scholarly journals SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particles formation from the photooxidation of a typical aromatic hydrocarbon

2021 ◽  
Author(s):  
Zhaomin Yang ◽  
Li Xu ◽  
Narcisse T. Tsona ◽  
Jianlong Li ◽  
Xin Luo ◽  
...  
Keyword(s):  
Fine Particles ◽  
Heterogeneous Reaction ◽  
Oxidation Mechanism ◽  
Unknown Origin ◽  
Formation Mechanisms ◽  
Chemical Compositions ◽  
Organosulfur Compounds ◽  
Aerosol Formation ◽  
Particle Volume ◽  
Secondary Aerosol

Abstract. Although atmospheric SO2 and NH3 levels can affect secondary aerosol formation, the influenced extent of their impact and their detailed driving mechanisms are not well understood. The focus of the present study is to examine the chemical compositions and formation mechanisms of secondary organic aerosols (SOA) from 1,2,4-trimethylbenzene (TMB) photooxidation influenced by SO2 and/or NH3. Here, we showed that SO2 emission could considerably enhance aerosol particle formation due to SO2-induced sulfates generation and acid-catalyzed heterogeneous reaction. Orbitrap mass spectrometry (MS) measurements revealed the generation of not only typical TMB products but also hitherto unidentified organosulfates (OSs) in SO2-added experiments. The OSs designated as unknown origin in earlier field measurements were also detected in TMB SOA, indicating that atmospheric OSs might be also originated from TMB photooxidation. For NH3-involved experiments, results demonstrated a positive correlation between NH3 levels and particle volume as well as number concentrations. The effects of NH3 on SOA composition was slight under SO2-free conditions but stronger in the presence of SO2. A series of multifunctional products with carbonyl, alcohols, and nitrate functional groups were tentatively characterized in NH3-involved experiments based on infrared spectra and HRMS analysis. Plausible formation pathways were proposed for detected products in the particle-phase. The volatility distributions of products, estimated using parameterization methods, suggested that the detected products gradually condense onto the nucleation particles to contribute to aerosol formation and growth. Our results suggest that strict control of SO2 and NH3 emissions might remarkably reduce organosulfates and secondary aerosol burden in the atmosphere. Updating the aromatic oxidation mechanism in models could result in more accurate treatment of particles formation for urban regions with considerable SO2, NH3, and aromatics emissions.

scholarly journals SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

2021 ◽  
Vol 21 (10) ◽  
pp. 7963-7981
Author(s):  
Zhaomin Yang ◽  
Li Xu ◽  
Narcisse T. Tsona ◽  
Jianlong Li ◽  
Xin Luo ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Oxidation Mechanism ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Mass Spectrometry Analysis ◽  
Formation Mechanisms ◽  
Chemical Compositions ◽  
Organosulfur Compounds ◽  
Aerosol Formation ◽  
Secondary Aerosol

Abstract. Aromatic hydrocarbons can dominate the volatile organic compound budget in the urban atmosphere. Among them, 1,2,4-trimethylbenzene (TMB), mainly emitted from solvent use, is one of the most important secondary organic aerosol (SOA) precursors. Although atmospheric SO2 and NH3 levels can affect secondary aerosol formation, the influenced extent of their impact and their detailed driving mechanisms are not well understood. The focus of the present study is to examine the chemical compositions and formation mechanisms of SOA from TMB photooxidation influenced by SO2 and/or NH3. Here, we show that SO2 emission could considerably enhance aerosol particle formation due to SO2-induced sulfate generation and acid-catalyzed heterogeneous reactions. Orbitrap mass spectrometry measurements revealed the generation of not only typical TMB products but also hitherto unidentified organosulfates (OSs) in SO2-added experiments. The OSs designated as being of unknown origin in earlier field measurements were also detected in TMB SOA, indicating that atmospheric OSs might also be originated from TMB photooxidation. For NH3-involved experiments, results demonstrated a positive correlation between NH3 levels and particle volume as well as number concentrations. The effects of NH3 on SOA composition were slight under SO2-free conditions but stronger in the presence of SO2. A series of multifunctional products with carbonyl, alcohols, and nitrate functional groups were tentatively characterized in NH3-involved experiments based on infrared spectra and mass spectrometry analysis. Plausible formation pathways were proposed for detected products in the particle phase. The volatility distributions of products, estimated using parameterization methods, suggested that the detected products gradually condense onto the nucleation particles to contribute to aerosol formation and growth. Our results suggest that strict control of SO2 and NH3 emissions might remarkably reduce organosulfates and secondary aerosol burden in the atmosphere. Updating the aromatic oxidation mechanism in models could result in more accurate treatment of particle formation for urban regions with considerable SO2, NH3, and aromatics emissions.

