Atmospheric NH3 Research Articles

Characterization of greenhouse gas emissions and stable isotopic composition of ammonia during industrial composting process

Carbon dioxide (CO2), nitrous oxide (N2O), methane (CH4) and ammonia (NH3) emitted during the composting of livestock and poultry waste are important gaseous atmospheric pollutants. However, most previous studies on compost-related anthropogenic emissions of these gases were based on small reactor composting. Our understanding of their in situ emissions during industrial composting remains extremely limited. In order to explore the influence of gas produced by industrial composting on regional environment, we monitored CO2, CH4, N2O and NH3 emissions during industrial composting for 19 days and characterized the isotopic composition of emitted NH3. On average, the emission rates of CO2, CH4, N2O, and NH3 during the composting cycle were 86.8 g CO2-C·d-1·m-2, 9.8 g CH4-C·d-1·m-2, 3.7 mg N2O-N·d-1·m-2 and 736.6 mg NH3-N·d-1·m-2, respectively. The contribution of CH4 to daily global warming potential (GWP) was the highest (65%), followed by CO2, NH3(indirect), and N2O. Moreover, ammonia emitted from industrial compost had a mean δ15N value of -11.6‰±1.2‰ (range: -21.8‰--7.2‰). Overall, this study provided useful information for understanding greenhouse gas emission dynamics and characterizing atmospheric NH3 sources during composting process in livestock and poultry breeding areas.

On-road tailpipe characterization of exhaust ammonia emissions from in-use light-duty gasoline motor vehicles

A Portable Emissions Monitoring System (PEMS) has been used to estimate ammonia emission rates from a representative fleet of 47 in-use light-duty gasoline motor vehicles over 145 on-road Real Driving Emissions (RDE) tests. The PEMS modules were carried onboard the tested vehicles and were wired such that their ceramic exhaust emission sensors were mounted directly in the tailpipe. The on-road RDE tests were conducted over an urban testing route that included residential and highway roads, uphill and downhill road segments, stop signs, traffic lights, and a school zone with a reduced speed limit. The entire vehicle test sample had an average ammonia emission rate of 114.7 mg/mile ±135.3 (StD). This would yield an estimated 2909 metric tons per year of NH3 emissions from the Wasatch fleet on-road gasoline motor vehicles. Old vehicles with aged Three-Way Catalyst (TWC) converters had higher NH3 emissions rates than newer vehicles with newer TWC converters. For instance, Tier 0, Tier I, NLEV, Tier II and Tier III vehicles had average emission rates of 563.1, 177.8, 213.6, 94.4 and 18.9 mg/mile, respectively. Carbon monoxide, and nitrogen oxides had a strong correlation with ammonia emission rates, with r ≥ 0.70. A Moderate correlation was found with vehicles’ mileage (r = 0.6), model year (r = −0.5), engine displacement (r = 0.4), and number of cylinders (r = 0.4). The outcomes highlight vehicle contributions to the atmospheric NH3 inventory and the impact of vehicle characteristics and ammonia precursor concentrations on ammonia emission rates from gasoline vehicles.

Air pollution monitoring: development of ammonia (NH<sub>3</sub>) dynamic reference gas mixtures at nanomoles per mole levels to improve the lack of traceability of measurements

Abstract. The measurement of ammonia (NH3) in ambient air is a sensitive and priority topic due to its impact on ecosystems. NH3 emissions have continuously increased over the last century in Europe because of intensive livestock practices and the enhanced use of nitrogen-based fertilizers. European air quality monitoring networks monitor atmospheric NH3 amount-of-substance fractions. However, the lack of stable reference gas mixtures (RGMs) of atmospheric amount-of-substance fractions of ammonia to calibrate NH3 analyzers is a common issue of the networks, which results in data that are not accurate, traceable, or, thus, geographically comparable. In order to cover this lack, LNE (Laboratoire National de Métrologie et d'Essais) developed, in close collaboration with the company 2M PROCESS, a gas reference generator to dynamically generate NH3 RGMs in air. The method is based on gas permeation and a further dynamic dilution to obtain an amount-of-substance fractions ranging between 1 and 400 nmol mol−1 (also well known as ppb or parts per billion; 1 ppb (NH3) to ≈ 0.7 µg m−3) to cover the amount-of-substance fractions of ammonia measured in ambient air (emissions) and the operating range of the NH3 analyzers used by the monitoring networks. The calibration of the elements of the generator against the LNE primary standards ensures the traceability of the RGMs to the international system of units. Furthermore, the highly accurate flow and oven temperature measurements of the reference generator, together with the associated calibration procedure defined by LNE, guarantee relative expanded uncertainties of the calibration of the NH3 analyzers that are lower than 2 % (coverage factor = 2). This result is very satisfactory, considering the low NH3 amount-of-substance fraction levels (1 to 400 nmol mol−1) and the phenomena of adsorption and desorption, especially in the presence of traces of water on contact surfaces. A bilateral comparison was organized between METAS (Swiss Federal Institute of Metrology) and LNE, which consisted of the calibration of a Picarro G2103 gas analyzer by both national metrology institutes (NMIs). The results highlighted the good agreement between the NH3 reference generators developed by the two institutes and allowed the validation of both LNE's reference generator and calibration procedure. Since the end of 2020, LNE has calibrated several NH3 analyzers from the French air quality monitoring networks (Associations Agréées de Surveillance de la Qualité de l'Air – AASQA) using the newly developed SI-traceable RGMs. The enhanced number of calibrations provided may increase the comparability, accuracy, and traceability of the NH3 measurements carried out on French territory.

