International journal of environmental research and public health, 2015
Mercury (Hg) is a global pollutant with adverse health effects on humans and wildlife. It is of s... more Mercury (Hg) is a global pollutant with adverse health effects on humans and wildlife. It is of special concern in the Arctic due to accumulation in the food web and exposure of the Arctic population through a rich marine diet. Climate change may alter the exposure of the Arctic population to Hg. We have investigated the effect of climate change on the atmospheric Hg transport to and deposition within the Arctic by making a sensitivity study of how the atmospheric chemistry-transport model Danish Eulerian Hemispheric Model (DEHM) reacts to climate change forcing. The total deposition of Hg to the Arctic is 18% lower in the 2090s compared to the 1990s under the applied Special Report on Emissions Scenarios (SRES-A1B) climate scenario. Asia is the major anthropogenic source area (25% of the deposition to the Arctic) followed by Europe (6%) and North America (5%), with the rest arising from the background concentration, and this is independent of the climate. DEHM predicts between a 6%...
ABSTRACT Persistent organic pollutants (POPs) are a group of chemical compounds with mainly anthr... more ABSTRACT Persistent organic pollutants (POPs) are a group of chemical compounds with mainly anthropogenic origin; they are semi-volatile, hydrophobic, they bioaccumulate, they have toxic effects on human and wildlife and they display low degradation rates in the environment (Jones and de Voogt, 1999). POPs are emitted to the atmosphere either from industrial production, as by-products from combustion, or intentionally as pesticides used on crops or for insect control. A number of POPs are banned or subject to regulation, e.g. under the UNEP Stockholm convention for POPs and emissions of them have decreased during the last decades (Jones and de Voogt, 1999). However, due to the great persistence large amounts are still cycling in the environment. The volatility of POPs is temperature dependent, which can lead to several consecutive deposition and re-emission events named multi-hop or grasshopper transport (Wania and Mackay, 1996). To contribute to the understanding of these processes several models are developed. The environmental fate of POPs is traditionally studied with box models (e.g. Wania et al., 1999). Recently, atmospheric transport models with high spatiotemporal resolution are also developed to address these issues (e.g. Koziol and Pudykiewicz, 2001; Hansen et al., 2004).
Cyclic volatile methyl siloxanes (cVMS) are present in technical applications and personal care p... more Cyclic volatile methyl siloxanes (cVMS) are present in technical applications and personal care products. They are predicted to undergo long-range atmospheric transport, but measurements of cVMS in remote areas remain scarce. An active air sampling method for decamethylcyclopentasiloxane (D5) was further evaluated to include hexamethylcyclotrisiloxane (D3), octamethylcyclotetrasiloxane (D4), and dodecamethylcyclohexasiloxane (D6). Air samples were collected at the Zeppelin observatory in the remote Arctic (79° N, 12° E) with an average sampling time of 81 ± 23 h in late summer (August-October) and 25 ± 10 h in early winter (November-December) 2011. The average concentrations of D5 and D6 in late summer were 0.73 ± 0.31 and 0.23 ± 0.17 ng/m(3), respectively, and 2.94 ± 0.46 and 0.45 ± 0.18 ng/m(3) in early winter, respectively. Detection of D5 and D6 in the Arctic atmosphere confirms their long-range atmospheric transport. The D5 measurements agreed well with predictions from a Eulerian atmospheric chemistry-transport model, and seasonal variability was explained by the seasonality in the OH radical concentrations. These results extend our understanding of the atmospheric fate of D5 to high latitudes, but question the levels of D3 and D4 that have previously been measured at Zeppelin with passive air samplers.
