scholarly journals Single-particle characterization of aerosols collected at a remote site in the Amazonian rainforest and an urban site in Manaus, Brazil

2018 ◽  
Author(s):  
Li Wu ◽  
Xue Li ◽  
Hye Kyeong Kim ◽  
Hong Geng ◽  
Ricardo H. M. Godoi ◽  
...  

Abstract. In this study, aerosol samples collected at a remote site in the Amazonian rainforest and an urban site in Manaus, Brazil, were investigated on a single particle basis using a quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA). Twenty-three aerosol samples were collected in four size ranges (0.25–0.5, 0.5–1.0, 1.0–2.0, and 2.0–4.0 µm) during the wet season in 2012 at two Amazon basin sites: 10 samples in Manaus, an urban area; and 13 samples at an 80-m high tower, located at the Amazon Tall Tower Observatory (ATTO) site in the middle of the rainforest, 150 km northeast of Manaus. The aerosol particles were classified into nine particle types based on the morphology on the secondary electron images (SEIs) together with the elemental concentrations of 3,162 individual particles: (i) secondary organic aerosols (SOA), (ii) ammonium sulfate (AS), (iii) SOA and AS mixtures, (iv) aged mineral dust, (v) reacted sea-salts, (vi) primary biological aerosol (PBA), (vii) carbon-rich or elemental carbon (EC) particles, such as soot, tar ball, and char, (viii) fly ash, and (ix) heavy metal (HM, such as Fe, Zn, Ni, and Ti)-containing particles. In submicron aerosols collected at the ATTO site, SOA and AS mixture particles were predominant (50–94 % in relative abundance) with SOA and ammonium sulfate comprising 73–100 %. In supermicron aerosols at the ATTO site, aged mineral dust and sea-salts (37–70 %) as well as SOA and ammonium sulfate (28–58 %) were abundant. PBAs were observed abundantly in the PM2–4 fraction (46 %), and EC and fly ash particles were absent in all size fractions. The analysis of a bulk PM0.25–0.5 aerosol sample from the ATTO site using Raman microspectrometry and attenuated total reflection Fourier transform infrared spectroscopy showed that ammonium sulfate, organics, and minerals are the major chemical species, which is consistent with the ED-EPMA results. In the submicron aerosols collected in Manaus, either SOA and ammonium sulfate (17–80 %) or EC particles (6–78 %) were dominant depending on the samples. In contrast, aged mineral dust, reacted sea-salt, PBA, SOA, ammonium sulfate, and EC particles comprised most of the supermicron aerosols collected in Manaus. The SOA, ammonium sulfate, and PBAs were mostly of a biogenic origin from the rainforest, whereas the EC and HM-containing particles were of an anthropogenic origin. Aged mineral dust and reacted sea-salt particles, including mineral dust mixed with sea-salts probably during long-range transatlantic transport, were abundant in the supermicron fractions at both sites. Among the aged mineral dust and reacted sea-salt particles, sulfate-containing ones outnumbered those containing nitrates and sulfate+nitrate in the ATTO samples. In contrast, particles containing sulfate+nitrate were comparable in number to particles containing sulfate only in the Manaus samples, indicating the different sources and formation mechanisms of secondary aerosols, i.e., the predominant presence of sulfate at the ATTO site from mostly biogenic emissions and the elevated influences of nitrates from anthropogenic activities at the Manaus site.

2019 ◽  
Vol 19 (2) ◽  
pp. 1221-1240 ◽  
Author(s):  
Li Wu ◽  
Xue Li ◽  
HyeKyeong Kim ◽  
Hong Geng ◽  
Ricardo H. M. Godoi ◽  
...  

