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Abstract While the ongoing increases in the deposition of atmospheric nitrogen (N) in China have attracted ever more attention, to date there has been little research in N deposition in inland aquatic ecosystems. In this study, we quantified the bulk and dry atmospheric N deposition around the Dongting Lake, which is connected to the Yangtze River and is the second largest freshwater lake in China. Bulk N deposition averaged 48.0 kg N ha−1 yr−1, of which ammonium (NH 4 N), nitrate (NO 3 N), and dissolved organic nitrogen (DON) accounted for 41.6%, 35.1%, and 23.3%, respectively. Dry N deposition averaged 27.0 kg N ha−1 yr−1, and was dominated by NH 3. Bulk N deposition was higher in spring and summer than in autumn and winter at the sites around the lake because of the high precipitation. NH 3 deposition was the highest in spring and summer due to fertilization, and NO x deposition was the highest in winter because of the combustion of coal for domestic heating. The concentrations of NH 3 significantly decreased with the concentration of NH 4 N, indicating below-cloud scavenging and local sources. The concentrations of NO x and NO 3 N were not correlated, indicating long-distance transfer of NO x. Bulk N deposition in our study was generally twice that reported in other studies, even when only inorganic N species in bulk deposition were considered. Total N deposition averaged 75.0 kg N ha−1 yr−1, which was much higher than that reported in other studies. Both N deposited directly into the lake and N deposited across the lake basin that was subsequently transported to the lake in runoff could enrich the N concentration of the lake water and increase the gross primary productivity (GPP). Our results highlighted the importance of integrated management that includes both aquatic and atmospheric systems at either the lake basin scale or regional scale, rather than at the individual lake-scale. Graphical abstract Image 1 Highlights • Total N deposition was much higher than that reported in other studies around the Dongting Lake. • DON deposition, which usually be ignored, is a significant contributor. • Potential eutrophication effects of N loading to the Dongting Lake from atmospheric N deposition should be re-evaluated. [ABSTRACT FROM AUTHOR]

Quantifying the similarities and differences in atmospheric nitrogen (N) deposition between different ecosystems is important to develop effective measures to reduce air pollution and maintain biodiversity. Here we show that the constitution of N deposition differed significantly between a grassland and a desert ecosystem in Northwestern China. Flux of bulk (wet plus part of dry deposition) and dry (gaseous NH 3 and NO 2) deposition were continuously monitored from 2018 to 2020. The grassland and desert sites had similar amount of total N deposition, being 7.29 and 6.33 kg N ha−1 yr−1, respectively. However, N deposition at the grassland was dominated by the bulk deposition (4.44 kg N ha−1 yr−1, 61% of the total N deposition), whereas that at the desert was dominated by dry deposition (4.20 kg N ha−1 yr−1, 66% of total deposition). The desert had greater ambient concentrations of NH 3 (3.66 μg N m−3) and NO 2 (1.52 μg N m−3) than the grassland (2.73 μg NH 3 –N m−3 and 0.72 μg NO 2 –N m−3). The amount of reduced N deposition (NH 4 + and NH 3) was around 3 times of that of oxidized N deposition (NO 3 − and NO 2) in both ecosystems. The N deposition rates in both ecosystems have exceeded the critical load for the fragile ecosystems (5–10 kg N ha−1 yr−1), highlighting the importance of reducing N emission sources that are related with anthropogenic disturbance. [Display omitted] • The boundary of Tarim Basin and Tibet Plateau has relatively low N deposition. • Bulk and dry deposition dominated in grassland and desert, respectively. • The reduced/oxidized N ratio in N deposition was close to 3 in both ecosystems. • N deposition exceeded the minimum critical load value for sensitive ecosystems. [ABSTRACT FROM AUTHOR]

Soils below croplands and grasslands have acidified significantly in China since the 1980s in terms of pH decline in response to acid inputs caused by intensified fertilizer application and/or acid deposition. However, it is unclear what the rate is of pH decline of forest soils in China in response to enhanced acid deposition and wood production over the same period. We therefore gathered soil pH data from the Second National Soil Inventory of China and publications from the China National Knowledge Infrastructure (CNKI) database in 1981–1985 and 2006–2010, respectively, to evaluate the long-term change of pH values in forest soils. We found that soil pH decreased on average by 0.36 units in the period 1981–1985 to 2006–2010., with most serious pH decline occurring in southwest China (0.63 pH units). The soil type with the strongest pH decline was the semi-Luvisol (0.44 pH units). The decrease in pH was significantly correlated with the acid input induced by atmospheric deposition and forest harvesting. On average, the contribution of atmospheric deposition to the total acid input was estimated at 84% whereas element uptake (due to forest wood growth and harvest) contributed 16% only. Atmospheric deposition is thus the major driver for the significant forest soil acidification across China. [ABSTRACT FROM AUTHOR]

