Trends in snowpack chemistry and comparison to National Atmospheric Deposition Program results for the Rocky Mountains, US, 1993–2004

Seasonal snowpack chemistry data from the Rocky Mountain region of the US was examined to identify long-term trends in concentration and chemical deposition in snow and in snow-water equivalent. For the period 1993–2004, comparisons of trends were made between 54 Rocky Mountain Snowpack sites and 16 National Atmospheric Deposition Program wetfall sites located nearby in the region. The region was divided into three subregions: Northern, Central, and Southern. A non-parametric correlation method known as the Regional Kendall Test was used. This technique collectively computed the slope, direction, and probability of trend for several sites at once in each of the Northern, Central, and Southern Rockies subregions. Seasonal Kendall tests were used to evaluate trends at individual sites.Significant trends occurred during the period in wetfall and snowpack concentrations and deposition, and in precipitation. For the comparison, trends in concentrations of ammonium, nitrate, and sulfate for the two networks were in fair agreement. In several cases, increases in ammonium and nitrate concentrations, and decreases in sulfate concentrations for both wetfall and snowpack were consistent in the three subregions. However, deposition patterns between wetfall and snowpack more often were opposite, particularly for ammonium and nitrate. Decreases in ammonium and nitrate deposition in wetfall in the central and southern rockies subregions mostly were moderately significant (p<0.11) in constrast to highly significant increases in snowpack (p<0.02). These opposite trends likely are explained by different rates of declining precipitation during the recent drought (1999–2004) and increasing concentration. Furthermore, dry deposition was an important factor in total deposition of nitrogen in the region. Sulfate deposition decreased with moderate to high significance in all three subregions in both wetfall and snowpack. Precipitation trends consistently were downward and significant for wetfall, snowpack, and snow-telemetry data for the central and southern rockies subregions (p<0.03), while no trends were noted for the Northern Rockies subregion.     

Aerosol physical,chemical and optical properties during the Rocky Mountain Airborne Nitrogen and Sulfur study

During the Rocky Mountain Airborne Nitrogen and Sulfur (RoMANS) study, conducted during the spring and summer of 2006, a suite of instruments located near the eastern boundary of Rocky Mountain National Park (RMNP) measured aerosol physical, chemical and optical properties. Three instruments, a differential mobility particle sizer (DMPS), an optical particle counter (OPC), and an aerodynamic particle sizer (APS), measured aerosol size distributions. Aerosols were sampled by an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampler and a URG denuder/filter-pack system for compositional analysis. An Optec integrating nephelometer measured aerosol light scattering. The spring time period had lower aerosol concentrations, with an average volume concentration of 2.2 ± 2.6 μm³ cm^?3 compared to 6.5 ± 3.9 μm³ cm^?3 in the summer. During the spring, soil was the single largest constituent of PM_2.5 mass, accounting for 32%. During the summer, organic carbon accounted for 60% of the PM_2.5 mass. Sulfates and nitrates had higher fractional contributions in the spring than the summer. Variability in aerosol number and volume concentrations and in composition was greater in the spring than in the summer, reflecting differing meteorological conditions. Aerosol scattering coefficients (b_sp) measured by the nephelometer compared well with those calculated from Mie theory using size distributions, composition data and modeled RH dependent water contents.     

High concentrations and dry deposition of reactive nitrogen species at two sites in the North China Plain

Atmospheric concentrations of major reactive nitrogen (N_r) species were quantified using passive samplers, denuders, and particulate samplers at Dongbeiwang and Quzhou, North China Plain (NCP) in a two-year study. Average concentrations of NH₃, NO₂, HNO₃, pNH₄⁺ and pNO₃⁻ were 12.0, 12.9, 0.6, 10.3, and 4.7 μg N m⁻³ across the two sites, showing different seasonal patterns of these N_r species. For example, the highest NH₃ concentration occurred in summer while NO₂ concentrations were greater in winter, both of which reflected impacts of N fertilization (summer) and coal-fueled home heating (winter). Based on measured N_r concentrations and their deposition velocities taken from the literature, annual N dry deposition was up to 55 kg N ha⁻¹. Such high concentrations and deposition rates of N_r species in the NCP indicate very serious air pollution from anthropogenic sources and significant atmospheric N input to crops.     

