To investigate the influence of pollution events on the chemical composition and formation processes of aerosol particles, 24-h integrated size-segregated particulate matter (PM) was collected during the fall season at an urban site of Gwangju, Korea and was used to determine the concentrations of mass, water-soluble organic carbon (WSOC) and ionic species. Furthermore, black carbon (BC) concentrations were observed with an aethalometer. The entire sampling period was classified into four periods, i.e., typical, pollution event I, pollution event II, and an Asian dust event. Stable meteorological conditions (e.g., low wind speed, high surface pressure, and high relative humidity) observed during the two pollution events led to accumulation of aerosol particles and increased formation of secondary organic and inorganic aerosol species, thus causing $PM_{2.5}$ increase. Furthermore, these stable conditions resulted in the predominant condensation or droplet mode size distributions of PM, WSOC, $NO_3{^-}$, and $SO{_4}^{2-}$. However, difference in the accumulation mode size distributions of secondary water-soluble species between pollution events I and II could be attributed to the difference in transport pathways of air masses from high-pollution regions and the formation processes for the secondary chemical species. The average absorption ${\AA}ngstr{\ddot{o}}m$ exponent ($AAE_{370-950}$) for 370-950 nm wavelengths > 1.0 indicates that the BC particles from traffic emissions were likely mixed with light absorbing brown carbon (BrC) from biomass burning (BB) emissions. It was found that light absorption by BrC in the near UV range was affected by both secondary organic aerosol and BB emissions. Overall, the pollution events observed during fall at the study site can be due to the synergy of unfavorable meteorological conditions, enhanced secondary formation, local emissions, and long-range transportation of air masses from upwind polluted areas.
To investigate the environmental adaptation and ecophysiological characteristics of Suaeda maritima and S. asparagoides under saline conditions, plant growth and density were analyzed according to environmental changes of habitats. The total ion content of soil decreased with time, which was caused by the predominance of exchangeable $Na^+$ and $Cl^-$ in the upper layers. The population of S. maritima was more densely distributed in the region with higher ion contents of $Cl^-$, $Mg^{2+}$, $K^+$ and $Na^+$ than the population of S. asparagoides. Both species were showed a decreased population density according to increases in plant growth. Under the conditions of a salt field, S. maritima and S. asparagoides contained high inorganic ions to maintain low water potential, but low water soluble carbohydrate contents. In the case of free amino acid, S. maritima showed an especially high proline content, and contained rather large amounts of free amino acids, whereas S. asparagoides did not. Both species showed high inorganic ion contents in the leaves, which might be a mechanism of avoiding the ionic toxicity by diluting the accumulated ionic concentration with a high ratio of water content to dry weight. This result suggests that S. maritima seems to adapt to saline conditions by accumulating proline in addition to inorganic ions. S. asparagoides seems to adapt by osmoregulation processes, using inorganic ions rather than free amino acids.
Saturated n-dicarboxylic acids ($C_2-C_7$, $C_9$), unsaturated dicarboxylic acids (maleic, fumaric, phthalic acid), ketocarboxylic acids (pyruvic, glyoxylic acid), and dicarbonyls (glyoxal, methylglyoxal) were determined in size-segregated samples with a high-volume Andersen air sampler at a suburban site in Saitama, Japan, May 12-17 and July 24-27, 2007 and January 22-31, 2008. The seasonal average concentrations of these detected organic acids were 670 $ng/m^3$, accounting for about 4.4-5.7% (C/C) of water-soluble organic carbon (WSOC) and 2.3-3.6% (C/C) of organic carbon (OC). The most abundant species of dicarboxylic acids was oxalic acid, followed by malonic, phthalic, or succinic acids. Glyoxylic acid and methyglyoxal were most abundant ketocarboxylic acid and dicarbonyl, respectively. Seasonal differences, size-segregated concentrations, and the correlations of these acids with ambient temperatures, oxidants, elemental carbon (EC), OC, WSOC, and ionic components were also discussed in terms of their corresponding sources and possible secondary formation pathways. The results suggested that photochemical reactions contributed more to the formation of particulate organic acids in Saitama suburban areas than did direct emissions from anthropogenic and natural sources. However, direct emissions of vehicles were also important sources of several organic acids in particles, such as phthalic and adipic acids, especially in winter.
