Controls on Mercury and Methylmercury Deposition for Two Watersheds in Acadia National Park, Maine

Throughfall and bulk precipitation samples were collected for two watersheds at Acadia National Park, Maine, from 3 May to 16 November 2000, to determine which landscape factors affected mercury (Hg) deposition. One of these watersheds, Cadillac Brook, burned in 1947, providing a natural experimental design to study the effects of forest type on deposition to forested watersheds. Sites that face southwest received the highest Hg deposition, which may be due to the interception of cross-continental movement of contaminated air masses. Sites covered with softwood vegetation also received higher Hg deposition than other vegetation types because of the higher scavenging efficiency of the canopy structure. Methyl mercury (MeHg) deposition was not affected by these factors. Hg deposition, as bulk precipitation and throughfall was lower in Cadillac Brook watershed (burned) than in Hadlock Brook watershed (unburned) because of vegetation type and watershed aspect. Hg and MeHg inputs were weighted by season and vegetation type because these two factors had the most influence on deposition. Hg volatilization was not determined. The total Hg deposition via throughfall and bulk precipitation was 9.4 μg/m²/year in Cadillac Brook watershed and 10.2 μg/m²/year in Hadlock Brook watershed. The total MeHg deposition via throughfall and bulk precipitation was 0.05 μg/m²/year in Cadillac Brook watershed and 0.10 μg/m²/year in Hadlock Brook watershed.     

Forest Vegetation Monitoring and Foliar Chemistry of Red Spruce and Red Maple at Acadia National Park in Maine

The USDA Forest Service Forest Health Monitoring (FHM) program indicators, including forest mensuration, crown condition classification, and damage and mortality indicators were used in the Cadillac Brook and Hadlock Brook watershed forests at Acadia National Park (ANP) along coastal Maine. Cadillac Brook watershed burned in a wildfire in 1947. Hadlock Brook watershed, undisturbed for several centuries, serves as the reference site. These two small watersheds have been gauged and monitored at ANP since 1998 as part of the Park Research and Intensive Monitoring of Ecosystems Network (PRIMENet). Forest vegetation at Hadlock Brook was dominated by late successional species such as Acer saccharum, Fagus grandifolia, Betula alleghaniensis, Acer rubrum and Picea rubens. Forest vegetation at Cadillac Brook, on the other hand, was younger and more diverse and included those species found in Hadlock as well as early successional species such as Betula papyrifera and Populus grandidentata. Differences in forest species composition and stand structure were attributed to the severe wildfire that affected the Cadillac Brook watershed. Overall, the forests at these ANP watersheds were healthy with a low percentage (相似文献   

Watershed Nitrogen and Mercury Geochemical Fluxes Integrate Landscape Factors in Long-term Research Watersheds at Acadia National Park, Maine, USA

This paper is an overview of this special issue devoted to watershed research in Acadia National Park (Acadia NP). The papers address components of an integrated research program on two upland watersheds at Acadia NP, USA (44° 20′ N latitude; 68° 15′ E longitude). These watersheds were instrumented in 1998 to provide a long-term foundation for regional ecological and watershed research. The research was initiated as part of EPA/NPS PRIMENet (Park Research and Intensive Monitoring of Ecosystems Network), a system of UV-monitoring stations and long-term watershed research sites located in US national parks. The initial goals at Acadia NP were to address research questions about mercury, acid rain, and nitrogen saturation developed from prior research. The project design was based on natural differences in forests and soils induced by an intense wildfire in one watershed in 1947. There is no evidence of fire in the reference watershed for several hundred years. We are testing hypotheses about controls on surface water chemistry, and bioavailability of contaminants in the contrasting watersheds. The unburned 47-ha Hadlock Brook watershed is 70% spruce-fir mature conifer forest. In contrast, burned 32-ha Cadillac Brook watershed, 4 km northeast of the Hadlock watershed, is 20% regenerating mixed northern hardwoods and 60% shrub/rocky balds. Differences in atmospheric deposition are controlled primarily by forest stand composition and age. The watersheds are gauged and have water chemistry stations at 122 m (Cadillac) and 137 m (Hadlock); watershed maximum elevations are 468 and 380 m, respectively. The stream water chemistry patterns reflect, in part, the legacy of the intense fire, which, in turn, controls differences in forest vegetation and soil characteristics. These factors result in higher nitrogen and mercury flux from the unburned watershed, reflecting differences in atmospheric deposition, contrasting ecosystem pools of nitrogen and mercury, and inferred differences in internal cycling and bioavailabilty.     

