Sea: spatial trends of PAHs, PCBs, OCPs and PBDEs. Environ Sci Pollut Res 22:11301–11313.  https://doi.org/10.1007/s11356-015-4363-4 CrossRefGoogle Scholar
  24. Lammel G, Mulder MD, Shahpoury P, Kukučka P, Lišková H, Přibylová P, Prokeš R, Wotawa G (2016). Nitropolyaromatic hydrocarbons—gas-particle partitioning, mass size distribution, and formation along transport in marine and continental background air in Europe, submittedGoogle Scholar
  25. Landlová L, Čupr P, Franců J, Klánová J, Lammel G (2014) Composition and effects of inhalable size fractions of atmospheric aerosols in the polluted atmosphere: part I. PAHs, PCBs and OCPs and the matrix chemical composition. Environ Sci Pollut Res 21:6188–6204.  https://doi.org/10.1007/s11356-014-2571-y CrossRefGoogle Scholar
  26. Li Y-F, Jia H-L (2014) Prediction of gas/particle partition quotients of polybrominated diphenyl ethers (PBDEs) in north temperate zone air: an empirical approach. Ecotoxicol Environ Saf 108:65–71.  https://doi.org/10.1016/j.ecoenv.2014.05.028 CrossRefGoogle Scholar
  27. Li YF, Ma WL, Yang M (2015) Prediction of gas/particle partitioning of polybrominated diphenyl ethers (PBDEs) in global air: a theoretical study. Atmos Chem Phys 15:1669–1681.  https://doi.org/10.5194/acp-15-1669-2015 CrossRefGoogle Scholar
  28. Li Y-F, Qiao L-N, Ren N-Q, Sverko E, Mackay D, Macdonald RW (2017) Decabrominated diphenyl ethers (BDE-209) in Chinese and global air: levels, gas/particle partitioning, and long-range transport: is long-range transport of BDE-209 really governed by the movement of particles? Environ Sci Technol 51:1035–1042.  https://doi.org/10.1021/acs.est.6b05395 CrossRefGoogle Scholar
  29. Luo P, Ni HG, Bao LJ, Li SM, Zeng EY (2014) Size distribution of airborne particle-bound polybrominated diphenyl ethers and its implications for dry and wet deposition Environ Sci Technol 48:13793–13799 doi: https://doi.org/10.1021/es5042018
  30. Lyu Y, Xu T, Li X, Cheng T, Yang X, Sun X, Chen J (2016) Size distribution of particle-associated polybrominated diphenyl ethers (PBDEs) and their implications for health. Atmospheric Measurement Techniques 9:1025–1037.  https://doi.org/10.5194/amt-9-1025-2016 CrossRefGoogle Scholar
  31. Mandalakis M, Besis A, Stephanou EG (2009) Particle-size distribution and gas/particle partitioning of atmospheric polybrominated diphenyl ethers in urban areas of Greece. Environ Pollut 157:1227–1233.  https://doi.org/10.1016/j.envpol.2008.12.010 CrossRefGoogle Scholar
  32. Mulder MD, Heil A, Kukučka P, Kuta J, Přibylová P, Prokeš R, Lammel G (2015) Long-range atmospheric transport of PAHs, PCBs and PBDEs to the central and eastern Mediterranean and changes of PCB and PBDE congener patterns in summer 2010. Atmos Environ 111:51–59.  https://doi.org/10.1016/j.atmosenv.2015.03.044 CrossRefGoogle Scholar
  33. Odabasi M et al (2009) Electric arc furnaces for steel-making: hot spots for persistent organic pollutants. Environ Sci Technol 43:5205–5211.  https://doi.org/10.1021/es900863s CrossRefGoogle Scholar
  34. Odabasi M et al (2015b) Biomonitoring the spatial and historical variations of persistent organic pollutants (POPs) in an industrial region. Environ Sci Technol 49:2105–2114.  https://doi.org/10.1021/es506316t CrossRefGoogle Scholar