Spatial variability of ammonium and nitrate in soils near a poultry farm

This paper assesses the distribution of ammonium (NH4+) and nitrate (NO3-) nitrogen deposition in native bushland soil adjacent to an open ventilated poultry farm. The farm is located in Thirlmere 150 km south west of Sydney, Australia. A total of 104 geographically referenced soil cores were obtained from the study area. Soil pH, electrical conductivity (EC), NH4(+) - and NO3(-)-nitrogen concentrations were analysed for variable trends at three depths, i.e. 0-30, 30-60, and 60-90 cm. Significantly higher concentrations of the two nitrogen forms and EC were observed nearer to the farm in the surface soil samples (0-30 cm). The distribution of NH4+, NO3- and EC were all correlated in surface samples throughout the study area. There was no indication of NH4+ and NO3- leaching within soil profile sampled and it appears that weeds and native vegetation had utilised the accumulated nitrogen. The level of N deposition adjacent to the poultry farm decreased downwind due to dispersion of plume and to the buffering effects from the bushland.     

Effects of Atmospheric Nitrogen Deposition on Remote Freshwater Ecosystems

We review known and hypothesized effects of nitrogen (N) deposition owing to human activities on the chemistry, organisms, and ecosystem processes of remote oligotrophic freshwaters. Acidification is the best-known effect of N deposition on water chemistry, but additional effects include increased nutrient availability and alteration of the balance between N and other nutrients. Our synthesis of the literature, framed in a comprehensive model for the effects of N deposition on natural ecosystems, shows that all these effects can reduce biological diversity and alter ecosystem processes in remote freshwaters. N deposition is projected to grow worldwide in the near future and will interact with other global changes. Present effects on these fragile ecosystems may be only early signs of more radical impacts ahead.     

Experimental field estimation of organic nitrogen formation in tree canopies

The content of organic N has been shown in many studies to increase during the passage of rain water through forest canopies. The source of this organic N is unknown, but generally assumed to come from canopy processing of wet or dry-deposited inorganic N. There have been very few experimental studies in the field to address the canopy formation or loss of organic N. We report two studies: a Scots pine canopy exposed to ammonia gas, and a Sitka spruce canopy exposed to ammonium and nitrate as wet deposition. In both cases, organic N deposition in throughfall was increased, but only represented a small fraction (<10%) of the additional inorganic N supplied, suggesting a limited capacity for net organic N production, similar in both conifer canopies under Scottish summertime conditions, of less than 1.6 mmol N m⁻² mth⁻¹ (equivalent to 3 kg N ha⁻¹ y⁻¹).     

Measurements and modeling of reactive nitrogen deposition in southeast Brazil

Increased reactive nitrogen (N_r) deposition due to expansion of agro-industry was investigated considering emission sources, atmospheric transport and chemical reactions. Measurements of the main inorganic nitrogen species (NO₂, NH₃, HNO₃, and aerosol nitrate and ammonium) were made over a period of one year at six sites distributed across an area of ∼130,000 km² in southeast Brazil. Oxidized species were estimated to account for ∼90% of dry deposited N_r, due to the region’s large emissions of nitrogen oxides from biomass burning and road transport. NO₂-N was important closer to urban areas, however overall HNO₃-N represented the largest component of dry deposited N_r. A simple mathematical modeling procedure was developed to enable estimates of total N_r dry deposition to be made from knowledge of NO₂ concentrations. The technique, whose accuracy here ranged from <1% to 29%, provides a useful new tool for the mapping of reactive nitrogen deposition.     

Nitrogen deposition threatens species richness of grasslands across Europe

Evidence from an international survey in the Atlantic biogeographic region of Europe indicates that chronic nitrogen deposition is reducing plant species richness in acid grasslands. Across the deposition gradient in this region (2-44 kg N ha⁻¹ yr⁻¹) species richness showed a curvilinear response, with greatest reductions in species richness when deposition increased from low levels. This has important implications for conservation policies, suggesting that to protect the most sensitive grasslands resources should be focussed where deposition is currently low. Soil pH is also an important driver of species richness indicating that the acidifying effect of nitrogen deposition may be contributing to species richness reductions. The results of this survey suggest that the impacts of nitrogen deposition can be observed over a large geographical range.     