Competitive Uptake of Dimethylamine and Trimethylamine against Ammonia on Acidic Particles in Marine Atmospheres.

Alkaline gases such as NH3 and amines play important roles in neutralizing acidic particles in the atmosphere. Here, two common gaseous amines (dimethylamine (DMA) and trimethylamine (TMA)), NH3, and their corresponding ions in PM2.5 were measured semicontinuously using an ambient ion monitor-ion chromatography (AIM-IC) system in marine air during a round-trip cruise of approximately 4000 km along the coastline of eastern China. The concentrations of particulate DMA, detected as DMAH+, varied from <4 to 100 ng m-3 and generally decreased with increasing atmospheric NH3 concentrations. Combining observations with thermodynamic equilibrium calculations using the extended aerosol inorganics model (E-AIM) indicated that the competitive uptake of DMA against NH3 on acidic aerosols generally followed thermodynamic equilibria and appeared to be sensitive to DMA/NH3 molar ratios, resulting in molar ratios of DMAH+ to DMA + DMAH+ of 0.31 ± 0.16 (average ± standard deviation) at atmospheric NH3 concentrations over 1.8 μg m-3 (with a corresponding DMA/NH3 ratio of (1.8 ± 1.0) × 10-3), 0.80 ± 0.15 at atmospheric NH3 concentrations below 0.3 μg m-3 (with a corresponding DMA/NH3 ratio of (1.3 ± 0.6) × 10-2), and 0.56 ± 0.19 in the remaining cases. Particulate TMA concentrations, detected as TMAH+, ranged from <2 to 21 ng m-3 and decreased with increasing concentrations of atmospheric NH3. However, TMAH+ was depleted concurrently with the formation of NH4NO3 under low concentrations of atmospheric NH3, contradictory to the calculated increase in the equilibrated concentration of TMAH+ by the E-AIM.

Robust Evidence of 14C, 13C, and 15N Analyses Indicating Fossil Fuel Sources for Total Carbon and Ammonium in Fine Aerosols in Seoul Megacity.

Carbon- and nitrogen-containing aerosols are ubiquitous in urban atmospheres and play important roles in air quality and climate change. We determined the 14C fraction modern (fM) and δ13C of total carbon (TC) and δ15N of NH4+ in the PM2.5 collected in Seoul megacity during April 2018 to December 2019. The seasonal mean δ13C values were similar to −25.1‰ ± 2.0‰ in warm and −24.2‰ ± 0.82‰ in cold seasons. Mean δ15N values were higher in warm (16.4‰ ± 2.8‰) than in cold seasons (4.0‰ ± 6.1‰), highlighting the temperature effects on atmospheric NH3 levels and phase-equilibrium isotopic exchange during the conversion of NH3 to NH4+. While 37% ± 10% of TC was apportioned to fossil-fuel sources on the basis of fM values, δ15N indicated a higher contribution of emissions from vehicle exhausts and electricity generating units (power-plant NH3 slip) to NH3: 60% ± 26% in warm season and 66% ± 22% in cold season, based on a Bayesian isotope-mixing model. The collective evidence of multiple isotope analysis reasonably supports the major contribution of fossil-fuel-combustion sources to NH4+, in conjunction with TC, and an increased contribution from vehicle emissions during the severe PM2.5 pollution episodes. These findings demonstrate the efficacy of a multiple-isotope approach in providing better insight into the major sources of PM2.5 in the urban atmosphere.