  35. Odabasi M, Cetin B, Bayram A (2015a) Persistent organic pollutants (POPs) on fine and coarse atmospheric particles measured at two (urban and industrial) sites. Aerosol Air Qual Res 15:1894–1905.  https://doi.org/10.4209/aaqr.2015.02.0118 Google Scholar
  36. Okonski K et al (2014) Particle size distribution of halogenated flame retardants and implications for atmospheric deposition and transport. Environ Sci Technol 48:14426–14434.  https://doi.org/10.1021/es5044547 CrossRefGoogle Scholar
  37. O’Shaughnessy PT, Raabe OG (2003) A comparison of cascade impactor data reduction methods. Aerosol Sci Technol 37:187–200.  https://doi.org/10.1080/02786820300956 CrossRefGoogle Scholar
  38. Pankow JF (1987) Review and comparative analysis of the theories on partitioning between the gas and aerosol particulate phases in the atmosphere. Atmospheric Environment (1967) 21:2275–2283.  https://doi.org/10.1016/0004-6981(87)90363-5 CrossRefGoogle Scholar
  39. Pankow JF (1998) Further discussion of the octanol/air partition coefficient Koa as a correlating parameter for gas/particle partitioning coefficients. Atmos Environ 32:1493–1497.  https://doi.org/10.1016/S1352-2310(97)00383-X CrossRefGoogle Scholar
  40. Ruijgrok W, Davidson CI, Nicholson KW (1995) Dry deposition of particles: implications and recommendations for mapping of deposition over Europe. Tellus Series B 47(B):587–601Google Scholar
  41. Samara C, Voutsa D, Kouras A, Eleftheriadis K, Maggos T, Saraga D, Petrakakis M (2014) Organic and elemental carbon associated to PM10 and PM2.5 at urban sites of northern Greece. Environ Sci Pollut Res 21:1769–1785.  https://doi.org/10.1007/s11356-013-2052-8 CrossRefGoogle Scholar
  42. Shy CG, Huang HL, Chao HR, Chang-Chien GP (2012) Cord blood levels of thyroid hormones and IGF-1 weakly correlate with breast milk levels of PBDEs in Taiwan. Int J Hyg Environ Health 215:345–351.  https://doi.org/10.1016/j.ijheh.2011.10.004 CrossRefGoogle Scholar
  43. Sofuoglu SC, Sofuoglu A, Holsen TM, Alexander CM, Pagano JJ (2013) Atmospheric concentrations and potential sources of PCBs, PBDEs, and pesticides to Acadia National Park. Environ Pollut 177:116–124.  https://doi.org/10.1016/j.envpol.2013.02.015 CrossRefGoogle Scholar
  44. Stohl A, Forster C, Frank A, Seibert P, Wotawa G (2005) Technical note: the Lagrangian particle dispersion model FLEXPART version 6.2. Atmos Chem Phys 5:2461–2474.  https://doi.org/10.5194/acp-5-2461-2005 CrossRefGoogle Scholar
  45. Tittlemier SA, Halldorson T, Stern GA, Tomy GT (2002) Vapor pressures, aqueous solubilities, and Henry’s law constants of some brominated flame retardants. Environ Toxicol Chem 21:1804–1810CrossRefGoogle Scholar
  46. Ugranli T et al (2016) POPs in a major conurbation in Turkey: ambient air concentrations, seasonal variation, inhalation and dermal exposure, and associated carcinogenic risks. Environ Sci Pollut Res 23:22500–22512.  https://doi.org/10.1007/s11356-016-7350-5 CrossRefGoogle Scholar
  47. UNEP/POPS/COP.4/17 Recommendations of the persistent organic pollutants review committee of the Stockholm convention to amend annexes A, B or C of the convention. In: Stockholm Convention on Persistent Organic Pollutants, Stockholm, 4/2/2009 2009Google Scholar
  48. Wang C et al (2012) Summer atmospheric polybrominated diphenyl ethers in urban and rural areas of northern China. Environ Pollut 171:234–240.  https://doi.org/10.1016/j.envpol.2012.07.041 CrossRefGoogle Scholar
