Trends in atmospheric reactive nitrogen for the Eastern United States

Reactive nitrogen can travel far from emission sources and impact sensitive ecosystems. From 2002 to 2006, policy actions have led to decreases in NO(x) emissions from power plants and motor vehicles. In this study, atmospheric chemical transport modeling demonstrates that these emissions reductions have led to a downward trend in ambient measurements of transported reactive nitrogen, especially atmospheric concentrations and wet deposition of nitrate. The trend in reduced nitrogen, namely ammonium, is ambiguous. As reduced nitrogen becomes a larger fraction of the reactive nitrogen budget, wide-spread NH(3) measurements and improved NH(3) emissions assessments are a critical need.     

Effects of geographical location and land use on atmospheric deposition of nitrogen in the State of Connecticut

A network of eight monitoring stations was established to study the atmospheric nitrogen concentration and deposition in the State of Connecticut. The stations were classified into urban, rural, coastal and inland categories to represent the geographical location and land use characteristics surrounding the monitoring sites. Nitrogen species including nitrate, ammonium, nitric acid vapor and organic nitrogen in the air and precipitation were collected, analyzed and used to infer nitrogen concentrations and dry and wet deposition flux densities for the sampling period from 1997 through 1999, with independently collected meteorological data. Statistical analyses were conducted to evaluate the spatial variations of atmospheric concentration and deposition fluxes of total nitrogen in Connecticut. A slightly higher atmospheric concentration of total nitrogen was observed along the Connecticut coastline of Long Island Sound compared to inland areas, while the differences of nitrogen deposition fluxes were insignificant between coastal and inland sites. The land use characteristics surrounding the monitoring sites had profound effects on the atmospheric nitrogen concentration and dry deposition flux. The ambient nitrogen concentration over the four urban sites was averaged 38.9% higher than that over the rural sites, resulting a 58.0% higher dry deposition flux in these sites compared to their rural counterparts. The local industrial activities and traffic emissions of nitrogen at urban areas had significant effects on the spatial distribution of atmospheric nitrogen concentration and dry deposition flux in the State. Wet and total deposition fluxes appeared to be invariant between the monitoring sites, except for high flux densities measured at Old Greenwich, a monitoring station near to and downwind of the New York and New Jersey industrial complexes.     

The effect of variable sub-grid deposition factors on the results of the lagrangian long-range transport model of EMEP

The EMEP/MSC-W routine model for long-range atmospheric transport of sulphur and nitrogen includes a correction for the unresolved sub-grid-scale deposition in emission grid-squares. A constant fraction of the emissions is assumed to be directly deposited inside the first grid-square. Experiments have been performed to estimate the effects of using factors which vary with emission height and meteorological conditions. Results indicate that the constant local deposition factor used for sulphur dioxide in the routine model, is an overestimate, in particular for high-level emission sources. The change in annual deposition caused by the new local deposition factor for sulphur dioxide, is most clearly seen as a decreased deposition in the grid-squares with the largest emissions such as due for the former German Democratic Republic. The amount of this decrease strongly depends on the source height distribution. With the presently available emission data, a decrease of maximum 36% can be expected in individual grid squares. In grid-squares dominated by transboundary deposition, the increase is typically lower than 10%.     

Can the foliar nitrogen concentration of upland vegetation be used for predicting atmospheric nitrogen deposition? Evidence from field surveys