scholarly journals Summertime and wintertime atmospheric processes of secondary aerosol in Beijing

2019 ◽  
Author(s):  
Jing Duan ◽  
Ru-Jin Huang ◽  
Yongjie Li ◽  
Qi Chen ◽  
Yan Zheng ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Seasonal Variations ◽  
Chemical Speciation ◽  
Fine Particles ◽  
Large Fraction ◽  
Formation Mechanisms ◽  
Urban Air ◽  
Aerosol Formation ◽  
Secondary Aerosol ◽  
Atmospheric Processes

Abstract. Secondary aerosol constitutes a large fraction of fine particles in urban air of China. However, its formation mechanisms and atmospheric processes remain largely uncertain despite considerable studies in recent years. To elucidate the seasonal variations of fine particles composition and secondary aerosol formation, an Aerodyne quadrupole aerosol chemical speciation monitor (Q-ACSM) combined with other online instruments were used to characterize the submicron particulate matter (diameter 

Summertime and wintertime atmospheric processes of secondary aerosol in Beijing

2020 ◽  
Author(s):  
Jing Duan ◽  
Rujin Huang ◽  
Chunshui Lin ◽  
Haiyan Ni ◽  
Meng Wang
Keyword(s):  
Aqueous Phase ◽  
Liquid Water ◽  
Fine Particles ◽  
Photochemical Oxidation ◽  
Formation Mechanisms ◽  
Phase Reaction ◽  
Aerosol Formation ◽  
Secondary Aerosol ◽  
Atmospheric Processes ◽  
Sulfate Formation

&lt;p&gt;Secondary aerosol constitutes a large fraction of fine particles in urban air of China. However, its formation mechanisms and atmospheric processes remain largely uncertain despite considerable studies in recent years. To elucidate the seasonal variations of fine particles composition and secondary aerosol formation, an Aerodyne quadrupole aerosol chemical speciation monitor (Q-ACSM) combined with other online instruments were used to characterize the submicron particulate matter (diameter &lt; 1 &amp;#956;m, PM&lt;sub&gt;1&lt;/sub&gt;) in Beijing during summer and winter 2015. Our results suggest that the photochemical oxidation was the major pathway for sulfate formation during summer, whereas aqueous-phase reaction became an important process for sulfate formation during winter. High concentration of nitrate (17% of the PM&lt;sub&gt;1&lt;/sub&gt; mass) was found during winter explained by enhanced gas-to-particle partitioning at low temperature, while high nitrate concentration (19%) was also observed under the conditions of high relative humidity (RH) during summer likely due to the hydrophilic property of NH&lt;sub&gt;4&lt;/sub&gt;NO&lt;sub&gt;3&lt;/sub&gt; and hydrolysis of N&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;5&lt;/sub&gt;. As for SOA formation, photochemical oxidation perhaps played an important role for summertime oxygenated OA (OOA) formation and wintertime less oxidized OOA (LO-OOA) formation. The wintertime more oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC), indicating more important contribution of aqueous-phase processing than photochemical production to MO-OOA. Meanwhile, the dependence of LO-OOA and the mass ratio of LO-OOA to MO-OOA on atmospheric oxidative tracer (i.e., O&lt;sub&gt;x&lt;/sub&gt;) both degraded when RH were greater than 60%, suggesting that RH or aerosol liquid water may also affect the LO-OOA formation.&lt;/p&gt;

scholarly journals Summertime and wintertime atmospheric processes of secondary aerosol in Beijing

2020 ◽  
Vol 20 (6) ◽  
pp. 3793-3807 ◽  
Author(s):  
Jing Duan ◽  
Ru-Jin Huang ◽  
Yongjie Li ◽  
Qi Chen ◽  
Yan Zheng ◽  
...  
Keyword(s):  
Aqueous Phase ◽  
Liquid Water ◽  
Fine Particles ◽  
Photochemical Oxidation ◽  
Formation Mechanisms ◽  
Phase Reaction ◽  
Aerosol Formation ◽  
Secondary Aerosol ◽  
Atmospheric Processes ◽  
Sulfate Formation

