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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 O 3 via reaction with isoprene or terpenes during the wet and dry seasons, respectively. This is reduced from ~50–70 % for within-canopy reactive O 3 loss attributed to the ozonolysis of highly reactive sesquiterpenes (e.g., β-caryophyllene) that are reacted away before reaching our measurement site. Wemore » 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.« 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];  [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
  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 Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1593306
Report Number(s):
PNNL-SA-138448
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
AC05-76RL01830; SC0014040; SC0004698; SC0016559
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.
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. doi:10.5194/acp-18-10433-2018.
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. doi:10.5194/acp-18-10433-2018. https://www.osti.gov/servlets/purl/1593306.
@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 = {2018},
month = {7}
}

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  • Loza, Christine L.; Chan, Arthur W. H.; Galloway, Melissa M.
  • Environmental Science & Technology, Vol. 44, Issue 13
  • DOI: 10.1021/es100727v

Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO 2 emission controls
journal, January 2016

  • Marais, E. A.; Jacob, D. J.; Jimenez, J. L.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 3
  • DOI: 10.5194/acp-16-1603-2016

Sources and properties of Amazonian aerosol particles
journal, January 2010

  • Martin, Scot T.; Andreae, Meinrat O.; Artaxo, Paulo
  • Reviews of Geophysics, Vol. 48, Issue 2
  • DOI: 10.1029/2008RG000280

Introduction: Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5)
journal, January 2016

  • Martin, S. T.; Artaxo, P.; Machado, L. A. T.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 8
  • DOI: 10.5194/acp-16-4785-2016

The Arm Climate Research Facility: A Review of Structure and Capabilities
journal, March 2013

  • Mather, James H.; Voyles, Jimmy W.
  • Bulletin of the American Meteorological Society, Vol. 94, Issue 3
  • DOI: 10.1175/BAMS-D-11-00218.1

Gas-Wall Partitioning of Organic Compounds in a Teflon Film Chamber and Potential Effects on Reaction Product and Aerosol Yield Measurements
journal, August 2010


Gas and aerosol wall losses in Teflon film smog chambers
journal, December 1985

  • McMurry, Peter H.; Grosjean, Daniel.
  • Environmental Science & Technology, Vol. 19, Issue 12
  • DOI: 10.1021/es00142a006

Vapor–Wall Deposition in Chambers: Theoretical Considerations
journal, August 2014

  • McVay, Renee C.; Cappa, Christopher D.; Seinfeld, John H.
  • Environmental Science & Technology, Vol. 48, Issue 17
  • DOI: 10.1021/es502170j

Organic aerosol formation from the reactive uptake of isoprene epoxydiols (IEPOX) onto non-acidified inorganic seeds
journal, January 2014

  • Nguyen, T. B.; Coggon, M. M.; Bates, K. H.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 7
  • DOI: 10.5194/acp-14-3497-2014

The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges
journal, February 2015

  • Nozière, Barbara; Kalberer, Markus; Claeys, Magda
  • Chemical Reviews, Vol. 115, Issue 10
  • DOI: 10.1021/cr5003485

Predicting Thermal Behavior of Secondary Organic Aerosols
journal, August 2017

  • Offenberg, John H.; Lewandowski, Michael; Kleindienst, Tadeusz E.
  • Environmental Science & Technology, Vol. 51, Issue 17
  • DOI: 10.1021/acs.est.7b01968

Sesquiterpenoid Emissions from Agricultural Crops: Correlations to Monoterpenoid Emissions and Leaf Terpene Content
journal, May 2010

  • Ormeño, Elena; Gentner, Drew R.; Fares, Silvano
  • Environmental Science & Technology, Vol. 44, Issue 10
  • DOI: 10.1021/es903674m

Unexpected Epoxide Formation in the Gas-Phase Photooxidation of Isoprene
journal, August 2009


Rainforest Aerosols as Biogenic Nuclei of Clouds and Precipitation in the Amazon
journal, September 2010


Trans - β -Caryophyllene: An Effective Antileishmanial Compound Found in Commercial Copaiba Oil ( Copaifera spp.)
journal, January 2013

  • Soares, Deivid C.; Portella, Nathalya A.; Ramos, Mônica Freiman de S.
  • Evidence-Based Complementary and Alternative Medicine, Vol. 2013
  • DOI: 10.1155/2013/761323

