Nitrogen Deposition Fluxes Research Articles

First Assessment of Inorganic Nitrogen Deposition Budget Following the Impoundment of a Subtropical Hydroelectric Reservoir (Nam Theun 2, Lao PDR)

AbstractWith around 490 km2 at full level of operation, the Nam Theun 2 Reservoir (NT2R) is one of the largest hydroreservoir in Southeast Asia. This study presents a first estimation of the atmospheric inorganic nitrogen deposition into the NT2R based on a 2‐year monitoring (June 2010 to July 2012) including gas concentrations and precipitation. Dry deposition fluxes are estimated by the inferential method using, on the one hand, surface measurements of gas concentrations (NO2, HNO3, NH3) from passive samplers and, on the other hand, modeled exchange rates. Wet deposition fluxes are calculated from NH4+ and NO3− concentrations determined in samples of rain from an automatic precipitation collector. The average nitrogen deposition flux is estimated at 1.26 ± 0.14 kgN·ha−1·year−1 from dry processes and 5.01 ± 0.92 kgN·ha−1·year−1 from wet ones, that is, an average annual total nitrogen flux of 6.27 ± 1.06 kgN·ha−1·year−1 deposited at the NT2R with 80% from wet deposition. Before impoundment, the mean N flux has been estimated at 3.42 ± 1.88 kgN·ha−1·year−1 for dry deposition and 5.01 ± 2.12 kgN·ha−1·year−1 for wet deposition, or a total N deposition flux of 8.43 ± 4.01 kgN·ha−1·year−1 over the studied area dominated by forests with little agriculture soil and water surfaces. Thus, the total N deposition over the studied area has been reduced of 26% (or 63% for dry deposition) following the reservoir impoundment based on our working hypothesis.

Chemical characteristics of airborne particles in Xi'an, inland China during dust storm episodes: Implications for heterogeneous formation of ammonium nitrate and enhancement of N-deposition

To identify the sources and heterogeneous reactions of sulfate and nitrate with dust in the atmosphere, airborne particles in Xi'an, inland China during the spring of 2017 were collected and measured for chemical compositions, along with a laboratory simulation of the heterogeneous formation of ammonium nitrate on the dust surface. Our results showed that concentrations of Ca2+, Na+ and Cl− in the TSP samples were enhanced in the dust events, with the values of 41.8, 5.4 and 4.0 μg m−3, respectively, while NO3− (7.1 μg m−3) and NH4+ (2.4 μg m−3) remarkably decreased, compared to those in the non-dust periods. During the dust events, NH4+ correlated only with NO3− (R2 = 0.52) and abundantly occurred in the coarse mode (>2.1 μm), in contrast to that in the non-dust periods, which well correlated with sulfate and nitrate and enriched in the fine mode (<2.1 μm). SO42− in Xi'an during the dust events existed mostly as gypsum (CaSO4·2H2O) and mirabilite (Na2SO4·10H2O) and dominated in the coarse mode, suggesting that they were directly transported from the upwind Gobi Desert region. Our laboratory simulation results showed that during the long-range transport hygroscopic salts in the Gobi dust such as mirabilite can absorb water vapor and form a liquid phase on the particle surface, then gaseous NH3 and HNO3 partition into the aqueous phase and form NH4NO3, resulting in the strong correlation of NH4+ with NO3− and their accumulation on dust particles. The dry deposition flux of total inorganic nitrogen (NH4+ + NO3−) in Xi'an during the dust events was 0.97 mg-N m−2 d−1 and 37% higher than that in the non-dust periods. Such a significant enhanced N-deposition is ascribed to the heterogeneous formation of NH4NO3 on the dust particle surface, which has been ignored and should be included in future model simulations.