Atmospheric transport models are used in studies of atmospheric chemistry as well as aerobiology.... more Atmospheric transport models are used in studies of atmospheric chemistry as well as aerobiology. Atmospheric transport models in general needs accurate emissions inventories, which includes biogenic emissions such as Volatile Organic Compounds (VOCs) and pollen. Trees are important VOC and pollen sources and a needed requirement is specie distribution which takes into account important species such as Betula and Alnus. We present here a detailed tree species inventory covering Europe, parts of Africa and parts of Asia. Forest inventories have been obtained for each European country, parts of Asia and parts of Africa. The national inventories vary with respect to number of species as well as the number of sub-regions each nation is divided into. The inventories are therefore harmonised within a GIS system and afterwards gridded to the model grid defined by the EMEP model: 50 km x 50 km. The inventory is designed to be used with existing land-use data, which separates forest cover into broad leaved, mixed and conifer forests. This will be exemplified by using two different remote sensing products with different grid resolution such as GLC2000 and CLC2000 in selected areas. The final inventory includes 16 conifer species and 23 broadleaved species that are important for biogenic VOCs or pollen emission calculations. For example: Oak (Quercus), poplar (Populus), pines (Pinus), spruce (Picea), birch (Betula) and alder (Alnus). 774 regions with forest inventories are included, mainly on sub-national level. The coverage of each specie ranges from national to European scale, where the latter includes VOC and allergy relevant species such as Quercus, Alnus and Betula. The inventory is gridded to the model grid defined by the EMEP model, which is also the basis for many emissions inventories throughout Europe. The inventory is therefore prepared for easy implementation into atmospheric transport models by providing an extension to already applied land use data such as the Corine Land Cover (CLC2000) or Global Land Cover (GLC2000). Possible applications of the inventory include emissions of VOCs and pollen, CO2 fluxes and dry deposition - in general calculations which are tree specie dependent.
So far reduction of the anthropogenic emissions of chemical species to the atmosphere has been pr... more So far reduction of the anthropogenic emissions of chemical species to the atmosphere has been profoundly investigated. However, new research indicates that climate change on its own also has a significant impact on the future air pollution levels. Climate Change and its impact on air pollution levels are currently studied by a number of research groups using, global, hemispherical and
Current aerobiological research applies the hypothesis that the main source of atmospheric birch ... more Current aerobiological research applies the hypothesis that the main source of atmospheric birch (Betula) pollen is forest trees. Our results indicate that the measured levels in Copenhagen are not only due to birch trees in Danish forests but that the urban areas also seem to be a significant source of birch pollen. A number of episodes in 2003 with enhanced
A dynamic snowpack module was implemented in the Danish Eulerian Hemispheric Model Persistant Org... more A dynamic snowpack module was implemented in the Danish Eulerian Hemispheric Model Persistant Organic Pollutants (DEHM-POP), an atmospheric chemistry-transport model designed to study the environmental fate of persistent organic pollutants in the Northern Hemisphere. The role of the snowpack on the fate of alpha-hexachlorocyclohexane (alpha-HCH) was investigated by making simulations both with and without the formation of a snowpack and comparing model results with data from 21 air monitoring sites. The inclusion of a dynamic snowpack module in the DEHM-POP model generally improves the fit between modeled and observed alpha-HCH air concentrations for the winter and spring seasons and the overall correlation coefficient between predicted and observed concentrations are improved at 8 of the sites. The predicted snowpack concentrations are in good agreement with the few available snow measurements from the Arctic. The presence of a snowpack increases surface boundary layer air concentrations of alpha-HCH at midlatitudes, while the effect is more pronounced in the Arctic due to the longer periods of snow cover. The results indicate that the snowpack module in DEHM-POP acts as a fast-exchanging temporary storage medium for alpha-HCH, as significant fractions were rapidly revolatilized back into the atmosphere following deposition with snowfall, although the current parametrization for vapor-exchange probably over emphasizes this process. Nonetheless, increased air concentrations observed between March and May ("spring maximum events"; SME) at several high latitude monitoring stations are also predicted by the model. The model results indicate that the SMEs are associated with the revolatilization of previously deposited chemical from the snowpack, following a reduction in the capacity of the snowpack to retain alpha-HCH with increasing temperatures toward the end of the winter period, rather than the actual melting of the snowpack. The SMEs are not predicted at all the Arctic monitoring sites by the model, and the significance of the snowpack in controlling these in the model is, therefore, open to question given the uncertainties in the snow-air partition coefficient (K(sa)) and the reliance of the model on a one-layer snowpack rather than a multilayered snowpack.
