NH3 Dry Deposition Research Articles

Multi-time Scale Variation of Atmospheric Ammonia Concentration and Dry Deposition in a Paddy Rice Region in Subtropical China

Meteorological factors and anthropogenic activities significantly affect atmospheric ammonia （NH3） concentration and its dry deposition. Former studies have examined the spatial and temporal variability in atmospheric NH3 concentrations at monthly scales. However, the characteristics of atmospheric concentrations at finer time scales such as hourly and daily scales and the influencing factors remain unclear. In this study, atmospheric NH3 concentration and related meteorological factors were continuously monitored online for one year in a double cropping rice region in subtropical China, and atmospheric NH3 concentration and its meteorological influencing factors as well as dry deposition were analyzed at different time scales （hourly, daily, and monthly）. The main results were as follows： The annual average daily concentration of NH3 in the rice area varied from 0.01 to 58.0 μg·m-3 （in N, same below）, and the annual average concentration was 5.3 μg·m-3. On the hourly scale, the 24-hour dynamics of atmospheric NH3 concentration showed a unimodal pattern, and the time of the NH3 peak appearance in different seasons was different； the time of the peak that appeared in winter lagged behind that in the other seasons. From the perspective of daily scale, NH3 concentration was mainly affected by fertilization in the paddy fields, peaking at 1-3 days after fertilization and then gradually decreasing. On the monthly scale, NH3 concentration peaked at 12.8 μg·m-3 in July and was the lowest in October at 1.6 μg·m-3. On the hourly scale, NH3 concentration varied seasonally due to the influences of meteorological factors, mainly as follows： NH3 concentration showed significant positive correlations with air temperature and solar radiation in all four seasons and with wind speed in spring and summer, whereas it showed significant negative correlations with relative humidity except in winter. On the daily scale, NH3 concentration showed a significant positive correlation with air temperature, rainfall, and solar radiation, whereas it showed a significant negative correlation with relative humidity. On the monthly scale, no significant correlation existed between each meteorological factor and NH3 concentration. The annual dry deposition flux （in N） calculated from the hourly average NH3 concentration was 8.5 kg·（hm2·a）-1, which was 11.6% higher than the annual flux calculated from the daily average and 12.4% higher than the annual flux calculated from the monthly average. In summary, there were significant daily and seasonal variations in atmospheric NH3 concentration in the paddy rice region in subtropical China, and conducting hourly-scale observations of NH3 concentration can help to reveal the multi-time scale variations in NH3 concentration and to quantify NH3 dry deposition more accurately.

Estimation of ammonia deposition to forest ecosystems in Scotland and Sri Lanka using wind-controlled NH3 enhancement experiments

Ammonia (NH3) pollution has emerged as a major cause of concern as atmospheric concentrations continue to increase globally. Environmentally damaging NH3 levels are expected to severely affect sensitive and economically important organisms, but evidence is lacking in many parts of the world. We describe the design and operation of a wind-controlled NH3 enhancement system to assess effects on forests in two contrasting climates. We established structurally identical NH3 enhancement systems in a temperate birch woodland in the UK and a tropical sub-montane forest in central Sri Lanka, both simulating real-world NH3 pollution conditions. Vertical and horizontal NH3 concentrations were monitored at two different time scales to understand NH3 transport within the forest canopies. We applied a bi-directional resistance model with four canopy layers to calculate net deposition fluxes. At both sites, NH3 concentrations and deposition were found to decrease exponentially with distance away from the source, consistent with expectations. Conversely, we found differences in vertical mixing of NH3 between the two experiments, with more vertically uniform NH3 concentrations in the dense and multi-layered sub-montane forest canopy in Sri Lanka. Monthly NH3 concentrations downwind of the source ranged from 3 to 29 μg m−3 at the UK site and 2–47 μg m−3 at the Sri Lankan site, compared with background values of 0.63 and 0.35 μg m−3, respectively. The total calculated NH3 dry deposition flux to all the canopy layers along the NH3 transects ranged from 12 to 162 kg N ha−1 yr−1 in the UK and 16–426 kg N ha−1 yr−1 in Sri Lanka, representative of conditions in the vicinity of a range of common NH3 sources. This multi-layer model is applicable for identifying the fate of NH3 in forest ecosystems where the gas enters the canopy laterally through the trunk space and exposes the understorey to high NH3 levels. In both study sites, we found that cuticular deposition was the dominant flux in the vegetation layers, with a smaller contribution from stomatal uptake. The new facilities are now allowing the first ever field comparison of NH3 impacts on forest ecosystems, with special focus on lichen bio-indicators, which will provide vital evidence to inform NH3 critical levels and associated nitrogen policy development in South Asia.

