Modelling the fate of persistent organic pollutants in Europe: parameterisation of a gridded distribution model

A regionally segmented multimedia fate model for the European continent is described together with an illustrative steady-state case study examining the fate of gamma-HCH (lindane) based on 1998 emission data. The study builds on the regionally segmented BETR North America model structure and describes the regional segmentation and parameterisation for Europe. The European continent is described by a 5 degrees x5 degrees grid, leading to 50 regions together with four perimetric boxes representing regions buffering the European environment. Each zone comprises seven compartments including; upper and lower atmosphere, soil, vegetation, fresh water and sediment and coastal water. Inter-regions flows of air and water are described, exploiting information originating from GIS databases and other georeferenced data. The model is primarily designed to describe the fate of Persistent Organic Pollutants (POPs) within the European environment by examining chemical partitioning and degradation in each region, and inter-region transport either under steady-state conditions or fully dynamically. A test case scenario is presented which examines the fate of estimated spatially resolved atmospheric emissions of lindane throughout Europe within the lower atmosphere and surface soil compartments. In accordance with the predominant wind direction in Europe, the model predicts high concentrations close to the major sources as well as towards Central and Northeast regions. Elevated soil concentrations in Scandinavian soils provide further evidence of the potential of increased scavenging by forests and subsequent accumulation by organic-rich terrestrial surfaces. Initial model predictions have revealed a factor of 5-10 underestimation of lindane concentrations in the atmosphere. This is explained by an underestimation of source strength and/or an underestimation of European background levels. The model presented can further be used to predict deposition fluxes and chemical inventories, and it can also be adapted to provide characteristic travel distances and overall environmental persistence, which can be compared with other long-range transport prediction methods.     

BETR North America: a regionally segmented multimedia contaminant fate model for North America

We present the Berkeley-Trent North American contaminant fate model (BETR North America), a regionally segmented multimedia contaminant fate model based on the fugacity concept. The model is built on a framework that links contaminant fate models of individual regions, and is generally applicable to large, spatially heterogeneous areas. The North American environment is modeled as 24 ecological regions, within each region contaminant fate is described using a 7 compartment multimedia fugacity model including a vertically segmented atmosphere, freshwater, freshwater sediment, soil, coastal water and vegetation compartments. Inter-regional transport of contaminants in the atmosphere, freshwater and coastal water is described using a database of hydrological and meteorological data compiled with Geographical Information Systems (GIS) techniques. Steady-state and dynamic solutions to the 168 mass balance equations that make up the linked model for North America are discussed, and an illustrative case study of toxaphene transport from the southern United States to the Great Lakes Basin is presented. Regionally segmented models such as BETR North America can provide a critical link between evaluative models of long-range transport potential and contaminant concentrations observed in remote regions. The continent-scale mass balance calculated by the model provides a sound basis for evaluating long-range transport potential of organic pollutants, and formulation of continent-scale management and regulatory strategies for chemicals.     

Analysis of atmospheric behavior of PCDDs/PCDFs by a one-compartment box model

The overall atmospheric behavior of PCDDs/PCDFs in the Kanto region, Japan, was simulated by a one-compartment box model. For each homologue the relative significance and temperature dependences of dry deposition, wet deposition, degradation, and advection in both gas and particulate phases were examined and compared. The results of the model calculation suggested that the rates for dry deposition are comparable to those for wet deposition, and the rates for advection are comparable to those for bulk (dry+wet) depositions in the Kanto region. On the other hand, the rates of degradation for PCDDs/PCDFs in the atmosphere in the Kanto region would be negligible. The emission rates and the bulk deposition fluxes in the entire Kanto region estimated by the model calculation based on observed air concentrations were 0.084-0.90 kg-TEQ/month and 0.045-0.43 kg-TEQ/month, respectively. These estimated emission rates and bulk deposition fluxes were slightly higher than the estimated emission rate based on observed emission concentrations and the estimated bulk deposition fluxes based on observed deposition fluxes collected on water deposition surface, respectively. This study showed the model calculation can be available for understanding of the overall atmospheric behavior, verification of the source inventory, and estimation of deposition flux on the actual environment including various deposition surfaces.     

