Assessing the long-range transport of PAH to a sub-Arctic site using positive matrix factorization and potential source contribution function

摘要

Gas-phase and particle-phase atmospheric samples collected in a sparsely populated sub-Arctic environment in the Yukon Territory, Canada were analyzed for a wide range of organic pollutants including polycyclic aromatic hydrocarbons (PAH). Receptor modeling using positive matrix factorization (PMF) was applied to a PAH data set from samples collected between August 2007 and December 2008 to afford four factors. These factors were designated as fossil fuel combustion emissions, particle-phase wood combustion emissions, gas-phase wood combustion emissions, and unburned petroleum/petrogenic emissions. The multiple linear regression-derived average contributions of these factors to the total PAH concentrations were 14% for fossil fuel combustion, 6% for particle-phase wood combustion emissions, 46% for gas-phase wood combustion emissions and 34% for petrogenic emissions. When the total PAH concentrations (defined as the sum of twenty-two PAH) and the PMF-modeled PAH concentrations set were compared, the correlation was excellent (R~2 = 0.97). Ten-day back trajectories starting at four different heights were used in a potential source contribution function analysis (PSCF) to assess the potential source regions of these PAH factors. Mapping the computed PSCF values for the four PMF factors revealed different source regions in the northern hemisphere for each PMF factor. Atmospheric transport of PAH occurred from both relatively short and long distances with both continental (North American) and trans-oceanic (Asian) sources contributing significantly to the total PAH. This study provides evidence of the transport of fossil fuel and wood combustion emissions from Asia, continental North America and northern Europe to sub-Arctic Canada (and by extension to the Canadian Arctic) primarily during cooler (fall-winter) months. This study demonstrates for the first time that the combined PMF-PSCF methodology can be used to identify geographically-disperse PAH source contributors on a hemispherical scale.