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Title: Urban influence on the concentration and composition of submicron particulate matter in central Amazonia

Abstract

An understanding of how anthropogenic emissions affect the concentrations and composition of airborne particulate matter (PM) is fundamental to quantifying the influence of human activities on climate and air quality. The central Amazon Basin, especially around the city of Manaus, Brazil, has experienced rapid changes in the past decades due to ongoing urbanization. Herein, changes in the concentration and composition of submicron PM due to pollution downwind of the Manaus metropolitan region are reported as part of the GoAmazon2014/5 experiment. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a suite of other gas- and particle-phase instruments were deployed at the T3 research site, 70km downwind of Manaus, during the wet season. At this site, organic components represented 79±7% of the non-refractory PM 1 mass concentration on average, which was in the same range as several upwind sites. However, the organic PM 1 was considerably more oxidized at T3 compared to upwind measurements. Positive-matrix factorization (PMF) was applied to the time series of organic mass spectra collected at the T3 site, yielding three factors representing secondary processes (73±15% of total organic mass concentration) and three factors representing primary anthropogenic emissions (27±15%). Fuzzy c-means clustering (FCM) was applied to the afternoon timemore » series of concentrations of NO y, ozone, total particle number, black carbon, and sulfate. Four clusters were identified and characterized by distinct air mass origins and particle compositions. Two clusters, Bkgd-1 and Bkgd-2, were associated with background conditions. Bkgd-1 appeared to represent near-field atmospheric PM production and oxidation of a day or less. Bkgd-2 appeared to represent material transported and oxidized for two or more days, often with out-of-basin contributions. Two other clusters, Pol-1 and Pol-2, represented the Manaus influence, one apparently associated with the northern region of Manaus and the other with the southern region of the city. A composite of the PMF and FCM analyses provided insights into the anthropogenic effects on PM concentration and composition. The increase in mass concentration of submicron PM ranged from 25% to 200% under polluted compared with background conditions, including contributions from both primary and secondary PM. Furthermore, a comparison of PMF factor loadings for different clusters suggested a shift in the pathways of PM production under polluted conditions. Nitrogen oxides may have played a critical role in these shifts. Increased concentrations of nitrogen oxides can shift pathways of PM production from HO 2-dominant to NO-dominant as well as increase the concentrations of oxidants in the atmosphere. Consequently, the oxidation of biogenic and anthropogenic precursor gases as well as the oxidative processing of preexisting atmospheric PM can be accelerated. This combined set of results demonstrates the susceptibility of atmospheric chemistry, air quality, and associated climate forcing to anthropogenic perturbations over tropical forests.« less