Impacts of Atmospheric Nitrogen Deposition and Coastal Nitrogen Fluxes on Oxygen Concentrations in Chesapeake Bay

AbstractAlthough rivers are the primary source of dissolved inorganic nitrogen (DIN) inputs to the Chesapeake Bay, direct atmospheric DIN deposition and coastal DIN concentrations on the continental shelf can also significantly influence hypoxia; however, the relative impact of these additional sources of DIN on Chesapeake Bay hypoxia has not previously been quantified. In this study, the estuarine‐carbon‐biogeochemistry model embedded in the Regional‐Ocean‐Modeling‐System (ChesROMS‐ECB) is used to examine the relative impact of these three DIN sources. Model simulations highlight that DIN from the atmosphere has roughly the same impact on hypoxia as the same gram‐for‐gram change in riverine DIN loading, although their spatial and temporal distributions are distinct. DIN concentrations on the continental shelf have a similar overall impact on hypoxia as DIN from the atmosphere (~0.2 mg L−1); however, atmospheric DIN impacts dissolved oxygen (DO) primarily via the decomposition of autochthonous organic matter, whereas coastal DIN concentrations primarily impact DO via the decomposition of allochthonous organic matter entering the Bay mouth from the shelf. The impacts of atmospheric DIN deposition and coastal DIN concentrations on hypoxia are greatest in summer and occur farther downstream (southern mesohaline) in wet years than in dry years (northern mesohaline). Integrated analyses of the relative contributions of all three DIN sources on summer bottom DO indicate that impacts of atmospheric deposition are largest in the eastern mesohaline shoals, riverine DIN has dominant impacts in the largest tributaries and the oligohaline Bay, while coastal DIN concentrations are most influential in the polyhaline region.

A modelling approach to assess the effects of atmospheric nitrogen deposition on the marine ecosystem in the Bohai Sea, China

Atmospheric deposited nitrogen (AD-N) approximates or exceeds riverine input in many coastal ecosystems, such as the Bohai Sea (BHS) which is one of the most eutrophic coastal waters in China. We construct a three-dimensional (3D) physical-biogeochemical model to understand the influence of atmospheric dissolved inorganic nitrogen (DIN) on the intra- and inter-annual variations of phytoplankton blooms and nutrient dynamics in the BHS. The biological component, which is coupled to the Regional Ocean Modelling System (ROMS), is a simple but widely used Nutrient-Phytoplankton-Zooplankton-Detritus (NPZD) model with eight state variables. The model simulation successfully reproduces the spatial and temporal variations of observed DIN and dissolved inorganic phosphorus (DIP) and the climatological features of phytoplankton biomasses (chlorophyll a), which confirms the major role of air-transported nutrients in controlling standing stocks and nutrient limitations. The modelling results show that the relative contributions of deposited nitrogen to the total DIN in the seawater for the Bohai, Laizhou and Liaodong Bays and Central Bohai Basin reach 84.8%, 49.3%, 37.4% and 44.4% on average, respectively. The relative contribution ratio is approximately 54% for the entire Bohai region, causing a 56.5% increase in the phytoplankton biomass on average. These results also indicate that the effects of AD-N on nutrient and phytoplankton dynamics vary widely in regional areas because of the uneven spatial distribution of nitrogen deposition fluxes and also partially because of the hydrodynamic conditions, shortwave radiation and water temperatures.

Nitrogen deposition in precipitation to a monsoon-affected eutrophic embayment: Fluxes, sources, and processes

Daya Bay in the South China Sea (SCS) has experienced rapid nitrogen pollution and intensified eutrophication in the past decade due to economic development. Here, we estimated the deposition fluxes of nitrogenous species, clarified the contribution of nitrogen from precipitation and measured ions and isotopic composition (δ15N and δ18O) of nitrate in precipitation in one year period to trace its sources and formation processes among different seasons. We found that the deposition fluxes of total dissolved nitrogen (TDN), NO3−, NH4+, NO2−, and dissolved organic nitrogen (DON) to Daya Bay were 132.5, 64.4 17.5, 1.0, 49.6 mmol m−2∙yr−1, respectively. DON was a significant contributor to nitrogen deposition (37% of TDN), and NO3− accounted for 78% of the DIN in precipitation. The nitrogen deposition fluxes were higher in spring and summer, and lower in winter. Nitrogen from precipitation contributed nearly 38% of the total input of nitrogen (point sources input and dry and wet deposition) in Daya Bay. The δ15N-NO3- abundance, ion compositions, and air mass backward trajectories implicated that coal combustion, vehicle exhausts, and dust from mainland China delivered by northeast monsoon were the main sources in winter, while fossil fuel combustion (coal combustion and vehicle exhausts) and dust from PRD and southeast Asia transported by southwest monsoon were the main sources in spring; marine sources, vehicle exhausts and lightning could be the potential sources in summer. δ18O results showed that OH pathway was dominant in the chemical formation process of nitrate in summer, while N2O5+ DMS/HC pathways in winter and spring.