The Danish Eulerian Hemispheric Model (DEHM) developed at the National Environmental Research Ins... more The Danish Eulerian Hemispheric Model (DEHM) developed at the National Environmental Research Institute (NERI) in Denmark has been applied for numerous studies of air pollution. DEHM was originally developed with the main purpose of investigating the atmospheric transport of pollutants to the Arctic region, but is now also applied for more local scale environmental problems. The DEHM model has therefore
Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is... more Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is released to the atmosphere in large quantities. Although D(5) is currently under consideration for regulation, there have been no field investigations of its atmospheric fate. We employed a recently developed, quality assured method to measure D(5) concentration in ambient air at a rural site in Sweden. The samples were collected with daily resolution between January and June 2009. The D(5) concentration ranged from 0.3 to 9 ng m(-3), which is 1-3 orders of magnitude lower than previous reports. The measured data were compared with D(5) concentrations predicted using an atmospheric circulation model that included both OH radical and D(5) chemistry. The model was parametrized using emissions estimates and physical chemical properties determined in laboratory experiments. There was good agreement between the measured and modeled D(5) concentrations. The results show that D(5) is clearly subject to long-range atmospheric transport, but that it is also effectively removed from the atmosphere via phototransformation. Atmospheric deposition has little influence on the atmospheric fate. The good agreement between the model predictions and the field observations indicates that there is a good understanding of the major factors governing D(5) concentrations in the atmosphere.
An arctic snow model was developed to predict the exchange of vapor-phase persistent organic poll... more 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 alpha- and gamma-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 concentrations) were largely dependent on the snow/air partition coefficients (K(sa)). Chemicals with relatively higher K(sa) values such as alpha- and gamma-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 K(sa) values (i.e., HCHs). Sensitivity analysis revealed that snow concentrations were more strongly influenced by K(sa) 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.
International journal of environmental research and public health, 2015
Mercury (Hg) is a global pollutant with adverse health effects on humans and wildlife. It is of s... more Mercury (Hg) is a global pollutant with adverse health effects on humans and wildlife. It is of special concern in the Arctic due to accumulation in the food web and exposure of the Arctic population through a rich marine diet. Climate change may alter the exposure of the Arctic population to Hg. We have investigated the effect of climate change on the atmospheric Hg transport to and deposition within the Arctic by making a sensitivity study of how the atmospheric chemistry-transport model Danish Eulerian Hemispheric Model (DEHM) reacts to climate change forcing. The total deposition of Hg to the Arctic is 18% lower in the 2090s compared to the 1990s under the applied Special Report on Emissions Scenarios (SRES-A1B) climate scenario. Asia is the major anthropogenic source area (25% of the deposition to the Arctic) followed by Europe (6%) and North America (5%), with the rest arising from the background concentration, and this is independent of the climate. DEHM predicts between a 6%...
ABSTRACT Persistent organic pollutants (POPs) are a group of chemical compounds with mainly anthr... more ABSTRACT Persistent organic pollutants (POPs) are a group of chemical compounds with mainly anthropogenic origin; they are semi-volatile, hydrophobic, they bioaccumulate, they have toxic effects on human and wildlife and they display low degradation rates in the environment (Jones and de Voogt, 1999). POPs are emitted to the atmosphere either from industrial production, as by-products from combustion, or intentionally as pesticides used on crops or for insect control. A number of POPs are banned or subject to regulation, e.g. under the UNEP Stockholm convention for POPs and emissions of them have decreased during the last decades (Jones and de Voogt, 1999). However, due to the great persistence large amounts are still cycling in the environment. The volatility of POPs is temperature dependent, which can lead to several consecutive deposition and re-emission events named multi-hop or grasshopper transport (Wania and Mackay, 1996). To contribute to the understanding of these processes several models are developed. The environmental fate of POPs is traditionally studied with box models (e.g. Wania et al., 1999). Recently, atmospheric transport models with high spatiotemporal resolution are also developed to address these issues (e.g. Koziol and Pudykiewicz, 2001; Hansen et al., 2004).