Development of continental scale multimedia contaminant fate models: integrating GIS

The incentives and approaches for modelling chemical fate at a continental scale are discussed and reviewed. It is suggested that a multi-media model consisting of some 20-30 regions, each of which contains typically seven environmental compartments represents a reasonable compromise between the issues of the need for detailed resolution, avoidance of excessive data demands and inherent complexity and transparency. Strategies adopted in compiling the Berkley-Trent (BETR) model for North America are discussed and used to illustrate the issues of selecting appropriate number and nature of segments, treatment of air and water flows and the acquisition of environmental data. It is suggested that GIS software can play a valuable role in gathering and processing such data and in the display and interpretation of the results of the model assessment. The BETR model will be a useful tool for describing the nature of persistence and long-range transport of chemicals of concern in the North American environment.     

Anthropogenic pollutants in the Russian Arctic atmosphere: sources and sinks in spring and summer

The 5-day forward and backward trajectories of air mass transport to three Russian Arctic points for each day in April and July over a 10-year period from 1986 to 1995 have been analyzed. The important features and seasonal differences in air exchange processes in various areas of the Arctic have been investigated. Taking into account seasonal variations in aerosol scavenging mechanisms and velocities, the average contributions of large highly industrialized regions of the Russian Arctic air pollution were estimated for April and July. Reasonable correspondence between the calculated mean concentrations for six anthropogenic chemical elements (As, Ni, Pb, V, Zn, Cd) and experimentally determined values have been obtained. The atmospheric pollution transport from the Arctic was studied as yet another way of cleaning the Arctic atmosphere, in addition to the traditionally considered wet and dry depositions onto the surface. The average apportionment of conservative contaminants after passing the observation points was estimated for spring and summer. The air masses passing through the observation points in spring may take about 20–40% of pollutants out of the Arctic. In summer, however, more than 90% of pollutants transported into the Russian Arctic deposit within 5 days onto the surface inside the Arctic region. The monthly average fluxes of six anthropogenic elements onto the surface in the Russian Arctic were estimated for April and July.     

The sensitivity of PM2.5 source-receptor relationships to atmospheric chemistry and transport in a three-dimensional air quality model

Air quality model simulations constitute an effective approach to developing source-receptor relationships (so-called transfer coefficients in the risk analysis framework) because a significant fraction of particulate matter (particularly PM2.5) is secondary (i.e., formed in the atmosphere) and, therefore, depends on the atmospheric chemistry of the airshed. In this study, we have used a comprehensive three-dimensional air quality model for PM2.5 (SAQM-AERO) to compare three approaches to generating episodic transfer coefficients for several source regions in the Los Angeles Basin. First, transfer coefficients were developed by conducting PM2.5 SAQM-AERO simulations with reduced emissions of one of four precursors (i.e., primary PM, sulfur dioxide (SO2), oxides of nitrogen (NOx), and volatile organic compounds) from each source region. Next, we calculated transfer coefficients using two other methods: (1) a simplified chemistry for PM2.5 formation, and (2) simplifying assumptions on transport using information limited to basin-wide emission reductions. Transfer coefficients obtained with the simplified chemistry were similar to those obtained with the comprehensive model for VOC emission changes but differed for NOx and SOz emission changes. The differences were due to the parameterization of the rates of secondary PM formation in the simplified chemistry. In 90% of the cases, transfer coefficients estimated using only basin-wide information were within a factor of two of those obtained with the explicit source-receptor simulations conducted with the comprehensive model. The best agreement was obtained for VOC emission changes; poor agreement was obtained for primary PM2.5.     

