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Title: Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene

Abstract

Abstract. The effect of relative humidity (RH) on the chemical composition of secondaryorganic aerosol (SOA) formed from low-NOx toluene oxidation in theabsence of seed particles was investigated. SOA samples were prepared in anaerosol smog chamber at <2%RH and 75%RH, collected on Teflonfilters, and analyzed with nanospray desorption electrospray ionizationhigh-resolution mass spectrometry (nano-DESI–HRMS). Measurements revealed asignificant reduction in the fraction of oligomers present in the SOAgenerated at 75%RH compared to SOA generated under dry conditions. In aseparate set of experiments, the particle mass concentrations were measuredwith a scanning mobility particle sizer (SMPS) at RHs ranging from <2 to90%. It was found that the particle mass loading decreased bynearly an order of magnitude when RH increased from <2 to75–90% for low-NOx toluene SOA. The volatility distributions of theSOA compounds, estimated from the distribution of molecular formulas usingthe “molecular corridor” approach, confirmed that low-NOx toluene SOAbecame more volatile on average under high-RH conditions. In contrast, theeffect of RH on SOA mass loading was found to be much smaller forhigh-NOx toluene SOA. The observed increase in the oligomer fraction andparticle mass loading under dry conditions were attributed to the enhancement ofcondensation reactions, which produce water and oligomers from smallercompounds in low-NOx toluene SOA. The reduction in the fraction ofoligomericmore » compounds under humid conditions is predicted to partly counteractthe previously observed enhancement in the toluene SOA yield driven by theaerosol liquid water chemistry in deliquesced inorganic seed particles.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  2. Purdue Univ., West Lafayette, IN (United States). Dept. of Chemistry
  3. Univ. of California, Irvine, CA (United States). Dept. of Mechanical and Aerospace Engineering
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USEPA; National Science Foundation (NSF)
OSTI Identifier:
1501910
Alternate Identifier(s):
OSTI ID: 1542076
Report Number(s):
PNNL-SA-124399
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0018349; AC06-76RL01830; 83588101; 1500284; AGS-1654104; MRI-0923323; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 3; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hinks, Mallory L., Montoya-Aguilera, Julia, Ellison, Lucas, Lin, Peng, Laskin, Alexander, Laskin, Julia, Shiraiwa, Manabu, Dabdub, Donald, and Nizkorodov, Sergey A. Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene. United States: N. p., 2018. Web. doi:10.5194/acp-18-1643-2018.
Hinks, Mallory L., Montoya-Aguilera, Julia, Ellison, Lucas, Lin, Peng, Laskin, Alexander, Laskin, Julia, Shiraiwa, Manabu, Dabdub, Donald, & Nizkorodov, Sergey A. Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene. United States. https://doi.org/10.5194/acp-18-1643-2018
Hinks, Mallory L., Montoya-Aguilera, Julia, Ellison, Lucas, Lin, Peng, Laskin, Alexander, Laskin, Julia, Shiraiwa, Manabu, Dabdub, Donald, and Nizkorodov, Sergey A. Tue . "Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene". United States. https://doi.org/10.5194/acp-18-1643-2018. https://www.osti.gov/servlets/purl/1501910.
@article{osti_1501910,
title = {Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene},
author = {Hinks, Mallory L. and Montoya-Aguilera, Julia and Ellison, Lucas and Lin, Peng and Laskin, Alexander and Laskin, Julia and Shiraiwa, Manabu and Dabdub, Donald and Nizkorodov, Sergey A.},
abstractNote = {Abstract. The effect of relative humidity (RH) on the chemical composition of secondaryorganic aerosol (SOA) formed from low-NOx toluene oxidation in theabsence of seed particles was investigated. SOA samples were prepared in anaerosol smog chamber at <2%RH and 75%RH, collected on Teflonfilters, and analyzed with nanospray desorption electrospray ionizationhigh-resolution mass spectrometry (nano-DESI–HRMS). Measurements revealed asignificant reduction in the fraction of oligomers present in the SOAgenerated at 75%RH compared to SOA generated under dry conditions. In aseparate set of experiments, the particle mass concentrations were measuredwith a scanning mobility particle sizer (SMPS) at RHs ranging from <2 to90%. It was found that the particle mass loading decreased bynearly an order of magnitude when RH increased from <2 to75–90% for low-NOx toluene SOA. The volatility distributions of theSOA compounds, estimated from the distribution of molecular formulas usingthe “molecular corridor” approach, confirmed that low-NOx toluene SOAbecame more volatile on average under high-RH conditions. In contrast, theeffect of RH on SOA mass loading was found to be much smaller forhigh-NOx toluene SOA. The observed increase in the oligomer fraction andparticle mass loading under dry conditions were attributed to the enhancement ofcondensation reactions, which produce water and oligomers from smallercompounds in low-NOx toluene SOA. The reduction in the fraction ofoligomeric compounds under humid conditions is predicted to partly counteractthe previously observed enhancement in the toluene SOA yield driven by theaerosol liquid water chemistry in deliquesced inorganic seed particles.},
doi = {10.5194/acp-18-1643-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 3,
volume = 18,
place = {United States},
year = {Tue Feb 06 00:00:00 EST 2018},
month = {Tue Feb 06 00:00:00 EST 2018}
}

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Free Publicly Available Full Text
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Cited by: 53 works
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Figures / Tables:

Figure 1 Figure 1: High-resolution mass spectra obtained in negative ion mode (a) and positive ion mode (b). The red upward-pointing mass spectra represent the low-NOx SOA sample made under low RH (< 2 %) and the blue inverted mass spectra represent the low-NOx SOA sample made under high RH (75 %).

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Works referencing / citing this record:

Trends in the oxidation and relative volatility of chamber-generated secondary organic aerosol
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