scholarly journals Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of Central Eastern China

2013 ◽  
Vol 13 (4) ◽  
pp. 10809-10858 ◽  
Author(s):  
W. W. Hu ◽  
M. Hu ◽  
B. Yuan ◽  
J. L. Jimenez ◽  
Q. Tang ◽  
...  
Keyword(s):  
High Resolution ◽  
Black Carbon ◽  
Coal Combustion ◽  
Eastern China ◽  
Organic Aerosols ◽  
Receptor Site ◽  
Organic Aerosol ◽  
Submicron Particles ◽  
Central Eastern ◽  
Photochemical Age

Abstract. In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas In Eastern China, CAPTAIN) was conducted in March–April at a receptor site (Changdao Island) in Central Eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM1nr). The average mass concentration of PM1 (PM1nr + black carbon) was 47 ± 36 μg m−3 during the campaign and showed distinct variation depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM1 (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by Positive Matrix Factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA), reported here for the first time. The mass spectrum of CCOA has high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178 etc.). The average atomic ratio of oxygen to carbon in OA (O/C) at Changdao is 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the Van Krevelen diagram (H/C vs. O/C) shows a slope of −0.63, however, the OA influenced by coal combution exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. with photochemical age was investigated. It is shown that OA/ΔCO, as well as LV-OOA/ΔCO and SV-OOA/ΔCO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation in the oldest plumes (photochemical age of 25 h). The kOH at Changdao by assuming SOA formation and aging as a first-order process proportional to OH was calculated to be is 5.2 × 10−12 cm3 molec−1 s−1 which is similar to those determined in recent studies of polluted air in other continents.

scholarly journals Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of central eastern China

2013 ◽  
Vol 13 (19) ◽  
pp. 10095-10112 ◽  
Author(s):  
W. W. Hu ◽  
M. Hu ◽  
B. Yuan ◽  
J. L. Jimenez ◽  
Q. Tang ◽  
...  
Keyword(s):  
High Resolution ◽  
Black Carbon ◽  
Coal Combustion ◽  
Eastern China ◽  
Organic Aerosols ◽  
Receptor Site ◽  
Organic Aerosol ◽  
Submicron Particles ◽  
Central Eastern ◽  
Photochemical Age

Abstract. In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas IN Eastern China, CAPTAIN) was conducted March–April at a receptor site (a Changdao island) in central eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) that was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM1nr). The average mass concentration of PM1(PM1nr+black carbon) was 47 ± 36 μg m−3 during the campaign and showed distinct variation, depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM1 (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by positive matrix factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA). The mass spectrum of CCOA had high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178, etc.). The average atomic ratio of oxygen to carbon in OA (O / C) at Changdao was 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the van Krevelen diagram (H / C vs. O / C) showed a slope of −0.63; however, the OA influenced by coal combustion exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. photochemical age was investigated. It was shown that OA / ΔCO, as well as LV-OOA / ΔCO and SV-OOA / ΔCO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation (SOA) in the oldest plumes (photochemical age of 25 h). The kOH at Changdao, by assuming SOA formation and aging as a first-order process proportional to OH, was calculated to be 5.2 × 10−12 cm3 molec.−1 s−1, which is similar to those determined in recent studies of polluted air in other continents.

scholarly journals Technical note: A new approach to discriminate different black carbon sources by utilising fullerene and metals in positive matrix factorisation analysis of high-resolution soot particle aerosol mass spectrometer data

2021 ◽  
Vol 21 (13) ◽  
pp. 10763-10777
Author(s):  
Zainab Bibi ◽  
Hugh Coe ◽  
James Brooks ◽  
Paul I. Williams ◽  
Ernesto Reyes-Villegas ◽  
...  
Keyword(s):  
High Resolution ◽  
Black Carbon ◽  
Source Apportionment ◽  
Atmospheric Aerosol ◽  
Soot Particle ◽  
Organic Aerosol ◽  
Positive Matrix ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Matrix Factorisation