Abstract. Secondary aerosol constitutes a large fraction of fine particles in urban air of China. However, its formation mechanisms and atmospheric processes remain largely uncertain despite considerable study in recent years. To elucidate the seasonal variations in fine-particle composition and secondary aerosol formation, an Aerodyne quadrupole aerosol chemical speciation monitor (Q-ACSM), combined with other online instruments, was used to characterize the sub-micrometer particulate matter (diameter < 1 µm, PM1) in Beijing during summer and winter 2015. Our results suggest that photochemical oxidation was the major pathway for sulfate formation during summer, whereas aqueous-phase reaction became an important process for sulfate formation during winter. High concentrations of nitrate (17 % of the PM1 mass) were found during winter, explained by enhanced gas-to-particle partitioning at low temperature, while high nitrate concentrations (19 %) were also observed under the conditions of high relative humidity (RH) during summer, likely due to the hydrophilic property of NH4NO3 and hydrolysis of N2O5. As for organic aerosol (OA) sources, secondary OA (SOA) dominated the OA mass (74 %) during summer, while the SOA contribution decreased to 39 % during winter due to enhanced primary emissions in the heating season. In terms of the SOA formation, photochemical oxidation perhaps played an important role for summertime oxygenated OA (OOA) formation and less-oxidized wintertime OOA (LO-OOA) formation. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC), indicating a more important contribution of aqueous-phase processing over photochemical production to MO-OOA. Meanwhile, the dependence of LO-OOA and the mass ratio of LO-OOA to MO-OOA on atmospheric oxidative tracer (i.e., Ox) both degraded when RH was greater than 60 %, suggesting that RH or aerosol liquid water may also affect LO-OOA formation.

scholarly journals Simultaneous Measurements of Chemical Compositions of Fine Particles during Winter Haze Period in Urban Sites in China and Korea

Atmosphere ◽  
2020 ◽  
Vol 11 (3) ◽  
pp. 292 ◽  
Author(s):  
Minhan Park ◽  
Yujue Wang ◽  
Jihyo Chong ◽  
Haebum Lee ◽  
Jiho Jang ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Fine Particles ◽  
Chemical Compositions ◽  
Aerosol Formation ◽  
Wind Speeds ◽  
Simultaneous Measurements ◽  
Dust Sources ◽  
Secondary Formation ◽  
Combustion Sources ◽  
Burning Coal

We performed simultaneous measurements of chemical compositions of fine particles in Beijing, China and Gwangju, Korea to better understand their sources during winter haze period. We identified PM2.5 events in Beijing, possibly caused by a combination of multiple primary combustion sources (biomass burning, coal burning, and vehicle emissions) and secondary aerosol formation under stagnant conditions and/or dust sources under high wind speeds. During the PM2.5 events in Gwangju, the contribution of biomass burning and secondary formation of nitrate and organics to the fine particles content significantly increased under stagnant conditions. We commonly observed the increases of nitrogen-containing organic compounds and biomass burning inorganic (K+) and organic (levoglucosan) markers, suggesting the importance of biomass burning sources during the winter haze events (except dust event cases) at both sites. Pb isotope ratios indicated that the fraction of Pb originated from possibly industry and coal combustion sources increased during the PM2.5 events in Gwangju, relative to nonevent days.

scholarly journals Real-time secondary aerosol formation during a fog event in London

2009 ◽  
Vol 9 (7) ◽  
pp. 2459-2469 ◽  
Author(s):  
M. Dall'Osto ◽  
R. M. Harrison ◽  
H. Coe ◽  
P. Williams
Keyword(s):  
Real Time ◽  
Chemical Properties ◽  
Formation Mechanisms ◽  
Aerosol Formation ◽  
Urban Background ◽  
Mass Spectrometers ◽  
Secondary Aerosol ◽  
Aerosol Mass ◽  
Heterogeneous Formation ◽  
Specific Particle

Abstract. A fog event was monitored with state-of-the art real-time aerosol mass spectrometers in an urban background location in London (England) during the REPARTEE-I experiment. Specific particle types rich in hydroxymethanesulphonate (HMS) were found only during the fog event. Formation of inorganic and organic secondary aerosol was observed as soon as fog was detected and two different mechanisms are suggested to be responsible for the production of two different types of aerosol. Nitrate aerosol is produced in the liquid phase within the droplet. Contrary to previous studies, the formation of HULIS was observed on interstitial particles rather than evaporated fog droplets, suggesting heterogeneous formation mechanisms depending on parameters other than the water content and not fully understood. Not only are secondary aerosol constituents produced during the fog event, but the primary aerosol is observed to be processed by the fog event, dramatically changing its chemical properties.