The deposition of atmospheric nitrogen can be enhanced at high altitude sites as a consequence of cloud droplet deposition and orographic enhancement of wet deposition on hills. The degree to which the increased deposition of nitrogen influences foliar nitrogen concentration in a range of upland plant species was studied in a series of field surveys in northern Britain. A range of upland plant species sampled along altitudinal transects at sites of known atmospheric nitrogen deposition showed marked increases in foliar nitrogen concentration with increasing nitrogen deposition and altitude (and hence with decreasing temperature). For Nardus stricta L., Deschampsia flexuosa (L.) Trin., Calluna vulgaris (L.) Hull, Erica cinerea L. and Hylocomium splendens (Hedw.) Br. Eur. on an unpolluted hill, foliar nitrogen increased by 0.07, 0.12, 0.15, 0.08 and 0.04% dry weight respectively for each 1 kg ha(-1) year(-1) increase in nitrogen deposition. Most species showed an approximately linear relationship between foliar nitrogen concentration and altitude but no trend with altitude for foliar phosphorus concentration. This provided evidence that the tissue nutrient status of upland plants reflects nutrient availability rather than the direct effects of climate on growth. However, differences in the relationship between foliar nitrogen concentration and atmospheric nitrogen deposition for N. stricta sampled on hills in contrasting pollution climates show that the possibility of temperature-mediated growth effects on foliar nitrogen concentration should not be ignored. Thus, there is potential to use upland plant species as biomonitors of nitrogen deposition, but the response of different species to nitrogen addition, in combination with climatic effects on growth, must be well characterised.     

Reconciling models and measurements to assess trends in atmospheric mercury deposition

Changes in atmospheric mercury deposition are used to evaluate the effectiveness of regulations controlling emissions. This analysis can be complicated by seemingly incongruent data from different model runs, model types, and field measurements. Here we present a case study example that describes how to identify trends in regional scale mercury deposition using best-available information from multiple data sources. To do this, we use data from three atmospheric chemistry models (CMAQ, GEOS-Chem, HYSPLIT) and multiple sediment archives (ombrotrophic bog, headwater lake, coastal salt marsh) from the Bay of Fundy region in Canada. Combined sediment and modeling data indicate that deposition attributable to US and Canadian emissions has declined in recent years, thereby increasing the relative significance of global sources. We estimate that anthropogenic emissions in the US and Canada account for 28-33% of contemporary atmospheric deposition in this region, with the rest from natural (14-32%) and global sources (41-53%).     

太湖北部藻类生长旺盛期大气氮、磷沉降特征

按照<大气降水样品的采集与保存标准>(GB/T 153580.2-92)收集大气N、P沉降物和降水量,并测定了2007年5～11月太湖北部梅梁湾藻类生长旺盛期间大气TN、TP的干、湿沉降通量.结果表明,太湖北部梅粱湾大气TN月湿沉降通量和月总沉降通量的变化趋势均呈双峰型特征,与当地梅雨和台风侵袭时的降水量呈明显正相关,并且TN的月湿沉降通量高于月干沉降适量,但降水量最少的11月则相反;大气TP月干、月湿沉降通量呈相互交替的变化趋势.大气N沉降物中主要以溶解性氮(TDN)为主,平均约占91.4%;而P沉降物中溶解性磷(TDP)占的比例相对较低,平均约为65.1%.经测定,2007年太湖北部梅梁湾TN和TP的年沉降通量分别为2 976、84.0 kg/km2,相比2002年7月至2003年6月分别下降34.4%和78.7%;2007年太湖北部梅粱湾大气TN的年沉降量高达6 958 t,远超过太湖湖泊生态系统理论允许的TN年沉降量.     

Changes in base cation deposition across New York State and adjacent New England following implementation of the 1990 Clean Air Act amendments

To reduce atmospheric deposition, in 1990 Congress passed amendments to the Clean Air Act requiring electric utility power plants to decrease emissions of sulfur dioxide and nitrogen oxides, with Phase I beginning in 1995. We analyzed precipitation volume, wet deposition, and concentration of the sum of base cations measured at 12 National Atmospheric Deposition Program sites in Massachusetts, New Hampshire, New York, and Vermont. We compared five-year means prior to and following passage of the amendments and for five years after the implementation of Phase I. Whereas only one of the monitoring stations recorded a decline in base cation deposition, three sites out of the 12 showed a decline in base cation concentration. None of the sites exhibited a significant change in precipitation volume. Continued deposition of base cations may help to reduce the detrimental effects of acidic deposition.     