Spatial Distribution of Ammonia Concentrations and Modeled Dry Deposition in an Intensive Dairy Production Region.

Agriculture generates ~83% of total US ammonia (NH3) emissions, potentially adversely impacting sensitive ecosystems through wet and dry deposition. Regions with intense livestock production, such as the dairy region of south-central Idaho, generate hotspots of NH3 emissions. Our objective was to measure the spatial and temporal variability of NH3 across this region and estimate its dry deposition. Ambient NH3 was measured using diffusive passive samplers at 8 sites in two transects across the region from 2018-2020. NH3 fluxes were estimated using the Surface Tiled Aerosol and Gaseous Exchange (STAGE) model. Peak NH3 concentrations were 4-5 times greater at a high-density dairy site compared to mixed agriculture/dairy or agricultural sites, and 26 times greater than non-agricultural sites with prominent seasonal trends driven by temperature. Annual estimated dry deposition rates in areas of intensive dairy production can approach 45 kg N ha-1 y-1, compared to <1 kg N ha-1 y-1 in natural landscapes. Our results suggest that the natural sagebrush steppe landscapes interspersed within and surrounding agricultural areas in southern Idaho receive NH3 dry deposition rates within and above the range of nitrogen critical loads for North American deserts. Finally, our results highlight a need for improved understanding of the role of soil processes in NH3 dry deposition to arid and sparsely vegetated natural ecosystems across the western US.

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 ammonia deposition and its role in a cool-temperate fragmented deciduous broad-leaved forest

Forest fragmentation can increase dry deposition of atmospheric ammonia (NH3) volatilized from agricultural areas, and consequently increase spatial variability of Nr deposition within the forest (“elevated reactive nitrogen (Nr) deposition”). However, little is known about this effect and its impact on forest production in a deciduous broad-leaved forest in Asian countries. Here, we performed the field observations of atmospheric concentration and deposition of inorganic Nr gases and particles in a Japanese fragmented forest from May 2018 to April 2019. Leaf traits and growth of Japanese oak tree and understory vegetation were also measured. Atmospheric concentration and deposition of dissolved inorganic Nr (DIN) to tree canopies were measured via filter sampling and throughfall methods, respectively. Canopy retention/exchange was also estimated as a part of dry deposition using the canopy budget model. The results demonstrated that annual dry deposition of NH3 to tree canopies (4.4 kgN ha−1 y−1) was dominant in the annual total DIN deposition (7.1 kgN ha−1 y−1) at the forest edge, including the elevated Nr deposition of approximately 2 kgN ha−1 y−1. Additionally, agricultural activities such as fertilization in the area surrounding the forest likely enhanced the potential of canopy retention of NH4+, readily absorbed by tree canopy. The growth rates of tree and understory vegetation (dwarf bamboo) were higher at the edge than that at the interior, emphasizing a need for further investigation to quantify the effect of low Nr deposition (<3–5 kgN ha−1 y−1) on forest production, along with the conventional experimental studies under a high Nr deposition.

Long-term declines in atmospheric nitrogen and sulfur deposition reduce critical loads exceedances at multiple Canadian rural sites, 2000–2018