Abstract. Atmospheric aerosol particles are known to have detrimental effects on human health and climate. Black carbon is an important constituent of atmospheric aerosol particulate matter (PM), emitted from incomplete combustion. Source apportionment of BC is very important, to evaluate the influence of different sources. The high-resolution soot particle aerosol mass spectrometer (HR-SP-AMS) instrument uses a laser vaporiser, which allows the real-time detection and characterisation of refractory black carbon (rBC) and its internally mixed particles such as metals, coating species, and rBC subcomponents in the form of HOA + fullerene. In this case study, the soot data were collected by using HR-SP-AMS during Guy Fawkes Night on 5 November 2014. Positive matrix factorisation was applied to positively discriminate between different wood-burning and bonfire sources for the first time, which no existing black carbon source apportionment technique is currently able to do. Along with this, the use of the fullerene signals in differentiating between soot sources and the use of metals as a tracer for fireworks has also been investigated, which did not significantly contribute to the rBC concentrations. The addition of fullerene signals and successful positive matrix factorisation (PMF) application to HR-SP-AMS data apportioned rBC into more than two sources. These bonfire sources are HOA + fullerene, biomass burning organic aerosol, more oxidised oxygenated organic aerosol (MO-OOA), and non-bonfire sources such as hydrocarbon-like OA and domestic burning. The result of correlation analysis between HR-SP-AMS data and previously published Aethalometer, MAAP, and CIMS data provides an effective way of gaining insights into the relationships between the variables and provide a quantitative estimate of the source contributions to the BC budget during this period. This research study is an important demonstration of using HR-SP-AMS for the purpose of BC source apportionment.

Seasonal variations in chemical characterization of submicron aerosol particles in Shanghai, China: Insights from a high-resolution aerosol mass spectrometry

2020 ◽  
Author(s):  
Wenfei Zhu ◽  
Shengrong Lou ◽  
Song Guo
Keyword(s):  
Particulate Matter ◽  
High Resolution ◽  
Photochemical Reaction ◽  
Chemical Characterization ◽  
Organic Aerosol ◽  
Submicron Particles ◽  
Chemical Components ◽  
Average Mass ◽  
Compound Pollution ◽  
Autumn And Winter

<p>As a characteristic pollutant of urban compound pollution, submicron particulate matter (PM1) has significantly impacted on human health and climate change. In this study, four intensive campaigns using a high-resolution time-of-flight AMS (HR-ToF-AMS) and other online instruments from 2016 to 2017 were conducted to investigate the seasonal characteristics of submicron particles in Shanghai. The average mass concentrations of submicron particulate matter during spring, summer, autumn and winter observations in Shanghai are 23.9 ± 20.7 μg/m3, 28.5 ± 17.6 μg/m3, 22.0 ± 17.2 μg/m3 and 31.9 ± 22.7 μg/m3, respectively. The major chemical components in submicron particulate matter showed obvious seasonal and daily variations. The increase of submicron particulate matter is mainly due to the contribution of nitrate in spring, autumn and winter, while the photochemical reaction promotes the rapid growth of sulfate in summer. Detailed source apportionment of organic aerosol showed that the fraction of more oxidized oxygenated organic aerosol in organic aerosol in spring was much lower than primary organic aerosol. Oxygenated organic aerosol dominated organic aerosol in summer (69%). More oxidized oxygenated organic aerosol account for 28% in autumn, suggesting that organic aerosol was aging. The liquid phase oxidation and the strong photochemical reaction concentration have a significant contribution to the formation of more oxidized oxygenated organic aerosol and less oxidized oxygenated organic aerosol in the spring, summer and winter observations, respectively. However, the photochemical reaction process dominated the formation of more oxidized oxygenated organic aerosol in autumn.</p>

scholarly journals VOC emissions, evolutions and contributions to SOA formation at a receptor site in eastern China

2013 ◽  
Vol 13 (17) ◽  
pp. 8815-8832 ◽  
Author(s):  
B. Yuan ◽  
W. W. Hu ◽  
M. Shao ◽  
M. Wang ◽  
W. T. Chen ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Emission Inventory ◽  
Eastern China ◽  
Receptor Site ◽  
Organic Aerosol ◽  
Inventory Data ◽  
Voc Oxidation ◽  
Volatile Organic ◽  
Emission Ratios