Wet deposition fluxes of atmospheric inorganic reactive nitrogen at an urban and rural site in the Indo-Gangetic Plain

Excess nitrogen deposition is a matter of concern for sensitive ecosystems. However, understanding the sources and transport of Nr species has been a challenge due to limited observations of atmospheric deposition of the key Nr species across India. In this study, wet deposition of atmospheric inorganic Nr species was investigated during the year 2013 at two regionally representative sites: Delhi (an urban site) and Jaunpur (a rural site). These sites are located in the Indo-Gangetic Plain (IGP) region, which is one of the most populated and fertile regions of India. The average NH4+ concentrations in rain water were found to be 25.4 μeql−1 and 98.5 μeql−1 at the rural and urban sites, respectively, whereas average NO3− concentrations were 12.4 μeql−1 and 28.7 μeql−1 at the rural and urban sites (respectively). The annual average wet deposition fluxes of NH4+ and NO3− at Delhi were calculated as 10.45 and 3.05 kgN ha−1 yr−1 respectively, whereas at Jaunpur the fluxes were 3.19 and 1.56 kgN ha−1 yr−1 respectively. In order to assess the Nr deposition, our estimates showed 486% increase in NO3− (from 0.52 to 3.05 kgN ha−1 yr−1) while 283% NH4+ (2.72–10.44 kgN ha−1 yr−1) between 1994 and 2013 at Delhi, clearly indicating the effect of urbanization and Land Use Land Cover (LULC) change. Reduced versus oxidized N deposition contribution was also estimated. This study provides key quantitative information to support regional nitrogen budget estimates in south Asia.

Atmospheric nitrogen deposition to China: A model analysis on nitrogen budget and critical load exceedance

We present a national-scale model analysis on the sources and processes of inorganic nitrogen deposition over China using the GEOS-Chem model at 1/2° × 1/3° horizontal resolution. Model results for 2008–2012 are evaluated with an ensemble of surface measurements of wet deposition flux and gaseous ammonia (NH3) concentration, and satellite measurements of tropospheric NO2 columns. Annual total inorganic nitrogen deposition fluxes are simulated to be generally less than 10 kg N ha−1 a−1 in western China (less than 2 kg N ha−1 a−1 over Tibet), 15–50 kg N ha−1 a−1 in eastern China, and 16.4 kg N ha−1 a−1 averaged over China. Annual total deposition to China is 16.4 Tg N, with 10.2 Tg N (62%) from reduced nitrogen (NHx) and 6.2 Tg N from oxidized nitrogen (NOy). Domestic anthropogenic sources contribute 86% of the total deposition; foreign anthropogenic sources 7% and natural sources 7%. Annually 23% of domestically emitted NH3 and 36% for NOx are exported outside the terrestrial land of China. We find that atmospheric nitrogen deposition is about half of the nitrogen input from fertilizer application (29.6 Tg N a−1), and is much higher than that from natural biological fixation (7.3 Tg N a−1) over China. A comparison of nitrogen deposition with critical load estimates for eutrophication indicates that about 15% of the land over China experiences critical load exceedances, demonstrating the necessity of nitrogen emission controls to avoid potential negative ecological effects.

Characteristics of Nitrogen Deposition in Daiyun Mountain National Nature Reserve

G78 nitrogen deposition collector was used to investigate the background value of local nitrogen deposition flux in Daiyun Mountain National Nature Reserve of Fujian province. The results showed that dry and wet nitrogen deposition of Daiyun Mountain National Nature Reserve was 2.30 kg·hm-2 and 14.79 kg·hm-2 from March to October in 2015. 53% of dry deposition was in the form of dissolved organic nitrogen (DON, 1.21 kg·hm-2). The main form of inorganic nitrogen (DIN) in dry deposition was NO3- deposition (0.71 kg·hm-2), with NH4+ deposition (0.37 kg·hm-2) being lower compared to NO3- deposition. DON and DIN flux in wet deposition was 5.38 kg·hm-2 and 9.41 kg·hm-2, respectively. DIN flux in wet deposition was mainly in the form of NH4+ deposition (6.07 kg·hm-2). Wet nitrogen deposition flux was found positively correlated with local precipitation. Wet nitrogen deposition in Daiyun Mountain National Nature Reserve might have significant negative effects on local water resource.

