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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 PM2.5 and other air pollutants. Here, we measured the water-soluble inorganic ions (WSII) and carbonaceous species in PM2.5, NH3 and NO2 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 NO3−, 68% for SO42−, 78% for NH4+, and 29–71% for other species), elemental carbon (EC, 43%) and organic carbon (OC, 45%) in PM2.5 were found during the APEC period. The contributions of secondary inorganic ions (SIA, including SO42−, NO3−, and NH4+) to PM2.5 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 PM2.5 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 NH3 and NO2 at all road sites were significantly reduced by 48 and 60% during the APEC period, which is consistent with clear reductions in satellite NH3 columns over Beijing city in the same period. This finding suggests that reducing traffic emissions could be a feasible method to control urban NH3 pollution. During the APEC period, concentrations of PM2.5, PM10, NO2, SO2 and CO from the Beijing city monitoring network showed significant reductions at urban (20–60%) and rural (18–57%) sites, whereas O3 concentrations increased significantly (by 93% and 53%, respectively). The control measures taken in the APEC period substantially decreased PM2.5 pollution but can increase ground O3, which also merits attention.

This study investigates the concentrations and δ15N values of NH3 in Beijing during and after the 2020 COVID-19 lockdown. Higher NH3 concentrations and lower δ15N-NH3(measured) were observed at most sites in 2020 compared to 2017. Except for a site inside a tunnel, NH3 concentrations did not increase significantly after the lockdown had ended compared to those during the lockdown, while δ15N-NH3(measured) increased by 2.1–9.9‰. Nonagricultural sources (fossil fuel and urban waste) overall contributed 81% and 62% of NH3 at on-road (tunnel interior) and nonroad (CAU) sites in 2020, respectively, comparable to those in 2017 (without significant difference). The contribution of nonagricultural sources slightly increased after the lockdown compared to the contribution during the lockdown at the nonroad site and hardly changed at the tunnel interior site. Our results suggest that (1) unfavorable meteorological conditions, especially lower boundary layer heights and changes in regional transport patterns, might play a more important role than reduced anthropogenic emissions in the temporal variations of Beijing NH3 and (2) the effect of reduced anthropogenic emissions, during the COVID-19 outbreak or with the future implementation of emission control strategies, on atmospheric NH3 can be better demonstrated by isotope-based source apportionment of NH3, rather than only by changes in NH3 concentrations.

In order to cope with heavy haze pollution in Beijing, the Air Pollution Prevention and Control Action Plan was issued in 2013. In this study, we took January observations from 2014 to 2018 as a case study to assess wintertime air quality improvement in Beijing after five years of continuous emission control measures and to investigate the causes of haze formation. SO2 and NO2 concentrations in January 2018 decreased by 84% and 41% from January 2014, while NH3 concentrations remained relatively stable during these years with an average of 7.28 μg m−3. The mean concentrations of PM2.5 and water-soluble inorganic ions declined over the study period, while compared with 2014, decreased SO42− ratio and increased NO3− contribution in PM2.5 were observed, highlighting the importance of reactive nitrogen (Nr) pollution control. High concentrations of NH3, NO2, as well as NH4+ and NO3− in PM2.5 at roadside monitoring sites, indicated that vehicle sources played a vital role in local urban Nr emissions. Finally, we found most NH3 existed in the gas phase in the Beijing atmosphere, even on polluted winter days, suggesting a considerable risk for additional secondary aerosol formation. Our findings demonstrate the effectiveness of the emissions control in alleviating Beijing's air pollution. Significant reductions of precursor emissions are needed to achieve the goals set by air quality standards in the future, especially for NH3. It is especially crucial to jointly consider and control multiple pollution sources to effectively reduce the high levels of air pollution that remain in Beijing.

