Polybrominated diphenyl ethers (PBDEs) in background air around the Aegean: implications for phase partitioning and size distribution
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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.
KeywordsAbsorption/adsorption models Gas/particle partitioning Long-range transport Aerosol mass size distribution
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.
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).
- 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
- 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
- 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
- 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
- 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
- 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
- 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
- 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
- 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