Wet Deposition Of Ammonium Research Articles

Long-term trends and response of wet ammonia deposition to changes in anthropogenic emissions in the Pearl River delta of China

The Pearl River Delta (PRD) region has been identified as a significant hotspot of wet ammonium deposition. However, the absence of long-term monitoring data in the area hinders the comprehension of the historical trends and changes in wet NH4+-N deposition in response to emissions, which interferes with the ability to make effective decisions. This study has analyzed the long-term trends of wet NH4+-N deposition flux and has quantified the effect of anthropogenic emissions and meteorological factors at a typical urban site and a typical forest site in the PRD region from 2009 to 2020. It revealed a significant decreasing trend in wet NH4+-N flux in both the typical urban and forest areas of the PRD region, at -6.2%/year (p < 0.001) and -3.3%/year (p < 0.001), respectively. Anthropogenic emissions are thought to have contributed 47–57% of the wet NH4+-N deposition trend over the past 12 years compared to meteorological factors. Meteorological conditions dominated the inter-annual fluctuations in wet NH4+-N deposition with an absolute contribution of 46%–52%, while anthropogenic emissions change alone explained 10%–31%. NH3 emissions have the greatest impact on the urban area among anthropogenic emission factors, while SO2 emissions have the greatest impact on the forest area. Additionally, precipitation was identified as the primary meteorological driver for both sites. Our findings also imply that the benefits of NH3 emissions reductions might not immediately emerge due to interference from weather-related factors.

Discerning the Concentration and Bi‐Directional Flux of Ammonia in an Urban Estuary Using the Relaxed Eddy Accumulation Method

AbstractNarragansett Bay, the largest estuary in New England, is a heavily urbanized watershed impacted by deposition and runoff. Nutrient budgets and local policy rely on deposition data from a 1990 study that did not include any direct observations of dry deposition of gaseous ammonia (NH3(g)) and particulate ammonium (p‐NH4+) due to uncertainties in their flux direction and measurement difficulty. Recent work has shown that wet deposition of ammonium (NH4+) to the Bay has increased by a factor of 6 over the past three decades, leading to a 2.5‐fold increase in wet nitrogen (N) deposition. This documented increase in wet deposition of NH4+ is concurrent with managed nutrient reductions in urbanized estuaries but has potentially increased the impacts of atmospheric N deposition, including the dry deposition of NH3(g) and p‐NH4+. However, the lack of NH3(g) and p‐NH4+ measurements hinders our interpretation of this important N source. For the first time over Narragansett Bay, and to our knowledge over open water, dry (particulate and gas phase) total ammonia (NHx = NH3(g) + p‐NH4+) and the bidirectional NH3(g) flux were quantified using a relaxed eddy accumulation sampling technique. We find that dry deposition of NHx comprises 9.6% of total (wet + dry) N deposition. During the fall season, the dominant flux direction for NH3(g) is upward, which also has implications for urban air quality. We estimate that NH3(g) emitted from the Bay to the atmosphere makes up to 10% of the local NH3(g) emission budget for fall.

Atmospheric deposition of reactive nitrogen to a deciduous forest in the southern Appalachian Mountains.

Assessing nutrient critical load exceedances requires complete and accurate atmospheric deposition budgets for reactive nitrogen (Nr). The exceedance is the total amount of Nr deposited to the ecosystem in excess of the critical load, which is the amount of Nr input below which harmful effects do not occur. Total deposition includes all forms of Nr (i.e., organic and inorganic) deposited to the ecosystem by wet and dry pathways. Here we present results from the Southern Appalachian Nitrogen Deposition Study (SANDS), in which a combination of measurements and field-scale modeling was used to develop a complete annual Nr deposition budget for a deciduous forest at the Coweeta Hydrologic Laboratory. Wet deposition of ammonium, nitrate, nitrite, and bulk organic N were measured directly. The dry deposited Nr fraction was estimated using a bidirectional resistance-based model driven with speciated measurements of Nr air concentrations (e.g., ammonia, ammonium aerosol, nitric acid, nitrate aerosol, bulk organic N in aerosol, total alkyl nitrates, and total peroxy nitrates), micrometeorology, canopy structure, and biogeochemistry. Total annual deposition was ~6.7 kg N ha-1 yr-1, which is on the upper end of Nr critical load estimates recently developed for similar ecosystems in the nearby Great Smoky Mountains National Park. Of the total (wet + dry) budget, 51.1% was contributed by reduced forms of Nr , with oxidized and organic forms contributing ~41.3% and 7.6%, respectively. Our results indicate that reductions in deposition would be needed to achieve the lowest estimates (~3.0 kg N ha-1 yr-1) of Nr critical loads in southern Appalachian forests.