Modeling transport and deposition of contaminants to ecosystems of concern: a case study for the Laurentian Great Lakes

Transfer efficiency (TE) is introduced as a model output that can be used to characterize the relative ability of chemicals to be transported in the environment and deposited to specific target ecosystems. We illustrate this concept by applying the Berkeley-Trent North American contaminant fate model (BETR North America) to identify organic chemicals with properties that result in efficient atmospheric transport and deposition to the Laurentian Great Lakes. By systematically applying the model to hypothetical organic chemicals that span a wide range of environmental partitioning properties, we identify combinations of properties that favor efficient transport and deposition to the Lakes. Five classes of chemicals are identified based on dominant transport and deposition pathways, and specific examples of chemicals in each class are identified and discussed. The role of vegetation in scavenging chemicals from the atmosphere is assessed, and found to have a negligible influence on transfer efficiency to the Great Lakes. Results indicate chemicals with octanol-water (K(ow)) and air-water (K(aw)) partition coefficients in the range of 10(5)-10(7) and 10(-4)-10(-1) combine efficient transport and deposition to the Great Lakes with potential for biaccumulation in the aquatic food web once they are deposited. A method of estimating the time scale for atmospheric transport and deposition process is suggested, and the effects of degrading reactions in the atmosphere and meteorological conditions on transport efficiency of different classes of chemicals are discussed. In total, this approach provides a method of identifying chemicals that are subject to long-range transport and deposition to specific target ecosystems as a result of their partitioning and persistence characteristics. Supported by an appropriate contaminant fate model, the approach can be applied to any target ecosystem of concern.     

Evaluation and comparison of multimedia mass balance models of chemical fate: application of EUSES and ChemCAN to 68 chemicals in Japan

The European Union System for Evaluation of Substances (EUSES) and the ChemCAN chemical fate model are applied to describe the fate of 68 chemicals on two spatial scales in Japan. Emission information on the chemicals has been obtained from Japan's Pollutant Release and Transfer Registry and available monitoring data gathered from government reports. Environmental concentrations calculated by the two models for the four primary environmental media of air, water, soil and sediment agree within a factor of 3 for over 70% of the data, and within a factor of 10 for over 87% of the data. Reasons for certain large discrepancies are discussed. Concentrations calculated by the models are generally consistent with the lower range of concentrations that are observed in the environment. Agreement between modeled and observed concentrations is considerably improved by including an estimate of the advective input of chemicals in air from outside Japan. The agreement between the EUSES and ChemCAN models suggests that results of individual chemical assessments are not likely to be significantly affected by the choice of chemical fate model. Primary sources of discrepancy between modeled and observed concentrations are believed to be uncertainties in emission rates, degradation half-lives, and the lack of data on advective inflow of contaminants in air.     

Model and input uncertainty in multi-media fate modeling: benzo[a]pyrene concentrations in Europe

This paper evaluates the contribution of (i) uncertainty in substance properties, (ii) lack of spatial variability, (iii) intermodel differences and (iv) neglecting sorption to black carbon (BC) to the uncertainty of Benzo[a]pyrene (BaP) concentrations in European air, soil and fresh water predicted by the multi-media fate model Simplebox. Uncertainty in substance properties was quantified using probabilistic modeling. The influence of spatial variability was quantified by estimating variation in predicted concentrations with three spatially explicit fate models (Impact 2002, EVn BETR and BETR Global). Intermodel differences were quantified by comparing concentration estimates of Simplebox, Impact 2002, EVn BETR and the European part of BETR Global. Finally, predictions of a BC-inclusive version of Simplebox were compared with predictions of a BC-exclusive version. For air concentrations of BaP, the lack of spatial variability in emissions was most influential. For freshwater concentrations of BaP, intermodel differences and lack of spatial variability in dimensions of fresh water bodies were the dominant sources of uncertainty. For soil, all sources of uncertainty were of comparable magnitude. Our results indicate that uncertainty in Simplebox can be as large as three orders of magnitude for BaP concentrations in the environment and would be substantially underestimated by focusing on one source of uncertainty only.     