The effects of atmospheric nitrogen deposition in the Rocky Mountains of Colorado and southern Wyoming, USA-a critical review

The Rocky Mountains of Colorado and southern Wyoming receive atmospheric nitrogen (N) deposition that ranges from 2 to 7 kg ha(-1) yr(-1), and some previous research indicates pronounced ecosystem effects at the highest rates of deposition. This paper provides a critical review of previously published studies on the effects of atmospheric N deposition in the region. Plant community changes have been demonstrated through N fertilization studies, however, N limitation is still widely reported in alpine tundra and subalpine forests of the Front Range, and sensitivity to changes in snow cover alone indicate the importance of climate sensitivity in these ecosystems. Retention of N in atmospheric wet deposition is <50% in some watersheds east of the Continental Divide, which reflects low biomass and a short growing season relative to the timing and N load in deposition. Regional upward temporal trends in surface water NO(3)(-) concentrations have not been demonstrated, and future trend analyses must consider the role of climate as well as N deposition. Relatively high rates of atmospheric N deposition east of the Divide may have altered nutrient limitation of phytoplankton, species composition of diatoms, and amphibian populations, but most of these effects have been inconclusive to date, and additional studies are needed to confirm hypothesized cause and effect relations. Projected future population growth and energy use in Colorado and the west increase the likelihood that the subtle effects of atmospheric N deposition now evident in the Front Range will become more pronounced and widespread in the future.     

An integrative analysis of the role of atmospheric deposition and land management practices on nitrogen in the US agricultural sector

Additions of anthropogenic nitrogen (N) compounds constitute one of the major classes of air pollutants of significance to human health and the environment. Reliance on wet deposition measurements alone can lead to considerable underestimates (by 40-60%) of the total (wet + dry) atmospheric N deposition. In addition, wet deposition of N are about 20% of the levels that are lost due to volatilization (primarily ammonia). Nevertheless, in the agricultural sectors of the Mississippi River basins, farm management practices, and recycling of N within cropping systems clearly outweigh the contributions of atmospheric deposition. As opposed to native vegetation and forests, there are no records of the negative effects of atmospheric N deposition on crop yield. Similarly, field studies on the interactions of atmospheric N compounds with the incidence and spread of pathogens does not permit any generalizations. Nitrogen applied as fertilizer affects disease probably more by its effect on the plant growth than by its effects on pathogens. In contrast, atmospheric nitrogen dioxide appears to be a stimulant of aphid performance. Under conditions of heavy weed infestation, N fertilization stimulates weed growth and competitiveness, rather than crop yield.     

Regional and historical variation in the nitrogen content of Racomitrium lanuginosum in Britain in relation to atmospheric nitrogen deposition

The moss Racomitrium lanuginosum (Hedw.) Brid. is an important component of the drier parts of ombrotrophic mires and montane heaths in north-western Britain. The extent and quality of the montane heaths dominated by R. lanuginosum has declined in recent decades, perhaps in part due to the effects of acidic deposition at high elevations. This paper examines the effect of atmospheric nitrogen deposition, which has increased during this century, on the nitrogen content of R. lanuginosum in Britain. The nitrogen content of the moss reflects the magnitude of the atmospheric supply being least in north-western Scotland and greatest (as much as six-fold greater) near to urban centres in northern England. This regional difference was less marked (only approx. two-fold) during the 19th century (as revealed from the analysis of herbarium specimens) when nitrogen concentrations were appreciably lower. Transplant studies both between regions and between sites within a mountain system demonstrated the importance of atmospheric deposition in determining the tissue nitrogen concentration of the moss. The results are discussed in relation to the potential importance of the enhanced atmospheric nitrogen supply to the normally nitrogen-impoverished montane heaths, and to the growth and persistence of the moss.     

Emissions of nitric oxide from 79 plant species in response to simulated nitrogen deposition

To assess the potential contribution of nitric oxide (NO) emission from the plants grown under the increasing nitrogen (N) deposition to atmospheric NO budget, the effects of simulated N deposition on NO emission and various leaf traits (e.g., specific leaf area, leaf N concentration, net photosynthetic rate, etc.) were investigated in 79 plant species classified by 13 plant functional groups. Simulated N deposition induced the significant increase of NO emission from most functional groups, especially from conifer, gymnosperm and C(3) herb. Moreover, the change rate of NO emission was significantly correlated with the change rate of various leaf traits. We conclude that the plants grown under atmospheric N deposition, especially in conifer, gymnosperm and C(3) herb, should be taken into account as an important biological source of NO and potentially contribute to atmospheric NO budget.     