An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals

Abstract. An ensemble-variational inversion system is developed for the estimation of ammonia emissions using ammonia retrievals from the Cross-track Infrared Sounder (CrIS) for use in the Global Environmental Multiscale – Modelling Air quality and Chemistry (GEM-MACH) chemical weather model. A novel hybrid method to compare logarithmic retrieval parameters to model profiles is presented. Inversions for the monthly mean ammonia emissions over North America were performed for May to August 2016. Inversions using the hybrid comparison method increased ammonia emissions at most locations within the model domain, with total monthly mean emissions increasing by 11 %–41 %. The use of these revised emissions in GEM-MACH reduced biases with surface ammonia observations by as much as 25 %. The revised ammonia emissions also improved the forecasts of total (fine + coarse) ammonium and nitrate, as well as ammonium wet deposition, with biases decreasing by as much as 13 %, but they did not improve the forecasts of just the fine components of ammonium and nitrate. A comparison of biases resulting from inversions using different comparison methods shows favourable results for the hybrid comparison method.

Highly concentrated atmospheric inorganic nitrogen deposition in an urban, coastal region in the US

Much of our understanding of atmospheric nitrogen deposition (AD) is based on important monitoring networks, such as the National Atmospheric Deposition Program (NADP) in the United States (US). However, it is likely that rural-based monitoring data are unrepresentative of reactive nitrogen concentrations found in urban areas. In this study, event-based precipitation was collected over one-year in Providence, RI - a mid-sized city situated at the head of Narragansett Bay, the largest estuary in the northeastern US Significant concentration enhancements in inorganic nitrogen (i.e., ammonium and nitrate) were found for wet deposition in the urban area compared to nearby NADP rural and non-urban coastal monitoring sites. Moreover, the annual ratio of ammonium to nitrate was highest in urban precipitation (>1.0). From 164 precipitation events, the mean volume-weighted ammonium and nitrate concentrations were 32.9 μmol l−1 and 28.4 μmol l−1, respectively, with total inorganic nitrogen concentrations exceeding 100 μmol l−1 in at least 30 events. AD data for Narragansett Bay is limited and outdated: our results suggest inorganic nitrogen is at least 2.5 times greater than currently estimated in policy decision-making related to improving water quality and ecosystem services. This underestimation is due to an increase (by as much as 6 times) in ammonium wet deposition since 1990, likely due to an increase in urban sources of precursor ammonia.

Projections of Atmospheric Nitrogen Deposition to the Chesapeake Bay Watershed.

Atmospheric deposition is among the largest pathways of nitrogen loading to the Chesapeake Bay Watershed (CBW). The interplay between future climate and emission changes in and around the CBW will likely shift the future nutrient deposition abundance and chemical regime (e.g., oxidized vs. reduced nitrogen). In this work, a Representative Concentration Pathway (RCP) from the Community Earth System Model is dynamically downscaled using the Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) model coupled to the agro-economic Environmental Policy Integrated Climate (EPIC) model. The relative impacts of emission and climate changes on atmospheric nutrient deposition are explored for a recent historical period and a period centered on 2050. The projected regional emissions in CMAQ reflect current federal and state regulations, which use baseline and projected emission years 2011 and 2040, respectively. The historical simulations of 2-m temperature and precipitation have cool and dry biases, and temperature and precipitation are projected to both increase. Ammonium wet deposition agrees well with observations, but nitrate wet deposition is underpredicted. Climate and deposition changes increase simulated future ammonium fertilizer application. In the CBW at 2050, these changes (along with widespread decreases in anthropogenic nitrogen oxide and sulfur oxide emissions, and relatively constant NH3 emissions) decrease total nitrogen deposition by 21%, decrease annual average oxidized nitrogen deposition by 44%, and increase reduced nitrogen deposition by 10%. These results emphasize the importance of decreased anthropogenic emissions on the control of future nitrogen loading to the Chesapeake Bay in a changing climate.

Reducing Wet Ammonium Deposition in Rocky Mountain National Park: the Development and Evaluation of A Pilot Early Warning System for Agricultural Operations in Eastern Colorado.