Towards a better spatial quantification of nitrogen deposition: A case study for Czech forests

The quantification of atmospheric deposition flux is essential for assessment of its impact on ecosystems. We present an advanced approach for the estimation of the spatial pattern of atmospheric nitrogen deposition flux over the Czech forests, collating all available measured data and model results. The aim of the presented study is to provide an improved, more complete, more reliable and more realistic estimate of the spatial pattern of nitrogen deposition flux over one country. This has so far usually been based on measurements of ambient NOx concentrations as dry deposition proxy, and NH4+ and NO3− in precipitation as wet deposition proxy. For estimation of unmeasured species contributing to dry deposition, we used the CAMx Eulerian photochemical dispersion model, coupled with the Aladin regional numeric weather prediction model. The contribution of fog and dissolved organic nitrogen was estimated using a geostatistical data driven model. We prepared individual maps for particular components applying the most relevant approach and then merged all layers to obtain a final map representing the best estimate of nitrogen deposition over the Czech Republic. Final maps accounting for unmeasured species clearly indicate that the approach used so far may result in a substantial underestimation of nitrogen deposition flux. Our results showed that nitrogen deposition over the Czech forested area in 2008 was well above 2 g N m−2 yr−1, with almost 70% of forested area receiving 3–4 g N m−2 yr−1. NH3 and gaseous HNO3, contributing about 80%, dominated the dry nitrogen deposition. Estimating the unmeasured nitrogen species by modeled values provides realistic approximations of total nitrogen deposition that also result in more realistic spatial patterns that could be used as input for further studies of likely nitrogen impacts on ecosystems.

Modeling inorganic nitrogen deposition in Guangdong province, China

Atmospheric nitrogen deposition is an essential component of acid deposition and serves as one of main sources of nitrogen of the ecosystem. Along with rapidly developed economy, it is expected that the nitrogen deposition in Guangdong province is considerably large, due to substantial anthropogenic reactive nitrogen lost to the Pearl River Delta (PRD) region, one of the most developed region in China. However, characterization of chemical compositions of inorganic nitrogen (IN) deposition and quantification of nitrogen deposition fluxes in time and space in Guangdong province were seldom conducted, especially using a numerical modeling approach. In this study, we established a WRF/SMOKE-PRD/CMAQ model system and expanded 2006-based PRD regional emission inventories to Guangdong provincial ones, including SO2, NOx, VOC, PM10, PM2.5, and NH3 emissions for modeling nitrogen deposition in Guangdong province. Observations, including meteorological observed data, rainfall data, ground-level criteria pollutant measurements, satellite-derived data, and nitrogen deposition fluxes from field measurements were employed in the evaluation of model performance. Results showed that annual nitrogen deposition fluxes in the PRD region and Guangdong province were 31.01 kg N hm−1 a−1 and 26.03 kg N hm−1 a−1, dominated by NHx (including NH3 and NH4+), with a percentage of 63% and 71% of the total deposition flux of IN, respectively. The ratio of dry deposition to wet deposition was approximately 2:1 in the PRD region and about 3:2 in the whole Guangdong province. IN deposition was mainly distributed in the PRD region, Chaozhou, and Maoming, which was similar to the spatial distributions of NOx and NH3 emissions. The spatial distributions of chemical compositions of IN deposition implied that NH3–N and NOx-N tended to deposit in places close to emission sources, while spatial distributions of aerosol NH4+−N and NO3−−N usually exhibited broader deposition areas, along with long-range transport of fine particles. Distinct temporal trends were found in IN components, especially for wet depositions, with peak values in August.

