scholarly journals Investigation of aged aerosols in size-resolved Asian dust storm particles transported from Beijing, China to Incheon, Korea using low-<i>Z</i> particle EPMA

2013 ◽  
Vol 13 (10) ◽  
pp. 27971-28016 ◽  
Author(s):  
H. Geng ◽  
H. J. Hwang ◽  
X. Liu ◽  
S. Dong ◽  
C.-U. Ro

Abstract. This is the first study of Asian dust storm (ADS) particles collected in Beijing, China and Incheon, Korea during the same spring ADS event. Using a seven-stage May impactor and a quantitative electron probe X-ray microanalysis (ED-EPMA, also known as low-Z particle EPMA), we examined the composition and morphology of 4200 aerosol particles at stages 1–6 (with a size cut-off of 16, 8, 4, 2, 1, and 0.5 μm in equivalent aerodynamic diameter, respectively) collected during an ADS event on 28–29 April 2005. The results showed that there were large differences in the chemical compositions between particles in sample S1 collected in Beijing immediately after the peak time of the ADS and in samples S2 and S3, which were collected in Incheon approximately 5 h and 24 h later, respectively. In sample S1, mineral dust particles accounted for more than 88% in relative number abundance at stages 1–5, and organic carbon (OC) and reacted NaCl-containing particles accounted for 24% and 32%, respectively, at stage 6. On the other hand, in samples S2 and S3, in addition to approximately 60% mineral dust, many sea salt particles reacted with airborne SO2 and NOx, often mixed with mineral dust, were encountered at stages 1–5, and (C, N, O, S)-rich particles (likely a mixture of water-soluble organic carbon with (NH4)2SO4 and NH4NO3) and K-containing particles were abundantly observed at stage 6. This suggests that the secondary aerosols and the internal mixture of mineral dust with sea spray aerosol increased when the ADS particles passed over the Yellow Sea. In the reacted or aged mineral dust and sea salt particles, nitrate-containing and both nitrate- and sulfate-containing species vastly outnumbered the sulfate-containing species, implying that ambient nitrogen oxides had a greater influence on the atmospheric particles during the ADS episode than SO2. In addition to partially- or totally-reacted CaCO3, reacted or aged Mg-containing aluminosilicates (likely including amesite, allophite, vermiculite, illite, and montmorillonite) were observed frequently in samples S2 and S3; and furthermore, both the atomic concentration ratios of [Mg]/[Al] and [Mg]/[Si] were elevated compared to that in sample S1. This shows that a great evolution or aging process must have occurred on the mineral dust. This indicates that the number abundance, reactivity with gaseous pollutants, and ratios of [Mg]/[Al] and [Mg]/[Si] of Mg-containing aluminosilicates are promising indices of the aging process of ADS particles during long-range transport.

2014 ◽  
Vol 14 (7) ◽  
pp. 3307-3323 ◽  
Author(s):  
H. Geng ◽  
H. Hwang ◽  
X. Liu ◽  
S. Dong ◽  
C.-U. Ro

Abstract. This is the first study of Asian dust storm (ADS) particles collected in Beijing, China, and Incheon, Korea, during a spring ADS event. Using a seven-stage May impactor and a quantitative electron probe X-ray microanalysis (ED-EPMA, also known as low-Z particle EPMA), we examined the composition and morphology of 4200 aerosol particles at stages 1–6 (with a size cut-off of 16, 8, 4, 2, 1, and 0.5 μm in equivalent aerodynamic diameter, respectively) collected during an ADS event on 28–29 April 2005. The results showed that there were large differences in the chemical compositions between particles in sample S1 collected in Beijing immediately after the peak time of the ADS and in samples S2 and S3, which were collected in Incheon approximately 5 h and 24 h later, respectively. In sample S1, mineral dust particles accounted for more than 88% in relative number abundance at stages 1–5; and organic carbon (OC) and reacted NaCl-containing particles accounted for 24% and 32%, respectively, at stage 6. On the other hand, in samples S2 and S3, in addition to approximately 60% mineral dust, many sea spray aerosol (SSA) particles reacted with airborne SO2 and NOx (accounting for 24% and 14% on average in samples S2 and S3, respectively), often mixed with mineral dust, were encountered at stages 1–5, and (C, N, O, S)-rich particles (likely a mixture of water-soluble organic carbon with (NH4)2SO4 and NH4NO3) were abundantly observed at stage 6 (accounting for 68% and 51% in samples S2 and S3, respectively). This suggests that an accumulation of sea-salt components on individual ADS particles larger than 1 μm in diameter occurred and many secondary aerosols smaller than 1 μm in diameter were formed when the ADS particles passed over the Yellow Sea. In the reacted or aged mineral dust and SSA particles, nitrate-containing and both nitrate- and sulfate-containing species vastly outnumbered the sulfate-containing species, implying that ambient NOx had a greater influence on the atmospheric particles than SO2 during this ADS episode. In addition to partially- or totally-reacted CaCO3, reacted or aged Mg-containing aluminosilicates were observed frequently in samples S2 and S3; furthermore, a student's t test showed that both their atomic concentration ratios of [Mg] / [Al] and [Mg] / [Si] were significantly elevated (P < 0.05) compared to those in samples S1 (for [Mg] / [Al], 0.34 ± 0.09 and 0.40 ± 0.03 in samples S2 and S3, respectively, vs. 0.24 ± 0.01 in sample S1; for [Mg] / [Si], 0.21 ± 0.05 and 0.22 ± 0.01 in samples S2 and S3, respectively, vs. 0.12 ± 0.02 in sample S1). The significant increase of [Mg] / [Al] and [Mg] / [Si] ratios in Mg-containing aluminosilicates indicates that a significant evolution or aging must have occurred on the ADS particles in the marine atmosphere during transport from China to Korea.