A number of field studies have provided evidence that biomass burning is one of the major global sources of atmospheric particles. In this study, we have collected $PM_{2.5}$ emitted from biomass burning combusted at open burning and laboratory chamber situations. The open burning experiment was conducted with the cooperation of 9 farmers in Chiba Prefecture, Japan, while the chamber experiment was designed to evaluate the characteristics of chemical components among 14 different plant species. The analyzed categories were $PM_{2.5}$ mass concentration, organic carbon (OC), elemental carbon (EC), ionic components ($Na^+$, ${NH_4}^+$, $Ca^{2+}$, $Mg^{2+}$, $K^+$, $Cl^-$, ${NO_3}^-$ and ${SO_4}^{2-}$), water-soluble organic carbon (WSOC), water-insoluble inorganic carbon (WIOC), char-EC and soot-EC. OC was the dominant chemical component, accounting for the major fraction of primary $PM_{2.5}$ derived from biomass burning, followed by EC. Ionic components contributed a small portion of $PM_{2.5}$, as well as that of $K^+$. In some cases, $K^+$ is used as biomass burning tracer; however, the observations obtained in this study suggest that $K^+$ may not always be suitable as a tracer for biomass burning emissions. Also, the results of all the samples tested indicate relatively low values of char-EC compared to soot-EC. From our results, careful consideration should be given to the usage of $K^+$ and char-EC as indicators of biomass burning. The calculated ratios of WSOC/OC and WIOC/OC were 55.7% and 44.3% on average for all samples, which showed no large difference between them. The organic materials to OC ratio, which is often used for chemical mass closure model, was roughly estimated by two independent methods, resulting in a factor of 1.7 for biomass burning emissions.
This study observed particulate matter ($PM_{2.5}$ and $PM_{10}$) in the downtown area of Jeju City, South Korea, to understand the chemical composition of particulates based on an analysis of the water-soluble ionic species contained in the particles. The mass fraction of the ionic species in the sampled $PM_{10}$ and $PM_{2.5}$ was 44.3% and 42.2%, respectively. In contrast, in Daegu City and Suwon City, the mass fraction of the ionic species in $PM_{2.5}$ was higher than that in $PM_{10}$. The chloride depletion percentage of $PM_{10}$ and $PM_{2.5}$ in Jeju City was higher than 61% and 66%, respectively. The contribution of sea-salt to the mass of $PM_{10}$ (5.9%) and $PM_{2.5}$ (2.6%) in Jeju City was similar to that in several coastal regions of South Korea. The mass ratio of $Cl^-$ to $Na^+$ in the downtown area of Jeju City was comparable to that in some coastal regions, such as the Gosan Area of Jeju Island, Deokjeok Island, and Taean City. The mass fraction of sea-salt in $PM_{10}$ and $PM_{2.5}$ was very low, and the concentration of sodium and chloride ions in $PM_{10}$ was not correlated with those in $PM_{2.5}$ ($R^2$ < 0.2), suggesting that the effects of sea-salt on the formation of particulate matter in Jeju City might be insignificant. The relationship between $NH_4{^+}$ and several anions such as $SO_4{^{2-}}$, $NO_3{^-}$, and $Cl^-$, as well as the relationship between the measurement and calculation of ammonium ion concentration, suggested that sea-salts may not react with $H_2SO_4$, and $(NH_4)_2SO_4$ may be a major secondary inorganic aerosol component of $PM_{2.5}$ and $PM_{10}$ in Jeju City.