Atmospheric deposition of nitrogen and sulfur over southern Europe with focus on the Mediterranean and the Black Sea

Atmospheric deposition provides significant amounts of nutrients to the continental and marine ecosystems. Using the mesoscale WRF/CMAQ modeling system, the nitrogen (N) and sulfur (S) atmospheric deposition fluxes over the Mediterranean and the Black seas and continental Europe are evaluated for the year 2008. The annual N and S deposition fluxes are calculated to be 4.89 Tg(N) yr−1 and 2.07 Tg(S) yr−1 over continental Europe, 0.92 Tg(N) yr−1 and 0.52 Tg(S) yr−1 over West Mediterranean, 1.10 Tg(N) yr−1 and 0.84 Tg(S) yr−1 over East Mediterranean and 0.36 Tg(N) yr−1 and 0.17 Tg(S) yr−1 over the Black Sea. Inorganic N deposition fluxes are calculated to be about 3 times higher than gaseous organic N deposition fluxes. Comparison to available observations associates the annual mean model estimates with about 40 ± 30% of uncertainty depending on location. Dry deposition dominates over wet deposition for both N and S in agreement with the observations. Results suggest that an important fraction of the N deposited over the Mediterranean basin can be attributed to transported N species while S deposition is dependent more on the local emissions. In Black Sea and West Mediterranean Sea waters the calculated atmospheric N inputs are comparable to the N export measured by sediment traps whereas in the East Mediterranean N input exceeds by a factor of about 5 the N export. Our simulations show that the critical N load of 1 g(N) m−2 yr−1 is exceeded over 84% of the European forested areas.

The cycling of organic nitrogen through the atmosphere

Atmospheric organic nitrogen (ON) appears to be a ubiquitous but poorly understood component of the atmospheric nitrogen deposition flux. Here, we focus on the ON components that dominate deposition and do not consider reactive atmospheric gases containing ON such as peroxyacyl nitrates that are important in atmospheric nitrogen transport, but are probably not particularly important in deposition. We first review the approaches to the analysis and characterization of atmospheric ON. We then briefly summarize the available data on the concentrations of ON in both aerosols and rainwater from around the world, and the limited information available on its chemical characterization. This evidence clearly shows that atmospheric aerosol and rainwater ON is a complex mixture of material from multiple sources. This synthesis of available information is then used to try and identify some of the important sources of this material, in particular, if it is of predominantly natural or anthropogenic origin. Finally, we suggest that the flux of ON is about 25 per cent of the total nitrogen deposition flux.

Trends in atmospheric deposition fluxes of sulphur and nitrogen in Czech forests

We present the temporal trends and spatial changes of deposition of sulphur and nitrogen in Czech forests based on records from long-term monitoring. A statistically significant trend for sulphur was detected at most of the sites measuring for wet, dry, and total deposition fluxes and at many of these the trend was also present for the period after 2000. The spatial pattern of the changes in sulphur deposition flux between 1995 and 2011 shows the decrease over the entire forested area in a wide range of 18.1–0.2 g m−2 year−1 with the most pronounced improvement in formerly most impacted regions. Nitrogen still represents a considerable stress in many areas. The value of nitrogen deposition flux of 1 g m−2 year−1 is exceeded over a significant portion of the country. On an equivalent basis, the ion ratios of NO3−/SO42− and NH4+/SO42− in precipitation show significantly increasing trends in time similarly to those of pH.

Atmospheric inorganic nitrogen input via dry, wet, and sea fog deposition to the subarctic western North Pacific Ocean

Abstract. Aerosol, rainwater, and sea fog water samples were collected during the cruise conducted over the subarctic western North Pacific Ocean in the summer of 2008, in order to estimate dry, wet, and sea fog deposition fluxes of atmospheric inorganic nitrogen (N). During sea fog events, mean number densities of particles with diameters larger than 0.5 μm decreased by 12–78%, suggesting that particles with diameters larger than 0.5 μm could act preferentially as condensation nuclei (CN) for sea fog droplets. Mean concentrations of nitrate (NO3−), methanesulfonic acid (MSA), and non sea-salt sulfate (nss-SO42−) in sea fog water were higher than those in rainwater, whereas those of ammonium (NH4+) in both sea fog water and rainwater were similar. These results reveal that sea fog scavenged NO3− and biogenic sulfur species more efficiently than rain. Mean dry, wet, and sea fog deposition fluxes for atmospheric total inorganic N (TIN; i.e. NH4+ + NO3−) over the subarctic western North Pacific Ocean were estimated to be 4.9 μmol m−2 d−1, 33 μmol m−2 d−1, and 7.8 μmol m−2 d−1, respectively. While NO3− was the dominant inorganic N species in dry and sea fog deposition, inorganic N supplied to surface waters by wet deposition was predominantly by NH4+. The contribution of dry, wet, and sea fog deposition to total deposition flux for TIN (46 μmol m−2 d−1) were 11%, 72%, and 17%, respectively, suggesting that ignoring sea fog deposition would lead to underestimate of the total influx of atmospheric inorganic N into the subarctic western North Pacific Ocean, especially in summer periods.

