Ammonia in a Changing Atmosphere

A special issue of Atmosphere (ISSN 2073-4433). This special issue belongs to the section "Aerosols".

Deadline for manuscript submissions: closed (23 May 2022) | Viewed by 20213

Special Issue Editors

School of Energy and Environment, City University of Hong Kong, Hong Kong, China
Interests: aerosol chemistry, air-sea interaction, organic pollutant lifecycles, biogeochemical cycles
Special Issues, Collections and Topics in MDPI journals
Environmental Science and Engineering, Harvard University, Cambridge, MA 02138, USA
Interests: air pollution; air quality modeling; atmospheric aerosol; atmospheric chemistry; heavy metals; greenhouse gases
School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham B15 2TT, UK
Interests: atmospheric biogeochemistry; air pollution; climate change
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Ammonia is the predominant basic gas in the atmosphere. It is also a major component of total reactive nitrogen. Agriculture activities and biomass burning are the largest global sources of ammonia. However, industrial activities and vehicles are important sources of ammonia in urban areas. Air quality regulations have led to substantial decreases in many traditional air pollutants such as sulfur dioxide and nitrogen oxides, and this trend is expected to continue in the future. In contrast, ammonia emissions have not decreased significantly. Ammonia emissions may even be substantially higher in the future due to increased agriculture activities and biomass burning caused by a growing world population and changing climate. These trends point to ammonia potentially playing an increasingly important role in atmospheric chemistry. In this Special Issue, we invite researchers to submit original research manuscripts on a broad range of laboratory, ambient (field and satellite measurements), and theoretical (fundamental chemistry and atmospheric modeling) studies related to the sources and distributions of ammonia in the atmosphere and how ammonia affects the formation and evolution of aerosols, climate properties and toxicity of aerosols, and nitrogen deposition. Manuscripts addressing topics which will be of interest to a broad audience are encouraged, but more focused studies are also welcomed.

Prof. Dr. Theodora Nah
Dr. Shaojie Song
Prof. Dr. Zongbo Shi
Guest Editors

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Keywords

  • aerosol formation
  • aerosol aging
  • aerosol properties and toxicity
  • laboratory studies
  • field studies
  • satellite measurements
  • modeling studies
  • ammonia and amines
  • nitrogen deposition

Published Papers (8 papers)