Estimating probabilities of correct identification from results of mass spectral library searches
journal, April 1994


Chemical Composition of Secondary Organic Aerosol Formed from the Photooxidation of Isoprene
journal, August 2006

  • Surratt, Jason D.; Murphy, Shane M.; Kroll, Jesse H.
  • The Journal of Physical Chemistry A, Vol. 110, Issue 31
  • DOI: 10.1021/jp061734m

Reactive intermediates revealed in secondary organic aerosol formation from isoprene
journal, December 2009

  • Surratt, J. D.; Chan, A. W. H.; Eddingsaas, N. C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911114107

3-methyl-1,2,3-butanetricarboxylic acid: An atmospheric tracer for terpene secondary organic aerosol
journal, January 2007

  • Szmigielski, Rafal; Surratt, Jason D.; Gómez-González, Yadian
  • Geophysical Research Letters, Vol. 34, Issue 24
  • DOI: 10.1029/2007GL031338

Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013
journal, September 2016

  • Thompson, Samantha L.; Yatavelli, Reddy L. N.; Stark, Harald
  • Aerosol Science and Technology, Vol. 51, Issue 1
  • DOI: 10.1080/02786826.2016.1254719

New tracer compounds for secondary organic aerosol formation from β-caryophyllene oxidation
journal, December 2013


Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall
journal, October 2016

  • Wang, Jian; Krejci, Radovan; Giangrande, Scott
  • Nature, Vol. 539, Issue 7629, p. 416-419
  • DOI: 10.1038/nature19819

An In-Situ Instrument for Speciated Organic Composition of Atmospheric Aerosols: T hermal Desorption A erosol G C/MS-FID (TAG)
journal, June 2006

  • Williams, Brent J.; Goldstein, Allen H.; Kreisberg, Nathan M.
  • Aerosol Science and Technology, Vol. 40, Issue 8
  • DOI: 10.1080/02786820600754631

The gas-phase ozonolysis of β-caryophyllene (C15H24). Part I: an experimental study
journal, January 2009

  • Winterhalter, Richard; Herrmann, Frank; Kanawati, Basem
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 21
  • DOI: 10.1039/b817824k

Embracing Complexity: Deciphering Origins and Transformations of Atmospheric Organics through Speciated Measurements
journal, April 2012

  • Worton, David R.; Gentner, Drew R.; Isaacman, Gabriel
  • Environmental Science & Technology, Vol. 46, Issue 10
  • DOI: 10.1021/es301199y

Effects of NO x on the Volatility of Secondary Organic Aerosol from Isoprene Photooxidation
journal, February 2014

  • Xu, Lu; Kollman, Matthew S.; Song, Chen
  • Environmental Science & Technology, Vol. 48, Issue 4
  • DOI: 10.1021/es404842g

Diel and seasonal changes of biogenic volatile organic compounds within and above an Amazonian rainforest
journal, January 2015

  • Yáñez-Serrano, A. M.; Nölscher, A. C.; Williams, J.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 6
  • DOI: 10.5194/acp-15-3359-2015

Monoterpene chemical speciation in a tropical rainforest:variation with season, height, and time of dayat the Amazon Tall Tower Observatory (ATTO)
journal, January 2018

  • Yáñez-Serrano, Ana María; Nölscher, Anke Christine; Bourtsoukidis, Efstratios
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 5
  • DOI: 10.5194/acp-18-3403-2018

Vapor wall loss of semi-volatile organic compounds in a Teflon chamber
journal, June 2016


Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol
journal, April 2014

  • Zhang, X.; Cappa, C. D.; Jathar, S. H.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 16
  • DOI: 10.1073/pnas.1404727111

Vapor wall deposition in Teflon chambers
journal, January 2015

  • Zhang, X.; Schwantes, R. H.; McVay, R. C.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 8
  • DOI: 10.5194/acp-15-4197-2015

Development of an In Situ Thermal Desorption Gas Chromatography Instrument for Quantifying Atmospheric Semi-Volatile Organic Compounds
journal, December 2012


A new processing scheme for ultra-high resolution direct infusion mass spectrometry data
journal, April 2018