Abstract. Daily air concentrations of inorganic nitrogen (N) species, including gaseous HNO3 and particulate-bound (p)NH4+ and pNO3-, and sulfur (S) species, including SO2 and pSO42-, and precipitation concentrations of NO3-, NH4+, and SO42-, have been routinely monitored by the Canadian Air and Precipitation Monitoring Network (CAPMoN) since 1983. Data at 15 rural sites from 2000–2018 were used to estimate dry and wet N and S deposition fluxes, which were then used to explore their spatiotemporal trends and assess ecosystem damage through a retrospective analysis of critical loads (CLs) exceedances. Total (dry + wet) N deposition ranged from 1.7–9.5 kgNha-1yr-1 among the 15 sites, though dry deposition of NH3 and some oxidized N species were not included due to lack of monitoring data. Based on additional N measurements in 2010 at one of the sites, annual total N deposition may be underestimated by up to 32 %. Total N deposition was dominated by wet NO3- and wet NH4+ deposition, which together comprised 71 %–95 %. Contributions to dry N deposition were 40 %–74 % by HNO3, 11 %–40 % by pNH4+, and 5 %–25 % by pNO3-. Total S deposition ranged from 1.3–8.5 kgSha-1yr-1 and was dominated by wet deposition of SO42- and dry deposition of SO2. Relative percentages of wet and dry S deposition were 45 %–89 % and 11 %–55 %, respectively. Acidic ion fluxes were greatest in southeastern Canada and were comparable among the west coast, prairie, remote, and eastern Canadian sites. Oxidized N (dry HNO3, dry pNO3-, wet NO3-) deposition was greater than that of reduced N (dry pNH4+, wet NH4+) in the early 2000s. In 2014–2018, reduced N deposition surpassed that of oxidized N in southeastern Canada. Total N and S deposition decreased significantly at a rate of −0.03 to −0.25 kgNha-1yr-1 (−1.1 % yr−1 to −3.3 % yr−1) and −0.08 to −0.66 kgSha-1yr-1 (−3.5 % yr−1 to −6.6 % yr−1), respectively, among the sites. The weak declining trend in total N deposition at the west coast site was consistent with the slower decline in NOx emissions in western Canada. Reductions in total N deposition were driven by its oxidized form as trends in reduced N were non-significant. As a result, reduced N contributions to total N deposition increased on average from 42 % in 2000–2004 to 53 % in 2014–2018. Anthropogenic NOx and SO2 emissions reductions in both eastern Canada and eastern US were highly effective in reducing total oxidized N and total S deposition, respectively, in eastern Canada. Acidic deposition exceeded terrestrial CL at 5 of the 14 sites and aquatic CL at 2 of the 5 sites in the early 2000s. However, exceedances have been trending downwards and acidic deposition fluxes were mostly near or below CL after 2012 for the subset of sites assessed, which support recovery from historical acidification. Further assessments of CL exceedances are required in other Canadian regions susceptible to acidification and affected by elevated or increasing N and S emissions.

Agricultural ammonia dry deposition and total nitrogen deposition to a Swiss mire

Mires are among the ecosystems most affected by eutrophication caused by excessive nitrogen (N) inputs via N deposition of ammonium (NH4+), nitrate (NO3–), nitric acid (HNO3), nitrogen dioxide (NO2), and ammonia (NH3). As NH3 emissions are mostly generated by agriculture, a particular conflict of interest exists in areas where agricultural production systems are located nearby sensitive ecosystems, as often is the case in Switzerland. Therefore, this study aimed at quantifying and evaluating total N inputs to a mire in the Swiss Alpine foothills during 2007–2019, focusing on NH3 dry deposition. Three surface–vegetation–atmosphere transfer models were used to estimate dry deposition of NH3 based on micrometeorological data in combination with monthly passive sampler NH3 concentration measurements. NH3-N dry deposition summed up to 1.5–5.2 kg N ha–1 a–1, while total N loads were 11.5–14.2 kg N ha–1 a–1, well beyond the critical N loads for raised bogs (5–10 kg N ha–1 a–1), and also higher than the lower limits for oligotrophic fens and mountain hay meadows (10 kg N ha–1 a–1). Hence, the mire studied is most likely negatively affected by eutrophication, which could ultimately lead to biodiversity loss and ecosystem instability. This is particularly remarkable as the monthly NH3 concentrations at the study site (0.4–4.7 µg m–3) are comparatively low for Switzerland.

