Environmental Science and Pollution Research

, Volume 21, Issue 22, pp 12638–12650 | Cite as

Persistent organic pollutant accumulation in seasonal snow along an altitudinal gradient in the Tyrolean Alps

  • Lourdes Arellano
  • Joan O. GrimaltEmail author
  • Pilar Fernández
  • Jordi F. Lopez
  • Ulrike Nickus
  • Hansjoerg Thies
Research Article


The snow capacity for storage of a large number of pollutants such as polybromodiphenyl ethers (PBDE), including BDE-209, polycyclic aromatic hydrocarbons (PAHs), polychlorobiphenyls (PCBs), hexachlorocyclohexanes (HCHs; α- and γ-isomers), endosulfans (α- and β-isomers and the sulphate residue) and hexachlorobenzene (HCB), in a steep altitudinal gradient (1,101–2,500 m above sea level (asl); maximum planar distance 16 km) in a typical European mountain system, the Tyrolean Alps (Austria), was studied here for the first time. Snow samples representing the whole snowpack accumulated at the end of the cold season were collected in all cases. The snow specific surface area (SSA) of these samples, 140–260 cm2 g−1, was characteristic of aged snow with low retention capacity. PAHs were the pollutant group in highest concentrations (500–8,400 pg L−1). PCBs and PBDEs were found in concentrations of 460–900 and 8.5–290 pg L−1, respectively. From the fourteen investigated BDE congeners, only BDE-47, BDE-99, BDE-100 and BDE-209 were found above the detection limit, which is consistent with the results found in the only previous study in the Tatra Mountains (Slovakia) which also involved a steep gradient (1,683–2,634 m asl; maximum planar distance 5 km; Arellano et al. 2011) and confirm the capacity of these low-volatile compounds for long-range transport from distant sources. HCB was found in a concentration range of 34–55 pg L−1. Snow deposition fluxes of PCB-118, PCB-153, γ-HCH, α-endosulfan and BDE-47 showed statistically significant correlations with altitude, involving higher values at higher elevation. This trend may reflect cold trapping effects in view of the snow particle contents and SSA values. However, these gradients were only significant for this limited number of compounds within each pollutant group which may be explained by differences in physical-chemical properties of the compounds and the limited capacity of the aged snow for organic pollutant retention. In some other cases, for example benzo[a]pyrene, the observed vertical gradients may reflect higher preservations at lower temperatures.


Snow Tyrolean Alps Polybromodiphenyl ethers Organochlorine compounds Polycyclic aromatic hydrocarbons Altitudinal gradients 



We thank Roberto Quiroz for his assistance with lab work with snow in Innsbruck. Financial support was provided by the EU Project EUROLIMPACS (GOCE-CT-2003-505540) and ArcRisk (FP7-ENV-2008-1-226534). Financial support from the Spanish Ministry of Research through the GRACCIE Project (CSD2007-00067) is also acknowledged. The paper was also sponsored by the research group 2009SGR1178 from the Government of Catalonia. L.A. is thankful for a grant from Banco de Santander-CSIC.