Evaluation of interactive and prescribed agricultural ammonia emissions for simulating atmospheric composition in CAM-chem

Abstract. Ammonia (NH3) plays a central role in the chemistry of inorganic secondary aerosols in the atmosphere. The largest emission sector for NH3 is agriculture, where NH3 is volatilized from livestock wastes and fertilized soils. Although the NH3 volatilization from soils is driven by the soil temperature and moisture, many atmospheric chemistry models prescribe the emission using yearly emission inventories and climatological seasonal variations. Here we evaluate an alternative approach where the NH3 emissions from agriculture are simulated interactively using the process model FANv2 (Flow of Agricultural Nitrogen, version 2) coupled to the Community Atmospheric Model with Chemistry (CAM-chem). We run a set of 6-year global simulations using the NH3 emission from FANv2 and three global emission inventories (EDGAR, CEDS and HTAP) and evaluate the model performance using a global set of multi-component (atmospheric NH3 and NH4+, and NH4+ wet deposition) in situ observations. Over East Asia, Europe and North America, the simulations with different emissions perform similarly when compared with the observed geographical patterns. The seasonal distributions of NH3 emissions differ between the inventories, and the comparison to observations suggests that both FANv2 and the inventories would benefit from more realistic timing of fertilizer applications. The largest differences between the simulations occur over data-scarce regions. In Africa, the emissions simulated by FANv2 are 200 %–300 % higher than in the inventories, and the available in situ observations from western and central Africa, as well as NH3 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument, are consistent with the higher NH3 emissions as simulated by FANv2. Overall, in simulating ammonia and ammonium concentrations over regions with detailed regional emission inventories, the inventories based on these details (HTAP, CEDS) capture the atmospheric concentrations and their seasonal variability the best. However these inventories cannot capture the impact of meteorological variability on the emissions, nor can these inventories couple the emissions to the biogeochemical cycles and their changes with climate drivers. Finally, we show with sensitivity experiments that the simulated time-averaged nitrate concentration in air is sensitive to the temporal resolution of the NH3 emissions. Over the CASTNET monitoring network covering the US, resolving the NH3 emissions hourly instead monthly reduced the positive model bias from approximately 80 % to 60 % of the observed yearly mean nitrate concentration. This suggests that some of the commonly reported overestimation of aerosol nitrate over the US may be related to unresolved temporal variability in the NH3 emissions.

Emission Characteristics, Transformation Mechanism, and Reduction Potential of Ammonia Emissions from a Crop Rotation System in Yangtze River Delta