The impact of nitrogen deposition on acid grasslands in the Atlantic region of Europe

A survey of 153 acid grasslands from the Atlantic biogeographic region of Europe indicates that chronic nitrogen deposition is changing plant species composition and soil and plant-tissue chemistry. Across the deposition gradient (2-44 kg N ha⁻¹ yr⁻¹) grass richness as a proportion of total species richness increased whereas forb richness decreased. Soil C:N ratio increased, but soil extractable nitrate and ammonium concentrations did not show any relationship with nitrogen deposition. The above-ground tissue nitrogen contents of three plant species were examined: Agrostis capillaris (grass), Galium saxatile (forb) and Rhytidiadelphus squarrosus (bryophyte). The tissue nitrogen content of neither vascular plant species showed any relationship with nitrogen deposition, but there was a weak positive relationship between R. squarrosus nitrogen content and nitrogen deposition. None of the species showed strong relationships between above-ground tissue N:P or C:N and nitrogen deposition, indicating that they are not good indicators of deposition rate.     

Nitrogen isotope variations in camphor (Cinnamomum Camphora) leaves of different ages in upper and lower canopies as an indicator of atmospheric nitrogen sources

Nitrogen isotopic composition of new, middle-aged and old camphor leaves in upper and lower canopies has been determined in a living area, near a motorway and near an industrial area (Jiangan Chemical Fertilizer Plant). We found that at sites near roads, more positive δ¹⁵N values were observed in the camphor leaves, especially in old leaves of upper canopies, and ?δ¹⁵N = δ¹⁵N_upper − δ¹⁵N_lower > 0, while those near the industrial area had more negative δ¹⁵N values and ?δ¹⁵N < 0. These could be explained by two isotopically different atmospheric N sources: greater uptake from isotopically heavy pools of atmospheric NO_x by old leaves in upper canopies at sites adjacent to roads, and greater uptake of ¹⁵N-depleted NH_y in atmospheric deposition by leaves at sites near the industrial area. This study presents novel evidence that ¹⁵N natural abundance of camphor leaves can be used as a robust indicator of atmospheric N sources.     

Precursors and nitrogen origins of trichloronitromethane and dichloroacetonitrile during chlorination/chloramination

The formation of trichloronitromethane (TCNM) and dichloroacetonitrile (DCAN) was investigated during chlorination and chloramination of 31 organic nitrogen (org-N) compounds, including amino acids, amines, dipeptides, purines, pyrimidones and pyrroles. Tryptophan and alanine generated the greatest amount of TCNM during chlorination process and asparagine and tyrosine yielded the highest amount of TCNM during chloramination process. Tryptophan, tyrosine, asparagine, and alanine produced more DCAN than other org-N compounds regardless of chlorination or chloramination. TCNM and DCAN formation was higher by chlorination than by chloramination. NH₂Cl:org-N molar ratios, reaction time, and pH affected N-DBPs formation in varying degrees. TCNM and DCAN yields were usually high during chloramination of tyrosine, asparagine, and methylpyrrole under the following reaction conditions: NH₂Cl:org-N molar ratios greater than 10, reaction time for 1 d, and at pH 7.2. NH₂Cl as a major nitrogen origin in TCNM and DCAN was confirmed via labeled ¹⁵N-monochloramine during chloramination of tyrosine, asparagine and methylpyrrole. In contrast, the majority of nitrogen in TCNM originated from glycine, and that in DCAN originated from pyrrole. Based on the intermediates identified by gas chromatography/mass spectrometry (GC/MS), a pathway scheme was proposed for TCNM and DCAN formation.     