  1. Aceves M, Grimalt JO (1993) Seasonally dependent size distributions of aliphatic and polycyclic aromatic hydrocarbons in urban aerosols from densely populated areas. Environ Sci Technol 27:2896–2908CrossRefGoogle Scholar
  2. Arellano L, Fernandez P, Tatosova J, Stuchlik E, Grimalt JO (2011) Long-range transported atmospheric pollutants in snowpacks accumulated at different altitudes in the Tatra Mountains (Slovakia). Environ Sci Technol 45:9268–9275CrossRefGoogle Scholar
  3. Bartrons M, Grimalt JO, Catalan J (2011) Altitudinal distributions of BDE-209 and other polybromodiphenyl ethers in high mountain lakes. Environ Pollut 159:1816–1822CrossRefGoogle Scholar
  4. Blais JM, Schinder DW, Muir DCG, Kimpe LE, Donald DB, Rosenberg B (1998) Accumulation of persistent organochlorine compounds in mountains of western Canada. Nature 395:585–588CrossRefGoogle Scholar
  5. Blais JM, Scheindler DW, Muir DCG, Sharp M, Donald D, Lafrenière M, Braekevelt E, Strachan WMJ (2001) Melting glaciers: a major source of persistent organochlorines to subalpine Bow Lake in Banff National Park, Canada. Ambio 30:410–415Google Scholar
  6. Blais JM, Charpentie S, Pick F, Kimpe LE, Amand AS, Regnault-Roger C (2006) Mercury, polybrominated diphenyl ether, organochlorine pesticide, and polychlorinated biphenyl concentrations in fish from lakes along an elevation transect in the French Pyrenees. Ecotoxicol Environ Saf 63:91–99CrossRefGoogle Scholar
  7. Burniston DA, Strachan WJM, Hoff JT, Wania F (2007) Changes in surface area and concentrations of semivolatile organic contaminants in aging snow. Environ Sci Technol 41:4932–4937CrossRefGoogle Scholar
  8. Carrera G, Fernández P, Vilanova RM, Grimalt JO, Ventura M, Camarero L, Catalan J, Nickus U, Thies H, Psenner R (1998) Analysis of trace polycyclic aromatic hydrocarbons and organochlorine compounds in atmospheric residues by solid-phase disk extraction. J Chromatogr A 823:189–196CrossRefGoogle Scholar
  9. Carrera G, Fernández P, Vilanova RM, Grimalt JO (2001) Persistent organic pollutants in snow from European high mountains areas. Atmos Environ 35:245–254CrossRefGoogle Scholar
  10. Carrera G, Fernández P, Grimalt JO (2002) Atmospheric deposition of organochlorine compounds to remote high mountain lakes of Europe. Environ Sci Technol 36:2581–2588CrossRefGoogle Scholar
  11. Daly GL, Wania F (2004) Simulating the influence of snow on the fate of organic compounds. Environ Sci Technol 38:4176–4186CrossRefGoogle Scholar
  12. de Wit CA, Herzke D, Vorkamp K (2010) Brominated flame retardants in the Arctic environment - trends and new candidates. Sci Total Environ 408:2885–2918CrossRefGoogle Scholar
  13. Estellano VH, Pozo K, Harner T, Franken M, Zaballa M (2008) Altitudinal and seasonal variations of persistent organic pollutants in the Bolivian Andes mountains. Environ Sci Technol 42:2528–2534CrossRefGoogle Scholar
  14. Fernandez P, Grimalt J (2003) On the global distribution of persistent organic pollutants. Chimia 57:514–521CrossRefGoogle Scholar
  15. Fernandez P, Vilanova RM, Grimalt JO (1999) Sediment fluxes of polycyclic aromatic hydrocarbons in European high altitude mountain lakes. Environ Sci Technol 33:3716–3722CrossRefGoogle Scholar
  16. Fernandez P, Grimalt JO, Vilanova RM (2002) Atmospheric gas-particle partitioning of polycyclic aromatic hydrocarbons in high mountain regions of Europe. Environ Sci Technol 36:1162–1168CrossRefGoogle Scholar
  17. Fernandez P, Carrera G, Grimalt JO, Ventura M, Camarero L, Catalan J, Nickus U, Thies H, Psenner R (2003) Factors governing the atmospheric deposition of polycyclic aromatic hydrocarbons to remote areas. Environ Sci Technol 37:3261–3267CrossRefGoogle Scholar
  18. Finizio A, Villa S, Raffaele F, Vighi M (2006) Variation of POP concentrations in fresh-fallen snow and air on an Alpine glacier (Monte Rosa). Ecotoxicol Environ Saf 63:25–32CrossRefGoogle Scholar
  19. Franz TP, Eisenreich SJ (1998) Snow scavenging of polychlorinated biphenyls and polycyclic aromatic hydrocarbons in Minnesota. Environ Sci Technol 32:1771–1778CrossRefGoogle Scholar