Ammonia in the atmosphere: a review on emission sources, atmospheric chemistry and deposition on terrestrial bodies

Gaseous ammonia (NH₃) is the most abundant alkaline gas in the atmosphere. In addition, it is a major component of total reactive nitrogen. The largest source of NH₃ emissions is agriculture, including animal husbandry and NH₃-based fertilizer applications. Other sources of NH₃ include industrial processes, vehicular emissions and volatilization from soils and oceans. Recent studies have indicated that NH₃ emissions have been increasing over the last few decades on a global scale. This is a concern because NH₃ plays a significant role in the formation of atmospheric particulate matter, visibility degradation and atmospheric deposition of nitrogen to sensitive ecosystems. Thus, the increase in NH₃ emissions negatively influences environmental and public health as well as climate change. For these reasons, it is important to have a clear understanding of the sources, deposition and atmospheric behaviour of NH₃. Over the last two decades, a number of research papers have addressed pertinent issues related to NH₃ emissions into the atmosphere at global, regional and local scales. This review article integrates the knowledge available on atmospheric NH₃ from the literature in a systematic manner, describes the environmental implications of unabated NH₃ emissions and provides a scientific basis for developing effective control strategies for NH₃.     

Modelling the atmospheric transport and deposition of sulphur and nitrogen over the United Kingdom and assessment of the influence of SO2 emissions from international shipping

A statistical Lagrangian atmospheric transport model was used to generate annual maps of deposition of sulphur and oxidised and reduced nitrogen for the UK at a 5×5 km² resolution. The model was run using emissions for the year 2002. The model was compared with measurements of gas concentrations (SO₂, NO_x, HNO₃ and NH₃) and of wet deposition and aerosol concentrations of SO₄²⁻, NO₃⁻ and NH₄⁺ from national monitoring networks. Good correlation was obtained, demonstrating that the model is capable of accurately estimating the mass balance and spatial distribution of sulphur and nitrogen compounds in the atmosphere. A future emissions scenario for the year 2020 was used to test the influence of shipping emissions on sulphur deposition in the UK. The results show that, if shipping emissions are assumed to increase at a rate of 2.5% per year, their relative contribution to sulphur deposition is expected to increase from 9% to 28% between 2002 and 2020. The model was compared to both a European scale and a global scale chemical transport model and found to give broad agreement with the magnitude and location of sulphur deposition associated with shipping emissions. Enforcement of the MARPOL convention to reduce the sulphur content in marine fuel to 1% was estimated to result in a 6% reduction in total sulphur deposition to the UK for the year 2020. The percentage area of sensitive habitats with exceedance of critical loads for acidity in the UK was predicted to decrease by 1% with the implementation of the MARPOL convention.     

Effects of atmospheric ammonia on vegetation--a review

Atmospheric ammonia does not only cause acute injuries at vegetation close to the source, but significantly contributes to large scale nitrogen eutrophication and acidification of ecosystems because the amount of sources is high and after conversion to ammonium it can reach remote areas by long-range atmospheric transport. Besides having acute toxic potential, NH(3) and NH(4)(+) (= NH(y)) may disturb vegetation by secondary metabolic changes due to increased NH(y) uptake and assimilation leading to higher susceptibility to abiotic (drought, frost) and biotic (pests) stress. Prevention of damage to natural and semi-natural ecosystems will only be achieved if NH(3) emissions are drastically reduced. In this paper, the current knowledge on NH(y) emission, deposition, and its effects on vegetation and ecosystems are reviewed. Critical levels and critical loads for nitrogen deposition are discussed.     