Streamwater acid-base chemistry and critical loads of atmospheric sulfur deposition in Shenandoah National Park, Virginia

A modeling study was conducted to evaluate the acid-base chemistry of streams within Shenandoah National Park, Virginia and to project future responses to sulfur (S) and nitrogen (N) atmospheric emissions controls. Many of the major stream systems in the park have acid neutralizing capacity (ANC) less than 20 μeq/L, levels at which chronic and/or episodic adverse impacts on native brook trout are possible. Model hindcasts suggested that none of these streams had ANC less than 50 μeq/L in 1900. Model projections, based on atmospheric emissions controls representative of laws already enacted as of 2003, suggested that the ANC of those streams simulated to have experienced the largest historical decreases in ANC will increase in the future. The levels of S deposition that were simulated to cause streamwater ANC to increase or decrease to three specified critical levels (0, 20, and 50 μeq/L) ranged from less than zero (ANC level not attainable) to several hundred kg/ha/year, depending on the selected site and its inherent acid-sensitivity, selected ANC endpoint criterion, and evaluation year for which the critical load was calculated. Several of the modeled streams situated on siliciclastic geology exhibited critical loads <0 kg/ha/year to achieve ANC >50 μeq/L in the year 2040, probably due at least in part to base cation losses from watershed soil. The median modeled siliciclastic stream had a calculated critical load to achieve ANC >50 μeq/L in 2100 that was about 3 kg/ha/year, or 77% lower than deposition in 1990, representing the time of model calibration.     

Characteristic Study of Dry Deposition, Concentration, Compositions for Particulates Mass and Ionic Species During Summer and Autumn Season at a Traffic Sampling Site

Aerosol samples for dry deposition and total suspend particulates (TSP) were collected from August to November of 2003 in central Taiwan. Ion chromatography was used to analyze the related water-soluble ionic species (Cl⁻, NO₃ ⁻, SO₄ ²⁻, Na⁺, NH₄ ⁺, K⁺, Mg²⁺ and Ca²⁺). The results obtained in this study indicated that the ambient air particulate mass concentrations in the daytime period (averaged 975.4 μg m⁻³) were higher than the nighttime period (averaged 542.1 μg m⁻³). And the daytime dry deposition fluxes (averaged 58.12 μg m⁻² sec⁻¹) were about 2.2 times as that of nighttime dry deposition fluxes (averaged 26.54 μg m⁻² sec⁻¹) of the downward dry deposition. The average values downward and upward of dry deposition fluxes for the weekend period were almost higher than the weekday period for either daytime or nighttime period. Furthermore, the average daytime dry deposition fluxes (averaged 26.37 μg m⁻² sec⁻¹) were also about 2.3 times as that of nighttime dry deposition fluxes (averaged 11.52 μg m⁻² sec⁻¹). Moreover, the results also indicate that SO₄ ²⁻ and Ca²⁺ have higher average composition for total suspended particulates in the daytime period while Ca²⁺, SO₄ ²⁻, and Na⁺ have the higher average composition for total suspends particulates in the nighttime period.     

