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

Abstract

Biogenic volatile organic compounds (BVOCs) from the Amazon forest region represent the largest source of organic carbon emissions to the atmosphere globally. These BVOC emissions dominantly consist of volatile and intermediate-volatility terpenoid compounds that undergo chemical transformations in the atmosphere to form oxygenated condensable gases and secondary organic aerosol (SOA). We collected quartz filter samples with 12 h time resolution and performed hourly in situ measurements with a semi-volatile thermal desorption aerosol gas chromatograph (SV-TAG) at a rural site ("T3") located to the west of the urban center of Manaus, Brazil as part of the Green Ocean Amazon (GoAmazon2014/5) field campaign to measure intermediate-volatility and semi-volatile BVOCs and their oxidation products during the wet and dry seasons. We speciated and quantified 30 sesquiterpenes and 4 diterpenes with mean concentrations in the range 0.01–6.04 ng m-3 (1–670 ppqv). We estimate that sesquiterpenes contribute approximately 14 and 12 % to the total reactive loss of O3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from ~50–70 % for within-canopy reactive O3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., β-caryophyllene) that are reacted away before reaching our measurement site. We further identify amore » suite of their oxidation products in the gas and particle phases and explore their role in biogenic SOA formation in the central Amazon region. Synthesized authentic standards were also used to quantify gas- and particle-phase oxidation products derived from β-caryophyllene. Using tracer-based scaling methods for these products, we roughly estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. By comparing our field data to laboratory-based sesquiterpene oxidation experiments we confirm that more than 40 additional observed compounds produced through sesquiterpene oxidation are present in Amazonian SOA, warranting further efforts towards more complete quantification.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [3];  [4];  [4]; ORCiD logo [4];  [4]; ORCiD logo [5];  [5];  [6]; ORCiD logo [6];  [7];  [7];  [8] more »; ORCiD logo [9]; ORCiD logo [9]; ORCiD logo [9]; ORCiD logo [9]; ORCiD logo [9]; ORCiD logo [7]; ORCiD logo [7]; ORCiD logo [10];  [11];  [11];  [12];  [12]; ORCiD logo [13];  [14]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States)
  2. Aerosol Dynamics, Inc., Berkeley, CA (United States)
  3. Aarhus Univ. (Denmark)
  4. Northwestern Univ., Evanston, IL (United States)
  5. Research Triangle Park, NC (United States)
  6. Univ. of Cambridge (United Kingdom)
  7. Harvard Univ., Cambridge, MA (United States)
  8. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  9. Univ. of Colorado, Boulder, CO (United States)
  10. Univ. of Sao Paulo (Brazil)
  11. Instituto Nacional de Pesquisas da Amazonia, Manaus, AM (Brazil)
  12. Universidade do Estado do Amazonas, Manaus, AM (Brazil)
  13. Instituto Nacional de Pesquisas Espiacais, São José dos Campos, SP (Brazil)
  14. Instituto Nacional de Pesquisas Espiacais, Cachoeira Paulista, SP (Brazil)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); University of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF); Brazilian National Council for Scientific and Technological Development (CNPq); USEPA; National Aeronautics and Space Administration (NASA); Alexander von Humboldt Foundation
OSTI Identifier:
1593306
Alternate Identifier(s):
OSTI ID: 1657284
Report Number(s):
PNNL-SA-138448
Journal ID: ISSN 1680-7324; TRN: US2100903
Grant/Contract Number:  
AC05-76RL01830; SC0014040; SC0004698; SC0016559; 1332998; CHE-1607640
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: 14; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Yee, Lindsay D., Isaacman-VanWertz, Gabriel, Wernis, Rebecca A., Meng, Meng, Rivera, Ventura, Kreisberg, Nathan M., Hering, Susanne V., Bering, Mads S., Glasius, Marianne, Upshur, Mary Alice, Gray Bé, Ariana, Thomson, Regan J., Geiger, Franz M., Offenberg, John H., Lewandowski, Michael, Kourtchev, Ivan, Kalberer, Markus, de Sá, Suzane, Martin, Scot T., Alexander, M. Lizabeth, Palm, Brett B., Hu, Weiwei, Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, Jose L., Liu, Yingjun, McKinney, Karena A., Artaxo, Paulo, Viegas, Juarez, Manzi, Antonio, Oliveira, Maria B., de Souza, Rodrigo, Machado, Luiz A. T., Longo, Karla, and Goldstein, Allen H. Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons. United States: N. p., 2018. Web. doi:10.5194/acp-18-10433-2018.