To study the characteristics and reduction potential of the ammonia emissions of a crop rotation system in the Yangtze River Delta, we monitored and compared the ammonia fluxes from two rotation systems:a conventional rice/winter wheat rotation system and a rice-shrimp cultivation/Chinese milk vetch rotation system. This study was conducted through closing chamber methods to investigate the influencing factors and transformation mechanism of ammonium emissions between the two studied cultivation patterns. Additionally, we established the temporal-spatial emission inventory by sorting out the local ammonia emission factors of farmland in the Yangtze River Delta in the last ten years. The emission reduction effects under different ammonia emission reduction paths were also obtained. The results showed that, the cumulative amount of ammonia emissions throughout the whole monitoring year for the conventional rice/winter wheat rotation system (CR-W) and the rice-shrimp cultivation/Chinese milk vetch rotation system (RS-C) were 65.95 and 20.31 kg·hm-2, respectively, whereas the ammonia loss rates of CR-W and RS-C were 10.86% and 9.20%, respectively. Field surface water NH4+-N, field surface water pH, and topsoil NH4+-N were the major internal factors of ammonia emissions from paddy fields, whereas topsoil NH4+-N and atmospheric temperature had an important impact on ammonia emissions in the wheat season. The ammonia flux/field NH4+-N ratio (ARN) of field surface water under the CR and RS modes in the rice season reached 0.35±0.27 and 0.14±0.19, respectively, which was 10-25 times that of topsoil in the wheat season, such that the ammonia emission flux in the rice season was significantly higher than that in the wheat season. Under the conditions of high field water pH (8.0-9.0), atmospheric temperature (>28℃), and wind speed (>5.0 m·s-1), the ammonia flux/field NH4+-N ratios (ARN) were around 1.6-4.6 times that under low pH, temperature, and wind speed conditions, indicating that those three factors were the main factors affecting the conversion of NH4+-N from farmland to atmospheric NH3. Fertilization types also had significant effects on ARN; under different conditions, the ARN of urea was 1.5-5.5 times that of organic fertilizer. In 2019, the ammonia emission flux of rice and wheat under a conventional planting pattern in the Yangtze River Delta were (49.2±17.6) kg·hm-2 and (16.0±13.5) kg·hm-2, respectively, whereas the ammonia loss rates of rice and wheat were (20.1±5.7)% and (5.9±3.6)%, respectively. The ammonia emission loss rate of the former was about three times that of the latter. The ammonia emission inventory built by local factors shows that the total ammonia emissions of the farmland rotation system in the Yangtze River Delta reached (400.3±206.4) kt in 2019, which was mainly concentrated in the central and northern regions of Anhui province and Jiangsu province, and the ammonia emission intensity reached (1.33±1.39) t·km-2. The selection of different emission factors had a relatively large impact on the change range of the inventory results, reaching the standard of -51.6%~51.6%. Through combing and analyzing the six main paths of ammonia emission reduction in farmland, it was found that nitrogen fertilizer synergism was the best way to reduce ammonia emissions, with the efficiency of (30.9±51.4)%; however, the grain yield increase rate was (-4.2±17.4)%, with great uncertainty. The ammonia emission reduction effect of adding soil additives was relatively poor (-5.4±45.1)%; however, the grain yield increase rate was the highest among those of the six emission reduction paths, reaching (6.8±23.9)%. The ammonia emission reduction effect and grain yield increase rate of the ecological planting and breeding mode were (22.3±15.1)% and (5.6±3.8)%, respectively, which had the advantages of reducing ammonia emissions and increasing crop yield.

Parallel plate wet denuder coupled ammonia transfer device-conductivity detector for near-real-time monitoring of gaseous ammonia

Gaseous ammonia (NH3) is a primary basic substance in the atmosphere, and its global emission has been increasing in recent decades. It is vital to continuously monitor the atmospheric NH3 to clarify the impact of NH3 on sensitive ecosystems. This paper proposes a simple gaseous NH3 monitor utilizing a parallel plate wet denuder (PPWD) and a conductometric flow injection analysis (FIA) with an ammonia transfer device (ATD). In the present study, water-soluble basic gases, NH3, are selectively detected by the conductivity detector (CD). The ATD-CD ammonium detector requires no coloring reagents commonly used in FIA. Five-day field measurement of ambient NH3 was successfully performed with 30 min time resolution. All the air samples over the observation period (n = 186) contained NH3 above the limit of quantification (11.4 nmol m−3). The NH3 data showed excellent agreement with the values using ion chromatography in the field measurements.

Overlooked Nonagricultural and Wintertime Agricultural NH3 Emissions in Quzhou County, North China Plain: Evidence from 15N-Stable Isotopes

Ammonia (NH3) plays a critical role in atmospheric chemistry and can exacerbate haze formation. Agricultural emissions have been known as a primary source of global atmospheric NH3. However, with accelerating urbanization and optimized agricultural production, the dominance of agricultural emissions has become less clear. We investigated the contributions of nonagricultural and agricultural sources to atmospheric NH3 based on measurements of NH3 isotopes at nine sites in Quzhou County, a typical agricultural county in the North China Plain. We found that Quzhou had extremely high NH3 concentrations (annual average across all sites of 40.3 ± 3.3 μg m–3). We compared the sources of seasonal NH3 contributions in rural and urban areas through 15N-stable isotope analyses, which provides new insights into NH3 sources compared with the traditional emission inventories. In rural areas, agricultural sources (fertilizer application and livestock production) make significant contributions (56 ± 3%) to NH3 emissions in the winter, whereas there were larger contributions of nonagricultural sources [fossil fuel, waste, and biomass burning (56 ± 2%)] relative to agricultural sources in urban areas. More effective strategies are still needed for better manure management and vegetable/fruit production in the winter and for controlling nonagricultural sources, even in counties dominated by agriculture.