Abstract. In this study, aerosol samples collected at a remote site in the Amazonian rainforest and an urban site in Manaus, Brazil, were investigated on a single-particle basis using a quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA). A total of 23 aerosol samples were collected in four size ranges (0.25–0.5, 0.5–1.0, 1.0–2.0, and 2.0–4.0 µm) during the wet season in 2012 at two Amazon basin sites: 10 samples in Manaus, an urban area; and 13 samples at an 80 m high tower, located at the Amazon Tall Tower Observatory (ATTO) site in the middle of the rainforest, 150 km northeast of Manaus. The aerosol particles were classified into nine particle types based on the morphology on the secondary electron images (SEIs) together with the elemental concentrations of 3162 individual particles: (i) secondary organic aerosols (SOA); (ii) ammonium sulfate (AS); (iii) SOA and AS mixtures; (iv) aged mineral dust; (v) reacted sea salts; (vi) primary biological aerosol (PBA); (vii) carbon-rich or elemental carbon (EC) particles, such as soot, tarball, and char; (viii) fly ash; and (ix) heavy metal (HM, such as Fe, Zn, Ni, and Ti)-containing particles. In submicron aerosols collected at the ATTO site, SOA and AS mixture particles were predominant (50 %–94 % in relative abundance) with SOA and ammonium sulfate comprising 73 %–100 %. In supermicron aerosols at the ATTO site, aged mineral dust and sea salts (37 %–70 %) as well as SOA and ammonium sulfate (28 %–58 %) were abundant. PBAs were observed abundantly in the PM2−4 fraction (46 %), and EC and fly ash particles were absent in all size fractions. The analysis of a bulk PM0.25−0.5 aerosol sample from the ATTO site using Raman microspectrometry and attenuated total reflection Fourier-transform infrared spectroscopy (ATR-FTIR) showed that ammonium sulfate, organics, and minerals are the major chemical species, which is consistent with the ED-EPMA results. In the submicron aerosols collected in Manaus, either SOA and ammonium sulfate (17 %–80 %) or EC particles (6 %–78 %) were dominant depending on the samples. In contrast, aged mineral dust, reacted sea salt, PBA, SOA, ammonium sulfate, and EC particles comprised most of the supermicron aerosols collected in Manaus. The SOA, ammonium sulfate, and PBAs were mostly of a biogenic origin from the rainforest, whereas the EC and HM-containing particles were of an anthropogenic origin. Based on the different contents of SOA, ammonium sulfate, and EC particles among the samples collected in Manaus, a considerable influence of the rainforest over the city was observed. Aged mineral dust and reacted sea-salt particles, including mineral dust mixed with sea salts probably during long-range transatlantic transport, were abundant in the supermicron fractions at both sites. Among the aged mineral dust and reacted sea-salt particles, sulfate-containing ones outnumbered those containing nitrates and sulfate + nitrate in the ATTO samples. In contrast, particles containing sulfate + nitrate were comparable in number to particles containing sulfate only in the Manaus samples, indicating the different sources and formation mechanisms of secondary aerosols, i.e., the predominant presence of sulfate at the ATTO site from mostly biogenic emissions and the elevated influences of nitrates from anthropogenic activities at the Manaus site.


2016 ◽  
Author(s):  
Weihua Chen ◽  
Xuemei Wang ◽  
Jason Blake Cohen ◽  
Shengzhen Zhou ◽  
Zhisheng Zhang ◽  
...  

Abstract. Measurements of size-resolved aerosols from 0.25 to 18 μm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 μm). Sulfate, was found to be strongly correlated with aerosol water, and anti-correlated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bi-modal distribution at the urban site, and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions were also found to be important in at least some of the sights on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the Monsoon over southern China.


2011 ◽  
Vol 11 (3) ◽  
pp. 1327-1337 ◽  
Author(s):  
H. Geng ◽  
J. Y. Ryu ◽  
S. Maskey ◽  
H.-J. Jung ◽  
C.-U. Ro

Abstract. A quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), called low-Z particle EPMA, was used to analyse individual aerosol particles collected in Incheon, Korea on 13–18 October 2008 (a typical haze episode occurred from 15 to 18 October). Overall 3600 individual particles in PM2.5-10 and PM1.0-2.5 fractions from 12 aerosol samples collected on haze and non-haze days were analysed. The analysed particles were classified, based on their X-ray spectral data together with their secondary electron images. The major particle types included organic carbon (OC), elemental carbon (EC), sea-salt, mineral dust (such as aluminosilicate, SiO2, CaCO3/CaMgCO3, etc.), (NH4)2SO4/NH4HSO4-containing, K-containing, Fe-rich and fly ash particles. Their relative number abundance results showed that OC particles were significantly increased while sea-salts and mineral dust particles were significantly decreased (especially in PM1.0-2.5 fraction) when haze occurred. For the other particle types (except Fe-rich particles in PM2.5-10 fraction), there were no significant differences in their relative abundances between haze and non-haze samples. On non-haze days, the nitrate-containing reacted sea-salt and mineral dust particles in PM1.0-2.5 fraction significantly outnumbered the sulfate-containing ones, whereas it was the reverse on haze days, implying that on haze days there were special sources or formation mechanisms for fine aerosol particles (≤2.5 μm in aerodynamic diameter). The emission of air pollutants from motor vehicles and stagnant meteorological conditions, such as low wind speed and high relative humidity, might be responsible for the elevated level of OC particles on haze days.


