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Stringent emission controls during the Asia Pacific Economic Cooperation Summit (APEC; November 5–11, 2014) provide a valuable opportunity to examine the impact of such measures on the chemical properties of PM 2.5 and other air pollutants. Here, we measured the water-soluble inorganic ions (WSII) and carbonaceous species in PM 2.5 , NH 3 and NO 2 at multiple sites in Beijing between September and November 2014. Relative to the pre-APEC period (September and October 2014), significant reductions in the average concentrations of WSII (69% for NO 3 −, 68% for SO 4 2−, 78% for NH 4 +, and 29–71% for other species), elemental carbon (EC, 43%) and organic carbon (OC, 45%) in PM 2.5 were found during the APEC period. The contributions of secondary inorganic ions (SIA, including SO 4 2−, NO 3 −, and NH 4 +) to PM 2.5 were significantly lower during the APEC period (9–44%), indicating a combination of lower gaseous precursor emissions and a relative weak secondary aerosol formation. Ion-balance calculations indicated that the PM 2.5 sample in the pre-APEC period was alkaline but was acidic during the APEC period. Relatively lower mean concentrations of EC (1.5 μg m−3), OC (10.5 μg m−3), secondary organic carbon (SOC, 3.3 μg m−3), secondary organic aerosol (SOA, 5.9 μg m−3) and primary organic aerosol (POA, 10.0 μg m−3) appeared during the APEC period. The average concentrations of NH 3 and NO 2 at all road sites were significantly reduced by 48 and 60% during the APEC period, which is consistent with clear reductions in satellite NH 3 columns over Beijing city in the same period. This finding suggests that reducing traffic emissions could be a feasible method to control urban NH 3 pollution. During the APEC period, concentrations of PM 2. 5 , PM 10 , NO 2 , SO 2 and CO from the Beijing city monitoring network showed significant reductions at urban (20–60%) and rural (18–57%) sites, whereas O 3 concentrations increased significantly (by 93% and 53%, respectively). The control measures taken in the APEC period substantially decreased PM 2.5 pollution but can increase ground O 3 , which also merits attention. • Concentrations of PM 2.5 and components reduced significantly during the APEC period. • Major components in PM 2.5 and other pollutants were comparable with other cities. • Vehicle restrictions could lower atmospheric NH 3 concentration over Beijing. • Emission control measures significantly increased ground-level O 3 concentrations. [ABSTRACT FROM AUTHOR]

Atmospheric reactive nitrogen (Nr) emissions and deposition have caused much damage to the global environment and also impacted human health. Determining long-term trends in atmospheric Nr concentrations and deposition is important for evaluating air quality and ecosystem effects and formulating control measures to reduce negative impacts. We measured monthly concentrations of NH 3 , pNH 4 +, HNO 3 , pNO 3 -, and NO 2 and calculated their dry deposition rates using an inferential method from 2011 to 2018 at an urban site in Zhengzhou in the North China Plain. Inorganic N (NH 4 + and NO 3 −) concentrations in precipitation and wet/bulk N deposition were also quantified in 2011, 2016, 2017 and 2018. The results showed high concentrations of atmospheric Nr species, with considerable variation in some species over the monitoring period. Annual mean NH 3 concentrations significantly increased from 2011 to 2018 (p < 0.001) with that in 2018 being twice that in 2011. However, pNO 3 - and pNH 4 + concentrations decreased after 2013. The annual mean NO 2 concentration in 2018 had decreased by 33.4% compared to the peak in 2011. Highest NH 3 concentrations were measured in spring or summer, and lowest concentrations in winter. pNH 4 + and pNO 3 - concentrations peaked mainly in winter. Total annual dry N deposition ranged from 21.9 to 41.2 kg N ha−1. Bulk NH 4 + and NO 3 − deposition was lower in 2016–2018 than in 2011. However, atmospheric Nr concentrations and N deposition remained high in this urban ecosystem. NH 3 emissions urgently need control measures, and Nr impacts on the surrounding ecosystems and human health should be considered. Continuous long-term measurements of atmospheric Nr concentrations and deposition at a regional scale are necessary to help formulate emission control measures and protect human and ecosystem health. • Significant changes in atmospheric reactive nitrogen were observed at an urban site in north China. • NH 3 concentrations increased by 110% from 2011 to 2018. • pNO 3 - and pNH 4 + concentrations in 2018 decreased by 65.1% and 62.8% compared to the maxima in 2012. • As a consequence, N deposition slightly decreased, with some improvement in air quality. [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]

Large uncertainties and challenges remain in the quantification of land-atmosphere exchanges of ammonia (NH 3), 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 NH 3 fluxes at a typical cropland in the North China Plain, one of the global NH 3 hotspots. It is the first attempt of measuring both NH 3 volatilization and deposition fluxes at an agricultural ecosystem using the open-path instrument-based EC technique. During the one-month experimental period, the NH 3 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 NH 3 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 NH 3 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 NH 3 exchanges. It also enables cross-validation between different methods to improve the understanding in the atmospheric reactive nitrogen cycling. • The open-path QCL-based eddy covariance instrument can detect small NH 3 fluxes. • Nitrogen loss rate from the wheat field through NH 3 volatilization was 0.57–0.71%. • NH 3 dry deposition averaged to 0.014 kg N ha−1 d−1 with a significant diurnal pattern. • Depositions estimated by inferential model were two times larger than the observed. [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]