scholarly journals Water-Soluble Ionic Characteristics of Aerosols in the Marine Boundary Layer over the Yellow Sea during the KORUS-AQ Campaign

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.

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.


2015 ◽  
Vol 72 (9) ◽  
pp. 3563-3573 ◽  
Author(s):  
Yan Zhang ◽  
Hong-Hai Zhang ◽  
Gui-Peng Yang ◽  
Qiu-Lin Liu

Abstract The total suspended particulate (TSP) samples over the Bohai Sea and the Yellow Sea were collected during two cruises in spring and autumn in 2012. Concentrations of water-soluble ions {Na+, K+, NH4+, Mg2+, Ca2+, Cl−, NO3 −, SO42−, and CH3SO3 − [methanesulfonic acid (MSA)]} and trace metals (Al, Pb, Zn, Cd, Cu, and V) were measured. Mass concentrations of TSP samples ranged from 65.2 to 136 μg m−3 in spring and from 15.9 to 70.3 μg m−3 in autumn, with average values of 100 ± 22.4 and 40.2 ± 17.8 μg m−3, respectively. The aerosol was acidic throughout the sampling periods according to calculation of equivalent concentrations of the cations (NH4+, nss-Ca2+, and nss-K+) and anions (nss-SO42− and NO3 −). Correlation analysis and enrichment factors revealed that the aerosol composition in the coastal marine atmosphere had a feature of a mixture of air masses: that is, crustal, marine, and anthropogenic emissions. Trace metals were enriched by a wide range of 1–103, and enrichment factors for crustal source (EFc) were relatively higher in spring. Species like Cd, Zn, and Pb had an overwhelming contribution from anthropogenic sources. In addition, the concentrations of MSA varied from 0.0075 to 0.17 and from 0.0019 to 0.018 μg m−3 during the spring and autumn cruises, respectively, with means of 0.061 and 0.012 μg m−3, respectively. Based on the observed MSA and nss-SO42− concentrations in spring and autumn, the relative biogenic sulfur contributions to nss-SO42− were estimated to be 8.0% and 3.5% on average, respectively, implying that anthropogenic sources had a dominant contribution to the sulfur budget over the observational area.


2012 ◽  
Vol 117 (D17) ◽  
pp. n/a-n/a ◽  
Author(s):  
Jin-Hui Shi ◽  
Hui-Wang Gao ◽  
Jing Zhang ◽  
Sai-Chun Tan ◽  
Jing-Ling Ren ◽  
...  

Atmosphere ◽  
2020 ◽  
Vol 11 (3) ◽  
pp. 310
Author(s):  
Hee-Jung Ko ◽  
Seung Joo Song ◽  
Jeong Eun Kim ◽  
Jung-Min Song ◽  
Joo Wan Cha

This study focuses on the temporal variation in the compositional characteristics of atmospheric aerosols in Seoul, South Korea, during the consecutive high aerosol concentration episode from 30 December 2013 to 2 January 2014. The temporal variations in the observed physical, optical, and chemical properties show that there were three distinct episodes during the period: haze, mixed haze/Asian dust, and Asian dust episodes. For the haze period, the concentration of secondary inorganic aerosols increased and both secondary inorganic aerosols and calcium species exhibited simultaneously high concentrations during the mixed haze/Asian dust period. The neutralization factors by ammonia in the haze periods were higher as 1.03 than the other periods, meanwhile the neutralization contribution by calcium carbonate was relatively higher as 1.39 during the Asian dust episode. The backward trajectory analysis showed that concentrations of SO42−, NO3−, and NH4+ were relatively high when air masses moved over East China. Principal component analysis showed that water-soluble components originated from soil dust/incineration, secondary aerosols/biomass burning, and road dust from the haze aerosol. For the mixed haze/Asian dust episode, the major source of aerosols was estimated to have originated from soil dust, pollutants from fossil fuel combustion, biomass burning, and sea-salt emissions. Furthermore, the main sources of ionic species in the Asian dust aerosols were estimated to be sea-salt/soil dust, secondary aerosols/coal combustion, and road dust.


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