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Research

20 pages, 16216 KiB  
Article
Road Traffic and Its Influence on Urban Ammonia Concentrations (France)
by Mélodie Chatain, Eve Chretien, Sabine Crunaire and Emmanuel Jantzem
Atmosphere 2022, 13(7), 1032; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos13071032 - 29 Jun 2022
Cited by 6 | Viewed by 2056
Abstract
Ammonia (NH3) is an unregulated atmospheric gaseous pollutant in ambient air, involved in the formation of fine particles. Ammonia is therefore a major precursor of particulate matter (PM), the health effects of which have been widely demonstrated. NH3 emissions are [...] Read more.
Ammonia (NH3) is an unregulated atmospheric gaseous pollutant in ambient air, involved in the formation of fine particles. Ammonia is therefore a major precursor of particulate matter (PM), the health effects of which have been widely demonstrated. NH3 emissions are clearly dominated by the agricultural sector (livestock and fertilizers), but other sources may also be important and less studied, such as road traffic with the increased use of catalytic converters in vehicles. This study is based on a long-term real-time measurements campaign (December 2019–September 2021) on two urban sites: a background site and a roadside site in the same agglomeration in France. The study of historical measurements at the background site clearly demonstrated the dominance of agriculture on the ammonia concentrations. This influence was also observed at both sites during the measurement campaign. The annual and monthly averages obtained in the study were similar to previous ones, with concentrations between 1–10 µg/m3 at both sites, indicating lower levels than previous studies for the roadside site. The ammonia levels measured during the campaign at the traffic site were significantly higher than those measured at the background site, highlighting the road traffic influence on ammonia in urban area. The biomass burning influence also seemed to be observed during this long measurement campaign at the agglomeration scale. The influences of road traffic and biomass burning on ammonia concentration remain small compared to agriculture. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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13 pages, 1938 KiB  
Article
Seasonal Aerosol Acidity, Liquid Water Content and Their Impact on Fine Urban Aerosol in SE Canada
by Andrea M. Arangio, Pourya Shahpoury, Ewa Dabek-Zlotorzynska and Athanasios Nenes
Atmosphere 2022, 13(7), 1012; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos13071012 - 23 Jun 2022
Cited by 2 | Viewed by 1639
Abstract
This study explores the drivers of aerosol pH and their impact on the inorganic fraction and mass of aerosol in the S.E. Canadian urban environments of Hamilton and Toronto, Ontario. We find that inter-seasonal pH variability is mostly driven by temperature changes, which [...] Read more.
This study explores the drivers of aerosol pH and their impact on the inorganic fraction and mass of aerosol in the S.E. Canadian urban environments of Hamilton and Toronto, Ontario. We find that inter-seasonal pH variability is mostly driven by temperature changes, which cause variations of up to one pH unit. Wintertime acidity is reduced, compared to summertime values. Because of this, the response of aerosol to precursors fundamentally changes between seasons, with a strong sensitivity of aerosol mass to levels of HNO3 in the wintertime. Liquid water content (LWC) fundamentally influences the aerosol sensitivity to NH3 and HNO3 levels. In the summertime, organic aerosol is mostly responsible for the LWC at Toronto, and ammonium sulfate for Hamilton; in the winter, LWC was mostly associated with ammonium nitrate at both sites. The combination of pH and LWC in the two sites also affects N dry deposition flux; NO3 fluxes were comparable between the two sites, but NH3 deposition flux at Toronto is almost twice what was seen in Hamilton; from November to March N deposition flux slows down leading to an accumulation of N as NO3 in the particle phase and an increase in PM2.5 levels. Given the higher aerosol pH in Toronto, aerosol masses at this site are more sensitive to the emission of HNO3 precursors compared to Hamilton. For both sites, NOx emissions should be better regulated to improve air quality during winter; this is specifically important for the Toronto site as it is thermodynamically more sensitive to the emissions of HNO3 precursors. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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13 pages, 2356 KiB  
Article
Continuous Measurement of Ammonia at an Intensive Pig Farm in Wuhan, China
by Kun Feng, Yan Wang, Ronggui Hu and Rongbiao Xiang
Atmosphere 2022, 13(3), 442; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos13030442 - 09 Mar 2022
Cited by 5 | Viewed by 2714
Abstract
Measurements with high time resolution are necessary to capture variation patterns and to facilitate the estimation of uncertainty in ammonia inventories. Continuous real-time monitoring of ammonia was carried out in a naturally ventilated nursery pig house during two periods in winter and summer, [...] Read more.