Agricultural emissions are the primary source of ammonia (NH3) deposition in Rocky Mountain National Park (RMNP), a Class I area, that is granted special air quality protections under the Clean Air Act. Between 2014 and 2016, the pilot phase of the Colorado agricultural nitrogen early warning system (CANEWS) was developed for agricultural producers to voluntarily and temporarily minimize emissions of NH3 during periods of upslope winds. The CANEWS was created using trajectory analyses driven by outputs from an ensemble of numerical weather forecasts together with the climatological expertize of human forecasters. Here, we discuss the methods for the CANEWS and offer preliminary analyses of 33 months of the CANEWS based on atmospheric deposition data from two sites in RMNP as well as responses from agricultural producers after warnings were issued. Results showed that the CANEWS accurately predicted 6 of 9 high N deposition weeks at a lower-elevation observation site, but only 4 of 11 high N deposition weeks at a higher-elevation site. Sixty agricultural producers from 39 of Colorado's agricultural operations volunteered for the CANEWS, and a two-way line of communication between agricultural producers and scientists was formed. For each warning issued, an average of 23 producers responded to a postwarning survey. Over 75% of responding CANEWS participants altered their practices after an alert. While the current effort was insufficient to reduce atmospheric deposition, we were encouraged by the collaborative spirit between agricultural, scientific, and resource management communities. Solving a broad and complex social-ecological problem requires both a technological approach, such as the CANEWS, and collaboration and trust from all participants, including agricultural producers, land managers, university researchers, and environmental agencies.

Implementation of a dynamical NH3 emissions parameterization in CMAQ for improving PM2.5 simulation in Taiwan

Ammonia (NH3) is an important precursor of inorganic fine particulate matter (PM2.5). Without specific information on the temporal variation in NH3 emissions, a simplified temporal variation in NH3 emissions is often used in chemical transport models. To better characterize NH3 emissions in an air quality model simulation for Taiwan, a dynamical NH3 emissions parameterization was applied to improve the temporal profile of NH3 emissions from livestock operations, synthetic nitrogen fertilizers, and standing crops. The Community Multiscale Air Quality (CMAQ) modeling simulation with a fixed NH3 emissions rate (the CONST experiment) presents a large positive bias in simulated nitrate and NH3, particularly during the nighttime and winter months. On the other hand, the CMAQ simulation with a dynamical NH3 emissions approach (the DYN experiment) improves the diurnal and seasonal variations and reduces the simulated bias. Moreover, according to the Taiwan emissions inventory, NH3 emissions from sewage accounts for a large portion (37%) of total NH3 emissions in Taiwan. The CMAQ simulation with the dynamical NH3 emissions approach and with a reduced level of NH3 emissions from sewage (the DYN1 experiment) was conducted to assess the possibility that the existing Taiwan emissions inventory may overestimate sewage NH3 emissions. The evaluations with observed NH3, nitrate, and ammonium wet deposition concentrations indicate that the DYN1 experiment performs better than the CONST and DYN experiments.

Long-term trends of wet inorganic nitrogen deposition in Rocky Mountain National Park: Influence of missing data imputation methods and associated uncertainty

Excess reactive nitrogen (Nr) deposition is occurring in Rocky Mountain National Park and impacting sensitive ecosystems. In 2006, the National Park Service, State of Colorado, and Environmental Protection Agency established the goal to reduce Nr deposition to below the ecosystem critical load by 2032. Progress is tracked using 5-year averages of annual wet inorganic nitrogen (IN) deposition measured at Loch Vale, Colorado, by the National Atmospheric Deposition Program (NADP). This remote high alpine site is challenging to operate, and large fractions of the annual precipitation, at times >40%, had invalid IN concentrations. Annual wet IN deposition is calculated using the NADP protocol, which replaces missing concentrations with the annual precipitation-weighted mean (PWM) concentration of valid samples. This protocol does not account for seasonal variations in IN concentrations and the inverse relationship between concentration and precipitation amounts. Invalid samples occurred more frequently in the winter and at high and low precipitation amounts, and the NADP protocol generally overestimated annual deposition rates, by as much as 20%. Here, a new method for imputing missing weekly IN concentrations that accounts for their seasonal and precipitation dependence is introduced. Using a bootstrapping analysis shows that the new method reduced the errors in the annual deposition rates by about 30% compared to the NADP protocol and the biases were near zero. The overall trend in the wet IN deposition rates was found to be flat from 1990 to 2017, but the nitrate contribution decreased about 33%, which was offset by a nearly equal increase in ammonium wet deposition. These trends are consistent with known changes in nitrate and ammonium precursor emissions. The long-term trends in the annual IN deposition rates were similar using both data imputation methods, but the 2013–2017 average was about 10% smaller using the new method.