A significant diurnal pattern of ammonia dry deposition to a cropland is detected by an open-path quantum cascade laser-based eddy covariance instrument

Large uncertainties and challenges remain in the quantification of land-atmosphere exchanges of ammonia (NH3), mainly due to limitations in measurement techniques. In this study, the eddy covariance (EC) technique based on an open-path quantum cascade laser (QCL) spectrometer was used to measure the NH3 fluxes at a typical cropland in the North China Plain, one of the global NH3 hotspots. It is the first attempt of measuring both NH3 volatilization and deposition fluxes at an agricultural ecosystem using the open-path instrument-based EC technique. During the one-month experimental period, the NH3 fluxes were characterized by enhanced emissions after fertilizer application and persistent dry depositions after ploughing practice, with the flux magnitude varying from −0.293 to 7.29 (median: −0.042) mg N m−2 h−1. Nearly 93% of the half-hourly fluxes (absolute values) exceeded the mean instrumental flux detection limit of 9.6 μg N m−2 h−1. Nitrogen loss rate from the wheat field through NH3 volatilization was 0.57–0.71% relative to the applied nitrogen fertilizers. Ammonia deposition dominated the period after the ploughing practice, showing an average deposition rate of 0.014 kg N ha−1 d−1 with a significant diurnal pattern. Both the local emission sources and meteorological conditions influenced the variation of NH3 dry deposition. The deposition fluxes measured by the EC technique were nearly one third the results modelled by the widely used inferential model method, but the difference needs to be validated by more observations that includes different surface and meteorological conditions. This study suggests that this open-path QCL-based EC instrument is an effective tool for long-term and high-frequency measurements of ecosystem NH3 exchanges. It also enables cross-validation between different methods to improve the understanding in the atmospheric reactive nitrogen cycling.

High NH3 deposition in the environs of a commercial fattening pig farm in central south China

Intensive livestock production has been increasing, and has resulted in the emission of more than seven teragram per year of ammonia (NH3) in China in recent years. However, little is known about the fate of the emitted NH3, especially the dry deposition of NH3 in the environs of intensive animal farms. In this study, the spatial and temporal variations of NH3 deposition in the environs of an intensive fattening pig farm were investigated in the central south of China. NH3 concentrations were measured at sites situated 50, 100, 200, 300, and 500 m in the downwind direction from the farm each month from July 2018 to June 2019. The NH3 deposition was calculated based on a bidirectional NH3 exchange model. The monthly NH3 emissions from the pig farm were estimated based on the breeding stock. The annual average NH3 concentrations ranged from 1200 to 14 μg m−3 at the downwind sites within 500 m of the pig farm, exhibiting exponential decay as distance increased. Strong seasonality in NH3 deposition was observed, with the highest season being in the summer and lowest in the winter, and air temperature was found to be an important factor affecting this seasonal variation. The estimated monthly total dry deposition within 500 m of the pig farm ranged from 92 to 1400 kg NH3–N mo−1, which accounted for 4.1%–14% of the total monthly NH3 emissions from the pig farm. The estimated total NH3 emissions and NH3 deposition from the pig farm were 63 000 kg NH3–N yr−1 and 5400 kg NH3–N yr−1, respectively, with the annual average ratio of NH3 deposition to NH3 emission being 8.6%. This study found NH3 deposition around intensive pig farms is high, and determined it as a significant fate of the NH3 emitted from pig farms.

Ammonia Dry Deposition in an Alpine Ecosystem Traced to Agricultural Emission Hotpots.

Elevated reactive nitrogen (Nr) deposition is a concern for alpine ecosystems, and dry NH3 deposition is a key contributor. Understanding how emission hotspots impact downwind ecosystems through dry NH3 deposition provides opportunities for effective mitigation. However, direct NH3 flux measurements with sufficient temporal resolution to quantify such events are rare. Here, we measured NH3 fluxes at Rocky Mountain National Park (RMNP) during two summers and analyzed transport events from upwind agricultural and urban sources in northeastern Colorado. We deployed open-path NH3 sensors on a mobile laboratory and an eddy covariance tower to measure NH3 concentrations and fluxes. Our spatial sampling illustrated an upslope event that transported NH3 emissions from the hotspot to RMNP. Observed NH3 deposition was significantly higher when backtrajectories passed through only the agricultural region (7.9 ng m-2 s-1) versus only the urban area (1.0 ng m-2 s-1) and both urban and agricultural areas (2.7 ng m-2 s-1). Cumulative NH3 fluxes were calculated using observed, bidirectional modeled, and gap-filled fluxes. More than 40% of the total dry NH3 deposition occurred when air masses were traced back to agricultural source regions. More generally, we identified that 10 (25) more national parks in the U.S. are within 100 (200) km of an NH3 hotspot, and more observations are needed to quantify the impacts of these hotspots on dry NH3 deposition in these regions.

