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Title: Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Abstract

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 μg m-3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air, and confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased withmore » increasing elemental O : C up to O : C ~ 1.0, and then decreased as O : C increased further. Some possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. And while measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign, multilinear regression analysis was performed between measured SOA formation and the concentration of gas-phase tracers representing different precursor sources. The majority of SOA-forming gases present during both seasons were of biogenic origin. Urban sources also contributed substantially in both seasons, while biomass burning sources were more important during the dry season. Our study enables a better understanding of SOA formation in environments with diverse emission sources.« less

Authors:
ORCiD logo; ; ORCiD logo; ORCiD logo; ; ORCiD logo; ; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ORCiD logo; ; ; ORCiD logo; more »; ORCiD logo; ; ; ; ; ORCiD logo « less
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); Large Scale Biosphere Atmosphere Experiment in Amazonia (LBA); National Institute of Amazonian Research (INPA); Amazonas State University (UEA); Amazonas State Research Foundation (FAPEAM); São Paulo State Research Foundation (FAPESP); National Science Foundation (NSF); Brazilian Scientific Mobility Program (CsF/CAPES); Brazilian National Council for Scientific and Technological Development (CNPq); United States Environmental Protection Agency (EPA)
OSTI Identifier:
1459726
Alternate Identifier(s):
OSTI ID: 1399678; OSTI ID: 1424985
Report Number(s):
BNL-114388-2017-JA; BNL-203222-2018-JAAM
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0016559; SC0011105; SC0011218; SC0004698; SC0012704; 001030/2012-4; AGS-1360834; 83587701-0; FP-91761701-0; DGE 1106400
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 18 Journal Issue: 1; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Palm, Brett B., de Sá, Suzane S., Day, Douglas A., Campuzano-Jost, Pedro, Hu, Weiwei, Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Brito, Joel, Wurm, Florian, Artaxo, Paulo, Thalman, Ryan, Wang, Jian, Yee, Lindsay D., Wernis, Rebecca, Isaacman-VanWertz, Gabriel, Goldstein, Allen H., Liu, Yingjun, Springston, Stephen R., Souza, Rodrigo, Newburn, Matt K., Alexander, M. Lizabeth, Martin, Scot T., and Jimenez, Jose L. Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia. Germany: N. p., 2018. Web. doi:10.5194/acp-18-467-2018.
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Palm, Brett B., de Sá, Suzane S., Day, Douglas A., Campuzano-Jost, Pedro, Hu, Weiwei, Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Brito, Joel, Wurm, Florian, Artaxo, Paulo, Thalman, Ryan, Wang, Jian, Yee, Lindsay D., Wernis, Rebecca, Isaacman-VanWertz, Gabriel, Goldstein, Allen H., Liu, Yingjun, Springston, Stephen R., Souza, Rodrigo, Newburn, Matt K., Alexander, M. Lizabeth, Martin, Scot T., & Jimenez, Jose L. Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia. Germany. https://doi.org/10.5194/acp-18-467-2018
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Palm, Brett B., de Sá, Suzane S., Day, Douglas A., Campuzano-Jost, Pedro, Hu, Weiwei, Seco, Roger, Sjostedt, Steven J., Park, Jeong-Hoo, Guenther, Alex B., Kim, Saewung, Brito, Joel, Wurm, Florian, Artaxo, Paulo, Thalman, Ryan, Wang, Jian, Yee, Lindsay D., Wernis, Rebecca, Isaacman-VanWertz, Gabriel, Goldstein, Allen H., Liu, Yingjun, Springston, Stephen R., Souza, Rodrigo, Newburn, Matt K., Alexander, M. Lizabeth, Martin, Scot T., and Jimenez, Jose L. Wed . "Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia". Germany. https://doi.org/10.5194/acp-18-467-2018.
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@article{osti_1459726,
title = {Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia},
author = {Palm, Brett B. and de Sá, Suzane S. and Day, Douglas A. and Campuzano-Jost, Pedro and Hu, Weiwei and Seco, Roger and Sjostedt, Steven J. and Park, Jeong-Hoo and Guenther, Alex B. and Kim, Saewung and Brito, Joel and Wurm, Florian and Artaxo, Paulo and Thalman, Ryan and Wang, Jian and Yee, Lindsay D. and Wernis, Rebecca and Isaacman-VanWertz, Gabriel and Goldstein, Allen H. and Liu, Yingjun and Springston, Stephen R. and Souza, Rodrigo and Newburn, Matt K. and Alexander, M. Lizabeth and Martin, Scot T. and Jimenez, Jose L.},
abstractNote = {Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 μg m-3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air, and confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ~ 1.0, and then decreased as O : C increased further. Some possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. And while measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign, multilinear regression analysis was performed between measured SOA formation and the concentration of gas-phase tracers representing different precursor sources. The majority of SOA-forming gases present during both seasons were of biogenic origin. Urban sources also contributed substantially in both seasons, while biomass burning sources were more important during the dry season. Our study enables a better understanding of SOA formation in environments with diverse emission sources.},
doi = {10.5194/acp-18-467-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 1,
volume = 18,
place = {Germany},
year = {Wed Jan 17 00:00:00 EST 2018},
month = {Wed Jan 17 00:00:00 EST 2018}
}
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  • DOI: 10.5194/acp-17-5331-2017