Data assimilation of CrIS NH&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; satellite observations for improving spatiotemporal NH&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; distributions in LOTOS-EUROS

Abstract. Atmospheric levels of ammonia (NH3) have substantially increased during the last century, posing a hazard to both human health and environmental quality. The atmospheric budget of NH3, however, is still highly uncertain due to an overall lack of observations. Satellite observations of atmospheric NH3 may help us in the current observational and knowledge gaps. Recent observations of the Cross-track Infrared Sounder (CrIS) provide us with daily, global distributions of NH3. In this study, the CrIS NH3 product is assimilated into the LOTOS-EUROS chemistry transport model using two different methods aimed at improving the modeled spatiotemporal NH3 distributions. In the first method NH3 surface concentrations from CrIS are used to fit spatially varying NH3 emission time factors to redistribute model input NH3 emissions over the year. The second method uses the CrIS NH3 profile to adjust the NH3 emissions using a local ensemble transform Kalman filter (LETKF) in a top-down approach. The two methods are tested separately and combined, focusing on a region in western Europe (Germany, Belgium and the Netherlands). In this region, the mean CrIS NH3 total columns were up to a factor 2 higher than the simulated NH3 columns between 2014 and 2018, which, after assimilating the CrIS NH3 columns using the LETKF algorithm, led to an increase in the total NH3 emissions of up to approximately 30 %. Our results illustrate that CrIS NH3 observations can be used successfully to estimate spatially variable NH3 time factors and improve NH3 emission distributions temporally, especially in spring (March to May). Moreover, the use of the CrIS-based NH3 time factors resulted in an improved comparison with the onset and duration of the NH3 spring peak observed at observation sites at hourly resolution in the Netherlands. Assimilation of the CrIS NH3 columns with the LETKF algorithm is mainly advantageous for improving the spatial concentration distribution of the modeled NH3 fields. Compared to in situ observations, a combination of both methods led to the most significant improvements in modeled monthly NH3 surface concentration and NH4+ wet deposition fields, illustrating the usefulness of the CrIS NH3 products to improve the temporal representativity of the model and better constrain the budget in agricultural areas.

Contributions of Ammonia to High Concentrations of PM2.5 in an Urban Area

Atmospheric ammonia (NH3) plays a critical role in PM2.5 pollution. Data on atmospheric NH3 are scanty; thus, the role of NH3 in the formation of ammonium ions (NH4+) in various environments is understudied. Herein, we measured concentrations of NH3, PM2.5, and its water-soluble SO42−, NO3−, and NH4+ ions (SNA) at an urban site in Jeonju, South Korea from May 2019 to April 2020. During the measurement period, the average concentrations of NH3 and PM2.5 were 10.5 ± 4.8 ppb and 24.0 ± 12.8 μg/m3, respectively, and SNA amounted to 4.3 ± 3.1, 4.4 ± 4.9, and 1.6 ± 1.8 μg/m3, respectively. A three-dimensional photochemical model analysis revealed that a major portion of NH3, more than 88%, originated from Korea. The enhancement of the ammonium-to-total ratio of NH3, NHX (NHR = [NH4+]/[NH4+] + [NH3]) was observed up to ~0.61 during the increase of PM2.5 concentration (PM2.5 ≥ 25 μg/m3) under low temperature and high relative humidity conditions, particularly in winter. The PM2.5 and SNA concentrations increased exponentially as NHR increased, indicating that NH3 contributed significantly to SNA formation by gas-to-particle conversion. Our study provided experimental evidence that atmospheric NH3 in the urban area significantly contributed to SNA formation through gas-to-particle conversion during PM2.5 pollution episodes.

Interannual variation of reactive nitrogen emissions and their impacts on PM2.5 air pollution in China during 2005–2015

Emissions of reactive nitrogen as ammonia (NH3) and nitrogen oxides (NO x ), together with sulfur dioxide (SO2), contribute to formation of secondary PM2.5 in the atmosphere. Satellite observations of atmospheric NH3, NO2, and SO2 levels since the 2000s provide valuable information to constrain the spatial and temporal variability of their emissions. Here we present a bottom-up Chinese NH3 emission inventory combined with top-down estimates of Chinese NO x and SO2 emissions using ozone monitoring instrument satellite observations, aiming to quantify the interannual variations of reactive nitrogen emissions in China and their contributions to PM2.5 air pollution over 2005–2015. We find small interannual changes in the total Chinese anthropogenic NH3 emissions during 2005–2016 (12.0–13.3 Tg with over 85% from agricultural sources), but large interannual change in top-down Chinese NO x and SO2 emissions. Chinese NO x emissions peaked around 2011 and declined by 22% during 2011–2015, and Chinese SO2 emissions declined by 55% in 2015 relative to that in 2007. Using the GEOS-Chem chemical transport model simulations, we find that rising atmospheric NH3 levels in eastern China since 2011 as observed by infrared atmospheric sounding interferometer and atmospheric infrared sounder satellites are mainly driven by rapid reductions in SO2 emissions. The 2011–2015 Chinese NO x emission reductions have decreased regional annual mean PM2.5 by 2.3–3.8 μg m−3. Interannual PM2.5 changes due to NH3 emission changes are relatively small, but further control of agricultural NH3 emissions can be effective for PM2.5 pollution mitigation in eastern China.