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [2];  [3];  [4]; ORCiD logo [5];  [6];  [7]; ORCiD logo [8]; ORCiD logo [9];  [10]; ORCiD logo [11];  [12];  [12]; ORCiD logo [13]; ORCiD logo [14]; ORCiD logo [15]; ORCiD logo [4] more »;  [7]; ORCiD logo [11];  [16]; ORCiD logo [15];  [17]; ORCiD logo [2];  [18] « less
  1. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences
  2. Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry and Cooperative Inst. for Research in Environmental Sciences
  3. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management; Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Civil and Environmental Engineering
  4. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management
  5. Univ. of São Paulo, São Paulo (Brazil). Inst. of Physics; Univ. Blaise Pascal, Aubiere (France). Lab. for Meteorological Physics (LaMP)
  6. Univ. of São Paulo, São Paulo (Brazil). Inst. of Physics; Federal Univ. of Uberlandia, Minas Gerais (Brazil). Inst. of Agricultural Sciences
  7. Amazonas State Univ., Manaus, Amazonas (Brazil). School of Technology
  8. National Inst. for Amazonian Research, Manaus, Amazonas (Brazil); Federal Univ. of Para, Belem (Brazil). Dept. of Meteorology and Geosciences Inst.
  9. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences; Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy, and Management
  10. Brookhaven National Lab. (BNL), Upton, NY (United States); Snow College, Richfield, UT (United States). Dept. of Chemistry
  11. Brookhaven National Lab. (BNL), Upton, NY (United States)
  12. Texas A & M Univ., College Station, TX (United States). Dept. of Atmospheric Sciences
  13. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC)
  14. Max Planck Society, Mainz (Germany). Max Planck Inst. for Chemistry, Particle Chemistry Dept.
  15. Univ. of São Paulo, São Paulo (Brazil). Inst. of Physics
  16. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences; Colby College, Waterville, MA (United States). Dept. of Chemistry
  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, Dept. of Earth and Planetary Sciences
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); US Environmental Protection Agency (EPA); Amazonas State Research Support Foundation (FAPEAM); National Science Foundation (NSF); Brazil Scientific Mobility Program (BSMP); Schlumberger Foundation; National Council for Scientific and Technological Development (CNPq)
OSTI Identifier:
1466575
Alternate Identifier(s):
OSTI ID: 1468615
Report Number(s):
BNL-208005-2018-JAAM; PNNL-SA-132381
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
SC0012704; SC0006680; SC0011115; SC0011105; FAPEAM 062.00568/2014; 134/2016; FAPESP 2013/05014-0; 1106400; 1332998; FP-91761701-0; AC0576RL01830
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: 16; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