Particulate matter emissions over the oil sands regions in Alberta, Canada

2017 ◽  
Vol 25 (4) ◽  
pp. 432-443 ◽  
Author(s):  
Zhenyu Xing ◽  
Ke Du
Keyword(s):  
Particulate Matter ◽  
Oil Sands ◽  
Secondary Organic Aerosol ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Open Pit ◽  
Open Pit Mining ◽  
Formation Mechanisms ◽  
Aerosol Formation ◽  
Secondary Aerosol

Particulate matter (PM) emissions from the expanded oil sands development in Alberta are becoming a focus among the aerosol science community because of its significant negative impact on the regional air quality and climate change. Open-pit mining, petroleum coke (petcoke) dust, and the transportation of oil sands and waste materials by heavy-duty trucks on unpaved roads could release PM into the air. Incomplete combustion of fossil fuels by engines and stationary boilers leads to the formation of carbonaceous aerosols. In addition, wildfire and biogenic emissions surrounding the oil sands regions also have the potential to contribute primary PM to the ambient air. Secondary organic aerosol formation has been revealed as an important source of PM over nearby and distant areas from the oil sands regions. This review summarizes the primary PM sources and some secondary aerosol formation mechanisms that are linked to oil sands development. It also reviews the approaches that can be applied in aerosol source apportionment. Meteorological condition is an important factor that may influence the primary PM emission and secondary aerosol formation in Alberta’s oil sands regions. Current concern should not be limited to the primary emission of atmospheric PM. Secondary formation of aerosols, especially secondary organic aerosol originating from photochemical reaction, should also be taken into consideration. To obtain a more comprehensive understanding of the sources and amount of PM emissions based on the bottom-up emission inventory approach, investigations on how to reduce the uncertainty in determination of real-world PM emission factors for the variable sources are needed. Long-range transport trajectories of fine PM from Alberta’s oil sands regions remain unknown.

scholarly journals Synergetic effect of NH<sub>3</sub> and NO<sub>x</sub> on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation

2021 ◽  
Author(s):  
Shijie Liu ◽  
Dandan Huang ◽  
Yiqian Wang ◽  
Si Zhang ◽  
Can Wu ◽  
...  
Keyword(s):  
Optical Absorption ◽  
Secondary Organic Aerosol ◽  
Heterogeneous Reaction ◽  
Synergetic Effect ◽  
Organic Aerosol ◽  
Chemical Compositions ◽  
Atmospheric Conditions ◽  
Aerosol Formation ◽  
Key Species ◽  
The Impact

Abstract. NH3 is the most important alkaline gas in the atmosphere and one of the key species affecting the behaviors of atmospheric aerosols. However, the impact of NH3 on secondary organic aerosol (SOA) formation remains poorly understood, especially the dynamic evolution of chemical compositions in the SOA formation process. A series of chamber experiments was performed to probe the individual and common effects of NH3 and NOx on toluene SOA formation through OH-photooxidation. The chemical compositions of toluene SOA were characterized using the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS). From 637 ± 14.6 μg m−3 (control), the SOA mass concentration increased to 867 ± 12.7 μg m−3 in the presence of NH3 and decreased to 452 ± 18.9 μg m−3 in the presence of NOx. However, the highest SOA concentration (1020 ± 10.6 μg m−3) and the lowest carbon oxidation state (OSC) occurred in the presence of both NH3 and NOx, indicating that the higher volatility products that formed in the presence of NOx could precipitate into the particle-phase when NH3 was added. This resulted in a synergetic effect on SOA formation when NH3 and NOx co-existed. The heterogeneous reaction was the main pathway by which NH3 participated in SOA formation in the photooxidation process. The synergetic effect of NH3 and NOx was also observed in SOA optical absorption. A peak at 280 nm, which is characteristic of organonitrogen imidazole compounds, was observed in the presence of NH3 and its intensity increased when NOx was added into the chamber. This work improves our understanding of how the synergistic interactions between NH3 and NOx influence SOA formation and offers new insights into mitigating aerosol pollution that factor in mixed atmospheric conditions.

