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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 O 3, over ranges from hours to days (O 3) 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 O 3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were 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 hygroscopicitymore » of the OA increased with increasing elemental O:C up to O:C~1.0, and then decreased as O:C increased further. 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. While measured ambient precursors were sufficient to explain the amount of SOA formed from O 3, 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. This study enables a better understanding of SOA formation in environments with diverse emission sources.« less

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [1]; ORCiD logo [3];  [4];  [5];  [6];  [3]; ORCiD logo [7];  [8]; ORCiD logo [8];  [9]; ORCiD logo [10];  [11];  [12];  [13];  [14];  [15] more »;  [10];  [16];  [17];  [17];  [18]; ORCiD logo [1] « less
  1. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES) and Dept. of Chemistry
  2. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS)
  3. Univ. of California, Irvine, CA (United States). Dept. of Earth System Science
  4. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Earth System Research Lab.
  5. National Center for Atmospheric Research, Boulder, CO (United States); National Inst. of Environmental Research (NIER), Incheon (Korea, Republic of). Climate and Air Quality Research Dept.
  6. Univ. of California, Irvine, CA (United States). Dept. of Earth System Science; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC)
  7. Univ. of Sao Paulo (Brazil). Inst. of Physics; Univ. of Clermont Auvergne, Clermont-Ferrand (France). Lab. for Meteorological Physics (LaMP)
  8. Univ. of Sao Paulo (Brazil). Inst. of Physics
  9. Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.; Snow College, Richfield, CT (United States). Dept. of Chemistry
  10. Brookhaven National Lab. (BNL), Upton, NY (United States). Biological, Environmental & Climate Sciences Dept.
  11. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management
  12. Univ. of California, Berkeley, CA (United States). Dept. of Civil and Environmental Engineering
  13. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; Virginia Tech, Blacksburg, VA (United States). Dept. of Civil and Environmental Engineering
  14. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; and Dept. of Civil and Environmental Engineering
  15. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS); Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management
  16. Univ. of the State of Amazonas, Manaus (Brazil)
  17. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  18. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS) and Dept. of Earth and Planetary Sciences
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); 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:
1424985
Alternate Identifier(s):
OSTI ID: 1399678
Report Number(s):
BNL-203222-2018-JAAM; BNL-114388-2017-JA
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0012704; 001030/2012-4; SC0016559; SC0011105; SC0011218; AGS-1360834; 83587701-0; FP-91761701-0; DGE 1106400; SC0004698
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: 1; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
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. United States: N. p., 2018. Web. doi:10.5194/acp-18-467-2018.
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. United States. doi:10.5194/acp-18-467-2018.
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". United States. doi:10.5194/acp-18-467-2018. https://www.osti.gov/servlets/purl/1424985.
@article{osti_1424985,
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 were 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. 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. 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. This 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 = {United States},
year = {2018},
month = {1}
}

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