Uncertainty analysis using a fugacity-based multimedia mass-balance model: Application of the updated EQC model to decamethylcyclopentasiloxane (D5)

The EQuilibrium Criterion (EQC) model developed and published in 1996 was recently revised to include improved treatment of input partitioning and reactivity data, temperature dependence and an easier sensitivity and uncertainty analysis. This New EQC model was used to evaluate the multimedia, fugacity-based fate of decamethylcyclopentasiloxane (D5; CAS No. 541-02-6) in the environment over a temperature range of 1–25 °C. In addition, Monte Carlo uncertainty analysis was used to quantitatively determine the influence of temperature and input partitioning and reactivity data on the behavior of D5 under various emission scenarios. Results indicated that emission mode was the most influential factor determining the fate and distribution of D5 in the model environment. When emitted to air and soil, D5 partitioned to and remained in the air compartment where rates of removal from degradation and advection processes were relatively rapid. In contrast, D5 emitted to water resulted in a substantial mass fraction of D5 being accumulated in the sediment compartment, where rates of removal from degradation and advection processes were slow. The mass distributions and fate of D5 in the model environment were strongly influenced by multiple input parameters, including temperature, the mode of emission (especially emission rate to water), K_OC and half-life in air. As temperature decreased from 25 °C to 1 °C, K_OC and half-life in air became increasingly more influential such that the mass distribution of D5 increased in air and decreased in sediment, resulting in decreased overall persistence.     

Air concentrations of polybrominated diphenyl ethers (PBDEs) in 2002–2004 at a rural site in the Great Lakes

Atmospheric PBDEs were measured on a monthly basis in 2002–2004 at Point Petre, a rural site in the Great Lakes. Average air concentrations were 7.0 ± 13 pg m^?3 for Σ₁₄BDE (excluding BDE-209), and 1.8 ± 1.5 pg m^?3 for BDE-209. Concentrations of 3 dominant congeners (i.e., BDE-47, 99, and 209) were comparable to previous measurements at remote/rural sites around the Great Lakes, but much lower than those at urban areas. Weak temperature dependence and strong linear correlations between relatively volatile congeners suggest importance of advective inputs of gaseous species. The significant correlation between BDE-209 and 183 implies their transport inputs associated with particles. Particle-bound percentages were found greater for highly brominated congeners than less brominated ones. These percentages increase with decreasing ambient temperatures. The observed gas/particle partitioning is consistent with laboratory measurements and fits well to the Junge–Pankow model. Using air mass back-trajectories, atmospheric transport to Point Petre was estimated as 76% for BDE-47, 67% for BDE-99, and 70% for BDE-209 from west–northwest and southwest directions. During the same time period, similar congener profiles and concentration levels were found at Alert in the Canadian High Arctic. Different inter-annual variations between Point Petre and Alert indicate that emissions from other regions than North America could also contribute PBDEs in the Arctic. In contrast to weak temperature effect at Point Petre, significant temperature dependence in the summertime implies volatilization emissions of PBDEs at Alert. Meanwhile, episodic observations in the wintertime were likely associated with enhanced inputs through long-range transport during the Arctic Haze period.     

The Sensitivity of PM25 Source-Receptor Relationships to Atmospheric Chemistry and Transport in a Three-Dimensional Air Quality Model

ABSTRACT

Air quality model simulations constitute an effective approach to developing source-receptor relationships (so-called transfer coefficients in the risk analysis framework) because a significant fraction of particulate matter (particularly PM_2.5) is secondary (i.e., formed in the atmosphere) and, therefore, depends on the atmospheric chemistry of the airshed. In this study, we have used a comprehensive three-dimensional air quality model for PM_{2 5} (SAQM-AERO) to compare three approaches to generating episodic transfer coefficients for several source regions in the Los Angeles Basin. First, transfer coefficients were developed by conducting PM_2.5 SAQM-AERO simulations with reduced emissions of one of four precursors (i.e., primary PM, sulfur dioxide (SO₂), oxides of nitrogen (NO_x), and volatile organic compounds) from each source region. Next, we calculated transfer coefficients using two other methods: (1) a simplified chemistry for PM_2.5 formation, and (2) simplifying assumptions on transport using information limited to basin-wide emission reductions. Transfer coefficients obtained with the simplified chemistry were similar to those obtained with the comprehensive model for VOC emission changes but differed for NO and SO emission changes. The differences were due to the parameterization of the rates of secondary PM formation in the simplified chemistry. In 90% of the cases, transfer coefficients estimated using only basin-wide information were within a factor of two of those obtained with the explicit source-receptor simulations conducted with the comprehensive model. The best agreement was obtained for VOC emission changes; poor agreement was obtained for primary PM_2.5.     