Abstract: Atmospheric emissions of reactive nitrogen (N) species are at high levels in China in recent years, but few studies have employed N deposition monitoring techniques that measure both dry and wet deposition for comprehensive evaluation of the impacts of N deposition on ecosystems. In this study, to quantify the total N deposition, both dry and wet N depositions were monitored using denuder/filter pack systems, passive samplers and wet-only samplers at three sites with different land use types (forest, paddy field and tea field) in a 135-km2 catchment in subtropical central China from September 2010 to August 2011. At the three sampling sites, the annual mean concentrations of total N (the sum of , and DON) in rainwater were 1.2–1.6 mg N L−1, showing small variation across sites. Annual mean concentrations of total N (the sum of NH3, NO2, HNO3, particulate and ) in the air were 13–18 μg N m−3. High NH3 concentrations in the air were observed at the agricultural sites of tea and paddy fields, indicating significant NH3 emissions from N fertiliser application; and high NO2 concentrations were found at the upland sites of forest and tea field, suggesting high NO emissions from soils due to high N deposition or high N fertiliser input. The annual total N deposition for the three sites of paddy field, tea field and forest was estimated as 22, 34 and 55 kg N ha−1 yr−1, in which the dry N deposition components contributed to 21%, 36% and 63% of the annual total N deposition, respectively. The annual deposition of reduced N species was 1.1–1.8 times of the annual deposition of oxidised N species. To minimise the adverse effects of atmospheric N deposition on natural/semi-natural ecosystems, it is crucial to reduce the reactive N emissions from anthropogenic activities (e.g., N fertiliser application, animal production and fossil fuel combustion) in subtropical central China. [Copyright &y& Elsevier]

Organic nitrogen (N) is an important component of the atmospheric deposition of reactive N, but its sources are essentially unknown. Assessing whether this dissolved organic N (DON) is of natural, anthropogenic or mixed origin is critically important in attempting to determine the scale of human perturbation of the global N cycle. Here we report evidence for atmospheric organic N deposition and its anthropogenic sources in China. Precipitation samples were collected and analyzed from 15 rural, suburban and urban sites during 2005 and 2006. The average deposition of DON was 8.6kgha−1 yr−1 with a volume-weighted concentration of 111μmolL−1, which was much higher than in other regions of the world. The contribution of DON to total dissolved N (TDN) was approximately 30% on average, agreeing well with other reported data in the literature. Parallel collections of wet-only and bulk deposition showed wet deposition to be 68% on average, indicating a significant dry deposition component. Combining data from the Chinese sites with those from elsewhere in the world, significant (p<0.0001) correlations between DON and NH4–N, NO3–N and TDN suggest that atmospheric organic N originates from similar sources to dissolved inorganic N (DIN) (NH4–N and NO3–N), which are largely attributed to anthropogenic emissions from both agricultural and industrial sources. [Copyright &y& Elsevier]

Abstract Very few comparative studies on atmospheric dry and wet nitrogen (N) deposition have been conducted in agro-pastoral catchment areas. In an effort to fill this knowledge gap, three interconnected land use types (cropland, mountain pasture, and plain pasture) with six sampling sites (Chinese cropland (CC), Chinese mountain pasture (CM), Chinese plain pasture (CP) Mongolia cropland (MC), Mongolia mountain pasture (MM) and Mongolia plain pasture (MP)) were selected in the transboundary regions of northwest China and western Mongolia. During 16 months from May 2014 to September 2015 atmospheric and precipitation samples were collected to assess levels of nitrogen deposition. Cropland had the highest NO 3 −N (1.0 mg N L−1 in China and 1.2 mg N L−1 in Mongolia) and NH 4 +-N concentrations (1.6 mg N L−1 in China and 2.0 mg N L−1 in Mongolia) in our six sampling sites. The CC experienced the highest wet deposition (5.2 kg N ha−1 yr−1), followed by MM pasture (3.2 kg N ha−1 yr−1) while wet deposition in other sites ranged from 2.1 to 2.8 kg N ha−1 yr−1. The ambient concentrations of NH 3 , NO 2 and dry N deposition were significant higher in cropland than being other land use with 3.0, 3.8 and 1.2 μg N m−3 respectively in China and 2.2, 2.8 and 0.6 μg N m−3 respectively in Mongolia. The highest total N deposition was at CC (14.5 kg N ha−1 yr−1) and MC (9.4 kg N ha−1 yr−1), followed by the mountain pasture (5.8–6.8 kg N ha−1 yr−1), and the plains pasture (5.6–5.7 kg N ha−1 yr−1). Overall, agro-pastoral catchments areas had relatively low total N deposition compared to other studies, and cropland had the highest wet and dry N deposition than mountain and plain pastures, and dry N deposition absolutely dominated the percentage (64–70% in cropland and 53–64% in pasture areas) of total atmospheric N deposition. Comparing the total N deposition in China and Mongolia, we found the CC had 54% higher value than in MC while the reverse was true for mountain pastures Mongolia received 17% more N. Graphical abstract Image 1 Highlights • Passive samplers, PM 10 samplers and rain gauges equipments were used to quantify the nitrogen deposition in six typical land use types. • The cropland sites had significant higher NH 3 and NO 2 concentration and total N deposition than pasture areas in our research area. • Dry deposition absolutely dominated the percentage of total atmospheric N deposition in agro-pastoral catchment areas of China and Mongolia. • Nitrogen deposition in CC had 54% higher value than in MC while the reverse was true for mountain pastures Mongolia received 17% more N. [ABSTRACT FROM AUTHOR]