The role of atmospheric deposition in the eutrophication of the North Sea: A model analysis

This study quantifies the relative contribution of atmospheric deposition to total nitrogen in the southern North Sea in a spatial and temporal context. This is done by means of a biogeochemical model analysis using the Delft3D Generic Ecological Model (GEM). Tracer based model results show that atmospheric deposition accounts for 6% of the external nitrogen inputs in the North Sea. This percentage, however, varies strongly per region. For example, in the OSPAR area NLO2 (Oystergrounds and vicinity), 16% of the total nitrogen originates from atmospheric deposition.To test whether atmospheric deposition also affects other eutrophication related variables, comparative model experiments were carried out in which model-based net deposition fluxes of nitrogen are included and excluded, respectively. Model results show that primary production rates are disproportionately affected by atmospheric deposition, which is due to a change in the carbon-to-nitrogen ratio. Furthermore, evaluation of O2 time series at Oystergrounds indicate that in offshore areas that are prone to hypoxia, the atmospheric nitrogen flux may just be a critical contribution to oxygen depletion.

Impact of declining atmospheric deposition on forest soil solution chemistry in Flanders, Belgium

Throughout Europe and the USA, forest ecosystem functioning has been impacted by long-term excessive deposition of acidifying compounds. In this study, we report on trends in stand deposition and soil solution fluxes of inorganic nitrogen (N) and sulphur (S) compounds over a 17-year period (1994–2010) in five ICP Forests monitoring plots in Flanders, northern Belgium. Deposition was dominated by N, and primarily NH4+. Deposition of SO42− and NH4+ declined by 56–68% and 40–59% respectively. Deposition of NO−3 decreased by 17–30% in deciduous forest plots, but remained stable in coniferous forest plots. The decrease of N and S deposition was parallelled by a simultaneous decline in base cation (BC = Ca2+ + K+ + Mg2+) deposition, resulting in a 45–74% decrease of potentially acidifying deposition. Trends in soil solution fluxes of NH4+, NO3−, SO42− and BC mirrored declining depositions. Nitrate losses below the rooting zone were eminent in both coniferous forest plots and in one deciduous forest plot, while net SO42− release was observed in two deciduous forest plots. Critical limits for BC/Al ratio were exceeded at the three plots on sandy soils with lower cation exchange capacity and base saturation. Soil solution acid neutralizing capacity increased but remained negative, indicating that soil acidification continued, as the start of recovery was delayed by a simultaneous decrease of BC depositions and short-term soil buffering processes. Despite substantial reductions, current N deposition levels still exceed 4–8 times the critical load for safeguarding sensitive lichen species, and are still 22–69% above the critical load for maintaining ground vegetation diversity.

Simulating dry deposition fluxes of PM10 and particulate inorganic nitrogen over the eastern China seas during a severe Asian dust event using WRF-Chem model

A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19–25 March, 2002. The modeling result well reproduced PM10 concentrations in various distances from the dust sources and the transport pathway of the dust strom. The results showed that both the concentrations and the dry deposition fluxes of PM10 increased over the China seas during the dust event following the passage of a cold front system. The maximum fluxes of PM10 in the Yellow Sea and the East China Sea during the dust event were 5.5 and 8.4 times of those before the event, respectively. However, the temporal variations of the dry deposition fluxes of particulate inorganic nitrogen differed over the Yellow Sea from those over the East China Sea. Nitrate and ammonium in the whole northern China rapidly decreased because of the intrusion of dust-loaded air on 19 March. The dust plume arrived in the Yellow Sea on 20 March, decreasing the particulate inorganic nitrogen in mass concentration accordingly. The minimum dry deposition fluxes of nitrate and ammonium in the Yellow Sea were about 3/5 and 1/6 of those before the dust arrival, respectively. In contrast, when the dust plume crossed over the Yangtze Delta area, it became abundant in nitrate and ammonium and increased the concentrations and dry deposition fluxes of particulate inorganic nitrogen over the East China Sea, where the maximum dry deposition fluxes of nitrate and ammonium increased approximately by 4.1 and 2.6 times of those prior to the dust arrival.