Cyclic volatile methyl siloxanes (cVMS) are present in technical applications and personal care p... more Cyclic volatile methyl siloxanes (cVMS) are present in technical applications and personal care products. They are predicted to undergo long-range atmospheric transport, but measurements of cVMS in remote areas remain scarce. An active air sampling method for decamethylcyclopentasiloxane (D5) was further evaluated to include hexamethylcyclotrisiloxane (D3), octamethylcyclotetrasiloxane (D4), and dodecamethylcyclohexasiloxane (D6). Air samples were collected at the Zeppelin observatory in the remote Arctic (79° N, 12° E) with an average sampling time of 81 ± 23 h in late summer (August-October) and 25 ± 10 h in early winter (November-December) 2011. The average concentrations of D5 and D6 in late summer were 0.73 ± 0.31 and 0.23 ± 0.17 ng/m(3), respectively, and 2.94 ± 0.46 and 0.45 ± 0.18 ng/m(3) in early winter, respectively. Detection of D5 and D6 in the Arctic atmosphere confirms their long-range atmospheric transport. The D5 measurements agreed well with predictions from a Eulerian atmospheric chemistry-transport model, and seasonal variability was explained by the seasonality in the OH radical concentrations. These results extend our understanding of the atmospheric fate of D5 to high latitudes, but question the levels of D3 and D4 that have previously been measured at Zeppelin with passive air samplers.
Atmospheric transport models are used in studies of atmospheric chemistry as well as aerobiology.... more Atmospheric transport models are used in studies of atmospheric chemistry as well as aerobiology. Atmospheric transport models in general needs accurate emissions inventories, which includes biogenic emissions such as Volatile Organic Compounds (VOCs) and pollen. Trees are important VOC and pollen sources and a needed requirement is specie distribution which takes into account important species such as Betula and Alnus. We present here a detailed tree species inventory covering Europe, parts of Africa and parts of Asia. Forest inventories have been obtained for each European country, parts of Asia and parts of Africa. The national inventories vary with respect to number of species as well as the number of sub-regions each nation is divided into. The inventories are therefore harmonised within a GIS system and afterwards gridded to the model grid defined by the EMEP model: 50 km x 50 km. The inventory is designed to be used with existing land-use data, which separates forest cover into broad leaved, mixed and conifer forests. This will be exemplified by using two different remote sensing products with different grid resolution such as GLC2000 and CLC2000 in selected areas. The final inventory includes 16 conifer species and 23 broadleaved species that are important for biogenic VOCs or pollen emission calculations. For example: Oak (Quercus), poplar (Populus), pines (Pinus), spruce (Picea), birch (Betula) and alder (Alnus). 774 regions with forest inventories are included, mainly on sub-national level. The coverage of each specie ranges from national to European scale, where the latter includes VOC and allergy relevant species such as Quercus, Alnus and Betula. The inventory is gridded to the model grid defined by the EMEP model, which is also the basis for many emissions inventories throughout Europe. The inventory is therefore prepared for easy implementation into atmospheric transport models by providing an extension to already applied land use data such as the Corine Land Cover (CLC2000) or Global Land Cover (GLC2000). Possible applications of the inventory include emissions of VOCs and pollen, CO2 fluxes and dry deposition - in general calculations which are tree specie dependent.