Inorganic nitrogen deposition in arid land ecosystems of Central Asia.

Atmospheric reactive nitrogen (Nr) pollution leads to enhanced Nr deposition. There still big gaps in understanding atmospheric nitrogen deposition because of limited monitoring sites in arid land ecosystems of Central Asia. To determine Nr concentrations and deposition in the study area, we have set up 20 monitoring sites to collect gaseous, particulate, and precipitation samples and measure their Nr components since 2009. Nr concentrations in air showed large spatial variations. Based on the Nr concentrations, dry deposition was calculated using the monthly average Nr concentrations by the corresponding deposition velocities modeled, which was varied between 3.15 and 27.92 kg N ha-1 yr-1 across desert, grassland, desert-grassland, forest, farmland, and city/suburb ecosystems. Ammonia N deposition varied between 0.50 asnd 8.66 kg N ha-1 yr-1, and nitrate N deposition c varied between 0.67 and 4.22 kg N ha-1 yr-1, respectively, in precipitation. Annual N deposition is following the order of desert (4.0) < grassland (6.0) < desert-grassland (7.6) < forest (16.1) < farmland (18.4) < city/suburb (35.4) ecosystems. Dry deposition contributed 52.7, 53.8, 100, 68.2, 73.7, and 78.9% of total N deposition in grassland, desert-grassland, desert, forest, farmland and city/suburb ecosystems, respectively. Reduced nitrogen deposition accounted for 62% of total N deposition in the arid area. Dry NH3 deposition made an important contribution (on average 40%) to total N deposition. Therefore, understanding the characteristics of Nr pollution especially NH3 emission is indispensable to atmospheric pollution control in arid region.

Atmospheric Nitrogen Deposition to a Southeast Tibetan Forest Ecosystem

With atmospheric reactive nitrogen (Nr) emissions increasing globally, research into Nr deposition has attracted increasing attention, especially in remote environments. These ecosystems are very sensitive to global change, especially enhanced Nr deposition. Forest environments, in particular, are highlighted because of their important ecological function. We quantified atmospheric Nr concentrations and deposition over four years of continuous monitoring in a southeast Tibetan boreal forest ecosystem, an ecosystem in which forest biomass and carbon density are high around the world. Average annual bulk Nr deposition was 3.00 kg N ha−1 y−1, with those of reduced and oxidized species estimated at 1.60 and 1.40 kg N ha−1 y−1, respectively. Bulk deposition of both NH4+ and NO3− were controlled by precipitation amount: both Nr deposition and precipitation were highest in summer and lowest in winter. Dry deposition of NH3 and NO2 were 1.18 and 0.05 kg N ha−1 y−1, respectively. Atmospheric NH3 concentrations were in the range 1.15–3.53 mg N L−1, highest in summer and lowest in winter. In contrast, no clear trend in seasonal NO2 concentrations was observed. Monthly NO2 concentrations were 0.79–1.13 mg N L−1. Total Nr deposition (bulk plus dry) was 4.23 (3.00 + 1.23) kg N ha−1 y−1 in the forest. Reduced nitrogen was the dominant species. In conclusion, Nr deposition was in the range at which forest net productivity and carbon sequestration are sensitive to any variation in nitrogen input, so quantification of Nr deposition should continue and with greater detail.

Changes in spatial patterns of ammonia dry deposition flux and deposition threshold exceedance according to dispersion model formalism and horizontal resolution.

Ammonia (NH3) emitted into the atmosphere from agricultural sources may affect nearby sensitive ecosystems due to high dry deposition fluxes on vegetation and soil surfaces, contributing to critical load exceedances. Ammonia fluxes near sources are simulated by either short-range atmospheric models or regional models using large grid cell sizes. However, studies are missing on the comparison of the results simulated by these two types of models. This paper presents the effect of model formalism, input factors, especially grid cell size and wind speed and the choice of deposition threshold on the spatial patterns of NH3 dry deposition fluxes and deposition threshold exceedances. We used the Eulerian chemistry-transport model CHIMERE and the Gaussian plume model OPS-ST on two study domains characterised by contrasting land use. We showed that the average annual NH3 dry deposition fluxes over each whole domain are similar for both models. By contrast, NH3 dry deposition fluxes near sources are higher when simulated with OPS-ST that provides analytical solutions that can be sampled with small grid cell sizes (i.e., from 25 to 1600m in this study), than with CHIMERE, which uses large grid cell sizes (i.e., 800 and 1600m). As a result, the spatial patterns of deposition threshold exceedance were very different between both models. These patterns depend mainly on grid cell size, the input factors and the choice of the deposition threshold value. We show that the model formalism has a relatively small effect on the results and that the differences result mainly from the spatial resolutions to which they can be applied. Simulation results must therefore be interpreted carefully, taking into account the simulation conditions.