2019 ◽  
Vol 12 (11) ◽  
pp. 6209-6239 ◽  
Author(s):  
Karl D. Froyd ◽  
Daniel M. Murphy ◽  
Charles A. Brock ◽  
Pedro Campuzano-Jost ◽  
Jack E. Dibb ◽  
...  

Abstract. Single-particle mass spectrometry (SPMS) instruments characterize the composition of individual aerosol particles in real time. Their fundamental ability to differentiate the externally mixed particle types that constitute the atmospheric aerosol population enables a unique perspective into sources and transformation. However, quantitative measurements by SPMS systems are inherently problematic. We introduce a new technique that combines collocated measurements of aerosol composition by SPMS and size-resolved absolute particle concentrations on aircraft platforms. Quantitative number, surface area, volume, and mass concentrations are derived for climate-relevant particle types such as mineral dust, sea salt, and biomass burning smoke. Additionally, relative ion signals are calibrated to derive mass concentrations of internally mixed sulfate and organic material that are distributed across multiple particle types. The NOAA Particle Analysis by Laser Mass Spectrometry (PALMS) instrument measures size-resolved aerosol chemical composition from aircraft. We describe the identification and quantification of nine major atmospheric particle classes, including sulfate–organic–nitrate mixtures, biomass burning, elemental carbon, sea salt, mineral dust, meteoric material, alkali salts, heavy fuel oil combustion, and a remainder class. Classes can be sub-divided as necessary based on chemical heterogeneity, accumulated secondary material during aging, or other atmospheric processing. Concentrations are derived for sizes that encompass the accumulation and coarse size modes. A statistical error analysis indicates that particle class concentrations can be determined within a few minutes for abundances above ∼10 ng m−3. Rare particle types require longer sampling times. We explore the instrumentation requirements and the limitations of the method for airborne measurements. Reducing the size resolution of the particle data increases time resolution with only a modest increase in uncertainty. The principal limiting factor to fast time response concentration measurements is statistically relevant sampling across the size range of interest, in particular, sizes D < 0.2 µm for accumulation-mode studies and D > 2 µm for coarse-mode analysis. Performance is compared to other airborne and ground-based composition measurements, and examples of atmospheric mineral dust concentrations are given. The wealth of information afforded by composition-resolved size distributions for all major aerosol types represents a new and powerful tool to characterize atmospheric aerosol properties in a quantitative fashion.


2010 ◽  
Vol 10 (11) ◽  
pp. 26641-26676
Author(s):  
H. Geng ◽  
J. Ryu ◽  
S. Maskey ◽  
H.-J. Jung ◽  
C.-U. Ro