  20. Gabrieli J, Decet F, Luchetta A, Valt M, Pastore P, Barbante C (2010) Occurrence of PAH in the seasonal snowpack of the eastern Italian Alps. Environ Pollut 158:3130–3137CrossRefGoogle Scholar
  21. Gallego E, Grimalt JO, Bartrons M, Lopez JF, Camarero L, Catalan J, Stuchlik E, Battarbee R (2007) Altitudinal gradients of PBDEs and PCBs in fish from European high mountain lakes. Environ Sci Technol 41:2196–2202Google Scholar
  22. Grimalt JO, Fernandez P, Berdie L, Vilanova RM, Catalan J, Psenner R, Hofer R, Appleby PG, Rosseland BO, Lien L, Massabuau JC, Battarbee RW (2001) Selective trapping of organochlorine compounds in mountain lakes of temperate areas. Environ Sci Technol 35:2690–2697CrossRefGoogle Scholar
  23. Grimalt JO, Fernandez P, Quiroz R (2009) Input of organochlorine compounds by snow to European high mountain lakes. Freshw Biol 54:2533–2542CrossRefGoogle Scholar
  24. Hageman KJ, Simonich SL, Campbell DH, Wilsoln GR, Landers DH (2006) Atmospheric deposition of current-use and historic-use pesticides in snow at National Parks in the western United States. Environ Sci Technol 40:3174–3180CrossRefGoogle Scholar
  25. Hageman KJ, Hafner WD, Campbell DH, Jaffe DA, Landers DH, Simonich SLM (2010) Variability in pesticide deposition and source contributions to snowpack in Western U.S. National Parks. Environ Sci Technol 44:4452–4458CrossRefGoogle Scholar
  26. Halsall JC (2004) Investigating the occurrence of persistent organic pollutants (POPs) in the Arctic: their atmospheric behaviour and interaction with the seasonal snow pack. Environ Pollut 128:163–175CrossRefGoogle Scholar
  27. Herbert BMJ, Halsall CJ, Fitzpatrick L, Villa S, Jones KC, Thomas GO (2004) Use and validation of novel snow samplers for hydrophobic, semi-volatile organic compounds (SVOCs). Chemosphere 56:227–235CrossRefGoogle Scholar
  28. Herbert BMJ, Halsall CJ, Villa S, Jones KC, Kallenborn R (2005) Rapid changes in PCB and OC pesticide concentrations in Arctic snow. Environ Sci Technol 39:2998–3005CrossRefGoogle Scholar
  29. Herbert BMJ, Halsall CJ, Jones KC, Kallenborn R (2006a) Field investigation into the diffusion of semi-volatile organic compounds into fresh and aged snow. Atmos Environ 40:1385–1393CrossRefGoogle Scholar
  30. Herbert BMJ, Villa S, Halsall CJ (2006b) Chemical interactions with snow: understanding the behavior and fate of semi-volatile organic compounds in snow. Ecotoxicol Environ Saf 63:3–16CrossRefGoogle Scholar
  31. Jantunen LM, Helm PA, Kylin H, Bidleman TF (2008) Hexachlorocyclohexanes (HCHs) in the Canadian Archipelago. 2. Air-water gas exchange of a- and g-HCH. Environ Sci Technol 42:465–470CrossRefGoogle Scholar
  32. Kang JH, Choi SD, Park H, Baek SY, Hong S, Chang YS (2009) Atmospheric deposition of persistent organic pollutants to the East Rongbuk Glacier in the Himalayas. Sci Total Environ 408:57–63CrossRefGoogle Scholar
  33. Kang JH, Son MH, Hur SD, Hong S, Motoyama H, Fukui K, Chang YS (2012) Deposition of organochlorine pesticides into the surface snow of East Antarctica. Sci Total Environ 433:290–295CrossRefGoogle Scholar
  34. Kirchgeorg T, Dreyer A, Gabrieli J, Kehrwald N, Sigl M, Schwikowski M, Boutron C, Gambaro A, Barbante C, Ebinghaus R (2013) Temporal variations of perfluoroalkyl substances and polybrominated diphenyl ethers in alpine snow. Environ Pollut 178:367–374CrossRefGoogle Scholar
  35. 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 40:6247–6254CrossRefGoogle Scholar
  36. Lei YD, Wania F (2004) Is rain or snow a more efficient scavenger of organic chemicals? Atmos Environ 38:3557–3571CrossRefGoogle Scholar
  37. Meyer T, Muir DCG, Teixeira C, Wang X, Young T, Wania F (2012) Deposition of brominated flame retardants to the Devon Ice Cap, Nunavut, Canada. Environ Sci Technol 46:826–833CrossRefGoogle Scholar
  38. Quiroz R, Arellano L, Grimalt JO, Fernández P (2008) Analysis of polybrominated diphenyl ethers in atmospheric deposition and snow samples by solid-phase disk extraction. J Chromatogr A 1192:147–151CrossRefGoogle Scholar