Changes in biomass burning, wetland extent, or agriculture drive atmospheric NH&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; trends in select African regions

Abstract. Atmospheric ammonia (NH3) is a precursor to fine particulate matter and a source of nitrogen (N) deposition that can adversely affect ecosystem health. The main sources of NH3 – agriculture and biomass burning – are undergoing are or expected to undergo substantial changes in Africa. Although evidence of increasing NH3 over parts of Africa has been observed, the mechanisms behind these trends are not well understood. Here we use observations of atmospheric NH3 vertical column densities (VCDs) from the Infrared Atmospheric Sounding Interferometer (IASI) along with other satellite observations of the land surface and atmosphere to evaluate how NH3 concentrations have changed over Africa from 2008 through 2018, and what has caused those changes. In West Africa NH3 VCDs are observed to increase during the late dry season, with increases of over 6 % yr−1 in Nigeria during February and March (p&lt;0.01). These positive trends are associated with increasing burned area and CO trends during these months, likely related to agricultural preparation. Increases are also observed in the Lake Victoria basin region, where they are associated with expanding agricultural area. In contrast, NH3 VCDs declined over the Sudd wetlands in South Sudan by over 1.5 % yr−1, though not significantly (p=0.28). Annual maxima in NH3 VCDs in South Sudan occur during February through May and are associated with the drying of temporarily flooded wetland soils, which favor emissions of NH3. The change in mean NH3 VCDs over the Sudd is strongly correlated with variation in wetland extent in the Sudd: in years when more area remained flooded during the dry season, NH3 VCDs were lower (r=0.64, p&lt;0.05). Relationships between biomass burning and NH3 may be observed when evaluating national-scale statistics: countries with the highest rates of increasing NH3 VCDs also had high rates of growth in CO VCDs; burned area displayed a similar pattern, though not significantly. Livestock numbers were also higher in countries with intermediate or high rates of NH3 VCD growth. Fertilizer use in Africa is currently low but growing; implementing practices that can limit NH3 losses from fertilizer as agriculture is intensified may help mitigate impacts on health and ecosystems.

Atmospheric NH3 Emission Inventory and Analysis of the Driving Force in Zhengzhou City

In this study, a 2017-based emission inventory of ammonia(NH3) was established for Zhengzhou by using the emission factor method. The 1 km×1 km gridded emission inventory was mapped using GIS technology. The NH3 emissions between 2007 and 2017 and driving force between 1989 and 2017 were also analyzed. Results showed that the total 2017-based NH3 emission in Zhengzhou was 18143.3 t, and the average emission intensity reached 2.4 t·km-2. The top emission source was from agriculture, accounting for 63.4% of the total emission, followed by fugacity(11.3%). The main contribution sources of livestock were egg poultry, pigs, and cattle. Dengfeng, Xingyang, and Xinmi had the highest emissions, accounting for 19.3%, 16.5%, and 15.6% of the total emission, respectively. The NH3 emission was higher in the southern and central western regions of Zhengzhou and lower in the northeastern region. The NH3 emission in Zhengzhou showed a downward trend from 2007 to 2017. The NH3 emissions from 1987 to 2017 were similar to the environmental Kuznets Curve, i.e., the emissions increased first and then decreased with the increase of per capita gross domestic product(GDP) and urbanization rate.