CCN activity of organic aerosols observed downwind of urban emissions during CARES
journal, January 2013

Estimates of non-traditional secondary organic aerosols from aircraft SVOC and IVOC emissions using CMAQ
journal, January 2015

  • Woody, M. C.; West, J. J.; Jathar, S. H.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 12
  • DOI: 10.5194/acp-15-6929-2015

Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol
journal, April 2014

  • Zhang, X.; Cappa, C. D.; Jathar, S. H.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 16
  • DOI: 10.1073/pnas.1404727111

Gas-phase tropospheric chemistry of biogenic volatile organic compounds: a review
journal, January 2003

Particle mass yield from β -caryophyllene ozonolysis
journal, January 2012

  • Chen, Q.; Li, Y. L.; McKinney, K. A.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 7
  • DOI: 10.5194/acp-12-3165-2012

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area
journal, January 2016

  • Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 11
  • DOI: 10.5194/acp-16-7411-2016

Contribution of isoprene-derived organosulfates to free tropospheric aerosol mass
journal, November 2010

  • Froyd, K. D.; Murphy, S. M.; Murphy, D. M.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 50
  • DOI: 10.1073/pnas.1012561107

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)
journal, January 2016

  • Hu, Weiwei; Palm, Brett B.; Day, Douglas A.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 18
  • DOI: 10.5194/acp-16-11563-2016

Cloud forming potential of oligomers relevant to secondary organic aerosols
journal, September 2014

  • Xu, Wen; Guo, Song; Gomez-Hernandez, Mario
  • Geophysical Research Letters, Vol. 41, Issue 18
  • DOI: 10.1002/2014GL061040

Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of α-pinene
journal, January 2008

  • Shilling, J. E.; Chen, Q.; King, S. M.
  • Atmospheric Chemistry and Physics, Vol. 8, Issue 7
  • DOI: 10.5194/acp-8-2073-2008

Aqueous chemistry and its role in secondary organic aerosol (SOA) formation
journal, January 2010

Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α -pinene ozonolysis
journal, January 2016

  • Nah, Theodora; McVay, Renee C.; Zhang, Xuan
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 14
  • DOI: 10.5194/acp-16-9361-2016

Sub-micrometre particulate matter is primarily in liquid form over Amazon rainforest
journal, December 2015

  • Bateman, Adam P.; Gong, Zhaoheng; Liu, Pengfei
  • Nature Geoscience, Vol. 9, Issue 1
  • DOI: 10.1038/ngeo2599

Reactive intermediates revealed in secondary organic aerosol formation from isoprene
journal, December 2009

  • Surratt, J. D.; Chan, A. W. H.; Eddingsaas, N. C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911114107

Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements
journal, January 2015

  • Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 20
  • DOI: 10.5194/acp-15-11807-2015

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

HO x radical chemistry in oxidation flow reactors with low-pressure mercury lamps systematically examined by modeling
journal, January 2015

  • Peng, Z.; Day, D. A.; Stark, H.
  • Atmospheric Measurement Techniques, Vol. 8, Issue 11
  • DOI: 10.5194/amt-8-4863-2015

Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data
journal, January 2009

  • Ulbrich, I. M.; Canagaratna, M. R.; Zhang, Q.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 9
  • DOI: 10.5194/acp-9-2891-2009

Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer
journal, January 2007

  • Canagaratna, M. R.; Jayne, J. T.; Jimenez, J. L.
  • Mass Spectrometry Reviews, Vol. 26, Issue 2
  • DOI: 10.1002/mas.20115

The gas-phase ozonolysis of β-caryophyllene (C15H24). Part I: an experimental study
journal, January 2009

  • Winterhalter, Richard; Herrmann, Frank; Kanawati, Basem
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 21
  • DOI: 10.1039/b817824k

A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
journal, January 2007

  • Petters, M. D.; Kreidenweis, S. M.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 8
  • DOI: 10.5194/acp-7-1961-2007

Cloud condensation nuclei (CCN) activity and oxygen-to-carbon elemental ratios following thermodenuder treatment of organic particles grown by α-pinene ozonolysis
journal, January 2011

  • Kuwata, Mikinori; Chen, Qi; Martin, Scot T.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 32
  • DOI: 10.1039/c1cp20253g

A high resolution and high sensitivity proton-transfer-reaction time-of-flight mass spectrometer (PTR-TOF-MS)
journal, September 2009

  • Jordan, A.; Haidacher, S.; Hanel, G.
  • International Journal of Mass Spectrometry, Vol. 286, Issue 2-3
  • DOI: 10.1016/j.ijms.2009.07.005

Atmospheric benzenoid emissions from plants rival those from fossil fuels
journal, July 2015

  • Misztal, P. K.; Hewitt, C. N.; Wildt, J.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep12064

Fine particle and organic vapor emissions from staged tests of an in-use aircraft engine
journal, July 2011

Modeling the Radical Chemistry in an Oxidation Flow Reactor: Radical Formation and Recycling, Sensitivities, and the OH Exposure Estimation Equation
journal, November 2014

  • Li, Rui; Palm, Brett B.; Ortega, Amber M.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 19
  • DOI: 10.1021/jp509534k

Airborne measurements of organosulfates over the continental U.S.: organosulfates over the continental US
journal, April 2015

  • Liao, Jin; Froyd, Karl D.; Murphy, Daniel M.
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 7
  • DOI: 10.1002/2014JD022378

A new software tool for the analysis of high resolution PTR-TOF mass spectra
journal, August 2013

Regional influence of wildfires on aerosol chemistry in the western US and insights into atmospheric aging of biomass burning organic aerosol
journal, January 2017

  • Zhou, Shan; Collier, Sonya; Jaffe, Daniel A.
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 3
  • DOI: 10.5194/acp-17-2477-2017

Effect of NO x on Secondary Organic Aerosol Concentrations
journal, August 2008

  • Lane, Timothy E.; Donahue, Neil M.; Pandis, Spyros N.
  • Environmental Science & Technology, Vol. 42, Issue 16
  • DOI: 10.1021/es703225a

Budget of organic carbon in a polluted atmosphere: Results from the New England Air Quality Study in 2002
journal, January 2005

Isoprene Epoxydiols as Precursors to Secondary Organic Aerosol Formation: Acid-Catalyzed Reactive Uptake Studies with Authentic Compounds
journal, November 2011

  • Lin, Ying-Hsuan; Zhang, Zhenfa; Docherty, Kenneth S.
  • Environmental Science & Technology, Vol. 46, Issue 1
  • DOI: 10.1021/es202554c

Cloud condensation nucleus activation properties of biogenic secondary organic aerosol
journal, January 2005

  • VanReken, Timothy M.
  • Journal of Geophysical Research, Vol. 110, Issue D7
  • DOI: 10.1029/2004JD005465

Aerosol Wall Losses in Electrically Charged Chambers
journal, January 1985

Simulating secondary organic aerosol formation using the volatility basis-set approach in a chemical transport model
journal, October 2008

Ozonolysis of β-Pinene: Temperature Dependence of Secondary Organic Aerosol Mass Fraction
journal, July 2008

  • Pathak, Ravikant; Donahue, Neil M.; Pandis, Spyros N.
  • Environmental Science & Technology, Vol. 42, Issue 14
  • DOI: 10.1021/es070721z

Modification of cloud condensation nucleus activity of organic aerosols by hydroxyl radical heterogeneous oxidation
journal, October 2009

Secondary aerosol formation from photochemical aging of aircraft exhaust in a smog chamber
journal, January 2011

  • Miracolo, M. A.; Hennigan, C. J.; Ranjan, M.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 9
  • DOI: 10.5194/acp-11-4135-2011
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