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 15 m 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 141 ng m−2 yr−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.