Measurements with high time resolution are necessary to capture variation patterns and to facilitate the estimation of uncertainty in ammonia inventories. Continuous real-time monitoring of ammonia was carried out in a naturally ventilated nursery pig house during two periods in winter and summer, respectively. A higher ventilation rate of about 73,799 ± 39,655 m3/h was obtained during the summer period in comparison with 1646 ± 604 m3/h in the winter. Correspondingly, ammonia level observed in summer (0.25 ± 0.10 mg/m3) was lower than that in winter (1.28 ± 0.74 mg/m3). Spatial variation of ammonia concentration was observed during the winter monitoring period. The mean ammonia emission factor was about 0.3221 ± 0.2921 g d−1 pig−1 in summer and 0.1039 ± 0.0550 g d−1 pig−1 in winter, ranging from 0.0094 to 1.9422 g d−1 pig−1 and 0.0046 to 0.2899 g d−1 pig−1, respectively. Significant correlation was found between ammonia emission and indoor temperature and relative humidity during the winter period. For the summer measurement, effects of ventilation rate and ammonia concentration on ammonia emission were significant. Prominent diurnal pattern existed for both ammonia concentration and emission, with higher emission rates during daytime. The results confirmed the existence of considerable uncertainty associated with the ammonia emission factor, acquired by snapshot measurements. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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15 pages, 5140 KiB  
Article
Partitioning of NH3-NH4+ in the Southeastern U.S.
by Bin Cheng, Lingjuan Wang-Li, Nicholas Meskhidze, John Classen and Peter Bloomfield
Atmosphere 2021, 12(12), 1681; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos12121681 - 15 Dec 2021
Cited by 2 | Viewed by 2260
Abstract
The formation of inorganic fine particulate matter (i.e., iPM2.5) is controlled by the thermodynamic equilibrium partitioning of NH3-NH4+. To develop effective control strategies of PM2.5, we aim to understand the impacts of changes in [...] Read more.
The formation of inorganic fine particulate matter (i.e., iPM2.5) is controlled by the thermodynamic equilibrium partitioning of NH3-NH4+. To develop effective control strategies of PM2.5, we aim to understand the impacts of changes in different precursor gases on iPM2.5 concentrations and partitioning of NH3-NH4+. To understand partitioning of NH3-NH4+ in the southeastern U.S., responses of iPM2.5 to precursor gases in four seasons were investigated using field measurements of iPM2.5, precursor gases, and meteorological conditions. The ISORROPIA II model was used to examine the effects of changes in total ammonia (gas + aerosol), total sulfuric acid (aerosol), and total nitric acid (gas + aerosol) on iPM2.5 concentrations and partitioning of NH3-NH4+. The results indicate that reduction in total H2SO4 is more effective than reduction in total HNO3 and total NH3 to reduce iPM2.5 especially under NH3-rich condition. The reduction in total H2SO4 may change partitioning of NH3-NH4+ towards gas-phase and may also lead to an increase in NO3 under NH3-rich conditions, which does not necessarily lead to full neutralization of acidic gases (pH < 7). Thus, future reduction in iPM2.5 may necessitate the coordinated reduction in both H2SO4 and HNO3 in the southeastern U.S. It is also found that the response of iPM2.5 to the change in total H2SO4 is more sensitive in summer than winter due to the dominance of SO42− salts in iPM2.5 and the high temperature in summer. The NH3 emissions from Animal Feeding Operations (AFOs) at an agricultural rural site (YRK) had great impacts on partitioning of NH3-NH4+. The Multiple Linear Regression (MLR) model revealed a strong positive correlation between cation-NH4+ and anions-SO42− and NO3. This research provides an insight into iPM2.5 formation mechanism for the advancement of PM2.5 control and regulation in the southeastern U.S. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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15 pages, 7814 KiB  
Article
Contributions of Ammonia to High Concentrations of PM2.5 in an Urban Area
by Junsu Park, Eunhye Kim, Sangmin Oh, Haeri Kim, Soontae Kim, Yong Pyo Kim and Mijung Song
Atmosphere 2021, 12(12), 1676; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos12121676 - 14 Dec 2021
Cited by 10 | Viewed by 3218
Abstract
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 [...] Read more.
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. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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19 pages, 4100 KiB  
Article
Seasonal and Spatial Variations of Atmospheric Ammonia in the Urban and Suburban Environments of Seoul, Korea
by Rahul Singh, Kyunghoon Kim, Gyutae Park, Seokwon Kang, Taehyun Park, Jihee Ban, Siyoung Choi, Jeongin Song, Dong-Gil Yu, Jung-Hun Woo, Yuri Choi and Taehyoung Lee
Atmosphere 2021, 12(12), 1607; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos12121607 - 02 Dec 2021
Cited by 8 | Viewed by 2976
Abstract
Atmospheric ammonia is a significant pollutant throughout the year, necessitating standardized measurement and identification of emission factors. We performed a quantized evaluation of ammonia concentrations at various locations in and around Seoul, South Korea. The established testing methods of the Radiello Passive Sampler [...] Read more.
