TY - JOUR

T1 - A dynamic model to study the exchange of gas-phase POPs between air and a seasonal snowpack.

AU - Hansen, Kaj M.

AU - Halsall, Crispin J.

AU - Christensen, Jesper H.

PY - 2006/4/15

Y1 - 2006/4/15

N2 - An arctic snow model was developed to predict the exchange of vapor-phase persistent organic pollutants between the atmosphere and the snowpack over a winter season. Using modeled meteorological data simulating conditions in the Canadian High Arctic, a single-layer snowpack was created on the basis of the precipitation rate, with the snow depth, snow specific surface area, density, and total surface area (TSA) evolving throughout the annual time series. TSA, an important parameter affecting the vapor-sorbed quantity of chemicals in snow, was within a factor of 5 of measured values. Net fluxes for fluorene, phenanthrene, PCB-28 and -52, and α- and γ-HCH (hexachlorocyclohexane) were predicted on the basis of their wet deposition (snowfall) and vapor exchange between the snow and atmosphere. Chemical fluxes were found to be highly dynamic, whereby deposition was rapidly offset by evaporative loss due to snow settling (i.e., changes in TSA). Differences in chemical behavior over the course of the season (i.e., fluxes, snow concentra tions) were largely dependent on the snow/air partition coefficients (Ksa). Chemicals with relatively higher Ksa values such as α- and γ-HCH were efficiently retained within the snowpack until later in the season compared to fluorene, phenathrene, and PCB-28 and -52. Average snow and air concentrations predicted by the model were within a factor of 5−10 of values measured from arctic field studies, but tended to be overpredicted for those chemicals with higher Ksa values (i.e., HCHs). Sensitivity analysis revealed that snow concentrations were more strongly influenced by Ksa than either inclusion of wind ventilation of the snowpack or other changes in physical parameters. Importantly, the model highlighted the relevance of the arctic snowpack in influencing atmospheric concentrations. For the HCHs, evaporative fluxes from snow were more pronounced in April and May, toward the end of the winter, providing evidence that the snowpack plays an important role in influencing the seasonal increase in air concentrations for these compounds at this time of year.

AB - An arctic snow model was developed to predict the exchange of vapor-phase persistent organic pollutants between the atmosphere and the snowpack over a winter season. Using modeled meteorological data simulating conditions in the Canadian High Arctic, a single-layer snowpack was created on the basis of the precipitation rate, with the snow depth, snow specific surface area, density, and total surface area (TSA) evolving throughout the annual time series. TSA, an important parameter affecting the vapor-sorbed quantity of chemicals in snow, was within a factor of 5 of measured values. Net fluxes for fluorene, phenanthrene, PCB-28 and -52, and α- and γ-HCH (hexachlorocyclohexane) were predicted on the basis of their wet deposition (snowfall) and vapor exchange between the snow and atmosphere. Chemical fluxes were found to be highly dynamic, whereby deposition was rapidly offset by evaporative loss due to snow settling (i.e., changes in TSA). Differences in chemical behavior over the course of the season (i.e., fluxes, snow concentra tions) were largely dependent on the snow/air partition coefficients (Ksa). Chemicals with relatively higher Ksa values such as α- and γ-HCH were efficiently retained within the snowpack until later in the season compared to fluorene, phenathrene, and PCB-28 and -52. Average snow and air concentrations predicted by the model were within a factor of 5−10 of values measured from arctic field studies, but tended to be overpredicted for those chemicals with higher Ksa values (i.e., HCHs). Sensitivity analysis revealed that snow concentrations were more strongly influenced by Ksa than either inclusion of wind ventilation of the snowpack or other changes in physical parameters. Importantly, the model highlighted the relevance of the arctic snowpack in influencing atmospheric concentrations. For the HCHs, evaporative fluxes from snow were more pronounced in April and May, toward the end of the winter, providing evidence that the snowpack plays an important role in influencing the seasonal increase in air concentrations for these compounds at this time of year.

U2 - 10.1021/es051685b

DO - 10.1021/es051685b

M3 - Journal article

VL - 40

SP - 2644

EP - 2652

JO - Environmental Science and Technology

JF - Environmental Science and Technology

SN - 0013-936X

IS - 8

ER -