Wet deposition of ammonium, nitrate and non-sea-salt sulphate in Sweden 1955 through 2017

Abstract Wet deposition to Sweden has been measured on a monthly basis since 1955. Data from all national and international precipitation chemistry networks operating in Sweden during 1955–2017 was collected in one unique database. During 1990–2000, 146 sites were operated on average and the spatial distribution of deposition across Sweden was determined. The measurement sites were divided into three regions representing southwestern, southeastern and northern Sweden. The three regions clearly differ in deposition amount while the temporal variations were similar between the regions. Non-sea-salt sulphate (nss-SO42-) wet deposition reached a maximum around 1970 and ammonium (NH4+) and nitrate (NO3−) in the mid-1980s. There was a reasonable agreement between the decreasing wet deposition trends of NH4+ and nss-SO42-, during 1990–2016 and the estimated decrease in the emissions in Sweden and Europe. The decreasing wet deposition trend of NO3− was, however, weaker than the corresponding estimated reduction in emissions of NOx. The wet depositions of NH4+ and NO3− were similar in magnitude during the whole measurement period and distributed in a similar manner between the three regions despite that these pollutants are transported over long distances and that the sources and atmospheric chemistry for NHx and NOx are different.

Ammonia Emissions from Subalpine Forest and Mountain Grassland Soils in Rocky Mountain National Park.

Atmospheric deposition of NH and NH contributes to eutrophication within sensitive subalpine ecosystems of Rocky Mountain National Park (RMNP) in the United States. However, little is known about the local contribution of NH from soils within the park. Thus, the goal of this study was to quantify and compare NH emissions from intact soil cores sampled from a subalpine grassland and forest within RMNP. Cores were collected at 2-wk intervals from 20 June 2011 to 12 Sept. 2011 and transferred to a laboratory chamber system for NH flux measurements. Additionally, N wet deposition was monitored at the sampling location to investigate possible impacts on NH soil emissions. The average quantifiable NH emissions (with SDs) from intact soil cores analyzed in the laboratory (23°C) were 0.42 ± 0.30 mg NH-N m d for grassland soil and 0.21 ± 0.03 mg NH-N m d for forest soil ( < 0.001). A mechanistic model was developed to estimate the impact of temperature on soil emissions using the chamber data and field-site air temperatures. Average estimated NH emissions from the field site over the study period were 0.21 and 0.082 mg NH-N m d for grasslands and forests, respectively. Ammonium wet deposition was not correlated to short term reemission of NH based on N isotope analysis. This work provides new information on the magnitude of NH emissions from native subalpine soils, indicating that natural emissions are not likely major sources of NH in the RMNP airshed.

Impact of Front Range sources on reactive nitrogen concentrations and deposition in Rocky Mountain National Park.

Human influenced atmospheric reactive nitrogen (RN) is impacting ecosystems in Rocky Mountain National Park (ROMO). Due to ROMO’s protected status as a Class 1 area, these changes are concerning, and improving our understanding of the contributions of different types of RN and their sources is important for reducing impacts in ROMO. In July–August 2014 the most comprehensive measurements (to date) of RN were made in ROMO during the Front Range Air Pollution and Photochemistry Éxperiment (FRAPPÉ). Measurements included peroxyacetyl nitrate (PAN), C1–C5 alkyl nitrates, and high-time resolution NOx, NOy, and ammonia. A limited set of measurements was extended through October. Co-located measurements of a suite of volatile organic compounds provide information on source types impacting ROMO. Specifically, we use ethane as a tracer of oil and gas operations and tetrachloroethylene (C2Cl4) as an urban tracer to investigate their relationship with RN species and transport patterns. Results of this analysis suggest elevated RN concentrations are associated with emissions from oil and gas operations, which are frequently co-located with agricultural production and livestock feeding areas in the region, and from urban areas. There also are periods where RN at ROMO is impacted by long-range transport. We present an atmospheric RN budget and a nitrogen deposition budget with dry and wet components. Total deposition for the period (7/1–9/30) was estimated at 1.58 kg N/ha, with 87% from wet deposition during this period of above average precipitation. Ammonium wet deposition was the dominant contributor to total nitrogen deposition followed by nitrate wet deposition and total dry deposition. Ammonia was estimated to be the largest contributor to dry deposition followed by nitric acid and PAN (other species included alkyl nitrates, ammonium and nitrate). All three species are challenging to measure routinely, especially at high time resolution.