2021 ◽  
Vol 253 ◽  
pp. 105486
Author(s):  
Qingyang Liu ◽  
Yanjiu Liu ◽  
Qiang Zhao ◽  
Tingting Zhang ◽  
James J. Schauer

1998 ◽  
Vol 76 (2) ◽  
pp. 275-288 ◽  
Author(s):  
Noriko Niimura ◽  
Kikuo Okada ◽  
Xiao-Bio Fan ◽  
Kenji Kai ◽  
Kimio Arao ◽  
...  

2019 ◽  
Vol 56 (3) ◽  
pp. 467-483
Author(s):  
Joo Wan Cha ◽  
Beomchel Shin ◽  
Hee-Jung Ko ◽  
Yun Kyu Lim ◽  
Sang-Boom Ryoo

AbstractMajor compositions of water-soluble ionic species in particulate matter less than 10 and 2.5 μm in diameter (PM10 and PM2.5, respectively) over the Yellow Sea were collected during the Korea–United States Air Quality (KORUS-AQ) campaign in 2016 onboard the research vessel Gisang 1. The secondary ionic species (NH4+, nss-SO42−, and NO3−) in PM10 and PM2.5 accounted for 84% and 89% of the total analyzed species. NH4+ was strongly correlated with non-sea salt (nss) SO42− (nss-SO42−) in PM10 and PM2.5; NO3− was closely correlated with Na+, Mg2+, and nss-Ca2+ in PM10 and NH4+ in PM2.5. High mass concentrations of methane sulfonic acid (MSA, CH3SO3−), the main source of natural sulfates over the Yellow Sea, were observed. The concentrations of MSA were found to show an increasing trend over the Yellow Sea in recent years. Biogenic sulfur contributions to the total nss-SO42− (MSA/nss-SO42− ratio) over the Yellow Sea ranged from 1.4% to 9.2% in PM10 and from 0.68% to 9.5% in PM2.5 during the cruise. Thus, biogenic nss-SO42− must be included, especially in the spring and early summer seasons, when biological activities are elevated in Northeast Asia. We classified the high aerosol mass concentration cases such as Asian dust and haze cases. In Asian dust cases, the ratio of NO3− to nss-SO42− in the aerosols showed that mobile (stationary) sources mainly affected PM10 (PM2.5). The major chemical species for Asian dust cases over the Yellow sea were CaCO3, Ca(NO3)2, Mg(NO3)2, Na(NO3)2, and sea salt. In haze cases over the Yellow sea, the contributions from stationary sources are high and the major species were (NH4)2SO4 and NH4NO3 in PM10 and PM2.5, respectively.


1994 ◽  
Vol 72 (5) ◽  
pp. 777-784 ◽  
Author(s):  
Noriko Niimura ◽  
Kikuo Okada ◽  
Xiao-Bio Fan ◽  
Kenji Kai ◽  
Kimio Arao ◽  
...  

2014 ◽  
Vol 14 (21) ◽  
pp. 11571-11585 ◽  
Author(s):  
G. H. Wang ◽  
C. L. Cheng ◽  
Y. Huang ◽  
J. Tao ◽  
Y. Q. Ren ◽  
...  