Premicellar precipitation, resolubilization and luminescing behaviors of $RuL_3^{2+}$ (L = bpy, phen, $Me_2bpy$) in aqueous alkylsulfate and sulfonate solutions were studied. Addition of the anionic surfactants to $RuL_3\;^{2+}$ solutions caused initial precipitation which was redissolved by further addition of the surfactants. The apparent solubility products $K_{sp}$'s of the precipitates were evaluated assuming 1:2 salt formation. The values were smaller as the ligand is more hydrophobic and the length of hydrocarbon chain of the surfactant is longer. The $K_{sp}$ values for L = bpy were constant over wide surfactant concentration range. However, those for L = $Me_2bpy$ and also for phen, but to less extent, increased with the surfactant concentration. The resolubilization of 1:2 salts was followed by red-shift of emission band and extensive emission quenching above critical concentration of the surfactants. The critical concentration was lower for more hydrophobic surfactant. For L = $Me_2bpy$, the blue-shifted emission band with enhanced emission intensity was observed in intermediate surfactant concentration region. The high ionic strength of media prevented the precipitate formation, but facilitated the red-shift of the emission bands. The results support that the precipitate is dissolved by accretion of surfactant anions to the salts to form water-soluble surfactant-rich $RuL_3$-surfactant anionic species. These species appeared to aggregate cooperatively to produce large clusters which exhibited the red-shifted emission.
Little information on HUmic-Like Substances (HULIS) in ambient particulate matter has been reported yet in Korea. HULIS makes up a significant fraction of the water-soluble organic mass in the atmospheric aerosols and influence their water uptake properties. In this study 24-hr $PM_{2.5}$ samples were collected between December 2013 and October 2014 at an urban site in Gwangju and analyzed for organic carbon (OC), elemental carbon (EC), water-soluble OC (WSOC), HULIS, and ionic species, to investigate possible sources and formation processes of HULIS. HULIS was separated using solid phase extraction method and quantified by total organic carbon analyzer. During the study period, HULIS concentration ranged from 0.19 to $5.65{\mu}gC/m^3$ with an average of $1.83{\pm}1.22{\mu}gC/m^3$, accounting for on average 45% of the WSOC (12~ 73%), with higher in cold season than in warm season. Strong correlation of WSOC with HULIS ($R^2=0.91$) indicates their similar chemical characteristics. On the basis of the relationships between HULIS and a variety of chemical species (EC, $K^+$, $NO_3{^-}$, $SO_4{^{2-}}$, and oxalate), it was postulated that HULIS observed during summer and winter were likely attributed to secondary formation and primary emissions from biomass burning (BB) and traffics. Stronger correlation of HULIS with $K^+$, which is a BB tracer, in winter ($R^2=0.81$) than in summer ($R^2=0.66$), suggests more significant contribution of BB emissions in winter to the observed HULIS. It is interesting to note that BB emissions may also have an influence on the HULIS in summer, but further study using levoglucosan that is a unique organic marker of BB emissions is required during summer. Higher correlation between HULIS and oxalate, which is mainly formed through cloud processing and/or photochemical oxidation processes, was found in the summer ($R^2=0.76$) than in the winter ($R^2=0.63$), reflecting a high fraction of secondary organic aerosol in the summer.
In order to investigate the chemical components of acid precipitation at Kangwha near the Yellow Sea and Seoul in Korea, the precipitation samples were collected by wetonly precipitation sampler from February 1991 to January 1992, and pH, electric conductivity(E. C.) and major water-soluble ionic components were analyzed. Strong negative linear correlations were observed between the rainfall amount and the sum of major ionic components in $\mu eq/\ell$ at two sites. The sum of major ionic components also correlated negatively with rain intensity. The analytical results of precipitation samples at two sites were compared each other. Average values of volume-weighted pH were found to be 5.21 at Kangwha and 5.09 at Seoul. The cationic abundance($\mu eq/\ell$) in rainwater showed the general trend $NH_4^+ > Na^+ > Ca^{2+} > Mg^{2-+} > H^+ > K^+$ at Kangwah and $NH_4^+ > Ca^{2+} > Na^+ > H^+ > Mg^{2+} > K^+$ at Seoul. The anionic abundance showed the general trend $SO_4^{2-} > Cl^- > NO_3^-$ at Kangwha and $SO_4^{2-} > NO_3^- > Cl^-$ at Seoul. The concentrations of seasalt such as $Na^+ and Cl^-$ were higher at Kangwha than Seoul. The concentrations of $nss-SO_4^{2-}, nss-Cl^- and NO_3^-$ which are acid composition were higher at Seoul(96.3 $\mu eq/\ell$) than Kangwha(69.0 $\mu eq/\ell$). The contribution of seasalt to the composition of precipitation were higher at Kangwha(34.1%) than Seoul(15.7%). Ammonia and calcium species in rainwater at Kangwha and Seoul are interpreted to have 91% of neutralizing capacity of the original sulfuric and nitric acids. Provided that the precipitation acidity originates primarily from sulfate and nitrate, sulfate was found to contribute about 73-75% of the free precipitation acidity.