Assessing the Impacts of Long-Range Sulfur and Nitrogen Deposition on Arctic and Sub-Arctic Ecosystems

For more than a decade, anthropogenic sulfur (S) and nitrogen (N) deposition has been identified as a key pollutant in the Arctic. In this study new critical loads of acidity (S and N) were estimated for terrestrial ecosystems north of 60° latitude by applying the Simple Mass Balance (SMB) model using two critical chemical criteria (Al/Bc = 1 and ANC_le = 0). Critical loads were exceeded in large areas of northern Europe and the Norilsk region in western Siberia during the 1990s, with the more stringent criterion (ANC_le = 0) showing the larger area of exceedance. However, modeled deposition estimates indicate that mean concentrations of sulfur oxides and total S deposition within the Arctic almost halved between 1990 and 2000. The modeled exceeded area is much reduced when currently agreed emission reductions are applied, and almost disappears under the implementation of maximum technically feasible reductions by 2020. In northern North America there was no exceedance under any of the deposition scenarios applied. Modeled N deposition was less than 5 kg ha⁻¹ y⁻¹ almost across the entire study area for all scenarios; and therefore empirical critical loads for the eutrophying impact of nitrogen are unlikely to be exceeded. The reduction in critical load exceedances is supported by observed improvements in surface water quality, whereas the observed extensive damage of terrestrial vegetation around the mining and smelter complexes in the area is mainly caused by direct impacts of air pollution and metals.     

Atmospheric nitrogen deposition: revisiting the question of the importance of the organic component

The organic component of atmospheric reactive nitrogen plays a role in biogeochemical cycles, climate and ecosystems. Although its deposition has long been known to be quantitatively significant, it is not routinely assessed in deposition studies and monitoring programmes. Excluding this fraction, typically 25-35%, introduces significant uncertainty in the determination of nitrogen deposition, with implications for the critical loads approach. The last decade of rainwater studies substantially expands the worldwide dataset, giving enough global coverage for specific hypotheses to be considered about the distribution, composition, sources and effects of organic-nitrogen deposition. This data collation and meta-analysis highlights knowledge gaps, suggesting where data-gathering efforts and process studies should be focused. New analytical techniques allow long-standing conjectures about the nature and sources of organic N to be investigated, with tantalising indications of the interplay between natural and anthropogenic sources, and between the nitrogen and carbon cycles.     

Soil type affects migration pattern of airborne Pb and Cd under a spruce-beech forest of the UN-ECE integrated monitoring site Zöbelboden, Austria

Anthropogenic trace element emissions have declined. However, top soils all over the world remain enriched in trace elements. We investigated Pb and Cd migration in forest soils of a remote monitoring site in the Austrian limestone Alps between 1992 and 2004. Large spatial variability masked temporal changes in the mineral soil of Lithic Leptosols (Skeltic), whereas a significant reduction of Pb concentrations in their forest floors occurred. Reductions of concentrations in the less heterogeneous Cambisols (Chromic) were significant. In contrast, virtually no migration of Pb and Cd were found in Stagnosols due to their impeded drainage. Very low element concentrations (<1 μg l⁻¹) in field-collected soil solutions using tension lysimeters (0.2 μm nylon filters) imply that migration largely occurred by preferential flow as particulate-bound species during intensive rainfall events. Our results indicate that the extent of Pb and Cd migration in soils is largely influenced by soil type.     

Nitrogen concentrations in mosses indicate the spatial distribution of atmospheric nitrogen deposition in Europe

In 2005/6, nearly 3000 moss samples from (semi-)natural location across 16 European countries were collected for nitrogen analysis. The lowest total nitrogen concentrations in mosses (<0.8%) were observed in northern Finland and northern UK. The highest concentrations (≥1.6%) were found in parts of Belgium, France, Germany, Slovakia, Slovenia and Bulgaria. The asymptotic relationship between the nitrogen concentrations in mosses and EMEP modelled nitrogen deposition (averaged per 50 km × 50 km grid) across Europe showed less scatter when there were at least five moss sampling sites per grid. Factors potentially contributing to the scatter are discussed. In Switzerland, a strong (r² = 0.91) linear relationship was found between the total nitrogen concentration in mosses and measured site-specific bulk nitrogen deposition rates. The total nitrogen concentrations in mosses complement deposition measurements, helping to identify areas in Europe at risk from high nitrogen deposition at a high spatial resolution.     

