Chemical Signatures of Seasonally Unique Anthropogenic Influences on Organic Aerosol Composition in the Central Amazon

Franklin, Emily B.; Yee, Lindsay D.; Wernis, Rebecca; Isaacman-VanWertz, Gabriel; Kreisberg, Nathan; Weber, Robert; Zhang, Haofei; Palm, Brett B.; Hu, Weiwei; Campuzano-Jost, Pedro; Day, Douglas A.; Manzi, Antonio; Artaxo, Paulo; De Souza, Rodrigo A. F.; Jimenez, Jose L.; Martin, Scot T.; Goldstein, Allen H.

doi:10.1021/acs.est.2c07260

Chemical Signatures of Seasonally Unique Anthropogenic Influences on Organic Aerosol Composition in the Central Amazon

Journal Article · Mon Apr 03 00:00:00 EDT 2023 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.2c07260· OSTI ID:1995728

^[1]; ^[2]; Wernis, Rebecca ^[2]; ^[3]; Kreisberg, Nathan ^[4]; Weber, Robert ^[2]; ^[5]; ^[6]; ^[7]; ^[8]; ^[8]; Manzi, Antonio ^[9]; Artaxo, Paulo ^[10]; De Souza, Rodrigo A. F. ^[11]; ^[8]; ^[12]; ^[2]

Univ. of California, Berkeley, CA (United States); Colorado State Univ., Fort Collins, CO (United States); University of California, Berkeley
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Aerosol Dynamics, Inc., Berkeley, CA (United States)
Univ. of California, Berkeley and Riverside, CA (United States)
Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES); National Center for Atmospheric Research (NCAR), Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES); Chinese Academy of Sciences (CAS), Guangzhou (China). Guangzhou Institute of Geochemistry
Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES)
National Institute for Space Research (INPE), São Paulo (Brazil)
Univ. of Sao Paulo (Brazil)
Amazonas State University, Manaus (Brazil)
Harvard Univ., Cambridge, MA (United States)

Urbanization and fires perturb the quantities and composition of fine organic aerosol in the central Amazon, with ramifications for radiative forcing and public health. These disturbances include not only direct emissions of particulates and secondary organic aerosol (SOA) precursors, but also changes in the pathways through which biogenic precursors form SOA. The composition of ambient organic aerosol is complex and incompletely characterized, encompassing millions of potential structures relatively few of which have been synthesized and characterized. Through analysis of submicron aerosol samples from the Green Ocean Amazon (GoAmazon2014/5) field campaign by two-dimensional gas chromatography coupled with machine learning, ~1300 unique compounds were traced and characterized over two seasons. Fires and urban emissions produced chemically and interseasonally distinct impacts on product signatures, with only ~50% of compounds observed in both seasons. Seasonally unique populations point to the importance of aqueous processing in Amazonian aerosol ageing, but further mechanistic insights are impeded by limited product identity knowledge. Further, less than 10% of compounds were identifiable at an isomer-specific level. Overall, the findings (i) provide compositional characterization of anthropogenic influence on submicron organic aerosol in the Amazon, (ii) identify key season-to-season differences in chemical signatures, and (iii) highlight high-priority knowledge gaps in current speciated knowledge.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Berkeley, CA (United States)

Sponsoring Organization:: National Science Fund (NSF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0011105; SC0020051

OSTI ID:: 1995728

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 15 Vol. 57; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (49)