To determine the size distributions of water-soluble inorganic ionic species (WSIS) in roadside aerosols, sampling experiments were carried out in the urban roadside area of Jeju City on August 2018 and January 2019 by using the eight-stage cascade impactor sampler. The mass of roadside aerosols were partitioned at 57% in fine fraction, 36-37% in coarse fraction, and 6-7% in giant fraction, regardless of summer and winter. The mass concentrations of WSIS except for Na+ and SO42- in roadside aerosols were higher in winter than in summer. The size distributions of Na+, Mg2+, Ca2+ and Cl- were characterized by bimodal types with coarse particle mode peaking around 3.3-4.7 ㎛ and 5.8-9.0 ㎛. The size distributions of NO3- and K+ shifted from a single fine mode peaking around 0.7-1.1 ㎛ in winter to bimodal and/or trimodal types with peaks around coarse mode in summer. SO42- and NH4+ showed a single fine mode peaking around 0.7-1.1 ㎛. The MMAD of roadside aerosols was lower than that of Na+, Mg2+, Ca2+ and Cl-. Based on the marine enrichment factors and the ratio values of WSIS and the corresponding value for sea water, the composition of roadside aerosols in Jeju City may be practically affected by terrestrial sources rather than marine source.
In this study, hourly measurements of $PM_{2.5}$ and its major chemical constituents such as organic and elemental carbon (OC and EC), and ionic species were made between January 15 and February 10, 2018 at the air pollution intensive monitering station in Gwangju. In addition, 24-hr integrated $PM_{2.5}$ samples were collected at the same site and analyzed for OC, EC, water-soluble OC (WSOC), humic-like substance (HULIS), and ionic species. Over the whole study period, the organic aerosols (=$1.6{\times}OC$) and $NO_3{^-}$ concentrations contributed 26.6% and 21.0% to $PM_{2.5}$, respectively. OC and EC concentrations were mainly attributed to traffic emissions with some contribution from biomass burning emissions. Moreover, strong correlations of OC with WSOC, HULIS, and $NO_3{^-}$ suggest that some of the organic aerosols were likely formed through atmospheric oxidation processes of hydrocarbon compounds from traffic emissions. For the period between January 18 and 22 when $PM_{2.5}$ pollution episode occurred, concentrations of three secondary ionic species ($=SO{_4}^{2-}+NO_3{^-}+NH_4{^+}$) and organic matter contributed on average 50.8 and 20.1% of $PM_{2.5}$, respectively, with the highest contribution from $NO_3{^-}$. Synoptic charts, air mass backward trajectories, and local meteorological conditions supported that high $PM_{2.5}$ pollution was resulted from long-range transport of haze particles lingering over northeastern China, accumulation of local emissions, and local production of secondary aerosols. During the $PM_{2.5}$ pollution episode, enhanced $SO{_4}^{2-}$ was more due to the long-range transport of aerosol particles from China rather than local secondary production from $SO_2$. Increasing rate in $NO_3{^-}$ was substantially greater than $NO_2$ and $SO{_4}^{2-}$ increasing rates, suggesting that the increased concentration of $NO_3{^-}$ during the pollution episode was attributed to enhanced formation of local $NO_3{^-}$ through heterogenous reactions of $NO_2$, rather than impact by long-range transportation from China.
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