In a publication in Atmospheric Environment ( http://dx.doi.org/10.1016/j.atmosenv.2015.10.081 ), Gu et al. (2015) estimated that “the total nitrogen (N) deposition in 2010 was 2.32 g N m −2 yr −1 ” in China. This value is comparable with previous estimations based on a synthesized dataset of wet/bulk inorganic N deposition observations, which underestimates the total N deposition since their algorithm (equations (2) and (3) in their paper) does not account for dry deposition of NH 3 , HNO 3 , NO x and wet/dry deposition of HONO and organic nitrogen (e.g. amines, amides, PAN). Indeed, Gu et al. (2015) mixed the terminology of wet/bulk deposition and total deposition. Another flawed assumption by Gu et al. (2015) is that all inorganic N in precipitation estimated by their algorithm originates from fertilizer and coal combustion. This is incorrect and almost certainly causes biases in the spatial and temporal distribution of estimated wet/bulk inorganic N deposition (Fig. 5 in their paper), further considering the fact that they neglected important N sources like livestock and they did not consider the nonlinearity between various sources and deposition. Besides the input data on N deposition, the model validation (Sect. 2.3.2) described in their paper also requires clarification because the detailed validation information about the time series of observational dataset versus modeling results was not given. As a result of these combined uncertainties in their estimation of N deposition and the lack of detail for model-measurement comparison, their estimates of the impacts of N deposition on carbon storage in Chinese forests may need further improvement. We suggest the clarification of the terminology regarding N deposition, especially for wet deposition, bulk deposition, gaseous and particulate dry deposition or total deposition since the accurate distinction between these terms is crucial to investigating and estimating the effects of N deposition on ecosystems. [ABSTRACT FROM AUTHOR]

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 (NH 3 ) concentration, and satellite measurements of tropospheric NO 2 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 (NH x ) and 6.2 Tg N from oxidized nitrogen (NO y ). Domestic anthropogenic sources contribute 86% of the total deposition; foreign anthropogenic sources 7% and natural sources 7%. Annually 23% of domestically emitted NH 3 and 36% for NO x 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. [ABSTRACT FROM AUTHOR]

Precipitation chemistry and atmospheric nitrogen (N) deposition are of great concern worldwide due to their close relationships with air quality and impacts on ecosystems. However, evaluation of the chemical composition of precipitation and N deposition flux in rural areas of Beijing has received little attention to date. This paper presents the chemical constituents, possible sources and wet deposition fluxes of water-soluble ions (NH 4 +, NO 3 −, SO 4 2−, Cl−, Na+, K+, Ca2+, Mg2+) in precipitation samples collected during 2017–2018 at a rural site located at northwest of Beijing city; meanwhile, dry deposition of reactive N species (gaseous ammonia, nitrogen dioxide, nitric acid, and particulate (p) NH 4 + and NO 3 −) were also quantified. During this 2-year period, the volume-weighted mean (VWM) pH of precipitation was 6.73, and all samples had pH values above 6.0. The VWM electric conductivity of precipitation and the mean sum of all measured ions was 43.8 μS cm−1 and 591.9 μeq L−1, respectively, indicating a significant impact of atmospheric pollution. Ca2+ and NH 4 + were the dominant neutralizing species for precipitation acidity. Positive matrix factorization analysis further confirmed five sources for water-soluble ions, including sea salt aging, secondary formation, agriculture, crust, and biomass burning. The annual mean wet N deposition was 4.6, 3.4 and 8.0 kg N ha−1 yr−1 for NH 4 +, NO 3 − and total inorganic N, respectively. The total dry N deposition was dominated by gaseous ammonia (11.5 kg N ha−1 yr−1). The total N deposition (wet plus dry) was 27.7 kg N ha−1 yr−1, where dry deposition contributed to 75% and wet deposition 25% of the total. The simulations from the GEOS-Chem model indicate that agricultural (fertilizer use and livestock) and nonagricultural sources (industry, power plant, and transportation) are both important contributors to total N deposition. These results could be useful in evaluating/developing emission control policies to protect the eco-environment in Beijing. • Precipitation chemistry and nitrogen (N) deposition were investigated in Beijing. • The pH values of precipitation samples were all above 6.0 and averaged 6.7. • Ion source was sea salt, secondary source, agriculture, crust, and biomass burning. • Total N deposition was 27.7 kg N ha−1 yr−1, of which 75% was from dry deposition. • Agricultural and nonagricultural sources contributed equally to total N deposition. [ABSTRACT FROM AUTHOR]