A note on the effects of inorganic seed aerosol on the oxidation state of secondary organic aerosol-α -Pinene ozonolysis

2016 ◽  
Vol 121 (20) ◽  
pp. 12,476-12,483 ◽  
Author(s):  
Dan Dan Huang ◽  
Xuan Zhang ◽  
Nathan F. Dalleska ◽  
Hanna Lignell ◽  
Matthew M. Coggon ◽  
...  
2013 ◽  
Vol 118 (20) ◽  
pp. 11,741-11,749 ◽  
Author(s):  
Chen Song ◽  
Madhu Gyawali ◽  
Rahul A. Zaveri ◽  
John E. Shilling ◽  
W. Patrick Arnott

2018 ◽  
Author(s):  
Changgeng Liu ◽  
Tianzeng Chen ◽  
Yongchun Liu ◽  
Jun Liu ◽  
Hong He ◽  
...  

Abstract. 2-Methoxyphenol (guaiacol) is derived from the lignin pyrolysis and taken as a potential tracer for wood smoke emissions. In this work, the effect of SO2 at atmospheric levels (0–56 ppb) on secondary organic aerosol (SOA) formation and its oxidation state during guaiacol photooxidation was investigated in the presence of various inorganic seed particles (NaCl and (NH4)2SO4). Without SO2 and seed particles, SOA yields (9.46–26.37 %) obtained at different guaiacol concentration (138.83–2197.36 μg m−3) could be well expressed by a one-product model. The presence of SO2 resulted in enhancing SOA yield by 14.05–23.66 %. With (NH4)2SO4 and NaCl seed particles, SOA yield was enhanced by 23.06 % and 29.57 %, respectively, which further increased significantly to 29.78–53.47 % in the presence of SO2, suggesting that SO2 and seed particles have a synergetic contribution to SOA formation. It should be noted that SO2 was found to be in favor of increasing the carbon oxidation state (OSC) of SOA, indicating that the functionalization reaction should be more dominant than oligomerization reaction. In addition, the average N/C ratio of SOA was 0.037, which revealed that NOx participated in the photooxidation process, consequently leading to the formation of organic nitrates. The experimental results demonstrate the importance of SO2 on the formation processes of SOA and organosulfates, and also are helpful to further understand SOA formation from the atmospheric photooxidation of guaiacol and its subsequent impacts on air quality and climate.


2011 ◽  
Vol 11 (12) ◽  
pp. 5917-5929 ◽  
Author(s):  
J. F. Hamilton ◽  
M. Rami Alfarra ◽  
K. P. Wyche ◽  
M. W. Ward ◽  
A. C. Lewis ◽  
...  

Abstract. The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES) project to study the effect of seed particles on the formation of secondary organic aerosol (SOA) from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulfate or diesel particles, a method was developed to use in-situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4–13 μg m−3). Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8 %. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90 % RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC × GC) and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS) was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.


2020 ◽  
Author(s):  
Juliane L. Fry ◽  
Bellamy Brownwood ◽  
Thorsten Hohaus ◽  
Avtandil Turdziladze ◽  
Philip Carlsson ◽  
...  

<p>Experiments at a set of atmospherically relevant conditions were performed in the atmospheric simulation chamber SAPHIR, investigating the oxidation of isoprene by the nitrate radical (NO3). A comprehensive set of instruments detected trace gases, radicals, aerosol properties and hydroxyl (OH) and NO3 radical reactivity. The chemical conditions in the chamber were varied to change the fate of the peroxy radicals (RO2) formed after the reaction between NO3 and isoprene, and seed aerosol of varying composition was added to initiate gas/aerosol partitioning. This presentation discusses observed gas/aerosol partitioning of the major organic nitrate products and summarizes the observations of secondary organic aerosol yield.</p>


2010 ◽  
Vol 10 (10) ◽  
pp. 25117-25151
Author(s):  
J. F. Hamilton ◽  
M. Rami Alfarra ◽  
K. P. Wyche ◽  
M. W. Ward ◽  
A. C. Lewis ◽  
...  

Abstract. The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES) project to study the effect of seed particles on the formation of secondary organic aerosol (SOA) from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulphate or diesel particles, a method was developed to use in situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4–13 μg m-3). Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8%. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90% RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC×GC) and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS) was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.


2014 ◽  
Vol 14 (22) ◽  
pp. 31441-31481 ◽  
Author(s):  
L. Hildebrandt Ruiz ◽  
A. L. Paciga ◽  
K. Cerully ◽  
A. Nenes ◽  
N. M. Donahue ◽  
...  

Abstract. Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form and transform SOA from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx. The effects of chemical aging on organic aerosol (OA) composition, mass yield, volatility and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state OSC) and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OS C ranged from −0.29 to 0.45 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.


2016 ◽  
Vol 47 ◽  
pp. 219-229 ◽  
Author(s):  
Mingqiang Huang ◽  
Jiahui Zhang ◽  
Shunyou Cai ◽  
Yingmin Liao ◽  
Weixiong Zhao ◽  
...  

2007 ◽  
Vol 7 (14) ◽  
pp. 3909-3922 ◽  
Author(s):  
N. L. Ng ◽  
J. H. Kroll ◽  
A. W. H. Chan ◽  
P. S. Chhabra ◽  
R. C. Flagan ◽  
...  

Abstract. Secondary organic aerosol (SOA) formation from the photooxidation of m-xylene, toluene, and benzene is investigated in the Caltech environmental chambers. Experiments are performed under two limiting NOx conditions; under high-NOx conditions the peroxy radicals (RO2) react only with NO, while under low-NOx conditions they react only with HO2. For all three aromatics studied (m-xylene, toluene, and benzene), the SOA yields (defined as the ratio of the mass of organic aerosol formed to the mass of parent hydrocarbon reacted) under low-NOx conditions substantially exceed those under high-NOx conditions, suggesting the importance of peroxy radical chemistry in SOA formation. Under low-NOx conditions, the SOA yields for m-xylene, toluene, and benzene are constant (36%, 30%, and 37%, respectively), indicating that the SOA formed is effectively nonvolatile under the range of Mo(>10 μg m−3) studied. Under high-NOx conditions, aerosol growth occurs essentially immediately, even when NO concentration is high. The SOA yield curves exhibit behavior similar to that observed by Odum et al. (1996, 1997a, b), although the values are somewhat higher than in the earlier study. The yields measured under high-NOx conditions are higher than previous measurements, suggesting a "rate effect" in SOA formation, in which SOA yields are higher when the oxidation rate is faster. Experiments carried out in the presence of acidic seed aerosol reveal no change of SOA yields from the aromatics as compared with those using neutral seed aerosol.


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