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Yee, Lindsay D., Isaacman-VanWertz, Gabriel, Wernis, Rebecca A., Meng, Meng, Rivera, Ventura, Kreisberg, Nathan M., Hering, Susanne V., Bering, Mads S., Glasius, Marianne, Upshur, Mary Alice, Gray Bé, Ariana, Thomson, Regan J., Geiger, Franz M., Offenberg, John H., Lewandowski, Michael, Kourtchev, Ivan, Kalberer, Markus, de Sá, Suzane, Martin, Scot T., Alexander, M. Lizabeth, Palm, Brett B., Hu, Weiwei, Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, Jose L., Liu, Yingjun, McKinney, Karena A., Artaxo, Paulo, Viegas, Juarez, Manzi, Antonio, Oliveira, Maria B., de Souza, Rodrigo, Machado, Luiz A. T., Longo, Karla, & Goldstein, Allen H. Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons. United States. https://doi.org/10.5194/acp-18-10433-2018
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Yee, Lindsay D., Isaacman-VanWertz, Gabriel, Wernis, Rebecca A., Meng, Meng, Rivera, Ventura, Kreisberg, Nathan M., Hering, Susanne V., Bering, Mads S., Glasius, Marianne, Upshur, Mary Alice, Gray Bé, Ariana, Thomson, Regan J., Geiger, Franz M., Offenberg, John H., Lewandowski, Michael, Kourtchev, Ivan, Kalberer, Markus, de Sá, Suzane, Martin, Scot T., Alexander, M. Lizabeth, Palm, Brett B., Hu, Weiwei, Campuzano-Jost, Pedro, Day, Douglas A., Jimenez, Jose L., Liu, Yingjun, McKinney, Karena A., Artaxo, Paulo, Viegas, Juarez, Manzi, Antonio, Oliveira, Maria B., de Souza, Rodrigo, Machado, Luiz A. T., Longo, Karla, and Goldstein, Allen H. Mon . "Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons". United States. https://doi.org/10.5194/acp-18-10433-2018. https://www.osti.gov/servlets/purl/1593306.
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@article{osti_1593306,
title = {Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons},
author = {Yee, Lindsay D. and Isaacman-VanWertz, Gabriel and Wernis, Rebecca A. and Meng, Meng and Rivera, Ventura and Kreisberg, Nathan M. and Hering, Susanne V. and Bering, Mads S. and Glasius, Marianne and Upshur, Mary Alice and Gray Bé, Ariana and Thomson, Regan J. and Geiger, Franz M. and Offenberg, John H. and Lewandowski, Michael and Kourtchev, Ivan and Kalberer, Markus and de Sá, Suzane and Martin, Scot T. and Alexander, M. Lizabeth and Palm, Brett B. and Hu, Weiwei and Campuzano-Jost, Pedro and Day, Douglas A. and Jimenez, Jose L. and Liu, Yingjun and McKinney, Karena A. and Artaxo, Paulo and Viegas, Juarez and Manzi, Antonio and Oliveira, Maria B. and de Souza, Rodrigo and Machado, Luiz A. T. and Longo, Karla and Goldstein, Allen H.},
abstractNote = {Biogenic volatile organic compounds (BVOCs) from the Amazon forest region represent the largest source of organic carbon emissions to the atmosphere globally. These BVOC emissions dominantly consist of volatile and intermediate-volatility terpenoid compounds that undergo chemical transformations in the atmosphere to form oxygenated condensable gases and secondary organic aerosol (SOA). We collected quartz filter samples with 12 h time resolution and performed hourly in situ measurements with a semi-volatile thermal desorption aerosol gas chromatograph (SV-TAG) at a rural site ("T3") located to the west of the urban center of Manaus, Brazil as part of the Green Ocean Amazon (GoAmazon2014/5) field campaign to measure intermediate-volatility and semi-volatile BVOCs and their oxidation products during the wet and dry seasons. We speciated and quantified 30 sesquiterpenes and 4 diterpenes with mean concentrations in the range 0.01–6.04 ng m-3 (1–670 ppqv). We estimate that sesquiterpenes contribute approximately 14 and 12 % to the total reactive loss of O3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from ~50–70 % for within-canopy reactive O3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., β-caryophyllene) that are reacted away before reaching our measurement site. We further identify a suite of their oxidation products in the gas and particle phases and explore their role in biogenic SOA formation in the central Amazon region. Synthesized authentic standards were also used to quantify gas- and particle-phase oxidation products derived from β-caryophyllene. Using tracer-based scaling methods for these products, we roughly estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. By comparing our field data to laboratory-based sesquiterpene oxidation experiments we confirm that more than 40 additional observed compounds produced through sesquiterpene oxidation are present in Amazonian SOA, warranting further efforts towards more complete quantification.},
doi = {10.5194/acp-18-10433-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 14,
volume = 18,
place = {United States},
year = {Mon Jul 23 00:00:00 EDT 2018},
month = {Mon Jul 23 00:00:00 EDT 2018}
}
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