A space view of agricultural and industrial changes during the Syrian civil war

The agricultural sector in Syria was heavily affected by the civil war that started in 2011. We investigate the war’s impact on the country’s atmospheric ammonia (NH3) from 2008 to 2019, using measurements from the infrared atmospheric sounding interferometer instrument on board the Metop satellites. We examine the changes in NH3 close to a fertilizer industry, whose activities were suspended due to conflict-related events. We also explore the effect of war-induced land use/land cover changes on agriculture-emitted ammonia in north-east Syria that has witnessed battles between different groups. The interpretation of the changes in NH3 is supported by different datasets: visible satellite imagery to assess the effect on industrial activity, reanalysis data from the European center for medium-range weather forecasts to look at the effect of meteorology (temperature, wind speed, and precipitation), and land cover and burned area products from the moderate resolution imaging spectroradiometer (MODIS) to examine land use/land cover changes and fire events during the study period. We show that the NH3 columns are directly affected by the war. Periods of intense conflict are reflected in lower values over the industry reaching –17%, –47%, and –32% in 2013, 2014, and 2016, respectively, compared to the [2008–2012] average, and a decrease reaching –14% and –15% in the croplands’ area in northeast Syria during 2017 and 2018 (compared to 2011), respectively. Toward the end of the control of Islamic State in Iraq and Syria, an increase in atmospheric NH3 was accompanied by an increase in croplands’ area that reached up to +35% in 2019 as compared to prewar (2011). This study shows the relevance of remote-sensing data of atmospheric composition in studying societal changes at a local and regional scale.

Spatial Distributions of Atmospheric Ammonia in a Rural Area in South Korea and the Associated Impact on a Nearby Urban Area

Ammonia (NH3) plays an important role in air quality and atmospheric chemistry, yet studies on the characteristics and impacts of NH3 are limited. Herein, we revealed the spatial distribution of atmospheric NH3, as measured by passive samplers, at three different sites (R1, R2, and R3) in the rural area (livestock environment) of Jeongeup, South Korea, from September 2019 to August 2020. At site R1, the boundary of a large-scale pig farm, dramatically high daily mean concentrations of NH3 were observed (118.7 ppb), whereas sites R2 and R3, located ~1 km from R1, exhibited lower concentrations of 18.2 and 30.4 ppb, respectively. In the rural environment, the monthly NH3 variations showed a peak in June (34.2 ppb), which was significantly higher than in the urban and remote areas. To examine the impact of NH3 from the rural area on a nearby urban area in June 2020, simultaneous measurements were performed using a real-time instrument in Jeonju. When high NH3 events occurred in the urban area in June, the results for the NH3 concentrations and observed meteorological conditions in the rural and urban areas showed that the rural area influenced the NH3 levels in the adjacent urban area.

Improved gridded ammonia emission inventory in China

Abstract. As a major alkaline gas in the atmosphere, NH3 significantly impacts atmospheric chemistry, ecological environment, and biodiversity. Gridded NH3 emission inventories can significantly affect the accuracy of model concentrations and play a crucial role in the refinement of mitigation strategies. However, several uncertainties are still associated with existing NH3 emission inventories in China. Therefore, in this study, we focused on improving fertilizer-application-related NH3 emission inventories. We comprehensively evaluated the dates and times of fertilizer application to the major crops that are cultivated in China, improved the spatial allocation methods for NH3 emissions from croplands with different rice types, and established a gridded NH3 emission inventory for mainland China with a resolution of 5 min × 5 min in 2016. The results showed that the atmospheric NH3 emissions in mainland China amounted to 12.11 Tg, with livestock waste (44.8 %) and fertilizer application (38.6 %) being the two main NH3 emission sources in China. Obvious spatial variability in NH3 emissions was also identified, and high emissions were predominantly concentrated in North China. Further, NH3 emissions tended to be high in summer and low in winter, and the ratio for the July–January period was 3.08. Furthermore, maize and rice fertilization in summer was primarily responsible for the increase in NH3 emissions in China, and the evaluation of the spatial and temporal accuracy of the NH3 emission inventory established in this study using the WRF-Chem and ground-station- and satellite-based observations showed that it was more accurate than other inventories.

Satellite-Based Analysis of Spatial–Temporal Distributions of NH3 and Factors of Influence in North China

NH3 is an important part of the global nitrogen cycle as the most important atmospheric alkaline gas. NH3 reacts rapidly with acidic substances and accelerates the generation of particulate matter (PM2.5), which has important effects on the atmosphere and climate change. In this study, satellite NH3 column data were used to analyze spatial and temporal distributions of NH3 in China, and because of high concentrations and rates of change, North China was selected for more detailed analysis. Qualitative analysis was conducted to understand the relations between concentrations of NH3 and those of SO2 and NO2. Last, the random forest method was used to quantify relations between concentrations of atmospheric NH3 and factors influencing those concentrations, such as meteorological factors, NH3 self-emission, and concentrations of SO2 and NO2. Satellite-retrieved NH3 column concentrations showed an increasing trend during the 11 years from 2008 to 2018, and the rate of increase in summer was faster than that in winter. In those 11 years, NH3 self-emission had the greatest influence on NH3 concentrations. Concentrations of SO2 and NO2 had some effect and were negatively correlated with NH3 concentrations. The effect of SO2 on NH3 concentration was greater than that of NO2. Atmospheric NH3 concentration was also affected by meteorological conditions (temperature, relative humidity, pressure, and wind). In summer, temperature is the most important factors of meteorological conditions and relative humidity is the most important factors in winter. Therefore, to better control atmospheric NH3 concentrations, it is particularly important to formulate practical NH3 emission reduction policies and to consider the effects of SO2 and NO2 emission reduction policies.