Nutrient Export from Watersheds on Mt. Desert Island, Maine, as a Function of Land Use and Fire History

A study of 13 small (less than 7.5 km²) watersheds on Mt. Desert Island, Maine, was conducted from January 1999 to September 2000 to determine nutrient export delivery to coastal waters around the island, and to determine whether a series of wildfires in 1947 have affected nutrient export in burned watersheds. Nutrient export (nitrate–nitrogen, total nitrogen, total phosphorus) was determined for each watershed during the study period, and was normalized by watershed area. The yield of nitrate–nitrogen (N) ranged from 10 to 140 kg/km²/year. Total N yield ranged from 42 to 250 kg/km²/year. Total phosphorus (P) yield ranged from 1.4 to 7.9 kg/km²/year. Watersheds entirely within Acadia National Park (lacking human land-based nutrient sources) exported significantly less total N and total P than watersheds that were partly or entirely outside the park boundary. Nitrate–N export was not significantly different in these two groups of watersheds, perhaps because atmospheric deposition is a dominant source of nitrate in the study area. No relation was observed between burn history and nutrient export. Any effect of burn history may be masked by other landscape-level factors related to nutrient export.     

Seasonal Variations of PM10 and TSP in Residential and Industrial Sites in an Urban Area of Kolkata, India

The objective of the study is to investigate seasonal and spatial variations of PM₁₀ (particulate matter with aerodynamic diameter less than or equal to 10 μm) and TSP (total suspended particulate matter) of an Indian Metropolis with high pollution and population density from November 2003 to November 2004. Ambient concentration measurements of PM₁₀ and TSP were carried out at two monitoring sites of an urban region of Kolkata. Monitoring sites have been selected based on the dominant activities of the area. Meteorological parameters such as wind speed, wind direction, rainfall, temperature and relative humidity were also collected simultaneously during the sampling period from Indian Meteorological Department, Kolkata. The 24 h average concentrations of PM₁₀ and TSP were found in the range 68.2–280.6 μg/m³ and 139.3–580.3 μg/m³ for residential (Kasba) area, while 62.4–401.2 μg/m³ and 125.7–732.1 μg/m³ for industrial (Cossipore) area, respectively. Winter concentrations of particulate pollutants were higher than other seasons, irrespective of the monitoring sites. It indicates a longer residence time of particulates in the atmosphere during winter due to low winds and low mixing height. Spread of air pollution sources and non-uniform mixing conditions in an urban area often result in spatial variation of pollutant concentrations. The higher particulate pollution at industrial area may be attributed due to resuspension of road dust, soil dust, automobile traffic and nearby industrial emissions. Particle size analysis result shows that PM₁₀ is about 52% of TSP at residential area and 54% at industrial area.     

Monitoring of Criteria Air Pollutants in Bursa, Turkey

The concentrations of criteria air pollutants such as CO, NO_x (NO + NO₂), SO₂ and PM were measured in the period of May 2001 and April 2003 in the city of Bursa, Turkey. The average concentrations for this period were 1115±1600 μg/m³, 29±50 μg/m³, 51±24 μg/m³, 79±65 μg/m³, 40±35 μg/m³, 98±220 μg/m³, for CO, NO, NO₂, NO_x, SO₂ and PM, respectively. Temporal changes in concentrations were analyzed using meteorological factors. Correlations among pollutant concentrations and meteorological parameters showed weak relations nearly in all data. Lower concentrations were observed in the summer months while higher concentrations were measured in the winter months. The increase in winter concentrations was probably due to residential heating. Pollutants were associated with each other in order to have information about their origin. NO_x/SO₂ ratio was also examined to bring out the source origin contributing on air pollution (i.e., traffic or stationary).     