  49. Wang Z-Y, Zeng X-L, Zhai Z-C (2008) Prediction of supercooled liquid vapor pressures and n-octanol/air partition coefficients for polybrominated diphenyl ethers by means of molecular descriptors from DFT method. Sci Total Environ 389:296–305.  https://doi.org/10.1016/j.scitotenv.2007.08.023 CrossRefGoogle Scholar
  50. Wania F, Dugani CB (2003) Assessing the long-range transport potential of polybrominated diphenyl ethers: a comparison of four multimedia models. Environ Toxicol Chem 22:1252–1261.  https://doi.org/10.1002/etc.5620220610 CrossRefGoogle Scholar
  51. Xiao H et al (2012) Atmospheric concentrations of halogenated flame retardants at two remote locations: the Canadian High Arctic and the Tibetan Plateau. Environ Pollut 161:154–161.  https://doi.org/10.1016/j.envpol.2011.09.041 CrossRefGoogle Scholar
  52. Xu H-Y, Zou J-W, Yu Q-S, Wang Y-H, Zhang J-Y, Jin H-X (2007) QSPR/QSAR models for prediction of the physicochemical properties and biological activity of polybrominated diphenyl ethers. Chemosphere 66:1998–2010.  https://doi.org/10.1016/j.chemosphere.2006.07.072 CrossRefGoogle Scholar
  53. Yang M et al (2013) Polybrominated diphenyl ethers in air across China: levels, compositions, and gas-particle partitioning. Environ Sci Technol 47:8978–8984.  https://doi.org/10.1021/es4022409 CrossRefGoogle Scholar
  54. Zhang B-Z, Zhang K, Li S-M, Wong CS, Zeng EY (2012) Size-dependent dry deposition of airborne polybrominated diphenyl ethers in urban Guangzhou, China. Environ Sci Technol 46:7207–7214.  https://doi.org/10.1021/es300944a CrossRefGoogle Scholar
  55. Zhou S, Lee AKY, McWhinney RD, Abbatt JPD (2012) Burial effects of organic coatings on the heterogeneous reactivity of particle-borne benzo[a]pyrene (BaP) toward ozone. J Phys Chem A 116:7050–7056.  https://doi.org/10.1021/jp3030705 CrossRefGoogle Scholar
  56. Zhou S, Shiraiwa M, McWhinney RD, Poschl U, JPD A (2013) Kinetic limitations in gas-particle reactions arising from slow diffusion in secondary organic aerosol. Faraday Discuss 165:391–406.  https://doi.org/10.1039/C3FD00030C CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany 2017

Authors and Affiliations

  • Athanasios Besis
    • 1
    Email author
  • Gerhard Lammel
    • 2
    • 3
  • Petr Kukučka
    • 2
    • 4
  • Constantini Samara
    • 1
  • Aysun Sofuoglu
    • 5
  • Yetkin Dumanoglu
    • 6
  • Kostas Eleftheriadis
    • 7
  • Giorgos Kouvarakis
    • 8
  • Sait C. Sofuoglu
    • 5
  • Vassiliki Vassilatou
    • 7
  • Dimitra Voutsa
    • 1
  1. 1.Department of Chemistry, Environmental Pollution Control LaboratoryAristotle University of ThessalonikiThessalonikiGreece
  2. 2.Research Centre for Toxic Compounds in the EnvironmentMasaryk UniversityBrnoCzech Republic
  3. 3.Multiphase Chemistry DepartmentMax Planck Institute for ChemistryMainzGermany
  4. 4.School of Science and Technology, Man-Technology-Environment Research Center (MTM)Örebro UniversityOrebroSweden
  5. 5.Department of Chemical Engineering and Environmental Research CenterIzmir Institute of TechnologyIzmirTurkey
  6. 6.Department of Environmental EngineeringDokuz Eylul UniversityIzmirTurkey
  7. 7.Institute of Nuclear Technology and Radiation ProtectionNCSR Demokritos InstituteAthensGreece
  8. 8.Department of Chemistry, Environmental Chemical Processes LaboratoryUniversity of CreteHeraklionGreece

Personalised recommendations