scholarly journals Particle size-dependent fluorescence properties of water-soluble organic compounds (WSOC) and their atmospheric implications on the aging of WSOC

2021 ◽  
Author(s):  
Juanjuan Qin ◽  
Jihua Tan ◽  
Xueming Zhou ◽  
Yanrong Yang ◽  
Yuanyuan Qin ◽  
...  

Abstract. Water-soluble organic compounds (WSOC) are essential in atmospheric particle formation, migration, and transformation processes. Size-segregated atmospheric particles were collected in a rural area of Beijing. Excitation-emission matrix (EEM) fluorescence spectroscopy was used to investigate the sources and optical properties of WSOC. Sophisticated data analysis on EEM data was performed to characteristically estimate the underlying connections among aerosol particles in different sizes. The WSOC concentrations and average fluorescence intensity (AFI) showed monomodal distribution in winter and bimodal distribution in summer, with dominant mode between 0.26 to 0.44 µm for both seasons. The EEM spectra of size-segregated WSOC were different among variant particle sizes, which could be the results of changing sources and/or chemical transformation of organics. Size distributions of fluorescence regional intensity (region Ⅲ and Ⅴ) and HIX indicate that humification degree or aromaticity of WSOC was highest between 0.26 to 0.44 µm. The Stokes shift (SS) and the harmonic mean of the excitation and emission wavelengths (WH) reflected that π-conjugated systems were high between 0.26 to 0.44 µm as well. The parallel factor analysis (PARAFAC) results showed that humic-like substances were abundant in fine particles (< 1 µm) and peaked at 0.26–0.44 µm. All evidence supported that the humification degree of WSOC increased in submicron mode (< 0.44 µm) and decreased gradually. Thus, it was conjectured that condensation of organics still goes on in submicron mode, resulting in the highest humification degree exhibit in particle size between 0.26 to 0.44 µm rather than < 0.26 µm. Synthetically analyzing 3-dimensional fluorescence data could efficiently present the secondary transformation processes of WSOC.

2022 ◽  
Vol 22 (1) ◽  
pp. 465-479
Author(s):  
Juanjuan Qin ◽  
Jihua Tan ◽  
Xueming Zhou ◽  
Yanrong Yang ◽  
Yuanyuan Qin ◽  
...  

Abstract. Water-soluble organic compounds (WSOCs) play important roles in atmospheric particle formation, migration, and transformation processes. Size-segregated atmospheric particles were collected in a rural area of Beijing. Three-dimensional fluorescence spectroscopy was used to investigate the optical properties of WSOCs as a means of inferring information about their atmospheric sources. Sophisticated analysis on fluorescence data was performed to characteristically estimate the connections among particles of different sizes. WSOC concentrations and the average fluorescence intensity (AFI) showed a monomodal distribution in winter and a bimodal distribution in summer, with the dominant mode in the 0.26–0.44 µm size range in both seasons. The excitation–emission matrix (EEM) spectra of WSOCs varied with particle size, likely due to changing sources and/or the chemical transformation of organics. Size distributions of the fluorescence regional integration (regions III and V) and humification index (HIX) indicate that the humification degree or aromaticity of WSOCs was the highest in the particle size range of 0.26–0.44 µm. The Stokes shift (SS) and the harmonic mean of the excitation and emission wavelengths (WH) reflected that π-conjugated systems were high in the same particle size range. The parallel factor analysis (PARAFAC) results showed that humic-like substances were abundant in fine particles (< 1 µm) and peaked at 0.26–0.44 µm. All evidence supported the fact that the humification degree of WSOCs increased with particle size in the submicron mode (< 0.44 µm) and then decreased gradually with particle size, which implied that the condensation of organics occurred in submicron particles, resulting in the highest degree of humification in the particle size range of 0.26–0.44 µm rather than in the < 0.26 µm range. Synthetically analyzing three-dimensional fluorescence data could efficiently reveal the secondary transformation processes of WSOCs.


2021 ◽  
Vol 9 ◽  
Author(s):  
Zhaoye Wu ◽  
Duanyang Liu ◽  
Tianliang Zhao ◽  
Yan Su ◽  
Bin Zhou