Trends in ammonia measurements in the Netherlands over the period 1993–2014

We present measurements of atmospheric concentrations of ammonia and ammonium in the Netherlands over the period 1993–2014 and measurements of wet deposition of ammonium for 1985–2014. The various time series have been obtained at 16 monitoring stations from the Dutch National Air Quality Monitoring Network. The monitoring stations are geographically homogenously spread over the Netherlands and are equally distributed over regions with relatively low, moderate and high ammonia emission.During the period covered, changes in the monitoring have occurred. To obtain consistent time series, data are revalidated or corrected when necessary, according to current validation procedures or latest technical insights. The time series of ammonia concentrations are gap filled and time series corrected for meteorological influences are constructed.The course in the ammonia concentrations shows roughly two periods. For 1993–2004, the ammonia concentrations show a downward trend of 36%, which is statistically significant with a confidence interval (CI) of 99%. For 2005–2014, an upward trend of 19% (CI 90%) is reported. Correcting time series of ammonia concentrations for meteorological influences enhances the statistical reliability of the derived trends. This resulted in trends of −40% (CI 99%) and 24% (CI 95%) respectively. For the full period there exists no trend in ammonia concentrations due to a trend in atmospheric conditions. For 2005–2014 ammonia concentrations increased especially in springtime, while showing no change in winter months. After correcting for meteorological influences, all seasons in this period show an increase in ammonia concentrations although the increase in the spring months is still the largest.For 1993–2014 the reported ammonia emissions in the Netherlands declined in both periods with respectively 51% and 22%. The trends in emissions and ammonia concentrations correspond in the period 1993–2004 whilst over the period 2005–2014, the trends in emissions and concentrations of ammonia diverge. This divergence is for roughly a third accounted for by processes related to changes in chemical climate (see accompanying modelling paper by Wichink Kruit et al., 2016) but it is not clear what explains the remaining difference in trends.For 1993–2014, downward trends of wet deposition of ammonium and ammonium in aerosol are found to be 47% and 68%, respectively. A split into two periods is not found as is the case with the ammonia concentration. However, although statistically not significant, both wet deposition of ammonium and ammonium in aerosol show a leveling off in decline between 2005 and 2014.

Increasing importance of deposition of reduced nitrogen in the United States

Rapid development of agriculture and fossil fuel combustion greatly increased US reactive nitrogen emissions to the atmosphere in the second half of the 20th century, resulting in excess nitrogen deposition to natural ecosystems. Recent efforts to lower nitrogen oxides emissions have substantially decreased nitrate wet deposition. Levels of wet ammonium deposition, by contrast, have increased in many regions. Together these changes have altered the balance between oxidized and reduced nitrogen deposition. Across most of the United States, wet deposition has transitioned from being nitrate-dominated in the 1980s to ammonium-dominated in recent years. Ammonia has historically not been routinely measured because there are no specific regulatory requirements for its measurement. Recent expansion in ammonia observations, however, along with ongoing measurements of nitric acid and fine particle ammonium and nitrate, permit new insight into the balance of oxidized and reduced nitrogen in the total (wet + dry) US nitrogen deposition budget. Observations from 37 sites reveal that reduced nitrogen contributes, on average, ∼65% of the total inorganic nitrogen deposition budget. Dry deposition of ammonia plays an especially key role in nitrogen deposition, contributing from 19% to 65% in different regions. Future progress toward reducing US nitrogen deposition will be increasingly difficult without a reduction in ammonia emissions.