The Bear Brook Watershed, Maine (BBWM), USA

The Bear Brook Watershed Manipulation project in Maine is a paired calibrated watershed study funded by the U. S. EPA. The research program is evaluating whole ecosystem response to elevated inputs of acidifying chemicals. The project consists of a 2.5 year calibration period (1987-1989), nine years of chemical additions of (NH4)2SO4 (15N- and 34S-enriched for several years) to West Bear watershed (1989-1998), followed by a recovery period. The other watershed, East Bear, serves as a reference. Dosing is in six equal treatments/yr of 1800 eq SO4 and NH4/ha/yr, a 200% increase over 1988 loading (wet plus dry) for SO4 and 300% for N (wet NO3 + NH4). The experimental and reference watersheds are forested with mixed hard- and softwoods, and have thin acidic soils, areas of 10.2 and 10.7 ha, and relief of 210 m. Thin till of variable composition is underlain by metasedimentary pelitic rocks and calc-silicate gneiss intruded by granite dikes and sills. For the period 1987-1995, precipitation averaged 1.4 m/yr, had a mean pH of 4.5, with SO4, NO3, and NH4 concentrations of 26, 14, and 7 eq/L, respectively. The nearly perrenial streams draining each watershed have discharges ranging from 0 (East Bear stops flowing for one to two months per year) to 150 L/sec. Prior to manipulation, East Bear and West Bear had a volume weighted annual mean pH of approximately 5.4, alkalinity = 0 to 4 eq/L, total base cations = 184 eq/L (sea-salt corrected = 118 eq/L), and SO4 = 100 to 111 eq/L. Nitrate ranged from 0 to 30 eq/L with an annual mean of 6 to 25 eq/L; dissolved organic carbon (DOC) ranged from 1 to 7 mg/L but was typically less than 3. Episodic acidification occurred at high discharge and was caused by dilution of cations, slightly increased DOC, significantly higher NO3, and the sea-salt effect. Depressions in pH were accompanied by increases in inorganic Al. The West Bear catchment responded to the chemical additions with increased export of base cations, Al, SO4, NO3, and decreased pH, ANC, and DOC. Silica remained relatively constant. Neutralization of the acidifying chemicals occurred dominantly by cation desorption and mobilization of Al.     

Characteristics of Hazardous Airborne Dust Around an Indian Surface Coal Mining Area

Surface coal mining creates more air pollution problems with respect to dust than underground mining . An investigation was conducted to evaluate the characteristics of the airborne dust created by surface coal mining in the Jharia Coalfield. Work zone air quality monitoring was conducted at six locations, and ambient air quality monitoring was conducted at five locations, for a period of 1 year. Total suspended particulate matter (TSP) concentration was found to be as high as 3,723 μg/m³, respirable particulate matter (PM10) 780 μg/m³, and benzene soluble matter was up to 32% in TSP in work zone air. In ambient air, the average maximum level of TSP was 837 μg/m³, PM10 170 μg/m³ and benzene soluble matter was up to 30%. Particle size analysis of TSP revealed that they were more respirable in nature and the median diameter was around 20 μm. Work zone air was found to have higher levels of TSP, PM10 and benzene soluble materials than ambient air. Variations in weight percentages for different size particles are discussed on the basis of mining activities. Anionic concentration in TSP was also determined. This paper concludes that more stringent air quality standards should be adopted for coal mining areas and due consideration should be given on particle size distribution of the air-borne dust while designing control equipment.     

Characterization of Rain and Roof Drainage Water Quality in Xanthi, Greece

Thirteen field campaigns were undertaken in the period from December 2, 2002 until September 1, 2004 to collect water samples in order to characterize the quality of rainfall and roof drainage in the city of Xanthi, a typical provincial city in Greece. In each campaign, water samples were collected from 10 representative sites in the city (in total 130 samples), representing areas of distinct land use and human activities (i.e., traffic volume, residence density and industrial activity). The water samples were analyzed according to drinking water criteria for total coliform (not detected), temperature (range: 0.9–20°C), pH (range: 3.6–11.4), alkalinity (range: 0–21.5 mg CaCO₃/L), nitrate (range: 0–2456 μg/L), ammonium (range: 0–2628 μg/L), sulfate (range: 0–0.5 mg/L), calcium (range: 259.1–3064 μeq/L), magnesium (range: 0.8–488.8 μeq/L), potassium (range: 0.0–110.6 μeq/L) and dissolved heavy metals (Fe, range: 0.01–0.18 mg/L; Mn, range: 0.01–0.09 mg/L; Zn, range: 0.01–0.54 mg/L; Cu, Cr and Ni, not detected). Pollutant concentrations were generally higher in roof drainage than in rainwater, but both were lower than drinking water standards. Dissolved heavy metal concentrations were generally higher in the areas of intensive human activities, such as roads with high traffic volume and densely populated residential areas. The satisfactory quality of rainwater, which results from this analysis, makes its use as grey water possible.     