Highly reactive light‐dependent monoterpenes in the Amazon Jardine, A. B.; Jardine, K. J.; Fuentes, J. D. Geophysical Research Letters, Vol. 42, Issue 5 https://doi.org/10.1002/2014GL062573	journal	March 2015
An assessment of the origin and composition of higher molecular weight organic matter in aerosols over Amazonia Simoneit, Bernd R. T.; Cardoso, J. N.; Robinson, N. Chemosphere, Vol. 21, Issue 10-11 https://doi.org/10.1016/0045-6535(90)90145-J	journal	January 1990
Monoterpene SOA – Contribution of first-generation oxidation products to formation and chemical composition Mutzel, Anke; Rodigast, Maria; Iinuma, Yoshiteru Atmospheric Environment, Vol. 130 https://doi.org/10.1016/J.ATMOSENV.2015.10.080	journal	April 2016
Observations of Manaus urban plume evolution and interaction with biogenic emissions in GoAmazon 2014/5 Cirino, Glauber; Brito, Joel; Barbosa, Henrique M. J. Atmospheric Environment, Vol. 191 https://doi.org/10.1016/J.ATMOSENV.2018.08.031	journal	October 2018
Levoglucosan as a tracer of biomass burning: Recent progress and perspectives Bhattarai, Hemraj; Saikawa, Eri; Wan, Xin Atmospheric Research, Vol. 220 https://doi.org/10.1016/J.ATMOSRES.2019.01.004	journal	May 2019
Characterization and biodegradation of water-soluble biomarkers and organic carbon extracted from low temperature chars Norwood, Matt J.; Louchouarn, Patrick; Kuo, Li-Jung Organic Geochemistry, Vol. 56 https://doi.org/10.1016/J.ORGGEOCHEM.2012.12.008	journal	March 2013
Identification and emission factors of molecular tracers in organic aerosols from biomass burning Part 2. Deciduous trees Oros, Daniel R.; Simoneit, Bernd R. T. Applied Geochemistry, Vol. 16, Issue 13 https://doi.org/10.1016/S0883-2927(01)00022-1	journal	October 2001
Formation of new particles in the gas-phase ozonolysis of monoterpenes Koch, Stephan; Winterhalter, Richard; Uherek, Elmar Atmospheric Environment, Vol. 34, Issue 23 https://doi.org/10.1016/S1352-2310(00)00133-3	journal	January 2000
Known and Unexplored Organic Constituents in the Earth's Atmosphere Goldstein, Allen H.; Galbally, Ian E. Environmental Science & Technology, Vol. 41, Issue 5 https://doi.org/10.1021/ES072476P	journal	March 2007
Impact of Urban Pollution on Organic-Mediated New-Particle Formation and Particle Number Concentration in the Amazon Rainforest Zhao, Bin; Fast, Jerome D.; Donahue, Neil M. Environmental Science & Technology, Vol. 55, Issue 8 https://doi.org/10.1021/acs.est.0c07465	journal	March 2021
Quantifying Atmospheric Parameter Ranges for Ambient Secondary Organic Aerosol Formation Porter, William C.; Jimenez, Jose L.; Barsanti, Kelley C. ACS Earth and Space Chemistry, Vol. 5, Issue 9 https://doi.org/10.1021/acsearthspacechem.1c00090	journal	July 2021
Secondary Organic Aerosol Formation from Healthy and Aphid-Stressed Scots Pine Emissions Faiola, Celia L.; Pullinen, Iida; Buchholz, Angela ACS Earth and Space Chemistry, Vol. 3, Issue 9 https://doi.org/10.1021/acsearthspacechem.9b00118	journal	August 2019
Gas-Phase OH Oxidation of Monoterpenes: Gaseous and Particulate Products Larsen, Bo. R.; Di Bella, Dario; Glasius, Marianne Journal of Atmospheric Chemistry, Vol. 38, Issue 3, p. 231-276 https://doi.org/10.1023/A:1006487530903	journal	January 2001
Water-soluble organic compounds in biomass burning aerosols over Amazonia1. Characterization by NMR and GC-MS Graham, Bim Journal of Geophysical Research, Vol. 107, Issue D20 https://doi.org/10.1029/2001JD000336	journal	January 2002
Water-soluble organic compounds in biomass burning aerosols over Amazonia 2. Apportionment of the chemical composition and importance of the polyacidic fraction Mayol-Bracero, O. L. Journal of Geophysical Research, Vol. 107, Issue D20 https://doi.org/10.1029/2001JD000522	journal	January 2002
Overview of the inorganic and organic composition of size-segregated aerosol in Rondônia, Brazil, from the biomass-burning period to the onset of the wet season Fuzzi, Sandro; Decesari, Stefano; Facchini, Maria Cristina Journal of Geophysical Research, Vol. 112, Issue D1 https://doi.org/10.1029/2005JD006741	journal	January 2007
Sources and properties of Amazonian aerosol particles Martin, Scot T.; Andreae, Meinrat O.; Artaxo, Paulo Reviews of Geophysics, Vol. 48, Issue 2 https://doi.org/10.1029/2008RG000280	journal	January 2010
Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin Chen, Q.; Farmer, D. K.; Schneider, J. Geophysical Research Letters, Vol. 36, Issue 20 https://doi.org/10.1029/2009GL039880	journal	January 2009
Premature Deaths in Brazil Associated With Long‐Term Exposure to PM _2.5 From Amazon Fires Between 2016 and 2019 Nawaz, M. O.; Henze, D. K. GeoHealth, Vol. 4, Issue 8 https://doi.org/10.1029/2020GH000268	journal	August 2020
The Amazon basin in transition Davidson, Eric A.; de Araújo, Alessandro C.; Artaxo, Paulo Nature, Vol. 481, Issue 7381 https://doi.org/10.1038/nature10717	journal	January 2012
Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol Kroll, Jesse H.; Donahue, Neil M.; Jimenez, Jose L. Nature Chemistry, Vol. 3, Issue 2 https://doi.org/10.1038/nchem.948	journal	January 2011
Urban pollution greatly enhances formation of natural aerosols over the Amazon rainforest Shrivastava, Manish; Andreae, Meinrat O.; Artaxo, Paulo Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08909-4	journal	March 2019
Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass burning conditions Artaxo, Paulo; Rizzo, Luciana V.; Brito, Joel F. Faraday Discussions, Vol. 165 https://doi.org/10.1039/C3FD00052D	journal	January 2013
Organosulfates in aerosols downwind of an urban region in central Amazon Glasius, Marianne; Bering, Mads S.; Yee, Lindsay D. Environmental Science: Processes & Impacts, Vol. 20, Issue 11 https://doi.org/10.1039/C8EM00413G	journal	January 2018
Direct observation of aqueous secondary organic aerosol from biomass-burning emissions Gilardoni, Stefania; Massoli, Paola; Paglione, Marco Proceedings of the National Academy of Sciences, Vol. 113, Issue 36 https://doi.org/10.1073/pnas.1602212113	journal	August 2016
Monoterpenes are the largest source of summertime organic aerosol in the southeastern United States Zhang, Haofei; Yee, Lindsay D.; Lee, Ben H. Proceedings of the National Academy of Sciences, Vol. 115, Issue 9 https://doi.org/10.1073/pnas.1717513115	journal	February 2018
Recent deforestation drove the spike in Amazonian fires Cardil, Adrián; de-Miguel, Sergio; Silva, Carlos A. Environmental Research Letters, Vol. 15, Issue 12 https://doi.org/10.1088/1748-9326/abcac7	journal	December 2020
Isoprene photo-oxidation products quantify the effect of pollution on hydroxyl radicals over Amazonia Liu, Yingjun; Seco, Roger; Kim, Saewung Science Advances, Vol. 4, Issue 4 https://doi.org/10.1126/sciadv.aar2547	journal	April 2018
The fuel of atmospheric chemistry: Toward a complete description of reactive organic carbon Heald, C. L.; Kroll, J. H. Science Advances, Vol. 6, Issue 6 https://doi.org/10.1126/sciadv.aay8967	journal	February 2020
Linking Meteorology, Turbulence, and Air Chemistry in the Amazon Rain Forest Fuentes, Jose D.; Chamecki, Marcelo; Nascimento dos Santos, Rosa Maria Bulletin of the American Meteorological Society, Vol. 97, Issue 12, p. 2329-2342 https://doi.org/10.1175/BAMS-D-15-00152.1	journal	December 2016
Impact of exposure to smoke from biomass burning in the Amazon rain forest on human health Urrutia-Pereira1,2,3, Marilyn; Varanda Rizzo4, Luciana; José Chong-Neto5,6,7,8, Herberto Jornal Brasileiro de Pneumologia https://doi.org/10.36416/1806-3756/E20210219	journal	October 2021
Aqueous chemistry and its role in secondary organic aerosol (SOA) formation Lim, Y. B.; Tan, Y.; Perri, M. J. Atmospheric Chemistry and Physics, Vol. 10, Issue 21 https://doi.org/10.5194/ACP-10-10521-2010	journal	January 2010
Insights into secondary organic aerosol formed via aqueous-phase reactions of phenolic compounds based on high resolution mass spectrometry Sun, Y. L.; Zhang, Q.; Anastasio, C. Atmospheric Chemistry and Physics, Vol. 10, Issue 10 https://doi.org/10.5194/ACP-10-4809-2010	journal	January 2010
Molecular transformations of phenolic SOA during photochemical aging in the aqueous phase: competition among oligomerization, functionalization, and fragmentation Yu, Lu; Smith, Jeremy; Laskin, Alexander Atmospheric Chemistry and Physics, Vol. 16, Issue 7 https://doi.org/10.5194/ACP-16-4511-2016	journal	January 2016
Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5 Shilling, John E.; Pekour, Mikhail S.; Fortner, Edward C. Atmospheric Chemistry and Physics, Vol. 18, Issue 14 https://doi.org/10.5194/ACP-18-10773-2018	journal	January 2018
Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A. Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/ACP-18-467-2018	journal	January 2018
Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions Liu, Lixia; Cheng, Yafang; Wang, Siwen Atmospheric Chemistry and Physics, Vol. 20, Issue 21 https://doi.org/10.5194/ACP-20-13283-2020	journal	November 2020
Exploration of oxidative chemistry and secondary organic aerosol formation in the Amazon during the wet season: explicit modeling of the Manaus urban plume with GECKO-A Mouchel-Vallon, Camille; Lee-Taylor, Julia; Hodzic, Alma Atmospheric Chemistry and Physics, Vol. 20, Issue 10 https://doi.org/10.5194/ACP-20-5995-2020	journal	May 2020
Molecular composition and photochemical evolution of water-soluble organic carbon (WSOC) extracted from field biomass burning aerosols using high-resolution mass spectrometry Cai, Jing; Zeng, Xiangying; Zhi, Guorui Atmospheric Chemistry and Physics, Vol. 20, Issue 10 https://doi.org/10.5194/ACP-20-6115-2020	journal	January 2020
Aerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basin Nascimento, Janaína P.; Bela, Megan M.; Meller, Bruno B. Atmospheric Chemistry and Physics, Vol. 21, Issue 9 https://doi.org/10.5194/ACP-21-6755-2021	journal	January 2021
Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies Ervens, B.; Turpin, B. J.; Weber, R. J. Atmospheric Chemistry and Physics, Vol. 11, Issue 21 https://doi.org/10.5194/acp-11-11069-2011	journal	January 2011
Introduction: Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Martin, S. T.; Artaxo, P.; Machado, L. A. T. Atmospheric Chemistry and Physics, Vol. 16, Issue 8 https://doi.org/10.5194/acp-16-4785-2016	journal	January 2016
Contributions of mobile, stationary and biogenic sources to air pollution in the Amazon rainforest: a numerical study with the WRF-Chem model Abou Rafee, Sameh A.; Martins, Leila D.; Kawashima, Ana B. Atmospheric Chemistry and Physics, Vol. 17, Issue 12 https://doi.org/10.5194/acp-17-7977-2017	journal	January 2017
Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons Yee, Lindsay D.; Isaacman-VanWertz, Gabriel; Wernis, Rebecca A. Atmospheric Chemistry and Physics, Vol. 18, Issue 14 https://doi.org/10.5194/acp-18-10433-2018	journal	January 2018
Urban influence on the concentration and composition of submicron particulate matter in central Amazonia de Sá, Suzane S.; Palm, Brett B.; Campuzano-Jost, Pedro Atmospheric Chemistry and Physics, Vol. 18, Issue 16 https://doi.org/10.5194/acp-18-12185-2018	journal	January 2018
Is there an aerosol signature of chemical cloud processing? Ervens, Barbara; Sorooshian, Armin; Aldhaif, Abdulmonam M. Atmospheric Chemistry and Physics, Vol. 18, Issue 21 https://doi.org/10.5194/acp-18-16099-2018	journal	January 2018
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 de Sá, Suzane S.; Rizzo, Luciana V.; Palm, Brett B. Atmospheric Chemistry and Physics, Vol. 19, Issue 12 https://doi.org/10.5194/acp-19-7973-2019	journal	January 2019
Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations Rissler, J.; Swietlicki, E.; Zhou, J. Atmospheric Chemistry and Physics, Vol. 4, Issue 8 https://doi.org/10.5194/acp-4-2119-2004	journal	January 2004
Comprehensive detection of analytes in large chromatographic datasets by coupling factor analysis with a decision tree Kim, Sungwoo; Lerner, Brian M.; Sueper, Donna T. Atmospheric Measurement Techniques, Vol. 15, Issue 17 https://doi.org/10.5194/amt-15-5061-2022	journal	September 2022

Similar Records

Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons

Journal Article · Sun Jul 22 20:00:00 EDT 2018 · Atmospheric Chemistry and Physics (Online) · OSTI ID:1593306

Related Subjects

54 ENVIRONMENTAL SCIENCES
air pollution
biomass burning
cheminformatics
secondary organic aerosol
urbanization

Chemical Signatures of Seasonally Unique Anthropogenic Influences on Organic Aerosol Composition in the Central Amazon

Citation Formats

References (49)

Similar Records

Related Subjects