Changes in wet nitrogen deposition in the United States between 1985 and 2012

The United States (US) is among the global hotspots of nitrogen (N) deposition and assessing the temporal trends of wet N deposition is relevant to quantify the effectiveness of existing N regulation policies and its consequent environmental effects. This study analyzed changes in observed wet deposition of dissolved inorganic N (DIN = ammonium + nitrate) in the US between 1985 and 2012 by applying a Mann–Kendall test and Regional Kendall test. Current wet DIN deposition (2011–2012) data were used to gain insight in the current pattern of N deposition. Wet DIN deposition generally decreased going from Midwest > Northeast > South > West region with a national mean rate of 3.5 kg N ha−1 yr−1. Ammonium dominated wet DIN deposition in the Midwest, South and West regions, whereas nitrate and ammonium both contributed a half in the Northeast region. Wet DIN deposition showed no significant change at the national scale between 1985 and 2012, but profound changes occurred in its components. Wet ammonium deposition showed a significant increasing trend at national scale (0.013 kg N ha−1 yr−2), with the highest increase in the Midwest and eastern part of the South region. Inversely, wet nitrate deposition decreased significantly at national scale (−0.014 kg N ha−1 yr−2), with the largest reduction in the Northeast region. Overall, ratios of ammonium versus nitrate in wet deposition showed a significant increase in all the four regions, resulting in a transition of the dominant N species from nitrate to ammonium. Distinct magnitudes, trends and patterns of wet ammonium and nitrate deposition suggest the needs to control N emissions by species and regions to avoid negative effects of N deposition on ecosystem health and function in the US.

Ammonia emissions in the United States, European Union, and China derived by high‐resolution inversion of ammonium wet deposition data: Interpretation with a new agricultural emissions inventory (MASAGE_NH3)

We use the adjoint of a global 3‐D chemical transport model (GEOS‐Chem) to optimize ammonia (NH3) emissions in the U.S., European Union, and China by inversion of 2005–2008 network data forwet deposition fluxes. Optimized emissions are derived on a 2° × 2.5° grid for individual months and years. Error characterization in the optimization includes model errors in precipitation. Annual optimized emissions are 2.8 Tg NH3−N a−1for the contiguous U.S., 3.1 Tg NH3−N a−1for the European Union, and 8.4 Tg NH3−N a−1for China. Comparisons to previous inventories for the U.S. and European Union show consistency (∼±15%) in annual totals but some large spatial and seasonal differences. We develop a new global bottom‐up inventory of NH3emissions (Magnitude And Seasonality of Agricultural Emissions model for NH3 (MASAGE_NH3)) to interpret the results of the adjoint optimization. MASAGE_NH3 provides information on the magnitude and seasonality of NH3emissions from individual crop and livestock sources on a 0.5° × 0.5° grid. We find that U.S. emissions peak in the spring in the Midwest due to corn fertilization and in the summer elsewhere due to manure. The seasonality of European emissions is more homogeneous with a well‐defined maximum in spring associated with manure and mineral fertilizer application. There is some evidence for the effect of European regulations of NH3emissions, notably a large fall decrease in northern Europe. Emissions in China peak in summer because of the summertime application of fertilizer for double cropping.

Wet deposition of acidifying substances in different regions of China and the rest of East Asia: Modeling with updated NAQPMS

The traditional way to study Sources–Receptor Relationships (SRRs) of wet deposition is based on sensitivity simulation, which has weakness in dealing with the non-linear secondary formation pollutants (e.g. ozone and nitrate). An on-line source tracking method has been developed in the Nested Air Quality Prediction Modeling System (NAQPMS) coupled with cloud-process module for the first time. The new model can not only quantify the total volume of the sulfate, nitrate and ammonium wet deposition with more accuracy, but also trace these acidic species to their emitted precursors. Compared with previous studies, our result clearly shows: (1) East China and Central China, which are the two primary export regions, have 15–30% and 10% effect on wet deposition in other areas, respectively; (2) Besides the above two regions, the total acid deposition in Southwestern and Northeastern China have reached or exceeded the critical loads under their own environmental conditions.

Atmospheric concentrations and deposition of reactive nitrogen in Grand Teton National Park

AbstractThe Grand Teton Reactive Nitrogen Deposition Study (GrandTReNDS) was conducted to provide a more complete look at atmospheric concentrations and deposition fluxes of various reactive nitrogen species in and around Grand Teton National Park (GTNP). Daily measurements of wet deposition, PM2.5 composition, and gaseous ammonia and nitric acid concentrations were made at three locations. Weekly measurements of gaseous ammonia were made at eight additional sites. Ammonia concentrations were higher at the western sites; the study average ammonia concentration west of GTNP was 35 nmol m−3 and on the east side of the park it was 18 nmol m−3. Concentrations of other measured reactive nitrogen species were lower than NH3 and fairly similar at all sites, with averages of approximately 9, 1, and 3 nmol m−3 for ammonium, nitrate, and nitric acid, respectively. Wet deposition of ammonium and dry deposition of ammonia were the largest reactive nitrogen deposition pathways, together accounting for 56% and 62% of the nitrogen deposition on the east and west sides of GTNP, respectively. Nitrogen deposition of measured species totaled 2.38 kg N ha−1 west of GTNP at Driggs, ID (6 April to 21 September 2011), 0.85 kg N ha−1 west of GTNP at a high‐elevation site (28 July to 21 September 2011) and 1.23 kg N · ha−1 at a location on the east side of GTNP (15 May to 21 September 2011). These measurements highlight the significant inputs of reactive nitrogen to regional ecosystems over the few months studied, the importance of including NH3 dry deposition in nitrogen deposition budgets, and the need to conduct further research to capture sources and the annual cycle of deposition.