Characterizing the spatiotemporal nitrogen stable isotopic composition of ammonia in vehicle plumes

Abstract. Vehicle emissions have been identified as an important urban source of ammonia (NH3). However, there are large uncertainties regarding the contribution of vehicle emissions to urban NH3 budgets, as well as the role of NH3 in spatiotemporal fine particulate matter (PM2.5) formation and nitrogen (N) deposition patterns. The N stable isotopic composition (δ15N) may be a useful observational constraint to track NH3 emission sources and chemical processing, but previously reported vehicle δ15N(NH3) emission signatures have reported a wide range of values, indicating the need for further refinement. Here we have characterized δ15N(NH3) spatiotemporal variabilities from vehicle plumes in stationary and on-road measurements in the USA and China using an active NH3 collection technique demonstrated to accurately characterize δ15N(NH3) on the order of hourly time resolution. Significant spatial and temporal δ15N(NH3) variabilities were observed and suggested to be driven by vehicle fleet composition and influences from NH3 dry deposition on tunnel surfaces. Overall, a consistent δ15N(NH3) signature of 6.6±2.1 ‰ (x‾±1σ; n=80) was found in fresh vehicle plumes with fleet compositions typical of urban regions. Our recommended vehicle δ15N(NH3) signature is significantly different from previous reports. This difference is due to a large and consistent δ15N(NH3) bias of approximately −15.5 ‰ between commonly employed passive NH3 collection techniques and the laboratory-tested active NH3 collection technique. This work constrains the δ15N(NH3) urban traffic plume signature, which has important implications for tracking vehicle NH3 in urban-affected areas and highlights the importance of utilizing verified collection methods for accurately characterizing δ15N(NH3) values.

Role of advection in atmospheric ammonia: A case study at a Japanese lake basin influenced by agricultural ammonia sources

The dry and wet depositions of atmospheric ammonia (NH3) is one of the important pathways of nitrogen loads to aquatic ecosystems and should be managed to mitigate lake eutrophication. Crop and livestock agriculture, one of the largest emitters of NH3 in Asian countries, are known to cause high spatial and seasonal variation of NH3 and influence the surrounding lake basin areas via its dry and wet deposition. However, the spatial characteristics of the NH3 concentration in basin scale are not completely understood for regulation in NH3 emission because a paucity of monitoring network is currently available for NH3 in many Asian countries. Here we aim to clarify dominant factors of spatial and seasonal variations of the NH3 concentration in a shallow eutrophic lake basin (Lake Kasumigaura basin) surrounded by agricultural areas in eastern Japan. Passive sampling over various land use categories in the basin was conducted at 36 sites in total from October 10, 2018 to January 14, 2020. Mean NH3 concentration in the observational period was in the order of farmland (6.6 ppbv), lake (5.9 ppbv), rural (3.5 ppbv), and forest (2.6 ppbv). Interestingly, the observed NH3 concentration near the livestock houses were higher in winter than summer, which was inconsistent with knowledge of seasonal changes of current NH3 emission inventory based on temperature-driven volatilization process. Comparing monthly NH3 concentrations at farmland and lake sites with various meteorological factors, we suggested the importance of seasonal advection of NH3 from high emission sources to which has been rarely paid attention by the previous past studies. Consequently, a higher nitrogen input by dry deposition of NH3 was preliminarily estimated over the lake than that of wet deposition of total nitrogen. Our finding of a role of seasonal advection in NH3 spatial pattens should be considered for lake ecosystem management since its deposition is known to be closely related to the ecological processes such as phytoplankton blooming.