Correlating emissions with time and temperature to predict worst-case emissions from open liquid area sources

The two primary factors influencing ambient air pollutant concentrations are emission rate and dispersion rate. Gaussian dispersion modeling studies for odors, and often other air pollutants, vary dispersion rates using hourly meteorological data. However, emission rates are typically held constant, based on one measured value. Using constant emission rates can be especially inaccurate for open liquid area sources, like wastewater treatment plant units, which have greater emissions during warmer weather, when volatilization and biological activity increase. If emission rates for a wastewater odor study are measured on a cooler day and input directly into a dispersion model as constant values, odor impact will likely be underestimated. Unfortunately, because of project schedules, not all emissions sampling from open liquid area sources can be conducted under worst-case summertime conditions. To address this problem, this paper presents a method of varying emission rates based on temperature and time of the day to predict worst-case emissions. Emissions are varied as a linear function of temperature, according to Henry's law, and a tenth order polynomial function of time. Equation coefficients are developed for a specific area source using concentration and temperature measurements, captured over a multiday period using a data-logging monitor. As a test case, time/temperature concentration correlation coefficients were estimated from field measurements of hydrogen sulfide (H2S) at the Rowlett Creek Wastewater Treatment Plant in Garland, TX. The correlations were then used to scale a flux chamber emission rate measurement according to hourly readings of time and temperature, to create an hourly emission rate file for input to the dispersion model ISCST3. ISCST3 was then used to predict hourly atmospheric concentrations of H2S. With emission rates varying hourly, ISCST3 predicted 384 acres of odor impact, compared with 103 acres for constant emissions. Because field sampling had been conducted on relatively cool days (85-90 degrees F), the constant emission rate underestimated odor impact significantly (by 73%).     

Inverse modeling of BTEX dissolution and biodegradation at the Bemidji, MN crude-oil spill site

The U.S. Geological Survey (USGS) solute transport and biodegradation code BIOMOC was used in conjunction with the USGS universal inverse modeling code UCODE to quantify field-scale hydrocarbon dissolution and biodegradation at the USGS Toxic Substances Hydrology Program crude-oil spill research site located near Bemidji, MN. This inverse modeling effort used the extensive historical data compiled at the Bemidji site from 1986 to 1997 and incorporated a multicomponent transport and biodegradation model. Inverse modeling was successful when coupled transport and degradation processes were incorporated into the model and a single dissolution rate coefficient was used for all BTEX components. Assuming a stationary oil body, we simulated benzene, toluene, ethylbenzene, m,p-xylene, and o-xylene (BTEX) concentrations in the oil and ground water, respectively, as well as dissolved oxygen. Dissolution from the oil phase and aerobic and anaerobic degradation processes were represented. The parameters estimated were the recharge rate, hydraulic conductivity, dissolution rate coefficient, individual first-order BTEX anaerobic degradation rates, and transverse dispersivity. Results were similar for simulations obtained using several alternative conceptual models of the hydrologic system and biodegradation processes. The dissolved BTEX concentration data were not sufficient to discriminate between these conceptual models. The calibrated simulations reproduced the general large-scale evolution of the plume, but did not reproduce the observed small-scale spatial and temporal variability in concentrations. The estimated anaerobic biodegradation rates for toluene and o-xylene were greater than the dissolution rate coefficient. However, the estimated anaerobic biodegradation rates for benzene, ethylbenzene, and m,p-xylene were less than the dissolution rate coefficient. The calibrated model was used to determine the BTEX mass balance in the oil body and groundwater plume. Dissolution from the oil body was greatest for compounds with large effective solubilities (benzene) and with large degradation rates (toluene and o-xylene). Anaerobic degradation removed 77% of the BTEX that dissolved into the water phase and aerobic degradation removed 17%. Although goodness-of-fit measures for the alternative conceptual models were not significantly different, predictions made with the models were quite variable.     