Evaluation of A Sampling Strategy for Estimation of Long-term Pm2.5 Exposure for Epidemiological Studies

As part of the European Community Respiratory Health Survey (ECRHS) PM_2.5 (particles collected with an upper 50% cut point of 2.5 μm aerodynamic diameter) was measured using an EPA-WINS (Environmetal Protection Agency Well Impactor Ninety-six) sampler. The monitoring schedule was restricted to 7 days per month for one year. Simultaneously, during this one year study period a collocated Harvard Impactor (HI) was run on a daily basis in Erfurt, Germany. Here we validated the reliability of annual, seasonal and monthly means estimated using the ECRHS scheme (measurements taken less than 25% of the whole study period) with the ‘true’ long-term averages, which were estimated using all available daily means.The daily PM_2.5 means, obtained by both instruments operated in parallel, were only slightly different (the mean difference between EPA-WINS and HI was 1.8 μg m⁻³ and 2.8 μg m⁻³ for the winter means). The values obtained by the two instruments were highly correlated (r = 0.95).In view of that negligible difference, no additional bias was seen with respect to the annual and the winter means estimated by the two different sampling strategies (the difference was 1.7 μg m⁻³ and 2.7 μg m⁻³, respectively). Monthly means, however, can only be considered to be a crude estimate that may substantially under- or overestimate the true monthly mean value.     

Appropriate Range of Quality Control Limit for Wet Deposition Monitoring

Precipitation chemistry programs in different regions of the world have different quality control limits for ion balance parameter IPD in wet deposition monitoring (R). The range of R values was calculated by assuming sample rainwater models in this paper. It was found that R was influenced by the inorganic ion types, total ion concentrations (IS) and the accuracy of the measurements (a _i ). R was defined and calculated as a function of a _i and ion concentration C _i . R values of different types of wet deposition (including ocean type, continent type and combined oceanic and continental deposition) were different. There were also differences between the samples of the same type if the samples had different total ion concentrations. When IS>100 μeq/L, the ranges of R of ocean type deposition, continent type deposition and combined oceanic and continental deposition were 5∼7%, 5∼9% and 5∼11%, respectively. When IS<50 μeq/L, if a _i was 100%, the range of R was 33∼71% because of the lower accuracy. It was also found that R of each criterion was in the range of R as calculated in this paper when IS≥50 μeq/L, but when IS<50 μeq/L, the criteria varied greatly in their R values.     

Atmospheric concentrations of nitric acid, sulfur dioxide, particulate nitrate and particulate sulfate, and estimation of their dry deposition on the urban- and mountain-facing sides of Mt. Gokurakuji, Western Japan

Atmospheric concentrations of nitric acid (HNO₃), sulfur dioxide (SO₂), particulate nitrate and particulate sulfate on the urban- and mountain-facing sides of Mt. Gokurakuji were measured from November 2002 to October 2003, in order to evaluate the effects of anthropogenic activity on air quality and dry deposited nitrate and sulfate on the surfaces of pine foliage. The results showed that HNO₃, SO₂ and concentrations were significantly higher (P < 0.05) on the urban-facing side (1.54, 2.48 and 0.65 μg m⁻³, respectively) than the mountain-facing side (0.67, 1.19 and 0.37 μg m⁻³, respectively), while concentrations did not differ significantly between the two sides (urban-facing: 2.80 μg m⁻³; mountain−facing: 2.05 μg m⁻³). Indirect estimates of dry deposition rates of nitrate and sulfate to the surfaces of pine foliage based on the measured concentrations approximately agreed with the measured values determined by the foliar rinsing technique in a previous study. It was found that HNO₃ was the major source (approximately 80%) of dry deposited nitrate on pine foliage, while the contribution from was about equal to that from SO₂. In conclusion, HNO₃ and SO₂ appear to be dominant species reflecting higher dry deposition rates of nitrate and sulfate on the urban-facing side compared to the mountain-facing side of Mt. Gokurakuji.     