So far reduction of the anthropogenic emissions of chemical species to the atmosphere has been pr... more So far reduction of the anthropogenic emissions of chemical species to the atmosphere has been profoundly investigated. However, new research indicates that climate change on its own also has a significant impact on the future air pollution levels. Climate Change and its impact on air pollution levels are currently studied by a number of research groups using, global, hemispherical and
Current aerobiological research applies the hypothesis that the main source of atmospheric birch ... more Current aerobiological research applies the hypothesis that the main source of atmospheric birch (Betula) pollen is forest trees. Our results indicate that the measured levels in Copenhagen are not only due to birch trees in Danish forests but that the urban areas also seem to be a significant source of birch pollen. A number of episodes in 2003 with enhanced
A dynamic snowpack module was implemented in the Danish Eulerian Hemispheric Model Persistant Org... more A dynamic snowpack module was implemented in the Danish Eulerian Hemispheric Model Persistant Organic Pollutants (DEHM-POP), an atmospheric chemistry-transport model designed to study the environmental fate of persistent organic pollutants in the Northern Hemisphere. The role of the snowpack on the fate of alpha-hexachlorocyclohexane (alpha-HCH) was investigated by making simulations both with and without the formation of a snowpack and comparing model results with data from 21 air monitoring sites. The inclusion of a dynamic snowpack module in the DEHM-POP model generally improves the fit between modeled and observed alpha-HCH air concentrations for the winter and spring seasons and the overall correlation coefficient between predicted and observed concentrations are improved at 8 of the sites. The predicted snowpack concentrations are in good agreement with the few available snow measurements from the Arctic. The presence of a snowpack increases surface boundary layer air concentrations of alpha-HCH at midlatitudes, while the effect is more pronounced in the Arctic due to the longer periods of snow cover. The results indicate that the snowpack module in DEHM-POP acts as a fast-exchanging temporary storage medium for alpha-HCH, as significant fractions were rapidly revolatilized back into the atmosphere following deposition with snowfall, although the current parametrization for vapor-exchange probably over emphasizes this process. Nonetheless, increased air concentrations observed between March and May ("spring maximum events"; SME) at several high latitude monitoring stations are also predicted by the model. The model results indicate that the SMEs are associated with the revolatilization of previously deposited chemical from the snowpack, following a reduction in the capacity of the snowpack to retain alpha-HCH with increasing temperatures toward the end of the winter period, rather than the actual melting of the snowpack. The SMEs are not predicted at all the Arctic monitoring sites by the model, and the significance of the snowpack in controlling these in the model is, therefore, open to question given the uncertainties in the snow-air partition coefficient (K(sa)) and the reliance of the model on a one-layer snowpack rather than a multilayered snowpack.
The Danish Eulerian Hemispheric Model (DEHM) developed at the National Environmental Research Ins... more The Danish Eulerian Hemispheric Model (DEHM) developed at the National Environmental Research Institute (NERI) in Denmark has been applied for numerous studies of air pollution. DEHM was originally developed with the main purpose of investigating the atmospheric transport of pollutants to the Arctic region, but is now also applied for more local scale environmental problems. The DEHM model has therefore
Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is... more Decamethylcyclopentasiloxane (D(5)) is a volatile compound used in personal care products that is released to the atmosphere in large quantities. Although D(5) is currently under consideration for regulation, there have been no field investigations of its atmospheric fate. We employed a recently developed, quality assured method to measure D(5) concentration in ambient air at a rural site in Sweden. The samples were collected with daily resolution between January and June 2009. The D(5) concentration ranged from 0.3 to 9 ng m(-3), which is 1-3 orders of magnitude lower than previous reports. The measured data were compared with D(5) concentrations predicted using an atmospheric circulation model that included both OH radical and D(5) chemistry. The model was parametrized using emissions estimates and physical chemical properties determined in laboratory experiments. There was good agreement between the measured and modeled D(5) concentrations. The results show that D(5) is clearly subject to long-range atmospheric transport, but that it is also effectively removed from the atmosphere via phototransformation. Atmospheric deposition has little influence on the atmospheric fate. The good agreement between the model predictions and the field observations indicates that there is a good understanding of the major factors governing D(5) concentrations in the atmosphere.
An arctic snow model was developed to predict the exchange of vapor-phase persistent organic poll... more 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 alpha- and gamma-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 concentrations) were largely dependent on the snow/air partition coefficients (K(sa)). Chemicals with relatively higher K(sa) values such as alpha- and gamma-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 K(sa) values (i.e., HCHs). Sensitivity analysis revealed that snow concentrations were more strongly influenced by K(sa) 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.
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