BETR global--a geographically-explicit global-scale multimedia contaminant fate model

We present two new software implementations of the BETR Global multimedia contaminant fate model. The model uses steady-state or non-steady-state mass-balance calculations to describe the fate and transport of persistent organic pollutants using a desktop computer. The global environment is described using a database of long-term average monthly conditions on a 15° × 15° grid. We demonstrate BETR Global by modeling the global sources, transport, and removal of decamethylcyclopentasiloxane (D5).     

Correlating Emissions with Time and Temperature to Predict Worst-Case Emissions from Open Liquid Area Sources

Abstract

The two primary factors influencing ambient air pollutant concentrations are emission rate and dispersion rate. Gaussian dispersion modeling studies for odors, and often other air pollutants, vary dispersion rates using hourly meteorological data. However, emission rates are typically held constant, based on one measured value. Using constant emission rates can be especially inaccurate for open liquid area sources, like wastewater treatment plant units, which have greater emissions during warmer weather, when volatilization and biological activity increase. If emission rates for a wastewater odor study are measured on a cooler day and input directly into a dispersion model as constant values, odor impact will likely be underestimated. Unfortunately, because of project schedules, not all emissions sampling from open liquid area sources can be conducted under worst-case summertime conditions. To address this problem, this paper presents a method of varying emission rates based on temperature and time of the day to predict worst-case emissions. Emissions are varied as a linear function of temperature, according to Henry’s law, and a tenth order polynomial function of time. Equation coefficients are developed for a specific area source using concentration and temperature measurements, captured over a multiday period using a data-logging monitor. As a test case, time/temperature concentration correlation coefficients were estimated from field measurements of hydrogen sulfide (H₂S) at the Rowlett Creek Wastewater Treatment Plant in Garland, TX. The correlations were then used to scale a flux chamber emission rate measurement according to hourly readings of time and temperature, to create an hourly emission rate file for input to the dispersion model ISCST3. ISCST3 was then used to predict hourly atmospheric concentrations of H₂S. With emission rates varying hourly, ISCST3 predicted 384 acres of odor impact, compared with 103 acres for constant emissions. Because field sampling had been conducted on relatively cool days (85–90 °F), the constant emission rate underestimated odor impact significantly (by 73%).     

Soot in the arctic snowpack: a cause for perturbations in radiative transfer

Recent data collected in the Arctic have demonstrated the transport of atmospheric aerosol of anthropogenic origin into that region. Concern over the radiative effect of the highly-absorbing soot component of this aerosol has resulted in a variety of atmospheric sampling efforts aimed at assessing the climatic impact of this component. However, little attention has been given to the measurement of soot deposited on the Arctic snowpack and the resulting perturbation of snow albedo, snowmelt rates and radiative transfer. Here we report measurements of light-absorbing material in the Arctic snowpack for longitudes from 25 E to 160 W. The contributions to light absorption due to natural crustal and soot aerosol are identified by their wavelength dependence. Reductions in Arctic snow albedo of one to several percent appear probable for the soot/ice mass fractions obtained to date. Estimates of the impact of this reduced albedo on the Arctic radiation budget over a season are shown to approximately equal that of the Arctic haze itself. The absorption of shortwave radiation by the springtime snowpack is estimated to be 5–10% higher than that of soot-free snow for this data.     