Changes of nitrogen deposition in China from 1980 to 2018

China has experienced a dramatic change in atmospheric reactive nitrogen (Nr) emissions over the past four decades. However, it remains unclear how nitrogen (N) deposition has responded to increases and/or decreases in Nr emissions. This study quantitatively assesses temporal and spatial variations in measurements of bulk and calculated dry N deposition in China from 1980 to 2018. A long-term database (1980–2018) shows that bulk N deposition peaked in around 2000, and had declined by 45% by 2016–2018. Recent bulk and dry N deposition (based on monitoring from 2011 to 2018) decreased from 2011 to 2018, with current average values of 19.4 ± 0.8 and 20.6 ± 0.4 kg N ha−1 yr−1, respectively. Oxidized N deposition, especially dry deposition, decreased after 2010 due to NOx emission controls. In contrast, reduced N deposition was approximately constant, with reductions in bulk NH4+-N deposition offset by a continuous increase in dry NH3 deposition. Elevated NH3 concentrations were found at nationwide monitoring sites even at urban sites, suggesting a strong influence of both agricultural and non-agricultural sources. Current emission controls are reducing Nr emissions and deposition but further mitigation measures are needed, especially of NH3, built on broader regional emission control strategies.

Global estimates of dry ammonia deposition inferred from space-measurements

Ammonia (NH3), as an alkaline gas, contributes substantially to atmospheric nitrogen deposition, which can cause biodiversity loss, water eutrophication and soil acidification. Advances in the application of satellite observations allow us to gain deeper insights into atmospheric NH3 concentrations at large spatial scales. A new satellite-based methodology is proposed for estimating dry NH3 deposition with consideration of bi-directional NH3 exchange. We estimate the global dry NH3 deposition for nine years (2008–2016) by using the Infrared Atmospheric Sounding Interferometer Instrument (IASI) NH3 retrievals. Satellite-based dry NH3 deposition is in general consistent with measured dry NH3 deposition over the monitoring sites (R2 = 0.65). Global dry NH3 deposition over 8 kg N ha−1 is mainly distributed in the Eastern China, Northern and Central Pakistan, and Northern India. An annual increase rate of 0.27 and 0.13 kg N ha−1 y−1 in dry NH3 deposition during 2008–2016 occurs in Eastern China and Sichuan Basin, which are the major Chinese agricultural regions. The NH3 compensation point is high during warm months, and can be above 1 μg m−3 such as in Eastern China, implying the importance of considering the NH3 compensation points for estimating dry NH3 deposition. We find, if the upward NH3 flux was ignored, it will cause 11%, 17%, 5% and 3% overestimation in dry NH3 deposition in Eastern China, Northern India, Eastern United States and Western Europe, respectively. This study presents the potential of using the satellite retrievals to estimate the large-scale dry NH3 deposition, and the methodology is able to provide temporally continuous and spatially complete fine-resolution datasets.

Modeling the Sources and Transport Processes During Extreme Ammonia Episodes in the U.S. Corn Belt

AbstractAtmospheric ammonia (NH3) is the primary form of reactive nitrogen (Nr) and a precursor of ammonium (NH4+) aerosols. Ammonia has been linked to adverse impacts on human health, the loss of ecosystem biodiversity, and plays a key role in aerosol radiative forcing. The midwestern United States is the major NH3 source in North America because of dense livestock operations and the high use of synthetic nitrogen fertilizers. Here, we combine tall‐tower (100 m) observations in Minnesota and Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) modeling to investigate high and low NH3 emission episodes within the U.S. Corn Belt to improve our understanding of the distribution of emission sources and transport processes. We examined observations and performed model simulations for cases in February through November of 2017 and 2018. The results showed the following: (1) Peak emissions in November 2017 were enhanced by above‐normal air temperatures, implying a Q10 (i.e., the change in NH3 emissions for a temperature increase of 10°C) of 2.5 for emissions. (2) The intensive livestock emissions rom northern Iowa, approximately 400 km away from the tall tower, accounted for 17.6% of the abundance in tall‐tower NH3 mixing ratios. (3) Ammonia mixing ratios in the innermost domain 3 frequently (i.e., 336 hr, 48% of November 2017) exceeded 5.3 ppb, an important air quality health standard. (4) In November 2017, simulated NH3 net ecosystem exchange (the difference between NH3 emissions and dry deposition) accounted for 60–65% of gross NH3 emissions for agricultural areas and was 2.8–3.1 times the emissions of forested areas. (5) We estimated a mean annual NH3 net ecosystem exchange of 1.60 ± 0.06 nmol · m−2 · s−1 for agricultural lands and −0.07 ± 0.02 nmol · m−2 · s−1 for forested lands. These results imply that future warmer fall temperatures will enhance agricultural NH3 emissions, increase the frequency of dangerous NH3 episodes, and enhance dry NH3 deposition in adjacent forested lands.