Abstract. A total suspended particulate (TSP) sample was collected hourly in Xi'an, an inland megacity of China near the Loess Plateau, during a dust storm event of 2013 (9 March 18:00−12 March 10:00 LT), along with a size-resolved aerosol sampling and an online measurement of PM2.5. The TSP and size-resolved samples were determined for elemental carbon (EC), organic carbon (OC), water-soluble organic carbon (WSOC) and nitrogen (WSON), inorganic ions and elements to investigate chemistry evolution of dust particles. Hourly concentrations of Cl−, NO3−, SO42−, Na+ and Ca2+ in the TSP samples reached up to 34, 12, 180, 72 and 28 μg m−3, respectively, when dust peak arrived over Xi'an. Chemical compositions of the TSP samples showed that during the whole observation period NH4+ and NO3− were linearly correlated with each other (r2=0.76) with a molar ratio of 1 : 1, while SO42− and Cl− were well correlated with Na+, Ca2+, Mg2+ and K+ (r2 > 0.85). Size distributions of NH4+ and NO3− presented a same pattern, which dominated in the coarse mode (> 2.1 μm) during the event and predominated in the fine mode (< 2.1 μm) during the non-event. SO42− and Cl− also dominated in the coarse mode during the event hours, but both exhibited two equivalent peaks in both the fine and the coarse modes during the non-event, due to the fine-mode accumulations of secondarily produced SO42− and biomass-burning-emitted Cl- and the coarse-mode enrichments of urban soil-derived SO42− and Cl−. Linear fit regression analysis further indicated that SO42− and Cl− in the dust samples possibly exist as Na2SO4, CaSO4 and NaCl, which directly originated from Gobi desert surface soil, while NH4+ and NO3− in the dust samples exist as NH4NO3. We propose a mechanism to explain these observations in which aqueous phase of dust particle surface is formed via uptake of water vapor by hygroscopic salts such as Na2SO4 and NaCl, followed by heterogeneous formation of nitrate on the liquid phase and subsequent absorption of ammonia. Our data indicate that 54 ± 20% and 60 ± 23% of NH4+ and NO3− during the dust period were secondarily produced via this pathway, with the remaining derived from the Gobi desert and Loess Plateau, while SO42− in the event almost entirely originated from the desert regions. Such cases are different from those in the East Asian continental outflow region, where during Asia dust storm events SO42− is secondarily produced and concentrates in sub-micrometer particles as (NH4)2SO4 and/or NH4HSO4. To the best of our knowledge, the current work for the first time revealed an infant state of the East Asian dust ageing process in the regions near the source, which is helpful for researchers to understand the panorama of East Asian dust ageing process from the desert area to the downwind region.


2012 ◽  
Vol 12 (24) ◽  
pp. 11985-11995 ◽  
Author(s):  
W. Nie ◽  
T. Wang ◽  
L. K. Xue ◽  
A. J. Ding ◽  
X. F. Wang ◽  
...  

Abstract. Heterogeneous processes on dust particles are important for understanding the chemistry and radiative balance of the atmosphere. This paper investigates an intense Asian dust storm episode observed at Mount Heng (1269 m a.s.l.) in southern China on 24–26 April 2009. A set of aerosol and trace gas data collected during the study was analyzed to investigate their chemical evolution and heterogeneous photochemistry as the dust traveled to southern China. Results show that the mineral dust arriving at Mt. Heng experienced significant modifications during transport, with large enrichments in secondary species (sulfate, nitrate, and ammonium) compared with the dust composition collected at an upwind mountain top site (Mount Hua). A photochemical age "clock" (−Log10(NOx/NOy)) was employed to quantify the atmospheric processing time. The result indicates an obvious increase in the abundance of secondary water-soluble ions in dust particles with the air mass atmospheric processing time. Based on the observations, a 4-stage evolution process is proposed for carbonate-containing Asian dust, starting from fresh dust to particles coated with hydrophilic and acidic materials. Daytime-enhanced nitrite formation on the dust particles was also observed, which indicates the recent laboratory result of the TiO2 photocatalysis of NO2 as a potential source of nitrite and nitrous acid.


2012 ◽  
Vol 12 (8) ◽  
pp. 19135-19161
Author(s):  
W. Nie ◽  
T. Wang ◽  
L. K. Xue ◽  
A. J. Ding ◽  
X. F. Wang ◽  
...  

Abstract. Heterogeneous processes on dust particles are important for understanding the chemistry and radiative balance of the atmosphere. This paper investigates an intense Asian dust storm episode observed at Mount Heng (1250 m a.s.l.) in Southern China on 24–26 April 2009. A set of aerosol and trace gas data collected during the study was analyzed to investigate their chemical evolution and heterogeneous photochemistry as the dust traveled to Southern China. Results show that the mineral dust arriving at Mt. Heng experienced significant modifications during transport, with large enrichments in secondary species (sulfate, nitrate, and ammonium) compared with the dust composition collected at an upwind mountain top site (Mount Hua). A photochemical age "clock" (−log10(NOx/NOy)) was employed to quantify the atmospheric processing time. The result indicates an obvious increase in the abundance of secondary water-soluble ions in dust particles with the air mass' photochemical age. Based on the observations, a 4-stage evolution process is proposed for carbonate-rich Asian dust, starting from fresh dust to particles coated with hydrophilic and acidic materials. Daytime-enhanced nitrite formation on the dust particles was also observed, which indicates the recent laboratory result of the TiO2 photocatalysis of NO2 as a potential source of nitrite and nitrous acid.


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