Abstract. Volatile organic compounds (VOCs) were measured by two online instruments (GC-FID/MS and PTR-MS) at a receptor site on Changdao Island (37.99° N, 120.70° E) in eastern China. Reaction with OH radical dominated chemical losses of most VOC species during the Changdao campaign. A photochemical-age-based parameterization method is used to calculate VOC emission ratios and to quantify the evolution of ambient VOCs. The calculated emission ratios of most hydrocarbons agree well with those obtained from emission inventory data, but determined emission ratios of oxygenated VOCs (OVOCs) are significantly higher than those from emission inventory data. The photochemical-age-based parameterization method is also used to investigate primary emissions and secondary formation of organic aerosol. The primary emission ratio of organic aerosol (OA) to CO is determined to be 14.9 μg m−3 ppm−1, and secondary organic aeorosols (SOA) are produced at an enhancement ratio of 18.8 μg m−3 ppm−1 to CO after 50 h of photochemical processing in the atmosphere. SOA formation is significantly higher than the level determined from VOC oxidation under both high-NOx (2.0 μg m−3 ppm−1 CO) and low-NOx conditions (6.5 μg m−3 ppm−1 CO). Polycyclic aromatic hydrocarbons (PAHs) and higher alkanes (> C10) account for as high as 17.4% of SOA formation, which suggests semi-volatile organic compounds (SVOCs) may be a large contributor to SOA formation during the Changdao campaign. The SOA formation potential of primary VOC emissions determined from field campaigns in Beijing and Pearl River Delta (PRD) is lower than the measured SOA levels reported in the two regions, indicating SOA formation is also beyond explainable by VOC oxidation in the two city clusters.

scholarly journals Volatility of mixed atmospheric Humic-like Substances and ammonium sulfate particles

2016 ◽  
Author(s):  
Wei Nie ◽  
Juan Hong ◽  
Silja A. K. Häme ◽  
Aijun Ding ◽  
Yugen Li ◽  
...  
Keyword(s):  
Ammonium Sulfate ◽  
Volume Fraction ◽  
Eastern China ◽  
Organic Aerosols ◽  
Organic Aerosol ◽  
Inorganic Salts ◽  
Transfer Model ◽  
Organic Part ◽  
Multi Phase ◽  
Mixed Samples

Abstract. The volatility of organic aerosols remains poorly understood due to the complexity of speciation and multi-phase processes. In this study, we extracted HUmic-LIke Substances (HULIS) from four atmospheric aerosol samples collected at the SORPES station in Nanjing, eastern China, and investigated the volatility behavior of particles at different sizes using a Volatility Tandem Differential Mobility Analyzer (VTDMA). In spite of the large differences in particle mass concentrations, the extracted HULIS from the four samples all revealed very high oxidation states (O : C > 0.95), indicating secondary formation as the major source of HULIS in Yangtze River Delta (YRD). An overall low volatility was identified for the HULIS samples, with the volume fraction remaining (VFR) higher than 55 % for all the re-generated HULIS particles at the temperature of 280 °C. A kinetic mass transfer model was applied to the thermodenuder (TD) data to interpret the observed evaporation pattern of HULIS, and to derive the mass fractions of semi-volatile (SVOC), low-volatility (LVOC) and extremely low-volatility components (ELVOC). The results showed that LVOC and ELVOC dominated (more than 80 %) the total volume of HULIS. Atomizing processes led to a size dependent evaporation of regenerated HULIS particles, and resulted in more ELVOCs in smaller particles. In order to understand the role of interaction between inorganic salts and atmospheric organic mixtures in the volatility of an organic aerosol, the evaporation of mixed samples of ammonium sulfate (AS) and HULIS was measured. The results showed a significant but nonlinear influence of ammonium sulfate on the volatility of HULIS. The estimated fraction of ELVOCs in the organic part of largest particles (145 nm) increased from 26 % in pure HULIS samples to 93 % in 1 : 3 (mass ratio of HULIS : AS) mixed samples, to 45 % in 2 : 2 mixed samples, and to 70 % in 3 : 1 mixed samples, suggesting that the interaction tends to decrease the volatility of atmospheric organic molecular once condensing on ammonium sulfate containing aerosols. Our results demonstrate that HULIS are important low volatile, or even extremely low volatile, compounds in the organic aerosol phase. As important formation pathways of atmospheric HULIS, multi-phase processes, including oxidation, oligomerization, polymerization and interaction with inorganic salts, are indicated to be important sources of low volatile and extremely low volatility species of organic aerosols.