In order to investigate the chemical composition distributions and pollution characteristics of Total water-soluble inorganic ions (TWSII) in the rain period (Meiyu) in the East Asian summer monsoon season, including the impact of Meiyu on air pollution in the Yangtze River Delta, East China, the gaseous pollutant concentrations, the 9 sizes segregated particles, and water-soluble inorganic ions of aerosols were measured on the north shore of Taihu Lake from June 4 to July 5, 2016. Results show that the mass concentrations of atmospheric particulate matters (PM2.5 and PM10) and main gaseous pollutants (SO2, NO2, CO, and O3) decrease during the Meiyu period, with the largest decline in PM10 and the smallest in CO. TWSII in atmospheric particles are mainly concentrated in fine particles during the Meiyu period. The values of ρ (TWSII) for PM1.1, PM1.1–2.1, and PM2.1–10 before the Meiyu onset are generally greater than those during the Meiyu period. During the first pollution process, the ρ(TWSII) for PM1.1 and PM1.1–2.1 first increase to the peak values, and then decrease during the moderate rainfall period, when the ρ(TWSII) in PM2.1–10 increase to its maximum before the Meiyu onset. The mass concentrations for anions, cations, and total ions at different particle-size sections all exhibit bimodal distributions before and after the Meiyu onset. The mass concentration peaks at a particle size of 1.1–2.1 μm for fine particles, while at 5.8–9.0 μm (before the Meiyu onset) and 9.0–10.0 μm (during the Meiyu period) for coarse particles, respectively. The peak particle size for mass concentration of coarse particles moves toward larger sizes during the Meiyu period. The mass concentrations of SO42− at different particle-size sections show a bimodal distribution before the Meiyu onset and a multi-modal distribution during the Meiyu period. The mass concentrations of NO3− at different particle-size sections show a bimodal distribution before the Meiyu onset and a unimodal distribution during the Meiyu period. The mass concentrations of NH4+ at different particle-size sections present a bimodal distribution before and after the Meiyu onset, with the particle-size for peak concentrations distributing in 1.1–2.1 and 5.8–9.0 μm before the Meiyu onset, and 9.0–10.0 μm during the Meiyu period. The mean value of nitrogen oxidation ratio (NOR) is higher before the Meiyu onset than after, indicating that the secondary conversion of NO2 before the Meiyu onset is enhanced. The sulfur oxidation ratio (SOR) values are greater than NOR values, but the concentrations of NO2 in the same period during the Meiyu period are higher than those of SO2, which indicates that the secondary conversion of SO2 during the Meiyu period on the north bank of Taihu Lake is stronger than that of NO2. During the whole observation, the contribution of stationary sources mainly contributed to the atmospheric particulate matters during the Meiyu period. The contributions of vehicle exhaust and coal combustion to fine particles are more obviously affected by the changes in meteorological conditions during the Meiyu period, and the vehicle emissions contribute more to PM1.1–2.1 than to PM1.1.


2010 ◽  
Vol 10 (7) ◽  
pp. 17467-17490
Author(s):  
G. Wang ◽  
K. Kawamura ◽  
M. Xie ◽  
S. Hu ◽  
B. Zhou ◽  
...  

Abstract. Primary (i.e., sugars and sugar alcohols) and secondary water-soluble organic compounds (WSOCs) (i.e., dicarboxylic acids and aromatic acids) were characterised on a molecular level in size-segregated aerosols from the urban and mountain atmosphere of China and from the marine atmosphere in the outflow region of East Asia. Levoglucosan is the most abundant WSOCs in the urban and mountain atmosphere, whose accumulated concentrations in all stages are 1–3 orders of magnitude higher than those of marine aerosols. In contrast, malic, succinic and phthalic acids are dominant in the marine aerosols, which are 3–6 times more abundant than levoglucosan. This suggests that a continuous formation of secondary organic aerosols is occurring in the marine atmosphere during the long-range transport of air mass from inland China to the North Pacific. Sugars and sugar-alcohols, except for levoglucosan, gave a bimodal size distribution in the urban and mountain areas, peaking at 0.7–1.1 μm and >3.3 μm, and a unimodal distribution in the marine region, peaking at >3.3 μm. In contrast, levoglucosan and all the secondary WSOCs, except for benzoic and azelaic acids, showed a unimodal size distribution with a peak at 0.7–1.1 μm. Geometric mean diameters (GMDs) of the WSOCs in fine particles (<2.1 μm) at the urban site are larger in winter than in spring, due to an enhanced coagulation effect under the development of an inversion layer. However, GMDs of levoglucosan and most of the secondary WSOCs in the coarse mode are larger in the mountain and marine air and smaller in the urban air. This is most likely caused by an enhanced hygroscopic growth due to the high humidity of the mountain and marine atmosphere.


2016 ◽  
Vol 9 (3) ◽  
pp. 1025-1037 ◽  
Author(s):  
Yan Lyu ◽  
Tingting Xu ◽  
Xiang Li ◽  
Tiantao Cheng ◽  
Xin Yang ◽  
...  

