scholarly journals High time-resolution chemical characterization of the water-soluble fraction of ambient aerosols with PILS-TOC-IC and AMS

2010 ◽  
Vol 3 (4) ◽  
pp. 1063-1074 ◽  
Author(s):  
H. Timonen ◽  
M. Aurela ◽  
S. Carbone ◽  
K. Saarnio ◽  
S. Saarikoski ◽  
...  

Abstract. A particle-into-liquid sampler (PILS) was coupled with a total organic carbon analyzer (TOC) and two ion chromatographs (IC) to enable high time-resolution measurements of water-soluble ions and water-soluble organic carbon (WSOC) by a single sampling and analytical set-up. The new high time-resolution measurement system, the PILS-TOC-IC, was able to provide essential chemical and physical information about fast changes in composition, concentrations and likely sources of the water-soluble fraction of atmospheric aerosol. The concentrations of major water-soluble ions and WSOC were measured by the PILS-TOC-IC system from 25 April to 28 May 2009. The data of the PILS-TOC-IC setup was compared with the data from the High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) data measured from 25 April to 8 May 2009. The measured water-soluble particulate organic matter (WSPOM) concentration varied typically from 0.10 to 8.8 μg m−3 (on average 1.5 μg m−3). The WSPOM contributed on average 51% to particulate organic matter (POM) measured with the AMS. The correlation between the data of all the online measurement devices (AMS, PILS-TOC-IC, semicontinuous EC/OC carbon analyzer and TEOM) was excellent. For sulfate, nitrate and ammonium the correlations between the PILS-TOC-IC and AMS were 0.93, 0.96 and 0.96, respectively. The correlation between WSPOM and POM was also strong (r = 0.88). The identified sources of WSPOM were long-range transported biomass burning and secondary organic aerosol (SOA) formation. WSPOM and oxalate produced in biomass burning were clearly correlated with carbon monoxide.

2010 ◽  
Vol 3 (2) ◽  
pp. 1775-1805 ◽  
Author(s):  
H. Timonen ◽  
M. Aurela ◽  
S. Carbone ◽  
K. Saarnio ◽  
S. Saarikoski ◽  
...  

Abstract. A particle-into-liquid sampler (PILS) was coupled with a total organic carbon analyzer (TOC) and two ion chromatographs (IC) to enable high time-resolution measurements of water-soluble ions and water-soluble organic carbon (WSOC) by a single sampling and analytical set-up. The new high time-resolution measurement system, the PILS-TOC-IC, was able to provide essential chemical and physical information about fast changes in composition, concentrations and likely sources of the water-soluble fraction of atmospheric aerosol. The concentrations of major water-soluble ions and WSOC were measured by the PILS-TOC-IC system from 25 April to 28 May 2009. The data of the PILS-TOC-IC setup was completed with the data from the High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) data measured from 25 April to 8 May 2009. The measured water-soluble particulate organic matter (WSPOM) concentration varied typically from 0.10 to 8.8 µg m−3 (on average 1.5 µg m−3). The WSPOM contributed on average 51% to particulate organic matter (POM) measured with the AMS. The correlation between the data of all the online measurement devices (AMS, PILS-TOC-IC, semicontinous EC/OC carbon analyzer and TEOM) was excellent. For sulfate, nitrate and ammonium the correlations between the PILS-TOC-IC and AMS were 0.93, 0.96 and 0.96, respectively. The correlation between WSPOM and POM was also strong (r=0.88). The identified sources of WSPOM were long-range transported biomass burning and secondary organic aerosol (SOA) formation. The WSPOM/POM-ratio followed the trends of the ambient daytime temperature. The temperature dependency of the WSPOM/POM-ratio suggest that in the absence of emissions from biomass burning, the SOA formation was the prevailing source for WSPOM. WSPOM produced in biomass burning was clearly correlated with carbon monoxide, confirming that biomass burning was producing primary WSPOM. In addition, elevated oxalate and potassium concentrations were measured during the biomass burning episode.


2018 ◽  
Vol 233 ◽  
pp. 1177-1187 ◽  
Author(s):  
Jian Xu ◽  
Qiongzhen Wang ◽  
Congrui Deng ◽  
V. Faye McNeill ◽  
Alison Fankhauser ◽  
...  

Atmosphere ◽  
2019 ◽  
Vol 10 (7) ◽  
pp. 397 ◽  
Author(s):  
Zhengxu Gao ◽  
Xiaoling Wang ◽  
Lijuan Shen ◽  
Hua Xiang ◽  
Honglei Wang

As the new core region of the haze pollution, the terrain effect of sub-basin and water networks over the Twin-Hu Basin (THB) in the Yangtze River Middle-Reach (YRMR) had great impacts on the variations and distributions of air pollutants. In this study, trace gases (NH3, HNO3, and HCl), water-soluble ions (WSIs), organic carbon (OC), and elemental carbon (EC) were measured in PM2.5 from 9 January to 27 January 2018, in Wuhan using monitoring for aerosols and gases (MARGA) and a semi-continuous OC/EC analyzer (Model RT-4). The characteristics of air pollutants during a haze episode were discussed, and the PM2.5 sources were quantitatively analyzed on haze and non-haze days using the principal component analysis/absolute principal component scores (PCA/APCS) model. The average PM2.5 concentration was 122.61 μg·m−3 on haze days, which was 2.20 times greater than it was on non-haze days. The concentrations of secondary water soluble ions (WSIs) including NO3−, SO42−, and NH4+ increased sharply on haze days, which accounted for 91.61% of the total WSIs and were 2.43 times larger than the values on non-haze days. The heterogeneous oxidation reactions of NO2 and SO2 during haze episodes were proven to be the major sources of sulfate and nitrate in PM2.5. On haze days, the concentrations of EC, primary organic carbon (POC), and secondary organic carbon (SOC) were 1.68, 1.69, and 1.34 times larger than those on non-haze days, the CO, HNO3, and NH3 concentrations enhanced and relatively low SO2, O3, and HNO2 levels were observed on haze days. The diurnal variations of different pollutants distinctly varied on haze days. The PM2.5 in Wuhan primarily originated from the secondary formation, combustion, dust, industry, and vehicle exhaust sources. The source contributions of the secondary formation + combustion sources to PM2.5 on haze days were 2.79 times larger than the level on non-haze days. The contribution of the vehicle exhaust + combustion source on haze days were 0.59 times the value on non-haze days. This description is supported by a summary of how pollutant concentrations and patterns vary in the THB compared to the variations in other pollution regions in China, which have been more completely described.