Historical nitrogen content of bryophyte tissue as an indicator of increased nitrogen deposition in the Cape Metropolitan Area, South Africa

Information on changes in precipitation chemistry in the rapidly expanding Cape Metropolitan Area (CMA) of South Africa is scarce. To obtain a long-term record of N deposition we investigated changes in moss foliar N, C:N ratios and nitrogen isotope values that might reflect precipitation chemistry. Tissue from 9 species was obtained from herbarium specimens collected between 1875 and 2000 while field samples were collected in 2001/2002. There is a strong trend of increasing foliar N content in all mosses collected over the past century (1.32-1.69 %N). Differences exist between ectohydric mosses which have higher foliar N than the mixohydric group. C:N ratios declined while foliar δ¹⁵N values showed no distinct pattern. From relationships between moss tissue N and N deposition rates we estimated an increase of 6-13 kg N ha⁻¹ a⁻¹ since 1950. Enhanced N deposition rates of this magnitude could lead to biodiversity losses in native ecosystems.     

氮沉降对香樟叶片光合及叶绿素荧光特性的影响研究

以香樟(Cinnamomum cam phora)为试验材料,通过模拟氮沉降的方法,研究了不同氮沉降条件下香樟叶片的光合、叶绿素荧光生理的表现,揭示了相应的生理生态机制.结果表明,适当浓度的氮沉降对香樟的生长具有促进作用,而过量的氮沉降会降低其净光合速率,从而对其生长产生抑制作用;不同处理组香樟的光补偿点(LCP)、光...     

Evaluation of surface runoff and road dust as sources of nitrogen using nitrate isotopic composition

Stable nitrogen and oxygen isotope ratios of nitrate (δ¹⁵N-NO₃ and δ¹⁸O-NO₃) have recently been used to identify nitrogen sources in water environments. However, there have been no investigations designed to determine nitrate isotopes in non-point sources in urban areas for evaluating the impact of surface deposits on nitrogen in surface runoff. In this study, we collected rainwater, surface runoff and surface deposits (road dust, roof dust and soil) to evaluate the nitrogen sources in surface runoff using nitrate isotopes. There were no large differences in δ¹⁵N-NO₃ among rainwater (−0.3‰ to 1.5‰), surface runoff (−2.7‰ to 0.4‰), leachates from road dust (−5.8‰ to 6.2‰) and soil (−11.5‰ to 0.6‰). In contrast, the δ¹⁸O-NO₃ in surface runoff (28.5-47.9‰) was lower than that in rainwater (62.7-78.6‰), and higher than that in leachates from road dust (6.1-27.6‰) and soil (−1.1‰ to 6.6‰). δ¹⁸O-NO₃ is a useful indicator for evaluating the NO₃-N sources in surface runoff. Using this indicator, NO₃-N from road dust was estimated to account for more than half of the NO₃-N in surface runoff. This is consistent with a result based on a comparison of their loads per unit surface between rainwater and surface runoff, which also showed that most of the nitrogen in surface runoff was derived from surface deposits.     

Dynamic modelling of atmospherically-deposited Ni, Cu, Zn, Cd and Pb in Pennine catchments (northern England)

Simulation modelling with CHUM-AM was carried out to investigate the accumulation and release of atmospherically-deposited heavy metals (Ni, Cu, Zn, Cd and Pb) in six moorland catchments, five with organic-rich soils, one with calcareous brown earths, in the Pennine chain of northern England. The model considers two soil layers and a third layer of weathering mineral matter, and operates on a yearly timestep, driven by deposition scenarios covering the period 1400-2010. The principal processes controlling heavy metals are competitive solid-solution partitioning of solutes, chemical interactions in solution, and chemical weathering. Agreement between observed and simulated soil metal pools and surface water concentrations for recent years was generally satisfactory, the results confirming that most contemporary soil metal is from atmospheric pollution. Metals in catchments with organic-rich soils show some mobility, especially under more acid conditions, but the calcareous mineral soils have retained nearly all anthropogenic metal inputs. Complexation by dissolved organic matter and co-transport accounts for up to 80% of the Cu in surface waters.     

南京市区植物叶片氮、硫、铅含量与大气污染评价

通过对南京市区的各功能区植物叶片中的氮、硫、铅元素含量的分析，研究了植物大气环境污染指数，探讨了植物叶片的氮、硫、铅元素含量的季节变化，以及与城市大气环境污染之间的关系。结果表明，植物叶片中，硫、铅元素的含量随季节变化不断增加，而氮元素含量相应减少；各功能区的硫、铅元素含量明显高于清洁对照区；用植物污染指数可以综合评价大气环境的质量状况。