Atmospheric ammonia is a significant pollutant throughout the year, necessitating standardized measurement and identification of emission factors. We performed a quantized evaluation of ammonia concentrations at various locations in and around Seoul, South Korea. The established testing methods of the Radiello Passive Sampler were used for ammonia sampling, and the method was validated using annular denuder sampling. Urban and suburban areas were studied to gain a deeper understanding of the factors responsible for ammonia pollution. This study aimed to establish the fluctuations in concentration over one year, by analyzing the seasonal and regional variation in ammonia concentration. Livestock and agricultural areas recorded the highest concentration of ammonia among all sites, with the highest concentration recorded in autumn. However, at most of the other studied sites, the highest and lowest ammonia concentrations were recorded during summer and winter, respectively. This study attempted to establish a correlation between ammonia concentration and temperature, as well as ammonia concentration and altitude. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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15 pages, 2569 KiB  
Article
Effect of Humidity on the Reactive Uptake of Ammonia and Dimethylamine by Nitrogen-Containing Secondary Organic Aerosol
by Natalie R. Smith, Julia Montoya-Aguilera, Donald Dabdub and Sergey A. Nizkorodov
Atmosphere 2021, 12(11), 1502; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos12111502 - 15 Nov 2021
Cited by 5 | Viewed by 2159
Abstract
This study investigated the uptake of ammonia (NH3) by secondary organic aerosol (SOA) particles generated via limonene photooxidation or ozonolysis as well as the uptake of dimethylamine (DMA) by limonene ozonolysis, α-cedrene photooxidation, or toluene photooxidation SOA in an environmental chamber [...] Read more.
This study investigated the uptake of ammonia (NH3) by secondary organic aerosol (SOA) particles generated via limonene photooxidation or ozonolysis as well as the uptake of dimethylamine (DMA) by limonene ozonolysis, α-cedrene photooxidation, or toluene photooxidation SOA in an environmental chamber between 0–50% relative humidity. In addition to the acid-base equilibrium uptake, NH3 and DMA can react with SOA carbonyl compounds converting them into nitrogen-containing organic compounds (NOCs). The effective reactive uptake coefficients for the formation of NOCs from ammonia were measured on the order of 10−5. The observed DMA reactive uptake coefficients ranged from 10−5 to 10−4. Typically, the reactive uptake coefficient decreased with increasing relative humidity. This is consistent with NOC formation by a condensation reaction between NH3 or DMA with SOA, which produces water as a product. Ammonia is more abundant in the atmosphere than amines. However, the larger observed reactive uptake coefficient suggests that amine uptake may also be a potential source of organic nitrogen in particulate matter. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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17 pages, 1817 KiB  
Article
Observations of Gas-Phase Alkylamines at a Coastal Site in the East Mediterranean Atmosphere
by Evangelia Tzitzikalaki, Nikos Kalivitis and Maria Kanakidou
Atmosphere 2021, 12(11), 1454; https://0-doi-org.brum.beds.ac.uk/10.3390/atmos12111454 - 03 Nov 2021
Cited by 4 | Viewed by 1640
Abstract
Atmospheric amines are ubiquitous compounds in the atmosphere, having both natural and anthropogenic origin. Recently, they have been identified as important contributors to new particle formation in the atmosphere, but observations of their atmospheric concentrations are scarce. In the present study we introduce [...] Read more.
Atmospheric amines are ubiquitous compounds in the atmosphere, having both natural and anthropogenic origin. Recently, they have been identified as important contributors to new particle formation in the atmosphere, but observations of their atmospheric concentrations are scarce. In the present study we introduce the first systematic long-term observations of gas-phase amines measurements in the East Mediterranean atmosphere. Air samples were collected at the Finokalia monitoring station of the University of Crete during a 3.5-year period from January 2013 to July 2016, and analyzed after extraction using a high-performance liquid chromatography triple quadrupole mass spectrometer. The detected alkylamines were the sum of dimethylamine and ethylamine (DMA+EA), trimethylamine (TMA), diethylamine (DEA) and triethylamine (TEA). DMA+EA and TMA were the most abundant alkylamines, with concentrations spanning from the detection limit to 78.0 and 69.8 pptv, and average concentrations of 7.8 ± 12.1 and 7.5 ± 12.4 pptv, respectively. Amines showed pronounced seasonal variability with DMA+EA and TMA concentrations being higher in winter. Statistical analysis of the observations showed different sources for each of the studied amines, except for DMA+ΕA and DEA that appear to have common sources in the region. This analysis points to a marine source of TMA and animal husbandry in the area as a potential source of TEA. None of the alkylamines is correlated with other anthropogenic sources. Furthermore, no clear association was found between the seasonality of NPF events and alkylamines concentrations, while a clear correlation was detected between the seasonality of nucleation mode particle (dp < 25 nm) number concentrations and alkylamine concentrations, indicating that amines may contribute to nucleation mode particles’ production. Full article
(This article belongs to the Special Issue Ammonia in a Changing Atmosphere)
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