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

Journal Article · · Atmospheric Chemistry and Physics (Online)
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  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

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 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.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER); 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)
Grant/Contract Number:
SC0012704; SC0006680; SC0011115; SC0011105; FAPEAM 062.00568/2014; 134/2016; FAPESP 2013/05014-0; 1106400; 1332998; FP-91761701-0; AC0576RL01830
OSTI ID:
1466575
Alternate ID(s):
OSTI ID: 1468615
Report Number(s):
BNL-208005-2018-JAAM; PNNL-SA-132381
Journal Information:
Atmospheric Chemistry and Physics (Online), Vol. 18, Issue 16; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 23 works
Citation information provided by
Web of Science

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  • C., Flagan, Richard; C., Eddingsaas, Nathan; L., Loza, Christine
  • The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/sz9v-nb58
text January 2009
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Cited By (10)

Unravelling the functions of biogenic volatiles in boreal and temperate forest ecosystems journal July 2019
CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions journal January 2017
Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region journal January 2018
Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia journal January 2018
Single-particle characterization of aerosols collected at a remote site in the Amazonian rainforest and an urban site in Manaus, Brazil journal January 2019
Chemical composition of ultrafine aerosol particles in central Amazonia during the wet season journal January 2019
Contributions of biomass-burning, urban, and biogenic emissions to the concentrations and light-absorbing properties of particulate matter in central Amazonia during the dry season journal January 2019
Aerosol optical depth retrievals in central Amazonia from a multi-filter rotating shadow-band radiometer calibrated on-site journal January 2019
Urban pollution greatly enhances formation of natural aerosols over the Amazon rainforest journal March 2019
Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5 journal January 2018

Figures / Tables (10)