Atmospheric sulfur and nitrogen deposition in the Athabasca oil sands region is correlated with foliar nutrient levels and soil chemical properties

The oil extraction industry and human activity in north eastern Alberta has been growing steadily since the 1960’s and is a source of air pollution. In the late 1990’s the Wood Buffalo Environmental Association was established to monitor air quality for both public and environmental health. A primary environmental concern was soil acidification caused by sulfur (S) and nitrogen (N) deposition. A network of forest health monitoring (FHM) sites was established in dry jack pine ecosystems to serve as an early indicator of negative impacts. A sampling campaign was executed in 2011 and this study examines soil properties and foliar nutrients in the context of measured and modeled acid deposition. Total N (TN), SO42−, pH, base cation to aluminum ratio (BC:Al), and base saturation (% BS) are reported for the organic layer (LFH) and 3 depths in the mineral soil, while foliar nutrients were analysed from current annual growth in jack pine needles. Atmospheric deposition of S, N, BC, and potential acid input (PAI) in the study area was recently provided by Edgerton et al. (2020) and soil and foliar chemistry was evaluated based on deposition estimates and measurements. Inverse distance weighting was used to examine spatial patterns and regression analysis was used to quantify relationships between variables. The results indicated that S deposition is spatially correlated with foliar SO42− concentration, and LFH SO42−, but not mineral topsoil (0–5 cm) SO42−. Nitrogen deposition was spatially correlated with foliar N concentration, but not LFH or topsoil TN indicating potential uptake by the foliage or rapid uptake by roots in the LFH layer. High BC deposition in the same areas with the highest potential acid inputs (PAI) did not correlate significantly with changes in soil pH. However, LFH pH was significantly related to dry NH3 deposition, which has not been reported previously and requires further investigation.

Estimating global surface ammonia concentrations inferred from satellite retrievals

Abstract. Ammonia (NH3), as an alkaline gas in the atmosphere, can cause direct or indirect effects on the air quality, soil acidification, climate change and human health. Estimating surface NH3 concentrations is critically important for modeling the dry deposition of NH3 and for modeling the formation of ammonium nitrate, which have important impacts on the natural environment. However, sparse monitoring sites make it challenging and difficult to understand the global distribution of surface NH3 concentrations in both time and space. We estimated the global surface NH3 concentrations for the years of 2008–2016 using satellite NH3 retrievals combining vertical profiles from GEOS-Chem. The accuracy assessment indicates that the satellite-based approach has achieved a high predictive power for annual surface NH3 concentrations compared with the measurements of all sites in China, the US and Europe (R2=0.76 and RMSE = 1.50 µg N m−3). The satellite-derived surface NH3 concentrations had higher consistency with the ground-based measurements in China (R2=0.71 and RMSE = 2.6 µg N m−3) than the US (R2=0.45 and RMSE = 0.76 µg N m−3) and Europe (R2=0.45 and RMSE = 0.86 µg N m−3) at a yearly scale. Annual surface NH3 concentrations higher than 6 µg N m−3 are mainly concentrated in the North China Plain of China and northern India, followed by 2–6 µg N m−3 mainly in southern and northeastern China, India, western Europe, and the eastern United States (US). High surface NH3 concentrations were found in the croplands in China, the US and Europe, and surface NH3 concentrations in the croplands in China were approximately double those in the croplands in the US and Europe. The linear trend analysis shows that an increase rate of surface NH3 concentrations (&gt; 0.2 µg N m−3 yr−1) appeared in eastern China during 2008–2016, and a middle increase rate (0.1–0.2 µg N m−3 yr−1) occurred in northern Xinjiang over China. NH3 increase was also found in agricultural regions in the central and eastern US with an annual increase rate of lower than 0.10 µg N m−3 yr−1. The satellite-derived surface NH3 concentrations help us to determine the NH3 pollution status in the areas without monitoring sites and to estimate the dry deposition of NH3 in the future.