scholarly journals Substantial changes in gaseous pollutants and chemical compositions in fine particles in the North China Plain during the COVID-19 lockdown period: anthropogenic vs. meteorological influences

2021 ◽  
Vol 21 (11) ◽  
pp. 8677-8692
Author(s):  
Rui Li ◽  
Yilong Zhao ◽  
Hongbo Fu ◽  
Jianmin Chen ◽  
Meng Peng ◽  
...  
Keyword(s):  
Fine Particles ◽  
Industrial Process ◽  
Road Dust ◽  
Pollutant Emissions ◽  
Chemical Compositions ◽  
Economic Activities ◽  
Secondary Aerosol ◽  
The North ◽  
Secondary Formation ◽  
Meteorological Influences

Abstract. The rapid response to the COVID-19 pandemic led to unprecedented decreases in economic activities, thereby reducing the pollutant emissions. A random forest (RF) model was applied to determine the respective contributions of meteorology and anthropogenic emissions to the changes in air quality. The result suggested that the strict lockdown measures significantly decreased primary components such as Cr (−67 %) and Fe (−61 %) in PM2.5 (p<0.01), whereas the higher relative humidity (RH) and NH3 level and the lower air temperature (T) remarkably enhanced the production of secondary aerosol, including SO42- (29 %), NO3- (29 %), and NH4+ (21 %) (p<0.05). The positive matrix factorization (PMF) result suggested that the contribution ratios of secondary formation (SF), industrial process (IP), biomass burning (BB), coal combustion (CC), and road dust (RD) changed from 36 %, 27 %, 21 %, 12 %, and 4 % before the COVID-19 outbreak to 44 %, 20 %, 20 %, 9 %, and 7 %, respectively. The rapid increase in the contribution ratio derived from SF to PM2.5 implied that the intermittent haze events during the COVID-19 period were characterized by secondary aerosol pollution, which was mainly contributed by the unfavorable meteorological conditions and high NH3 level.

scholarly journals Synergetic effects of NH<sub>3</sub> and NO<sub><i>x</i></sub> on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation

2021 ◽  
Vol 21 (23) ◽  
pp. 17759-17773
Author(s):  
Shijie Liu ◽  
Dandan Huang ◽  
Yiqian Wang ◽  
Si Zhang ◽  
Xiaodi Liu ◽  
...  
Keyword(s):  
Optical Absorption ◽  
Secondary Organic Aerosol ◽  
Heterogeneous Reaction ◽  
Synergetic Effect ◽  
Organic Aerosol ◽  
Chemical Compositions ◽  
Aerosol Formation ◽  
Haze Pollution ◽  
Key Species ◽  
The Impact

Abstract. NH3 is the most important alkaline gas in the atmosphere and one of the key species affecting the behaviors of atmospheric aerosols. However, the impact of NH3 on secondary organic aerosol (SOA) formation remains poorly understood, especially the dynamic evolution of chemical compositions in the SOA formation process. In this study, a series of chamber experiments were performed to probe the individual and common effects of NH3 and NOx on toluene SOA formation through OH photooxidation. The chemical compositions of toluene SOA were characterized using the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS). The SOA yield increased from 28.1 % in the absence of NH3 to 34.7 % in the presence of NH3 but decreased to 19.5 % in the presence of NOx. However, the highest SOA yield of 42.7 % and the lowest carbon oxidation state (OSC) occurred in the presence of both NH3 and NOx, indicating that the higher-volatility products that formed in the presence of NOx could partition into the particle phase when NH3 was added. This resulted in a synergetic effect on SOA formation when NH3 and NOx co-existed. The heterogeneous reaction was the main pathway by which NH3 participated in SOA formation in the photooxidation process. The synergetic effect of NH3 and NOx was also observed in SOA optical absorption. A peak at 280 nm, which is characteristic of organonitrogen imidazole compounds, was observed in the presence of NH3, and its intensity increased when NOx was added into the chamber. This work improves our understanding of how the synergistic interactions between NH3 and NOx influence SOA formation and offers new insights into mitigating haze pollution.

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