A seasonal nitrogen deposition budget for Rocky Mountain National Park

Nitrogen deposition is a concern in many protected ecosystems around the world, yet few studies have quantified a complete reactive nitrogen deposition budget including all dry and wet, inorganic and organic compounds. Critical loads that identify the level at which nitrogen deposition negatively affects an ecosystem are often defined using incomplete reactive nitrogen budgets. Frequently only wet deposition of ammonium and nitrate are considered, despite the importance of other nitrogen deposition pathways. Recently, dry deposition pathways including particulate ammonium and nitrate and gas phase nitric acid have been added to nitrogen deposition budgets. However, other nitrogen deposition pathways, including dry deposition of ammonia and wet deposition of organic nitrogen, still are rarely included. In this study, a more complete seasonal nitrogen deposition budget was constructed based on observations during a year-long study period from November 2008 to November 2009 at a location on the east side of Rocky Mountain National Park (RMNP), Colorado, USA. Measurements included wet deposition of ammonium, nitrate, and organic nitrogen, PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 microm, nitrate, and ammonium) concentrations of ammonium, nitrate, and organic nitrogen, and atmospheric gas phase concentrations of ammonia, nitric acid, and NO2. Dry deposition fluxes were determined from measured ambient concentrations and modeled deposition velocities. Total reactive nitrogen deposition by all included pathways was found to be 3.65 kg N x ha(-1) yr(-1). Monthly deposition fluxes ranged from 0.06 to 0.54 kg N x ha(-1)yr(-1), with peak deposition in the month of July and the least deposition in December. Wet deposition of ammonium and nitrate were the two largest deposition pathways, together contributing 1.97 kg N x ha(-1)yr(-1) or 54% of the total nitrogen deposition budget for this region. The next two largest deposition pathways were wet deposition of organic nitrogen and dry deposition of ammonia; combined they contributed 1.37 kg N x ha(-1)yr(-1) or 37% of the total nitrogen deposition budget. To better understand the nitrogen cycle and key interactions between the atmosphere and biosphere we need to include as many sources and types of nitrogen as possible and understand their variability throughout the year. Here we examine the components of the nitrogen deposition budget to better understand the factors that influence the different deposition pathways and their seasonal variations.

Nitrogen deposition to the United States: distribution, sources, and processes

Abstract. We simulate nitrogen deposition over the US in 2006–2008 by using the GEOS-Chem global chemical transport model at 1/2°×2/3° horizontal resolution over North America and adjacent oceans. US emissions of NOx and NH3 in the model are 6.7 and 2.9 Tg N a−1 respectively, including a 20% natural contribution for each. Ammonia emissions are a factor of 3 lower in winter than summer, providing a good match to US network observations of NHx (≡NH3 gas + ammonium aerosol) and ammonium wet deposition fluxes. Model comparisons to observed deposition fluxes and surface air concentrations of oxidized nitrogen species (NOy) show overall good agreement but excessive wintertime HNO3 production over the US Midwest and Northeast. This suggests a model overestimate N2O5 hydrolysis in aerosols, and a possible factor is inhibition by aerosol nitrate. Model results indicate a total nitrogen deposition flux of 6.5 Tg N a−1 over the contiguous US, including 4.2 as NOy and 2.3 as NHx. Domestic anthropogenic, foreign anthropogenic, and natural sources contribute respectively 78%, 6%, and 16% of total nitrogen deposition over the contiguous US in the model. The domestic anthropogenic contribution generally exceeds 70% in the east and in populated areas of the west, and is typically 50–70% in remote areas of the west. Total nitrogen deposition in the model exceeds 10 kg N ha−1 a−1 over 35% of the contiguous US.