2018 ◽  
Author(s):  
Ke Zhang ◽  
Lijun Han ◽  
Sumei Liu ◽  
Lingyan Wang

Abstract. A series of high time-resolution nutrient dissolution experiments were designed to determine the soluble fraction of atmospheric nutrients and reveal the short-time dissolution processes, patterns and kinetics of nutrient elements in aerosols. Aerosols that represented an important part of atmospheric transport path over the East Asian to West Pacific were leached by Milli-Q water and aged seawater at gradient pHs for certain time duration. Varied nutrient dissolution curves indicated that aerosol inorganic N, P and Si species dissolution reactions were quasi-first-order. Particularly, prominent factors influenced P solubility were source and acidity. Ratios of acid-soluble to water-soluble nutrient concentrations in high time-resolution dissolution experiments and ultra-sound extractions were 1.0 (0.9–1.1) for NH4+ and NO3−, 2.4 (2.1–2.6) for PO43− and 2.5 for SiO32−, demonstrating that inorganic N species were inclined to immediate and complete dissolution due to fine particles formed by gas-particle transformation, inorganic P (Fe-P, Ca-P and De-P) and Si were tended to dissolve more in strong acidity mainly because of coarse soil-derived mineral particles. Compared with the slow dissolution of inorganic P and Si, the rapid dissolution of inorganic N can affect the composition of marine nutrients and marine primary productivity.


2017 ◽  
Vol 17 (18) ◽  
pp. 11591-11604 ◽  
Author(s):  
Jing Chen ◽  
Sri Hapsari Budisulistiorini ◽  
Masayuki Itoh ◽  
Wen-Chien Lee ◽  
Takuma Miyakawa ◽  
...  

Abstract. The relationship between hygroscopic properties and chemical characteristics of Indonesian biomass burning (BB) particles, which are dominantly generated from peatland fires, was investigated using a humidified tandem differential mobility analyzer. In addition to peat, acacia (a popular species at plantation) and fern (a pioneering species after disturbance by fire) were used for experiments. Fresh Indonesian peat burning particles are almost non-hygroscopic (mean hygroscopicity parameter, κ < 0.06) due to predominant contribution of water-insoluble organics. The range of κ spans from 0.02 to 0.04 (dry diameter = 100 nm, hereinafter) for Riau peat burning particles, while that for Central Kalimantan ranges from 0.05 to 0.06. Fern combustion particles are more hygroscopic (κ = 0. 08), whereas the acacia burning particles have a mediate κ value (0.04). These results suggest that κ is significantly dependent on biomass types. This variance in κ is partially determined by fractions of water-soluble organic carbon (WSOC), as demonstrated by a correlation analysis (R = 0.65). κ of water-soluble organic matter is also quantified, incorporating the 1-octanol–water partitioning method. κ values for the water extracts are high, especially for peat burning particles (A0 (a whole part of the water-soluble fraction): κ = 0.18, A1 (highly water-soluble fraction): κ = 0.30). This result stresses the importance of both the WSOC fraction and κ of the water-soluble fraction in determining the hygroscopicity of organic aerosol particles. Values of κ correlate positively (R = 0.89) with the fraction of m∕z 44 ion signal quantified using a mass spectrometric technique, demonstrating the importance of highly oxygenated organic compounds to the water uptake by Indonesian BB particles. These results provide an experimentally validated reference for hygroscopicity of organics-dominated particles, thus contributing to more accurate estimation of environmental and climatic impacts driven by Indonesian BB particles on both regional and global scales.


2020 ◽  
pp. geochem2020-052
Author(s):  
I.N. Myagkaya ◽  
B.Yu. Saryg-ool ◽  
Oleg N. Surkov ◽  
S.M. Zhmodik ◽  
E.V. Lazareva ◽  
...  

We study the contents of elements and group composition in natural organic matter (NOM) that interacts with acid mine drainage (АMD) and high-sulfide tailings at the Ursk site (Southwestern Siberia, Russia). AMD causes biomass changes in NOM, related changes in the composition of fractions, and hydrolysis of hydrolyzable compounds; it increases the water-soluble fraction and maintains depolymerization of humic acids to fulvic acids, but exerts no effect on substances soluble in organics (bitumen) and on poorly hydrolyzable compounds. Accumulation of inorganic elements and precipitation of minerals obscure the true fraction composition of NOM: the superposed mineral component contributes significantly to the water-soluble, humic acid, hydrolyzable, and non-hydrolyzable fractions, and may reach 26.4 % per total of all fractions. Rock-forming and potentially toxic elements partition among NOM fractions and predominate in the water-soluble fraction. The contents of Au and Ag are the highest in the fractions of humic acids and hydrolyzable compounds but are lower in the non-hydrolyzable residue. The obtained data have implications for possible migration of potentially toxic elements and noble metals and thus for remediation of polluted areas. The observed fractionation of Ag and Au in NOM helps understand the mechanisms of their distribution in organic-bearing environments, such as peatlands or coal basins.


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