Due to increasing global demand for crop production and energy use, more and more reactive nitrogen (Nr) has been generated and emitted to the environment. As a result, global atmospheric nitrogen (N) deposition has tripled since the industrial revolution and the ecological environment and human health have been harmed. In this study, we measured dry and wet/bulk N deposition from July 2013 to December 2015 in a semi-arid grassland of Duolun County, Inner Mongolia, China. The samples of dry and wet/bulk N deposition were collected monthly with a DELTA (DEnuder for Long Term Atmospheric sampling) system and with Gradko passive samplers and a precipitation gauge. The measured results show that the annual mean concentrations of NH3, NO2, HNO3, particulate NH4+ (pNH4+) and particulate NO3− (pNO3−) in atmosphere were 2.33, 1.90, 0.18, 1.42 and 0.42 μg N/m3, respectively, and that the annual mean volume-weighted concentrations ofNH4+-N and NO3−-N in precipitation were 2.71 and 1.99 mg N/L, respectively. The concentrations of Nr components (including NH3, NO2, HNO3, pNH4+, pNO3−,NH4+-N and NO3−-N) exhibited different seasonal variations. Specifically, NO2 and HNO3 exhibited higher concentrations in autumn than in summer, while the other Nr components (NH3, pNH4+, pNO3−,NH4+-N and NO3−-N) showed the highest values in summer. Based on measured concentrations of Nr components and their deposition velocities estimated using the GEOS-Chem global atmospheric chemical transport model, the calculated annual mean dry deposition fluxes were 3.17, 1.13, 0.63, 0.91 and 0.36 kg N/(hm2•a) for NH3, NO2, HNO3, pNH4+ and pNO3−, respectively, and the calculated annual mean wet/bulk deposition fluxes were 5.37 and 3.15 kg N/(hm2•a) forNH4+-N and NO3−-N, respectively. The estimated annual N deposition (including dry N deposition and wet/bulk N deposition) reached 14.7 kg N/(hm2•a) in grassland of Duolun County, approaching to the upper limit of the N critical load (10–15 kg N/(hm2•a)). Dry and wet/bulk deposition fluxes of all Nr components (with an exception of HNO3) showed similar seasonal variations with the maximum deposition flux in summer and the minimum in winter. Reduced Nr components (e.g., gaseous NH3 and pNH4+ in atmosphere andNH4+-N in precipitation) dominated the total N deposition at the sampling site (accounted for 64% of the total N deposition), suggesting that the deposited atmospheric Nr mainly originated from agricultural activities. Considering the projected future increases in crop and livestock production in Inner Mongolia, the ecological and human risks to the negative effects of increased N deposition could be increased if no mitigation measures are taken.

Atmospheric reactive nitrogen (N) has induced large impacts on air pollution and ecosystem health worldwide. Atmospheric reactive N emission and deposition have largely increased in China since 1980 due to rapid agricultural, industrial, and urban development. But scientific gaps still remain in the regional and temporal variability in atmospheric N emissions and deposition. Meanwhile, the environmental impacts of N pollution and deposition are of great concern in China. This paper overviews the status of anthropogenic N emissions and deposition and their linkages to air pollution in China. The major findings include two aspects: (1) anthropogenic reactive N (e.g., NH3 and NOx) emissions contribute greatly to secondary inorganic aerosol formation and haze pollution and (2) dry N deposition is comparable in importance to wet N deposition, suggesting that both dry and wet deposition should be quantified simultaneously. Future research challenges on atmospheric N emission and deposition are discussed as well. China needs to (1) reduce the uncertainties of national emission inventory of various N species, especially organic N compounds; (2) establish national networks for atmospheric N concentration and deposition monitoring; and (3) evaluate ecological and environmental impacts of N pollution and deposition in typical ecosystems. Last but not least, N deposition modeling tools should be improved based on localized parameters and further used in future N regulation.

Air pollution especially of PM_(2.5) pollution is a serious problem in Beijing. In order to quantify the effect of a festival in which pollution was expected to be reduced, we collected and analyzed PM_(2.5) samples in urban Beijing during the 2015 Spring Festival (from February 9^(th) to March 6^(th) 2015). We divided the sampling period into three phases: non-haze, haze and firework days. The average concentration of PM_(2.5) was highest on firework days at 248.9 μg m^(-3), followed by haze days (199.9 μg m^(-3)) and non-haze days (90.8 μg m^(-3)). The air quality of non-haze days during the holiday was better than that during non-holiday periods. Secondary inorganic ions (SO_4^(2-), NO_3^- and NH_4^+) were enriched on the haze days, while those on firework days contained large amounts of Cl^- and K^+, but small amounts of NO_3^- and NH_4^+. Ratios of NO_3^-/SO_4^(2-), SO_4^(2-)/K^+ and Cl^-/K^+ effectively distinguished the characteristics of PM_(2.5) between firework events and haze days. Ion balance calculations indicated that the acidity of PM_(2.5) from firework days was higher than that from haze and non-haze days. A method using enrichment factors (EF) found that crustal elements (EF ＜ 10 on all three types of days) included Ca, Al, Fe, Na, Co, Ni, P, Ti, and V; firework elements (EF ＞ 10 on firework days, significantly higher than haze days) were made up of Ba, Cr, Cu, Mg, Pb, S, Si, and Zn; common anthropogenic pollution elements (EF ＞ 10 in all three types of days) were As, Cd, Cu, Pb, S, Sb, Zn. Differences in chemical characteristics indicated that holidays such as the Spring Festival can affect air pollution patterns in two ways: a decrease in the population and vehicles but an increase in activities such as firework displays.