Status of insecticide contamination of soil and water in Haryana, India

Twelve samples each of soil and ground water were collected from paddy-wheat, paddy-cotton, sugarcane fields and tube wells from same or near by fields around Hisar, Haryana, India during 2002–2003 to monitor pesticide residues. Residues were estimated by GC-ECD and GC-NPD systems equipped with capillary columns for organochlorine, synthetic pyrethroid and organophosphate insecticides. In soil, HCH (0.002–0.051 μg g⁻¹), DDT (0.001–0.066 μg g⁻¹), endosulfan (0.002–0.039 μg g⁻¹) and chlordane (0.0002–0.019 μg g⁻¹) among organochlorines, cypermethrin (0.001–0.035 μg g⁻¹) and fenvalerate (0.001–0.022 μg g⁻¹) among synthetic pyrethroids and chlorpyriphos (0.002–0.172 μg g⁻¹), malathion (0.002–0.008 μg g⁻¹), quinalphos (0.001–0.010 μg g⁻¹) among organophosphates were detected. Dominant contaminants were DDT, cypermethrin and chlorpyriphos from the respective groups. In water samples, HCH, DDT, endosulfan and cypermethrin residues were observed frequently. Only chlorpyriphos among organophosphates was detected in 10 samples. On consideration of tube well water for drinking purpose, about 80% samples were found to contain residues above the regulatory limits.     

Estimation Of Selenium Concentration In Shallow Groundwater In Alluvial Fan Area In Tsukui, Central Japan

Total selenium (Se) and water-soluble Se in soil, and Se in a shallow groundwater were hydrogeochemically researched in an alluvial fan area in Tsukui, Central Japan. The water-soluble Se was estimated at average level of 2.6 ± 1.2μg Se kg⁻¹ dry soil (± SD, n = 25), showing less than 1% of the total Se (349–508μg Se kg⁻¹ dry soil) in soil. The monthly Se concentration in groundwater was average 2.2μg,L⁻¹, ranging 1.6–2.4μg,L⁻¹ during 2001–2003. The Se in groundwater significantly decreased with increasing groundwater level after rainfall. This result indicated that Se-bearing water percolated with relatively low Se concentration through the soil layer. According to our prediction model of linear regression curve on the observation data, Se concentration in the groundwater was estimated to be increasing with the very low rate of 4.35 × 10⁻³μg Se L⁻¹,yr⁻¹. The hydrogeochemical research and the result of the prediction model showed that any explosive increase of Se will hardly occur in this groundwater without an anthropogenic Se contamination.     

Ambient Aerosol and its Carbon Content in Gainesville, a Mid-Scale City in Florida

Ambient aerosols were collected during 2000–2001 in Gainesville, Florida, using a micro-orifice uniform deposit impactor (MOUDI) to study mass size distribution and carbon composition. A bimodal mass distribution was found in every sample with major peaks for aerosols ranging from 0.32 to 0.56 μm, and 3.2 to 5.6 μm in diameter. The two distributions represent the fine mode (<2.5 μm) and the coarse mode (>2.5 μm) of particle size. Averaged over all sites and seasons, coarse particles consisted of 15% carbon while fine particles consisted of 22% carbon. Considerable variation was noted between winter and summer seasons. Smoke from fireplaces in winter appeared to be an important factor for the carbon, especially the elemental carbon contribution. In summer, organic carbon was more abundant. The maximum secondary organic carbon was also found in this season (7.0 μg m⁻³), and the concentration is between those observed in urban areas (15–20 μg m⁻³) and in rural areas (4–5 μg m⁻³). However, unlike in large cities where photochemical activity of anthropogenic emissions are determinants of carbon composition, biogenic sources were likely the key factor in Gainesville. Other critical factors that affect the distribution, shape and concentration were precipitation, brushfire and wind.     