Natural attenuation of chlorinated ethene compounds: model development and field-scale application at the Dover site

A multi-dimensional and multi-species reactive transport model was developed to aid in the analysis of natural attenuation design at chlorinated solvent sites. The model can simulate several simultaneously occurring attenuation processes including aerobic and anaerobic biological degradation processes. The developed model was applied to analyze field-scale transport and biodegradation processes occurring at the Area-6 site in Dover Air Force Base, Delaware. The model was calibrated to field data collected at this site. The calibrated model reproduced the general groundwater flow patterns, and also, it successfully recreated the observed distribution of tetrachloroethene (PCE), trichloroethene (TCE), dichloroethylene (DCE), vinyl chloride (VC) and chloride plumes. Field-scale decay rates of these contaminant plumes were also estimated. The decay rates are within the range of values that were previously estimated based on lab-scale microcosm and field-scale transect analyses. Model simulation results indicated that the anaerobic degradation rate of TCE, source loading rate, and groundwater transport rate are the important model parameters. Sensitivity analysis of the model indicated that the shape and extent of the predicted TCE plume is most sensitive to transmissivity values. The total mass of the predicted TCE plume is most sensitive to TCE anaerobic degradation rates. The numerical model developed in this study is a useful engineering tool for integrating field-scale natural attenuation data within a rational modeling framework. The model results can be used for quantifying the relative importance of various simultaneously occurring natural attenuation processes.     

Seasonal change of persistent organic pollutant concentrations in air at Niigata area,Japan

The concentrations of persistent organic pollutants (POPs), such as HCB, alpha-, beta-, gamma- and delta-HCH, trans- and cis-chlordane (t-CHL, c-CHL), DDE, DDD and DDT, in ambient air have been measured at five sampling points in Niigata area, Japan (Niigata, Maki, Tsubame, Jouzo and Yahiko) during the period from September 1999 to November 2001. HCB, alpha-HCH, t-CHL and c-CHL showed higher concentrations than the other chemicals in all locations. All the POPs except t-CHL and c-CHL collected at urban sites of the Niigata Plain was almost the same in their concentration levels. Higher concentrations of t-CHL and c-CHL in residential areas should be attributed to the past usage of the chemical as a termiticide. At Yahiko (remote site), most of the POPs showed lower concentrations than those measured at the other sampling sites, although alpha-HCH and gamma-HCH were comparable with the concentrations found at the other sampling sites. All POPs except alpha-HCH and gamma-HCH tend to decrease 41-80% in their concentrations from 2000 to 2001. The lower POPs concentrations in winter and the higher POPs concentrations in summer at every sampling point can be partly explained by temperature differences. Applying the equation of the logarithm of the POP partial pressure in air versus reciprocal temperature (lnPa=m/T+b) to our data, linear relations were observed. HCB gave a poor linearity and the smallest slope, while beta-HCH, t-CHL and c-CHL gave good linearities and large slopes in the equation. The results suggest that HCB level is influenced by not only the emission from terrestrial sources but the global-scale background pollution. A peculiar observation is that beta-HCH concentration measured in our study showed large temperature dependence, indicating there could be a source of contamination in the surrounding areas.     

Past and future trends in concentrations of sulphur and nitrogen compounds in the Arctic

Recent trends in nitrogen and sulphur compounds in air and precipitation from a range of Arctic monitoring stations are presented, with seasonal data from the late 70s to 2004 or 2005. Earlier findings of declining sulphur concentrations are confirmed for most stations, while the pattern is less clear for reduced and oxidized nitrogen. In fact there are positive trends for nitrogen compounds in air at several stations. Acidity is generally reduced at many stations while the precipitation amount is either increasing or stable. Variability of sulphate concentrations in air for the period 1991–2000 is reasonably well reproduced at most stations using an Eulerian, hemispherical model. Results for nitrogen compounds are weaker. Scenario studies show that even if large sulphur emission reductions take place in important source regions in South-East Asia in the coming decades, only small changes in Arctic deposition can be expected. This is because South-East Asian emissions have small influence north of the Arctic circle.