Few related studies have been carried out for northwest China's the inland, although the increasing inorganic reactive nitrogen (Nr) deposition and severe air pollution in China have attracted considerable attention. Based on eight-year measurements of the concentrations of NH3, HNO3, particulate (p) NH4+, pNO3−, and NO2 in the air and inorganic nitrogen (NH4+, NO3−) in the precipitation at a rural site in Wuwei, Gansu Province, we quantified the dry and bulk/wet Nr deposition fluxes and analyzed their temporal trends in combination with air pollution data (2015–2018). The concentrations of the single Nr species in the air did not exhibit significant seasonal variations, except for that of pNO3− which were the highest in summer and the lowest in winter. The average annual total Nr (dry + bulk) deposition was 27.2 ± 6.7 kg N ha−1 with a significant (p

With rapid economic growth in China, anthropogenic reactive nitrogen (Nr) emissions have more than doubled over the last two or three decades. Atmospheric Nr pollution is an environmental concern in China especially in megacities such as Beijing. In order to identify the impact of emission sources on atmospheric Nr pollution, we measured atmospheric Nr concentrations and their isotopic composition (δ15N) dynamics at three typical sites: landfill, pig farm and road traffic sites in Beijing from April 2010 to March 2011. Passive samplers were used for monitoring ammonia (NH3) and nitrogen dioxide (NO2), two major Nr species, while their δ15N values were measured by a diffusion method combined with mass spectrometer approach. The raw water pool of the landfill and fattening house of the pig farm were important NH3 sources with mean NH3 concentrations being 2,829 and 2,369 µg/m3, respectively, while the road traffic site was a minor NH3 source (10.6 µg/m3). NH3 concentrations at sites besides the landfill and roads were high in summer and low in winter due to the annual variation of temperature and the change of emission source intensity. In contrast, the NH3 concentrations inside the pig farm house were high in winter and low in summer, for the barn windows were open in summer and closed in winter. The mean NO2 concentrations were 89.8, 32.9 and 23.0 µg/m3 at the road traffic, the landfill and pig farm sites, respectively. Due to vehicle fuel combustion, NO2 concentration at the road traffic was the highest among the three sources, and the road traffic was a main NO2 emission source. PM10, pNH4 + and pNO3–concentrations in particulate matter were higher in summer than in winter (except PM10 for the pig farm). The δ15NH3 values ranged from–19.14‰ to 7.82‰, with an average of–0.05‰ for the landfill site, and the lowest values were observed in June and July. The δ15NH3 values for the pig farm site ranged from–29.78‰ to–14.05‰ with an average of–24.51‰, and the δ15NH3 values were more negative in summer than in the other seasons. The δ15NO2 values were–9.63‰ to 7.04‰ with an average of–3.72‰ for the road traffic site. The δ15NO2 values were more negative in summer than those in the other seasons. The different δ15N values for the various Nr species in different sources may serve as important indicators for identifying atmospheric Nr sources in megacities. The results may also provide the theoretical basis for research on the atmospheric N deposition and its sources.

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 (NH4+, NO3−, SO42−, 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) NH4+ and NO3−) 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 NH4+ 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 NH4+, NO3− 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.