A dynamic modelling approach for estimating critical loads of nitrogen based on plant community changes under a changing climate

A dynamic model of forest ecosystems was used to investigate the effects of climate change, atmospheric deposition and harvest intensity on 48 forest sites in Sweden (n = 16) and Switzerland (n = 32). The model was used to investigate the feasibility of deriving critical loads for nitrogen (N) deposition based on changes in plant community composition. The simulations show that climate and atmospheric deposition have comparably important effects on N mobilization in the soil, as climate triggers the release of organically bound nitrogen stored in the soil during the elevated deposition period. Climate has the most important effect on plant community composition, underlining the fact that this cannot be ignored in future simulations of vegetation dynamics. Harvest intensity has comparatively little effect on the plant community in the long term, while it may be detrimental in the short term following cutting. This study shows: that critical loads of N deposition can be estimated using the plant community as an indicator; that future climatic changes must be taken into account; and that the definition of the reference deposition is critical for the outcome of this estimate.     

Long-range transport of acidifying substances in East Asia—Part II: Source–receptor relationships

Region-to-grid source–receptor (S/R) relationships are established for sulfur and reactive nitrogen deposition in East Asia, using the Eulerian-type Community Multiscale Air Quality (CMAQ) model with emission and meteorology data for 2001. We proposed a source region attribution methodology by analyzing the non-linear responses of the CMAQ model to emission changes. Sensitivity simulations were conducted where emissions of SO₂, NO_x, and primary particles from a source region were reduced by 25%. The difference between the base and sensitivity simulations was multiplied by a factor of four, and then defined as the contribution from that source region. The transboundary influence exhibits strong seasonal variation and generally peaks during the dry seasons. Long-range transport from eastern China contributes a significant percentage (>20%) of anthropogenic reactive nitrogen as well as sulfur deposition in East Asia. At the same time, northwestern China receives approximately 35% of its sulfur load and 45% of its nitrogen load from foreign emissions. Sulfur emissions from Miyakejima and other volcanoes contribute approximately 50% of the sulfur load in Japan in 2001. Sulfur inflows from regions outside the study domain, which is attributed by using boundary conditions derived from the MOZART global atmospheric chemistry model, are pronounced (10–40%) over most parts of Asia. Compared with previous studies using simple Lagrangian models, our results indicate higher influence from long-range transport. The estimated S/R relationships are believed to be more realistic since they include global influence as well as internal interactions among different parts of China.     

Uncertainties in the current knowledge of some atmospheric trace gases associated with U.S. agriculture: a review

Approximately 80 different crop species are grown in the United States in widely differing geographic areas, climatic and edaphic conditions, and management practices. Although the majority of cultivated acreage in the United States is planted with only about 10 primary crops, uncertainties associated with trace gas emissions arise from: (1) limited data availability, (2) inaccurate estimates because of large temporal and spatial variability in trace gas composition and magnitude of trace gas emissions from agricultural activities, (3) differing characteristics of pollutant emissions from highly dispersed animal feed-lots, and (4) limited understanding of the emissions of semi-volatile organic compounds (SVOCs) associated with agriculture. Although emission issues are of concern, so also is atmospheric deposition to cropping systems, including wet and dry nitrogen, minerals, and organic compounds. These can have feedback effects on trace gas emissions. Overall, the many gaps in our understanding of these aspects of agricultural systems deserve serious attention.     

