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Elevated atmospheric reactive nitrogen (Nr) emissions and the subsequent nitrogen (N) deposition have negatively impacted the global environment, particularly in China. In order to assess the long-term trends in atmospheric N deposition in the south of China, Taojiang County in Hunan Province was selected as a representative rural area for study. We analyzed interannual variation in atmospheric Nr, including gaseous ammonia (NH3), nitrogen dioxide (NO2), nitrate acid (HNO3) vapor, particulate ammonium (NH4+), and nitrate (NO3−) in air and NH4+-N and NO3−-N in precipitation from 2011 to 2020. The 10-year average atmospheric wet-plus-dry N deposition was 41.9 kg N ha−1 yr−1, which decreased by approximately 24% after 2012, indicating that NH3 and NOx emissions were effectively reduced by emission controls introduced in 2013. Wet deposition accounted for approximately 74% of the total N deposition and was significantly influenced by annual precipitation amount. Reduced N (NH3, pNH4+, and NH4+ in rainwater) was the dominant form, comprising approximately 58% of the total N deposition, while oxidized N (pNO3−, NO2, HNO3, and NO3− in rainwater) accounted for 42% of the total N deposition. Atmospheric HNO3, NO2, and NH3 concentrations and deposition declined by 30–80% over the decade, while particulate NH4+ and NO3− concentrations and deposition remained at relatively stable levels, which suggests that ongoing research and policy should focus on rural particulate pollution. Future strategies must concentrate on the integrated control of NH3 and NOx emissions to mitigate air pollution and protect human health, particularly in rural areas because current abatement efforts are primarily directed toward urban areas and the industrial sector, whereas non-point source NH3 pollution, influenced mainly by agricultural activities, dominates in rural regions. [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]

• Atmospheric N deposition in China was evaluated by two time-scale deposition databases. • Bulk and dry N deposition reached a peak between 2000 and 2010 and then began a steady decline. • Significant decrease of oxidized N deposition proved the effectiveness of NO x emissions control. • Increase of NH 3 dry deposition highlighted the importance of regional NH 3 mitigation. 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 NO x emission controls. In contrast, reduced N deposition was approximately constant, with reductions in bulk NH 4 +-N deposition offset by a continuous increase in dry NH 3 deposition. Elevated NH 3 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 NH 3 , built on broader regional emission control strategies. [ABSTRACT FROM AUTHOR]