Sulphate, Nitrogen and Base Cation Budgets at 21 Forested Catchments in Canada, the United States and Europe

To assess the concern over declining base cation levels in forest soils caused by acid deposition, input-output budgets (1990s average) for sulphate (SO₄), inorganic nitrogen (NO₃-N; NH₄-N), calcium (Ca), magnesium (Mg) and potassium (K) were synthesised for 21 forested catchments from 17 regions in Canada, the United States and Europe. Trend analysis was conducted on monthly ion concentrations in deposition and runoff when more than 9 years of data were available (14 regions, 17 sites). Annual average SO₄ deposition during the 1990s ranged between 7.3 and 28.4 kg ha⁻¹ per year, and inorganic nitrogen (N) deposition was between 2.8 and 13.8 kg ha⁻¹ per year, of which 41–67% was nitrate (NO₃-N). Over the period of record, SO₄ concentration in deposition decreased in 13/14 (13 out of 14 total) regions and SO₄ in runoff decreased at 14/17 catchments. In contrast, NO₃-N concentrations in deposition decreased in only 1/14 regions, while NH₄-N concentration patterns varied; increasing at 3/14 regions and decreasing at 2/14 regions. Nitrate concentrations in runoff decreased at 4/17 catchments and increased at only 1 site, whereas runoff levels of NH₄-N increased at 5/17 catchments. Decreasing trends in deposition were also recorded for Ca, Mg, and K at many of the catchments and on an equivalent basis, accounted for up to 131% (median 22%) of the decrease in acid anion deposition. Base cation concentrations in streams generally declined over time, with significant decreases in Ca, Mg and K occurring at 8, 9 and 7 of 17 sites respectively, which accounted for up to 133% (median 48%) of the decrease in acid anion concentration. Sulphate export exceeded input at 18/21 catchments, likely due to dry deposition and/or internal sources. The majority of N in deposition (31–100%; median 94%) was retained in the catchments, although there was a tendency for greater NO₃-N leaching at sites receiving higher (<7 kg ha^-1 per year) bulk inorganic N deposition. Mass balance calculations show that export of Ca and Mg in runoff exceeds input at all 21 catchments, but K export only exceeds input at 16/21 sites. Estimates of base cation weathering were available for 18 sites. When included in the mass balance calculation, Ca, Mg and K exports exceeded inputs at 14, 10 and 2 sites respectively. Annual Ca and Mg losses represent appreciable proportions of the current exchangeable soil Ca and Mg pools, although losses at some of the sites likely occur from weathering reactions beneath the rooting zone and there is considerable uncertainty associated with mineral weathering estimates. Critical loads for sulphur (S) and N, using a critical base cation to aluminium ratio of 10 in soil solution, are currently exceeded at 7 of the 18 sites with base cation weathering estimates. Despite reductions in SO₄ and H⁺ deposition, mass balance estimates indicate that acid deposition continues to acidify soils in many regions with losses of Ca and Mg of primary concern. The U.S. Government's right to retain a non-exclusive, royalty free licence in and to any copyright is acknowledged. The Canadian Crown reserves the right to retain a non-exclusive, royalty free licence in and to any copyright.     