Abstract. Haze is an atmospheric phenomenon that leads to low visibility, and is mostly due to elevated levels of fine particulate matter. It can have effects on cloud formation, public health, agriculture, and even the global climate. Although urban haze has been increasing in occurrence over the past several years over the Seoul-Incheon metropolis, Korea, studies of the morphology and chemical composition of ambient aerosol particles by single-particle analysis during haze episodes have rarely been conducted. Herein, a quantitative energy-dispersive electron probe microanalysis (ED-EPMA), called low-Z particle EPMA, was used to analyze individual aerosol particles collected in Incheon, Korea on 13–18 October 2008 (a typical haze episode occurred from 15 to 18 October). Overall, 3600 particles in 12 aerosol samples collected on haze and non-haze days were measured by low-Z particle EPMA. Based on quantitative X-ray analysis, together with secondary electron images of individual particles, we successfully identified the aerosol particle types as follows: elemental carbon (EC), organic carbon (OC), (NH4)2SO4/NH4HSO4-containing, genuine (fresh) and reacted (aged) sea-salt, mineral dust (such as aluminosilicate, SiO2, CaCO3/CaMg(CO3)2, etc.), and K-containing, Fe-rich, and fly ash particles. By analyzing the relative abundances of different particle types, it was concluded that (a) on non-haze days, reacted sea-salts and reacted mineral dust particles were abundant in both the PM2.5–10 and PM1.0–2.5 fractions (with relative abundances of 65.0% and 57.7%, respectively); whereas on haze days, the relative abundances of OC and (NH4)2SO4/NH4HSO4-containing particles were significantly elevated, indicating that organic matter and secondary aerosols were abundant in the atmosphere when haze occurred. (b) in PM2.5–10 fractions, sea-salt and mineral dust particles reacted with NOx/HNO3 significantly outnumbered those reacted with SO2/H2SO4, no matter whether they were collected on haze or non-haze days; but in PM1.0–2.5 fractions on non-haze days, the nitrate-containing reacted particles significantly outnumbered the sulfate-containing ones, whereas it was the reverse on haze days, implying that on haze days there were special sources or formation mechanisms for the reacted fine aerosol particles (aerodynamic diameter<2.5 μm). It is hypothesized that motor vehicles, biomass burning from the areas surrounding Incheon, and haze transported from Eastern China are the major contributors to urban haze formation in Incheon under stagnant meteorological conditions such as low wind speed, high relative humidity, etc.


2016 ◽  
Vol 16 (20) ◽  
pp. 13271-13289 ◽  
Author(s):  
Weihua Chen ◽  
Xuemei Wang ◽  
Jason Blake Cohen ◽  
Shengzhen Zhou ◽  
Zhisheng Zhang ◽  
...  

Abstract. Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm). Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.


2019 ◽  
Author(s):  
Karl D. Froyd ◽  
Daniel M. Murphy ◽  
Charles A. Brock ◽  
Pedro Campuzano-Jost ◽  
Jack E. Dibb ◽  
...  

Abstract. Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. Their fundamental ability to differentiate the externally mixed particle types that constitute the atmospheric aerosol population enables a unique perspective into sources and transformation. However, quantitative measurements by SPMS systems are inherently problematic. We introduce a new technique that combines collocated measurements of aerosol composition by SPMS and size-resolved absolute particle concentrations on aircraft platforms. Quantitative number, surface area, volume, and mass concentrations are derived for climate-relevant particle types such as mineral dust, sea salt, and biomass burning smoke. Additionally, relative ion signals are calibrated to derive mass concentrations of internally mixed sulfate and organic material that are distributed across multiple particle types. The NOAA Particle Analysis by Laser Mass Spectrometry (PALMS) instrument measures size-resolved aerosol chemical composition from aircraft. We describe the identification and quantification of nine major atmospheric particle classes, including sulfate/organic/nitrate mixtures, biomass burning, elemental carbon, sea salt, mineral dust, meteoric material, alkali salts, heavy fuel oil combustion, and a remainder class. Classes can be sub-divided as necessary based on chemical heterogeneity, accumulated secondary material during aging, or other atmospheric processing. Concentrations are derived for sizes that encompass the accumulation and coarse size modes. A statistical error analysis indicates that particle class concentrations can be determined within a few minutes for abundances above ~ 10 ng m−3. Rare particle types require longer sampling times. We explore the instrumentation requirements and the limitations of the method for airborne measurements. Reducing the size resolution of the particle data increases time resolution with only a modest increase in uncertainty. The principal limiting factor to fast time response concentration measurements is statistically relevant sampling across the size range of interest, in particular, sizes D  2 μm for coarse mode analysis. We demonstrate the use of a virtual impactor to enhance sampling statistics for the inherently sparse coarse mode. Performance is compared to other airborne and ground-based composition measurements, and examples of atmospheric mineral dust concentrations are given. The wealth of information afforded by composition-resolved size distributions for all major aerosol types represents a new and powerful tool to characterize atmospheric aerosol properties in a quantitative fashion.


Author(s):  
Yeny A. Tobon ◽  
Danielle El Hajj ◽  
Samantha Seng ◽  
Ferdaous Bengrad ◽  
Myriam Moreau ◽  
...  

Sodium chloride (NaCl) is the main constituent of sea-salt aerosols. During atmospheric transport, sea-salt aerosols can interact with gases and other particles including secondary aerosols containing ammonium sulfate ((NH4)2SO4). This...


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