Abstract. In order to better understand the size distribution of particle-associated PBDEs and their deposition pattern in the human respiratory tract, we carried out a 1-year campaign during 2012–2013 for the measurement of size-resolved particles at the urban site of Shanghai. The results showed that particulate PBDEs exhibited a bimodal distribution with a mode peak in the accumulation particle size range and the second mode peak in the coarse particle size ranges. As the number of bromine atoms in the molecule increases, accumulation-mode peak intensity increased while coarse-mode peak intensity decreased. This change was consistent with the variation of PBDEs' subcooled vapor pressure. Absorption and adsorption processes dominated the distribution of PBDEs among the different size particles. The evaluated deposition flux of Σ13 PBDEs was 26.8 pg h−1, in which coarse particles contributed most PBDEs in head and tracheobronchial regions, while fine-mode particles contributed major PBDEs in the alveoli region. In association with the fact that fine particles can penetrate deeper into the respiratory system, fine-particle-bound highly brominated PBDEs can be inhaled more deeply into human lungs and cause a greater risk to human health.


2018 ◽  
Vol 15 (3) ◽  
pp. 150 ◽  
Author(s):  
Jingyi Zhang ◽  
Bin Jiang ◽  
Zhiheng Wang ◽  
Yongmei Liang ◽  
Yahe Zhang ◽  
...  

Environmental contextOrganic compounds generally make a large contribution to ambient aerosol fine particles, and can influence atmospheric chemistry. Solvent extraction before mass spectrometry is widely used for the determination of organic compounds in aerosols, but the molecular selectivity of different solvents is unclear. We extracted an aerosol sample with various solvents and show how the organic compound profile obtained by mass spectrometry changes depending on the extracting solvent. AbstractFor a comprehensive characterisation of organic compounds in aerosols, samples collected on a hazy day from Beijing were sequentially extracted with various solvents and analysed by Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Electrospray ionisation (ESI) was used for the MS analysis. Aerosol samples were extracted in an apolar-to-polar solvent order of n-hexane (n-C6), dichloromethane (DCM), acetonitrile (ACN) and water, and also extracted in reverse sequence. The separated fractions were defined as non-polar, low-polarity, mid-polarity and high-polarity organic compounds respectively. Approximately 70 % of the total organic carbon (TOC) was extractable, of which the water-soluble organic carbon (WSOC) and non-polar organic carbon accounted for 30 and 25 % of the TOC respectively. Non-polar and low-polarity compounds with a high degree of molecular condensation such as oxidised polycyclic aromatic hydrocarbons (PAHs) and nitrogen-containing compounds (CHN) were extracted by n-C6 and DCM. Water-soluble organic matter (WSOM) was predominant with aliphatic and aromatic organosulfates (CHOS) and nitrooxy-organosulfates (CHONS). Most oxygen-containing compounds (CHO) and oxygen- and nitrogen-containing compounds (CHON) with high double-bond equivalents (DBEs) and long carbon chains tended to be extracted into organic solvents.


2016 ◽  
Vol 12 (3) ◽  
pp. 4307-4321 ◽  
Author(s):  
Ahmed Hassan Ibrahim ◽  
Yehia Abbas

The physical properties of ferrites are verysensitive to microstructure, which in turn critically dependson the manufacturing process.Nanocrystalline Lithium Stannoferrite system Li0.5+0.5XFe2.5-1.5XSnXO4,X= (0, 0.2, 0.4, 0.6, 0.8 and 1.0) fine particles were successfully prepared by double sintering ceramic technique at pre-sintering temperature of 500oC for 3 h andthepre-sintered material was crushed and sintered finally in air at 1000oC.The structural and microstructural evolutions of the nanophase have been studied using X-ray powder diffraction (XRD) and the Rietveld method.The refinement results showed that the nanocrystalline ferrite has a two phases of ordered and disordered phases for polymorphous lithium Stannoferrite.The particle size of as obtained samples were found to be ~20 nm through TEM that increases up to ~ 85 nmand isdependent on the annealing temperature. TEM micrograph reveals that the grains of sample are spherical in shape. (TEM) analysis confirmed the X-ray results.The particle size of stannic substituted lithium ferrite fine particle obtained from the XRD using Scherrer equation.Magneticmeasurements obtained from lake shore’s vibrating sample magnetometer (VSM), saturation magnetization ofordered LiFe5O8 was found to be (57.829 emu/g) which was lower than disordered LiFe5O8(62.848 emu/g).Theinterplay between superexchange interactions of Fe3+ ions at A and B sublattices gives rise to ferrimagnetic ordering of magnetic moments,with a high Curie-Weiss temperature (TCW ~ 900 K).


Tellus B ◽  
2011 ◽  
Vol 63 (5) ◽  
Author(s):  
Puja Khare ◽  
B. P. Baruah ◽  
P. G. Rao

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