  39. Ueno D, Darling C, Alaee M, Pacepavicius G, Teixeira C, Campbell L, Letcher RL, Bergman A, Marsh G, Muir D (2008) Hydroxylated polybrominated diphenyl ethers (OH-PBDEs) in the abiotic environment: surface water and precipitation from Ontario, Canada. Environ Sci Technol 42:1657–1664CrossRefGoogle Scholar
  40. Usenko S, Simonich SLM, Hageman KJ, Schrlau JE, Geiser L, Campbell DH, Appleby PG, Landers DH (2010) Sources and deposition of polycyclic aromatic hydrocarbons to western U.S. National Parks. Environ Sci Technol 44:4512–4518CrossRefGoogle Scholar
  41. Van Drooge BL, Grimalt JO, Garcia CJT, Cuevas E (2002) Semivolatile organochlorine compounds in the free troposphere of the northeastern Atlantic. Environ Sci Technol 36:1155–1161CrossRefGoogle Scholar
  42. Van Drooge BL, Fernández P, Grimalt JO, Stuchlík E, Torres García CJ, Cuevas E (2010) Atmospheric polycyclic aromatic hydrocarbons in remote European and Atlantic sites located above the boundary mixing layer. Environ Sci Pollut Res 17:1207–1216CrossRefGoogle Scholar
  43. Vilanova RM, Fernandez P, Martinez C, Grimalt JO (2001a) Organochlorine pollutants in remote mountain lake waters. J Environ Qual 30:1286–1295CrossRefGoogle Scholar
  44. Vilanova RM, Fernandez P, Martínez C, Grimalt JO (2001b) Polycyclic aromatic hydrocarbons in remote mountain lake waters. Wat Res 35:3916–3926CrossRefGoogle Scholar
  45. Villa S, Negrelli C, Maggi V, Finizio A, Vighi M (2006) Analysis of a firn core for assessing POP seasonal accumulation on an Alpine glacier. Ecotoxicol Environ Saf 63:17–24CrossRefGoogle Scholar
  46. Vives I, Grimalt JO, Fernandez P, Rosseland B (2004a) Polycyclic aromatic hydrocarbons in fish from remote and high mountian lakes in Europe and Greenland. Sci Total Environ 324:67–77CrossRefGoogle Scholar
  47. Vives I, Grimalt JO, Catalan J, Rosseland BO, Battarbee RW (2004b) Influence of altitude and age in the accumulation of organochlorine compounds in fish from high mountain lakes. Environ Sci Technol 38:690–698CrossRefGoogle Scholar
  48. Vizcaino E, Arellano L, Fernandez P, Grimalt JO (2009) Analysis of whole congener mixtures of polybromodiphenyl ethers by gas chromatography-mass spectrometry in both environmental and biological samples at femtogram levels. J Chromatogr A 1216:5045–5051CrossRefGoogle Scholar
  49. Wang X, Ding X, Mai B, Xie Z, Xiang C, Sun L, Sheng G, Fu J, Zeng E (2005) Polybrominated diphenyl ethers in airborne particulates collected during a research expedition from the Bohai Sea to Arctic. Environ Sci Technol 39:7803–7809CrossRefGoogle Scholar
  50. Wang X, Yao T, Wang P, Yang W, Tian L (2008) The recent deposition of persistent organic pollutants and mercury to de Dasuopu glacier, Mt. Xixiabangma, central Himalayas. Sci Total Environ 394:134–143CrossRefGoogle Scholar
  51. Wania F, Mackay D (1996) Tracking the distribution of persistent organic pollutants. Environ Sci Technol 30:390A–396ACrossRefGoogle Scholar
  52. Wania F, Mackay D, Hoff JT (1999) The importance of snow scavenging of polychlorinated biphenyl and polycyclic aromatic hydrocarbons vapors. Environ Sci Technol 33:195–197CrossRefGoogle Scholar
  53. Weber J, Halsall CJ, Muir D, Teixeira C, Small J, Solomon K, Hermanson M, Hung H, Bidleman T (2010) Endosulfan, a global pesticide: a review of its fate in the environment and occurrence in the Arctic. Sci Total Environ 408:2966–2984CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2014

Authors and Affiliations

  • Lourdes Arellano
    • 1
  • Joan O. Grimalt
    • 1
    Email author
  • Pilar Fernández
    • 1
  • Jordi F. Lopez
    • 1
  • Ulrike Nickus
    • 2
  • Hansjoerg Thies
    • 3
  1. 1.Department of Environmental ChemistryInstitute of Environmental Assessment and Water Research (IDÆA-CSIC)BarcelonaSpain
  2. 2.Institute of Meteorology and GeophysicsUniversity of InnsbruckInnsbruckAustria
  3. 3.Institute of EcologyUniversity of InnsbruckInnsbruckAustria

Personalised recommendations