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Volume 18, issue 7 | Copyright
Atmos. Chem. Phys., 18, 5045-5058, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 13 Apr 2018

Research article | 13 Apr 2018

Continuous non-marine inputs of per- and polyfluoroalkyl substances to the High Arctic: a multi-decadal temporal record

Heidi M. Pickard1, Alison S. Criscitiello2, Christine Spencer3, Martin J. Sharp2, Derek C. G. Muir3, Amila O. De Silva3, and Cora J. Young1,a Heidi M. Pickard et al.
  • 1Department of Chemistry, Memorial University, St. John's, NL, A1B 3X7, Canada
  • 2Department of Earth and Atmospheric Sciences, University of Alberta, Edmonton, AB, T6G 2E3, Canada
  • 3Aquatic Contaminants Research Division, Environment and Climate Change Canada, Burlington, ON, L7S 1A1, Canada
  • anow at: Department of Chemistry, York University, Toronto, ON, M3J 1P3, Canada

Abstract. Perfluoroalkyl acids (PFAAs) are persistent, in some cases, bioaccumulative compounds found ubiquitously within the environment. They can be formed from the atmospheric oxidation of volatile precursor compounds and undergo long-range transport (LRT) through the atmosphere and ocean to remote locations. Ice caps preserve a temporal record of PFAA deposition making them useful in studying the atmospheric trends in LRT of PFAAs in polar or mountainous regions, as well as in understanding major pollutant sources and production changes over time. A 15m ice core representing 38 years of deposition (1977–2015) was collected from the Devon Ice Cap in Nunavut, providing us with the first multi-decadal temporal ice record in PFAA deposition to the Arctic. Ice core samples were concentrated using solid phase extraction and analyzed by liquid and ion chromatography methods. Both perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkyl sulfonic acids (PFSAs) were detected in the samples, with fluxes ranging from <LOD to 141ngm−2yr−1. Our results demonstrate that the PFCAs and perfluorooctane sulfonate (PFOS) have continuous and increasing deposition on the Devon Ice Cap, despite recent North American and international regulations and phase-outs. We propose that this is the result of on-going manufacture, use and emissions of these compounds, their precursors and other newly unidentified compounds in regions outside of North America. By modelling air mass transport densities, and comparing temporal trends in deposition with production changes of possible sources, we find that Eurasian sources, particularly from Continental Asia, are large contributors to the global pollutants impacting the Devon Ice Cap. Comparison of PFAAs to their precursors and correlations of PFCA pairs showed that deposition of PFAAs is dominated by atmospheric formation from volatile precursor sources. Major ion analysis confirmed that marine aerosol inputs are unimportant to the long-range transport mechanisms of these compounds. Assessments of deposition, homologue profiles, ion tracers, air mass transport models, and production and regulation trends allow us to characterize the PFAA depositional profile on the Devon Ice Cap and further understand the LRT mechanisms of these persistent pollutants.

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Perfluoroalkyl acids (PFAAs) are persistent, bioaccumulative compounds found in the environment far from source regions, including the remote Arctic. We collected a 15 m ice core from the Canadian High Arctic to measure a 38-year deposition record of PFAAs, proving information about major pollutant sources and production changes over time. Our results demonstrate that PFAAs have continuous and increasing deposition, despite recent North American regulations and phase-outs.
Perfluoroalkyl acids (PFAAs) are persistent, bioaccumulative compounds found in the environment...