de Sá, Suzane S., Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Hu, Weiwei, Isaacman-VanWertz, Gabriel, Yee, Lindsay D., Brito, Joel, Carbone, Samara, Ribeiro, Igor O., Cirino, Glauber G., Liu, Yingjun, Thalman, Ryan, Sedlacek, Arthur, Funk, Aaron, Schumacher, Courtney, Shilling, John E., Schneider, Johannes, Artaxo, Paulo, Goldstein, Allen H., Souza, Rodrigo A. F., Wang, Jian, McKinney, Karena A., Barbosa, Henrique, Alexander, M. Lizabeth, Jimenez, Jose L., and Martin, Scot T. Urban influence on the concentration and composition of submicron particulate matter in central Amazonia. United States: N. p., 2018. Web. doi:10.5194/acp-18-12185-2018.
de Sá, Suzane S., Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Hu, Weiwei, Isaacman-VanWertz, Gabriel, Yee, Lindsay D., Brito, Joel, Carbone, Samara, Ribeiro, Igor O., Cirino, Glauber G., Liu, Yingjun, Thalman, Ryan, Sedlacek, Arthur, Funk, Aaron, Schumacher, Courtney, Shilling, John E., Schneider, Johannes, Artaxo, Paulo, Goldstein, Allen H., Souza, Rodrigo A. F., Wang, Jian, McKinney, Karena A., Barbosa, Henrique, Alexander, M. Lizabeth, Jimenez, Jose L., & Martin, Scot T. Urban influence on the concentration and composition of submicron particulate matter in central Amazonia. United States. doi:10.5194/acp-18-12185-2018.
de Sá, Suzane S., Palm, Brett B., Campuzano-Jost, Pedro, Day, Douglas A., Hu, Weiwei, Isaacman-VanWertz, Gabriel, Yee, Lindsay D., Brito, Joel, Carbone, Samara, Ribeiro, Igor O., Cirino, Glauber G., Liu, Yingjun, Thalman, Ryan, Sedlacek, Arthur, Funk, Aaron, Schumacher, Courtney, Shilling, John E., Schneider, Johannes, Artaxo, Paulo, Goldstein, Allen H., Souza, Rodrigo A. F., Wang, Jian, McKinney, Karena A., Barbosa, Henrique, Alexander, M. Lizabeth, Jimenez, Jose L., and Martin, Scot T. Thu . "Urban influence on the concentration and composition of submicron particulate matter in central Amazonia". United States. doi:10.5194/acp-18-12185-2018. https://www.osti.gov/servlets/purl/1466575.
@article{osti_1466575,
title = {Urban influence on the concentration and composition of submicron particulate matter in central Amazonia},
author = {de Sá, Suzane S. and Palm, Brett B. and Campuzano-Jost, Pedro and Day, Douglas A. and Hu, Weiwei and Isaacman-VanWertz, Gabriel and Yee, Lindsay D. and Brito, Joel and Carbone, Samara and Ribeiro, Igor O. and Cirino, Glauber G. and Liu, Yingjun and Thalman, Ryan and Sedlacek, Arthur and Funk, Aaron and Schumacher, Courtney and Shilling, John E. and Schneider, Johannes and Artaxo, Paulo and Goldstein, Allen H. and Souza, Rodrigo A. F. and Wang, Jian and McKinney, Karena A. and Barbosa, Henrique and Alexander, M. Lizabeth and Jimenez, Jose L. and Martin, Scot T.},
abstractNote = {An understanding of how anthropogenic emissions affect the concentrations and composition of airborne particulate matter (PM) is fundamental to quantifying the influence of human activities on climate and air quality. The central Amazon Basin, especially around the city of Manaus, Brazil, has experienced rapid changes in the past decades due to ongoing urbanization. Herein, changes in the concentration and composition of submicron PM due to pollution downwind of the Manaus metropolitan region are reported as part of the GoAmazon2014/5 experiment. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a suite of other gas- and particle-phase instruments were deployed at the T3 research site, 70km downwind of Manaus, during the wet season. At this site, organic components represented 79±7% of the non-refractory PM1 mass concentration on average, which was in the same range as several upwind sites. However, the organic PM1 was considerably more oxidized at T3 compared to upwind measurements. Positive-matrix factorization (PMF) was applied to the time series of organic mass spectra collected at the T3 site, yielding three factors representing secondary processes (73±15% of total organic mass concentration) and three factors representing primary anthropogenic emissions (27±15%). Fuzzy c-means clustering (FCM) was applied to the afternoon time series of concentrations of NOy, ozone, total particle number, black carbon, and sulfate. Four clusters were identified and characterized by distinct air mass origins and particle compositions. Two clusters, Bkgd-1 and Bkgd-2, were associated with background conditions. Bkgd-1 appeared to represent near-field atmospheric PM production and oxidation of a day or less. Bkgd-2 appeared to represent material transported and oxidized for two or more days, often with out-of-basin contributions. Two other clusters, Pol-1 and Pol-2, represented the Manaus influence, one apparently associated with the northern region of Manaus and the other with the southern region of the city. A composite of the PMF and FCM analyses provided insights into the anthropogenic effects on PM concentration and composition. The increase in mass concentration of submicron PM ranged from 25% to 200% under polluted compared with background conditions, including contributions from both primary and secondary PM. Furthermore, a comparison of PMF factor loadings for different clusters suggested a shift in the pathways of PM production under polluted conditions. Nitrogen oxides may have played a critical role in these shifts. Increased concentrations of nitrogen oxides can shift pathways of PM production from HO2-dominant to NO-dominant as well as increase the concentrations of oxidants in the atmosphere. Consequently, the oxidation of biogenic and anthropogenic precursor gases as well as the oxidative processing of preexisting atmospheric PM can be accelerated. This combined set of results demonstrates the susceptibility of atmospheric chemistry, air quality, and associated climate forcing to anthropogenic perturbations over tropical forests.},
doi = {10.5194/acp-18-12185-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 16,
volume = 18,
place = {United States},
year = {2018},
month = {8}
}

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Works referenced in this record:

The Green Ocean Amazon Experiment (GoAmazon2014/5) Observes Pollution Affecting Gases, Aerosols, Clouds, and Rainfall over the Rain Forest
journal, May 2017

  • Martin, S. T.; Artaxo, P.; Machado, L.
  • Bulletin of the American Meteorological Society, Vol. 98, Issue 5, p. 981-997
  • DOI: 10.1175/BAMS-D-15-00221.1