Atmospheric nitrogen inputs to the Delaware Inland Bays: the role of ammonia

A previous assessment of nitrogen loading to the Delaware Inland Bays indicates that atmospheric deposition provides 15-25% of the total, annual N input to these estuaries. A large and increasing fraction of the atmospheric wet flux is NH(4)(+), which for most aquatic organisms represents the most readily assimilated form of this nutrient. Particularly noteworthy is a 60% increase in the precipitation NH(4)(+) concentration at Lewes, DE over the past 20 years, which parallels the increase in poultry production on the Delmarva Peninsula over this period (currently standing at nearly 585 million birds annually). To further examine the relationship between local NH(3) emissions and deposition, biweekly-integrated gaseous NH(3) concentrations were determined using Ogawa passive samplers deployed at 13 sampling sites throughout the Inland Bays watershed over a one-year period. Annual mean concentrations at the 13 sites ranged from <0.5 microg NH(3)m(-3) to >6 microg NH(3)m(-3), with a mean of 1.6+/-1.0 microg NH(3)m(-3). At most sites, highest NH(3) concentrations were evident during spring and summer, when fertilizer application and poultry house ventilation rates are greatest, and seasonally elevated temperatures induce increased rates of microbial activity and volatilization from soils and animal wastes. The observed north-to-south concentration gradient across the watershed is consistent with the spatial distribution of poultry houses, as revealed by a GIS analysis of aerial photographs. Based on the average measured NH(3) concentration and published NH(3) deposition rates to water surfaces (5-8 mm s(-1)), the direct atmospheric deposition of gaseous NH(3) to the Inland Bays is 3.0-4.8 kg ha(-1)yr(-1). This input, not accounted for in previous assessments of atmospheric loading to the Inland Bays, would effectively double the estimated direct dry deposition rate, and is on par with the NO(3)(-) and NH(4)(+) wet fluxes. A second component of this study examined spatial differences in NO(3)(-) and NH(4)(+) wet deposition within the Inland Bays watershed. In a pilot study, precipitation composition at the Lewes NADP-AIRMoN site (DE 02) was compared with that at a satellite site established at Riverdale on the Indian River Estuary, approximately 21 km southwest. While the volume-weighted mean precipitation NO(3)(-) concentrations did not differ significantly between sites, the NH(4)(+) concentration observed at Riverdale (26.3 micromoles L(-1)) was 73% greater than at Lewes (15.2 micromoles L(-1)). More recently, a NADP site was established at Trap Pond, DE (DE 99), which was intentionally located within the region of intense poultry production. A comparison of the initial two years (6/2001-5/2003) of precipitation chemistry data from Trap Pond with other nearby NADP-AIRMoN sites (Lewes and Smith Island) reveals fairly homogeneous NO(3)(-) wet deposition, but significant spatial differences ( approximately 60%) in the NH(4)(+) wet flux. Overall, these results suggest that local emissions and below-cloud scavenging provide a significant contribution to regional atmospheric N deposition.     

Cost-effective reduction of NOx emissions from electricity generation.

This paper analyzes the benefits and costs of policies to reduce NOx emissions from electricity generation in the United States. Because emissions of NO contribute to the high concentration of atmospheric ozone in the eastern states associated with health hazards, the U.S. Environmental Protection Agency (EPA) has called on eastern states to formulate state implementation plans (SIPs) for reducing NOx emissions. Our analysis considers three NOx reduction scenarios: a summer seasonal cap in the eastern states covered by EPA's NOx SIP Call, an annual cap in the same SIP Call region, and a national annual cap. All scenarios allow for emissions trading. Although EPA's current policy is to implement a seasonal cap in the SIP Call region, this analysis indicates that an annual cap in the SIP Call region would yield about $400 million more in net benefits (benefits less costs) than would a seasonal policy, based on particulate-related health effects only. An annual cap in the SIP Call region is also the policy that is most likely to achieve benefits in excess of costs. Consideration of omissions from this accounting, including the potential benefits from reductions in ozone concentrations, strengthens the finding that an annual program offers greater net benefits than does a seasonal program.     

Translating science into policy: using ecosystem thresholds to protect resources in Rocky Mountain National Park

Concern over impacts of atmospheric nitrogen deposition to ecosystems in Rocky Mountain National Park, Colorado, has prompted the National Park Service, the State of Colorado Department of Public Health and Environment, the Environmental Protection Agency, and interested stakeholders to collaborate in the Rocky Mountain National Park Initiative, a process to address these impacts. The development of a nitrogen critical load for park aquatic resources has provided the basis for a deposition goal to achieve resource protection, and parties to the Initiative are now discussing strategies to meet that goal by reducing air pollutant emissions that contribute to nitrogen deposition in the Park. Issues being considered include the types and locations of emissions to be reduced, the timeline for emission reductions, and the impact of emission reductions from programs already in place. These strategies may serve as templates for addressing ecosystem impacts from deposition in other national parks.