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.

Monitoring nitrogen deposition in typical forest ecosystems along a large transect in China

The nitrogen (N) deposition fluxes were investigated in eight typical forest ecosystems along the North-South Transect of Eastern China (NSTEC; based on the ChinaFLUX network) by ion-exchange resin (IER) columns from May 2008 to April 2009. Our results demonstrated that the method of IER columns was both labor cost saving and reliable for measuring dissolved inorganic nitrogen (DIN) deposition at the remote forest stations. The deposition of DIN in the throughfall ranged from 1.3 to 29.5 kg N ha(-1) a(-1), increasing from north to south along NSTEC. The relatively high average ratio of ammonium to nitrate in deposition (1.83) indicated that the N deposition along the NSTEC in China mostly originated in farming and animal husbandry rather than in industry and vehicle activities. For seasonal variability, the DIN deposition showed a single peak in the growing season in the northern part of NSTEC, while, in the southern part, it exhibited double-peaks in the early spring and the mid-summer, respectively. On the annual scale, the DIN deposition variations of the eight sites could be mainly explained by precipitation and the distances from forest stations to provincial capital cities.

Long term monitoring of the chemical composition of precipitation and wet deposition fluxes over three Sahelian savannas

The purpose of this study is to analyze a long term database of the chemical composition of precipitation at three African dry savanna sites in the Sahel. The precipitation samples were collected during the monsoon season at Agoufou (15°20′N, 01°29′W, Mali) from 2004 to 2006, Banizoumbou (13°31′N, 02°38′E, Niger) from 1994 to 2009 and Katibougou (12°56′N, 07°32′ W, Mali) from 1997 to 2008. pH and major inorganic and organic ions in precipitation were analyzed by ionic chromatography. A characterization of mean precipitation chemistry with the associated wet deposition fluxes for each species is presented. The first important result is that interannual variability of all volume-weighted mean (VWM) concentrations is low, ranging between ±5% and ±25%. Acidity in dry savannas is low and indicates the strong alkaline nature of the precipitation. The average annual pH at Agoufou is 6.28, 5.75 at Banizoumbou and 5.54 at Katibougou. This result is correlated with the important terrigenous contribution measured in the chemical content of precipitation, implying acidity neutralization by mineral species such as Ca2+ and NH4+. Mg2+ and K+ are found to play a minor role in neutralization. Enrichment factor calculations for Ca2+, SO42−, K+ and Mg2+ with respect to the sea reference reveal a significant influence of Saharan and Sahelian crustal sources. VWM concentrations of these species dominate the composition of measured precipitation. An estimation of the potential particulate and gas contribution to the total precipitation composition is given for each site: At Agoufou, the mean relative contribution in rainwater is 80% for particles and 20% for gases, while at the Banizoumbou and Katibougou sites, results indicate 70% for particles and 30% for gases. The high particulate phase contribution to precipitation emphasizes the importance of multiphase processes between gases and particles in the atmospheric chemistry typical of African semi-arid savanna ecosystems. The second highest contribution is nitrogenous, with high VWM concentrations of NO3− and NH4+ measured at the three sites. Monthly evolution of NO3− and NH4+ concentrations are studied in relation to gaseous emission sources in the Sahelian region, i.e. biogenic soil emission and ammonia sources from animals. The calculated wet nitrogen deposition flux presents a regular increase throughout the wet season at the three sites. Results suggest total mean nitrogen deposition fluxes of 1.80 kg N ha−1 yr−1 at Agoufou, 2.10 kg N ha−1 yr−1 at Banizoumbou, and 3.30 kg N ha−1 yr−1 at Katibougou. The marine contribution is lower, 23% at Agoufou, 17% at Banizoumbou and 13% at Katibougou. The last contribution concerns organic acidity, which ranges from 5% at Agoufou, 10% at Banizoumbou to 14% at Katibougou. Terrigenous and marine contributions present a negative gradient, whereas nitrogenous and organic contributions a positive gradient along the Sahelian transect defined by Agoufou–Banizoumbou–Katibougou.