scholarly journals Emissions of organic aerosol mass, black carbon, particle number, and regulated and unregulated gases from scooters and light and heavy duty vehicles with different fuels

2014 ◽  
Vol 14 (11) ◽  
pp. 16591-16639 ◽  
Author(s):  
R. Chirico ◽  
M. Clairotte ◽  
T. W. Adam ◽  
B. Giechaskiel ◽  
M. F. Heringa ◽  
...  
Keyword(s):  
High Resolution ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Aromatic Compounds ◽  
Particle Number ◽  
Time Of Flight ◽  
Organic Aerosol ◽  
Heavy Duty ◽  
Diesel Vehicles ◽  
Gasoline Vehicles

Abstract. A sampling campaign with seven different types of vehicles was conducted in 2009 at the vehicle test facilities of the Joint Research Centre (JRC) in Ispra (Italy). The vehicles chosen were representative of some categories circulating in Europe and were fueled either with standard gasoline or diesel and some with blends of rapeseed methyl ester biodiesel. The aim of this work was to improve the knowledge about the emission factors of gas phase and particle-associated regulated and unregulated species from vehicle exhaust. Unregulated species such as black carbon (BC), primary organic aerosol (OA) content, particle number (PN), monocyclic and polycyclic aromatic hydrocarbons (PAHs) and a~selection of unregulated gaseous compounds, including nitrous acid (N2O), ammonia (NH3), hydrogen cyanide (HCN), formaldehyde (HCHO), acetaldehyde (CH3CHO), sulfur dioxide (SO2), and methane (CH4), were measured in real time with a suite of instruments including a high-resolution aerosol time-of-flight mass spectrometer, a resonance enhanced multi-photon ionization time-of-flight mass spectrometer, and a high resolution Fourier transform infrared spectrometer. Diesel vehicles, without particle filters, featured the highest values for particle number, followed by gasoline vehicles and scooters. The particles from diesel and gasoline vehicles were mostly made of BC with a low fraction of OA, while the particles from the scooters were mainly composed of OA. Scooters were characterized by super high emissions factors for OA, which were orders of magnitude higher than for the other vehicles. The heavy duty diesel vehicle (HDDV) featured the highest nitrogen oxides (NOx) emissions, while the scooters had the highest emissions for total hydrocarbons and aromatic compounds due to the unburned and partially burned gasoline and lubricant oil mixture. Generally, vehicles fuelled with biodiesel blends showed lower emission factors of OA and total aromatics than those from the standard fuels. The scooters were the main emitters of aromatic compounds, followed by the gasoline vehicle, the diesel vehicles and the HDDV.

scholarly journals Volatility of mixed atmospheric humic-like substances and ammonium sulfate particles

2017 ◽  
Vol 17 (5) ◽  
pp. 3659-3672 ◽  
Author(s):  
Wei Nie ◽  
Juan Hong ◽  
Silja A. K. Häme ◽  
Aijun Ding ◽  
Yugen Li ◽  
...  
Keyword(s):  
Ammonium Sulfate ◽  
Volume Fraction ◽  
Eastern China ◽  
Organic Aerosols ◽  
Organic Aerosol ◽  
Yangtze River Delta ◽  
Inorganic Salts ◽  
Transfer Model ◽  
Organic Part ◽  
Mixed Samples