Significant decrease in SO2 emission and enhanced atmospheric oxidation trigger changes in sulfate formation pathways in China during 2008–2016

Understanding the changes in the sulfate (SO42−) formation pathway is important to further control particle pollution owing to the significant reduction of SO2 emission and enhanced atmospheric oxidation. This study applied the Community Multiscale Air Quality (CMAQ) model coupled with the sulfur tracking model (STM) to quantify sources of atmospheric SO42− in China and their changes during 2008–2016. The results showed that the surface SO42− concentration decreased by 51.1%, 40.8%, 37.5%, and 36.2% for Beijing–Tianjin–Hebei (BTH), Yangtze River Delta (YRD), Pearl River Delta (PRD), and Sichuan Basin (SCB), respectively. In addition, the SO42− formation pathways also changed in a sustained manner. The gas-phase reaction of SO2 with OH (SO4_GAS) and the reaction catalyzed by Fe3+ and Mn2+ (SO4_FEMN) decreased significantly (63.4% and 61.7%), whereas the aqueous-phase reaction of SO2 with O3 (SO4_O3) increased by 39.9% from 2008 to 2016. Primary SO42− emission (SO4_EMIS) played an important role in autumn and winter with over 30% contribution, whereas SO4_GAS and the aqueous-phase reaction of SO2 with H2O2 (SO4_H2O2) dominated in spring and summer, respectively. The sensitivity simulation results showed that sharp SO2 reduction significantly decreased SO4_GAS (over 60%); however, it was less sensitive to SO4_O3 (8%–11%). In addition, the SO2 emission reduction resulted in a large increase in atmospheric NH3 concentrations due to less neutralization reaction, thus increasing NO3− concentration in some regions. These results suggest that multi-pollutants control for SO2-NOx-VOC should be implemented to prevent the enhanced atmospheric oxidation furtherly deteriorating secondary air pollution, particularly in spring and summer. In addition, limiting primary emissions from residential combustion in winter is important to achieve coordinated control of SO2 and SO42− in northern China.

Selective photocatalytic oxidation of gaseous ammonia at ppb level over Pt and F modified TiO2

Ammonia (NH3) as an important precursor to form atmospheric fine particles and secondary inorganic aerosols, should be strictly controlled. Photocatalysis has provided a facile and an effective way to eliminate NH3 pollution under mild conditions, whereas the undesirable products, such as NO, NO2 would be generated during the reaction and the mechanism remains unclear. In this study, F or Pt modified TiO2 were explored to reduce the formation of NOx during photocatalytic oxidation of low-concentration NH3, and its photocatalytic activity, selectivity and mechanism of NH3 conversion were systematically studied. Results indicate that surface fluorination on TiO2 contribute to the reduction of noxious NOx, especially for NO2, since the modified TiO2 achieved enhanced adsorption of NH3 and strong electron-trapping ability, which can retard the recombination of photo-generated electrons and holes. In addition, the deposition of Pt could further extend the lifetime of the electron-hole pairs by strongly capture the electron, and enhance the oxidation of NH3 into nitrates and nitrites species. From the in-situ DRIFT spectroscopy and XPS results, we can deduce that reactive amino radical (•NH2) would be formed on TiO2 under photoirradiation after the adsorption of NH3 on Lewis acid cites. The formed •NH2 can react with reactive oxygen species in the presence of H2O, and produce NOx and HNOx. By both enhancing the adsorption of NH3 and separation efficiency of electron-hole pairs, the presence of F and Pt modification on the TiO2 changes the photocatalytic pathway of NH3 conversion. The proposed selective oxidation mechanism may offer a novel insight into the photocatalytic oxidation of atmospheric NH3 on other metal oxide with surface modification and can be broadly employed in air pollution control in indoor environments.