Twenty-year inter-annual trends and seasonal variations in precipitation and stream water chemistry at the Bear Brook Watershed in Maine, USA

Mean annual concentration of ${\textrm{SO}}_{4}^{2-}$ in wet-only deposition has decreased between 1988 and 2006 at the paired watershed study at Bear Brook Watershed in Maine, USA (BBWM) due to substantially decreased emissions of SO₂. Emissions of NO_x have not changed substantially, but deposition has declined slightly at BBWM. Base cations, ${\textrm{NH}}_{4}^{+}$ , and Cl^??? concentrations were largely unchanged, with small irregular changes of <1 μeq L^???1 per year from 1988 to 2006. Precipitation chemistry, hydrology, vegetation, and temperature drive seasonal stream chemistry. Low flow periods were typical in June–October, with relatively greater contributions of deeper flow solutions with higher pH; higher concentrations of acid-neutralizing capacity, Si, and non-marine Na; and low concentrations of inorganic Al. High flow periods during November–May were typically dominated by solutions following shallow flow paths, which were characterized by lower pH and higher Al and DOC concentrations. Biological activity strongly controlled ${\textrm{NO}}_{3}^{-}$ and K^?+?. They were depressed during the growing season and elevated in the fall. Since 1987, East Bear Brook (EB), the reference stream, has been slowly responding to reduced but still elevated acid deposition. Calcium and Mg have declined fairly steadily and faster than ${\textrm{SO}}_{4}^{2-}$ , with consequent acidification (lower pH and higher inorganic Al). Eighteen years of experimental treatment with (NH₄)₂SO₄ enhanced acidification of West Bear Brook’s (WB) watershed. Despite the manipulation, ${\textrm{NH}}_{4}^{+}$ concentration remained below detection limits at WB, while leaching of ${\textrm{NO}}_{3}^{-}$ increased. The seasonal pattern for ${\textrm{NO}}_{3}^{-}$ concentrations in WB, however, remained similar to EB. Mean monthly concentrations of ${\textrm{SO}}_{4}^{2-}$ have increased in WB since 1989, initially only during periods of high flow, but gradually also during base flow. Increases in mean monthly concentrations of Ca^2?+?, Mg^2?+?, and K^?+? due to the manipulation occurred from 1989 until about 1995, during the depletion of base cations in shallow flow paths in WB. Progressive depletion of Ca and Mg at greater soil depth occurred, causing stream concentrations to decline to pre-manipulation values. Mean monthly Si concentrations did not change in EB or WB, suggesting that the manipulation had no effect on mineral weathering rates. DOC concentrations in both streams did not exhibit inter- or intra-annual trends.     

Concentrations of PM2.5-associated OC, EC, and PCDD/Fs measured during the 2003 wildfire season in Missoula, Montana

Throughout August and September, 2003, wildfires burned in close proximity to Missoula, Montana, with smoke emanating from the fires impacting the valley for much of the summer. This presented the perfect opportunity to measure the levels of polychlorinated dibenzodioxins and dibenzofurans (PCDD/F) comprising ambient forest fire smoke particles impacting the Missoula Valley. An air sampler at the Montana Department of Environmental Quality's (DEQ) compliance site in Missoula measured hourly averages of PM₁₀ throughout the fire season. Three collocated PM_2.5 cyclones collected 24-h smoke samples using quartz filters and Polyurethane Foam (PUF) sorbent cartridges. From the quartz filters, concentrations of Organic and Elemental Carbon (OC/EC) were measured, while PCDD/F were measured from one set of a filter (particle phase) and PUF (vapor phase) aggregate of samples in an attempt to also investigate the different phases of PCDD/F in forest fire smoke impaired communities.Hourly PM₁₀ concentrations peaked at 302.9 μg m⁻³ on August 15. The highest OC concentration (115.6 μg m⁻³) was measured between August 21–22, and the highest EC concentration of 10.5 μg m⁻³ was measured August 20–21. Measurable concentrations of PM_2.5 associated PCDD/Fs were not detected from a representative aggregate sample, with the exception of small amounts of 1,2,3,4,6,7,8-heptachlorodibenzodioxin and octachlorodibenzodioxin. PM_2.5 samples collected during the smoke events were composed of approximately 65% OC. However, the OC fraction of the particles collected in the smoke impaired Missoula valley was not composed of significant amounts of PCDD/F.