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Molecular composition of organic aerosols in central Amazonia: An ultra-high-resolution mass spectrometry study

Published version
Peer-reviewed

Type

Article

Change log

Authors

Kourtchev, I 
Godoi, RHM 
Connors, S 
Levine, JG 
Archibald, AT 

Abstract

The Amazon Basin plays key role in atmospheric chemistry, biodiversity and climate change. In this study we applied nanoelectrospray (nanoESI) ultra-high-resolution mass spectrometry (UHRMS) for the analysis of the organic fraction of PM2.5 aerosol samples collected during dry and wet seasons at a site in central Amazonia receiving background air masses, biomass burning and urban pollution. Comprehensive mass spectral data evaluation methods (e.g. Kendrick mass defect, Van Krevelen diagrams, carbon oxidation state and aromaticity equivalent) were used to identify compound classes and mass distributions of the detected species. Nitrogen-and/or sulfur-containing organic species contributed up to 60% of the total identified number of formulae. A large number of molecular formulae in organic aerosol (OA) were attributed to later-generation nitrogen-and sulfur-containing oxidation products, suggesting that OA composition is affected by biomass burning and other, potentially anthropogenic, sources. Isoprene-derived organosulfate (IEPOX-OS) was found to be the most dominant ion in most of the analysed samples and strongly followed the concentration trends of the gas-phase anthropogenic tracers confirming its mixed anthropogenic-biogenic origin. The presence of oxidised aromatic and nitro-aromatic compounds in the samples suggested a strong influence from biomass burning especially during the dry period. Aerosol samples from the dry period and under enhanced biomass burning conditions contained a large number of molecules with high carbon oxidation state and an increased number of aromatic compounds compared to that from the wet period. The results of this work demonstrate that the studied site is influenced not only by biogenic emissions from the forest but also by biomass burning and potentially other anthropogenic emissions from the neighbouring urban environments.

Description

Keywords

37 Earth Sciences, 3701 Atmospheric Sciences, 13 Climate Action

Journal Title

Atmospheric Chemistry and Physics

Conference Name

Journal ISSN

1680-7316
1680-7324

Volume Title

16

Publisher

Copernicus Publications
Sponsorship
European Research Council (279405)
National Centre for Atmospheric Science (NERC) (via University of Leeds) (R8H12/83/009)
National Centre for Atmospheric Science (NERC) (via University of Leeds) (R8/H12/83/003)
National Centre for Atmospheric Science (NERC) (via University of Leeds) (R8/H12/83/003)
Research at the University of Cambridge was supported by European Research Council grant no. 279405. The authors would like to thank Jason Surratt (University of North Carolina) for providing a synthesised IEPOX-OS standard. O3, CO, NOy , RH and rain data were obtained from the Atmospheric Radiation Measurement (ARM) Climate Research Facility, a U.S. Department of Energy (grant DE-SC0011122) Office of Science user facility sponsored by the Office of Biological and Environmental Research. We acknowledge the support from the Central Office of the Large Scale Biosphere Atmosphere Experiment in Amazonia (LBA), the Instituto Nacional de Pesquisas da Amazonia (INPA), and the Universidade do Estado do Amazonia (UEA). The work was conducted under 001030/2012-4 of the Brazilian National Council for Scientific and Technological Development (CNPq).