Weekly vertical profiles of ammonia (NH3) were measured at 16 heights on the Beijing 325 m meteorological tower for 1 year from March 2016 to March 2017. The average NH3 concentrations exceeded 4 µg m−3 at all heights with an overall average (±1σ) value of 13.3 (±4.8) µg m−3. The highest NH3 concentrations along the vertical profiles mostly occurred from 32 to 63 m, decreasing both towards the surface and at higher altitudes. Significant decreases in NH3 concentrations were only found at the top two heights (280 and 320 m). These results suggest an NH3 rich atmosphere during all seasons in urban Beijing, from the ground to at least 320 m. The highest seasonal NH3 concentrations across the profile were observed in summer (18.2 µg m−3) with high temperature, followed by spring (13.4 µg m−3), autumn (12.1 µg m−3) and winter (8.3 µg m−3). A significant vertical variation in the NH3 concentration was only found in summer. Source region analyses suggest that air masses from intensive agricultural regions to the south contribute most to the high NH3 concentrations in Beijing. Local sources such as traffic emissions also appear to be important contributors to atmospheric NH3 in this urban environment.

The implementation of strict emission control measures in Beijing and surrounding regions during the 2015 China Victory Day Parade provided a valuable opportunity to investigate related air quality improvements in a megacity. We measured NH3, NO2 and PM2.5 at multiple sites in and outside Beijing and summarized concentrations of PM2.5, PM10, NO2, SO2 and CO in 291 cities across China from a national urban air quality monitoring network between August and September 2015. Consistently significant reductions of 12–35 % for NH3 and 33–59 % for NO2 in different areas of Beijing during the emission control period (referred to as the Parade Blue period) were observed compared with measurements in the pre- and post-Parade Blue periods without emission controls. Average NH3 and NO2 concentrations at sites near traffic were strongly correlated and showed positive and significant responses to traffic reduction measures, suggesting that traffic is an important source of both NH3 and NOx in urban Beijing. Daily concentrations of PM2.5 and secondary inorganic aerosol (sulfate, ammonium and nitrate) at the urban and rural sites both decreased during the Parade Blue period. During (after) the emission control period, concentrations of PM2.5, PM10, NO2, SO2 and CO from the national city-monitoring network showed the largest decrease (increase) of 34–72 % (50–214 %) in Beijing, a smaller decrease (a moderate increase) of 1–32 % (16–44 %) in emission control regions outside Beijing and an increase (decrease) of 6–16 % (−2–7 %) in non-emission-control regions of China. Integrated analysis of modelling and monitoring results demonstrated that emission control measures made a major contribution to air quality improvement in Beijing compared with a minor contribution from favourable meteorological conditions during the Parade Blue period. These results show that controls of secondary aerosol precursors (NH3, SO2 and NOx) locally and regionally are key to curbing air pollution in Beijing and probably in other mega cities worldwide.

Air pollution is one of the most serious environmental problems in China due to its rapid economic development alongside a very large consumption of fossil fuel, particularly in the North China Plain (NCP). During the period 2011–2014, we integrated active and passive sampling methods to perform continuous measurements of NH3, HNO3, NO2, and PM2.5 at two urban, one suburban, and two rural sites in the NCP. The annual average concentrations of NH3, NO2, and HNO3 across the five sites were in the ranges 8.5–23.0, 22.2–50.5, and 5.5–9.7 μg m−3, respectively, showing no significant spatial differences for NH3 and HNO3 but significantly higher NO2 concentration at the urban sites. At each site, annual average concentrations of NH3 and NO2 showed increasing and decreasing trends, respectively, while there was no obvious trend in annual HNO3 concentrations. Daily PM2.5 concentrations ranged from 11.8 to 621.0 μg m−3 at the urban site, from 19.8 to 692.9 μg m−3 at the suburban site, and from 23.9 to 754.5 μg m−3 at the two rural sites, with more than 70 % of sampling days exceeding 75 μg m−3. Concentrations of water-soluble ions in PM2.5 ranked differently between the non-rural and rural sites. The three dominant ions were NH4+, NO3−, and SO42− and mainly existed as (NH4)2SO4, NH4HSO4, and NH4NO3, and their concentrations averaged 48.6 ± 44.9, 41.2 ± 40.8, and 49.6 ± 35.9 μg m−3 at the urban, suburban, and rural sites, respectively. Ion balance calculations indicated that PM2.5 was neutral at the non-rural sites but acidic at the rural sites. Seasonal variations of the gases and aerosols exhibited different patterns, depending on source emission strength and meteorological conditions. Our results suggest that a feasible pathway to control PM2.5 pollution in the NCP should target ammonia and acid gases together. Electronic supplementary material The online version of this article (doi:10.1007/s11356-015-5648-3) contains supplementary material, which is available to authorized users.

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.