Abstract. The volatility of organic aerosols remains poorly understood due to the complexity of speciation and multiphase processes. In this study, we extracted humic-like substances (HULIS) from four atmospheric aerosol samples collected at the SORPES station in Nanjing, eastern China, and investigated the volatility behavior of particles at different sizes using a Volatility Tandem Differential Mobility Analyzer (VTDMA). In spite of the large differences in particle mass concentrations, the extracted HULIS from the four samples all revealed very high-oxidation states (O : C > 0.95), indicating secondary formation as the major source of HULIS in Yangtze River Delta (YRD). An overall low volatility was identified for the extracted HULIS, with the volume fraction remaining (VFR) higher than 55 % for all the regenerated HULIS particles at the temperature of 280 °C. A kinetic mass transfer model was applied to the thermodenuder (TD) data to interpret the observed evaporation pattern of HULIS, and to derive the mass fractions of semi-volatile (SVOC), low-volatility (LVOC) and extremely low-volatility components (ELVOC). The results showed that LVOC and ELVOC dominated (more than 80 %) the total volume of HULIS. Atomizing processes led to a size-dependent evaporation of regenerated HULIS particles, and resulted in more ELVOC in smaller particles. In order to understand the role of interaction between inorganic salts and atmospheric organic mixtures in the volatility of an organic aerosol, the evaporation of mixed samples of ammonium sulfate (AS) and HULIS was measured. The results showed a significant but nonlinear influence of ammonium sulfate on the volatility of HULIS. The estimated fraction of ELVOC in the organic part of the largest particles (145 nm) increased from 26 %, in pure HULIS samples, to 93 % in 1 : 3 (mass ratio of HULIS : AS) mixed samples, to 45 % in 2 : 2 mixed samples, and to 70 % in 3 : 1 mixed samples, suggesting that the interaction with ammonium sulfate tends to decrease the volatility of atmospheric organic compounds. Our results demonstrate that HULIS are important low-volatility, or even extremely low-volatility, compounds in the organic-aerosol phase. As important formation pathways of atmospheric HULIS, multiphase processes, including oxidation, oligomerization, polymerization and interaction with inorganic salts, are indicated to be important sources of low-volatility and extremely low-volatility species of organic aerosols.

scholarly journals Urban organic aerosol composition in Eastern China differs from North to South: Molecular insight from a liquid chromatography-Orbitrap mass spectrometry study

2019 ◽  
Author(s):  
Kai Wang ◽  
Ru-Jin Huang ◽  
Martin Brüggemann ◽  
Yun Zhang ◽  
Lu Yang ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Liquid Chromatography ◽  
Eastern China ◽  
Organic Aerosol ◽  
Photochemical Oxidation ◽  
Lower Latitude ◽  
Molecular Formula ◽  
Aerosol Composition ◽  
Orbitrap Mass Spectrometry ◽  
Low Degrees

Abstract. Particulate air pollution in China is influencing human health, ecosystem and climate. However, the chemical composition of particulate aerosol, especially of the organic fraction, is still not well understood. In this study, particulate aerosol samples with a diameter ≤ 2.5 μm (PM2.5) were collected in January 2014 in three cities located in Northeast, East and Southeast China, i.e., Changchun, Shanghai and Guangzhou, respectively. Organic aerosol (OA) in the PM2.5 samples was analyzed by ultrahigh performance liquid chromatography (UHPLC) coupled to high-resolution Orbitrap mass spectrometry in both negative mode (ESI−) and positive mode electrospray ionization (ESI+). After a non-target screening including molecular formula assignments, compounds were classified into five groups based on their elemental composition, i.e., CHO, CHON, CHN, CHOS and CHONS. The CHO, CHON and CHN compounds present the dominant signal abundances of 81–99.7 % in the mass spectra and the majority of these compounds were assigned to mono- and polyaromatics, suggesting that anthropogenic emissions are a large source of urban OA in all three cities. However, the chemical characteristics of these compounds varied among different cities. The degree of aromaticity and the number of polyaromatic compounds were significantly higher in samples from Changchun, which could be attributed to the large emissions from residential heating (i.e., coal combustion) during winter time in Northeast China. Moreover, the ESI− analysis showed higher H / C and O / C ratios for organic compounds in Shanghai and Guangzhou compared to samples from Changchun, indicating that OA in lower latitude regions of China experiences more intense photochemical oxidation processes. The majority of sulfur-containing compounds (CHOS and CHONS) in all cities were assigned to aliphatic compounds with low degrees of unsaturation and aromaticity. Again, samples from Shanghai and Guangzhou exhibit a larger chemical similarity but largely differ from those from Changchun.

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