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Title: An ecosystem-scale perspective of the net land methanol flux. Synthesis of micrometeorological flux measurements

Abstract

Methanol is the second most abundant volatile organic compound in the troposphere and plays a significant role in atmospheric chemistry. While there is consensus about the dominant role of living plants as the major source and the reaction with OH as the major sink of methanol, global methanol budgets diverge considerably in terms of source/sink estimates, reflecting uncertainties in the approaches used to model and the empirical data used to separately constrain these terms. Here we compiled micrometeorological methanol flux data from eight different study sites and reviewed the corresponding literature in order to provide a first cross-site synthesis of the terrestrial ecosystem-scale methanol exchange and present an independent data-driven view of the land–atmosphere methanol exchange. Our study shows that the controls of plant growth on production, and thus the methanol emission magnitude, as well as stomatal conductance on the hourly methanol emission variability, established at the leaf level, hold across sites at the ecosystem level. Unequivocal evidence for bi-directional methanol exchange at the ecosystem scale is presented. Deposition, which at some sites even exceeds methanol emissions, represents an emerging feature of ecosystem-scale measurements and is likely related to environmental factors favouring the formation of surface wetness. Methanol may adsorbmore » to or dissolve in this surface water and eventually be chemically or biologically removed from it. Management activities in agriculture and forestry are shown to increase local methanol emission by orders of magnitude; however, they are neglected at present in global budgets. While contemporary net land methanol budgets are overall consistent with the grand mean of the micrometeorological methanol flux measurements, we caution that the present approach of simulating methanol emission and deposition separately is prone to opposing systematic errors and does not allow for full advantage to be taken of the rich information content of micrometeorological flux measurements.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8];  [9];  [10];  [11];  [12]; ORCiD logo [9];  [13];  [3];  [14]; ORCiD logo [14];  [15];  [16]; ORCiD logo [17] more »;  [2] « less
  1. Univ. of Innsbruck (Austria); Eurpean Academy of Bolzano (Italy)
  2. Belgian Institute for Space Aeronomy (Belgium)
  3. Research Station Agroscope (Switzerland)
  4. Karlsruhe Inst. of Technology (KIT) Garmisch-Partenkirchen (Germany). IMK-IFU
  5. ETH Zurich (Switzerland). Institute of Agricultural Sciences; Karlsruhe Inst. of Technology (KIT) Garmisch-Partenkirchen (Germany). IMK-IFU
  6. Univ. of California, Berkeley, CA (United States)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  8. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  9. Univ. of Innsbruck (Austria)
  10. Univ. of Liege, (Belgium). Exchanges Ecosystems-Atmosphere, Department Biosystem Engineering (BIOSE)
  11. Lund Univ. (Sweden)
  12. ETH Zurich (Switzerland). Institute of Agricultural Sciences
  13. Royal Meteorological Inst. (Belgium)
  14. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences (SEAS)
  15. Univ. of Missouri, Columbia, MO (United States)
  16. Texas A & M Univ., College Station, TX (United States)
  17. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1214422
Alternate Identifier(s):
OSTI ID: 1265745
Grant/Contract Number:  
P19849-B16; P23267-B16; L518-N20; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 15; Journal Issue: 13; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Wohlfahrt, G., Amelynck, C., Ammann, C., Arneth, A., Bamberger, I., Goldstein, A. H., Gu, L., Guenther, A., Hansel, A., Heinesch, B., Holst, T., Hörtnagl, L., Karl, T., Laffineur, Q., Neftel, A., McKinney, K., Munger, J. W., Pallardy, S. G., Schade, G. W., Seco, R., and Schoon, N.. An ecosystem-scale perspective of the net land methanol flux. Synthesis of micrometeorological flux measurements. United States: N. p., 2015. Web. doi:10.5194/acp-15-7413-2015.
Wohlfahrt, G., Amelynck, C., Ammann, C., Arneth, A., Bamberger, I., Goldstein, A. H., Gu, L., Guenther, A., Hansel, A., Heinesch, B., Holst, T., Hörtnagl, L., Karl, T., Laffineur, Q., Neftel, A., McKinney, K., Munger, J. W., Pallardy, S. G., Schade, G. W., Seco, R., & Schoon, N.. An ecosystem-scale perspective of the net land methanol flux. Synthesis of micrometeorological flux measurements. United States. https://doi.org/10.5194/acp-15-7413-2015
Wohlfahrt, G., Amelynck, C., Ammann, C., Arneth, A., Bamberger, I., Goldstein, A. H., Gu, L., Guenther, A., Hansel, A., Heinesch, B., Holst, T., Hörtnagl, L., Karl, T., Laffineur, Q., Neftel, A., McKinney, K., Munger, J. W., Pallardy, S. G., Schade, G. W., Seco, R., and Schoon, N.. Thu . "An ecosystem-scale perspective of the net land methanol flux. Synthesis of micrometeorological flux measurements". United States. https://doi.org/10.5194/acp-15-7413-2015. https://www.osti.gov/servlets/purl/1214422.
@article{osti_1214422,
title = {An ecosystem-scale perspective of the net land methanol flux. Synthesis of micrometeorological flux measurements},
author = {Wohlfahrt, G. and Amelynck, C. and Ammann, C. and Arneth, A. and Bamberger, I. and Goldstein, A. H. and Gu, L. and Guenther, A. and Hansel, A. and Heinesch, B. and Holst, T. and Hörtnagl, L. and Karl, T. and Laffineur, Q. and Neftel, A. and McKinney, K. and Munger, J. W. and Pallardy, S. G. and Schade, G. W. and Seco, R. and Schoon, N.},
abstractNote = {Methanol is the second most abundant volatile organic compound in the troposphere and plays a significant role in atmospheric chemistry. While there is consensus about the dominant role of living plants as the major source and the reaction with OH as the major sink of methanol, global methanol budgets diverge considerably in terms of source/sink estimates, reflecting uncertainties in the approaches used to model and the empirical data used to separately constrain these terms. Here we compiled micrometeorological methanol flux data from eight different study sites and reviewed the corresponding literature in order to provide a first cross-site synthesis of the terrestrial ecosystem-scale methanol exchange and present an independent data-driven view of the land–atmosphere methanol exchange. Our study shows that the controls of plant growth on production, and thus the methanol emission magnitude, as well as stomatal conductance on the hourly methanol emission variability, established at the leaf level, hold across sites at the ecosystem level. Unequivocal evidence for bi-directional methanol exchange at the ecosystem scale is presented. Deposition, which at some sites even exceeds methanol emissions, represents an emerging feature of ecosystem-scale measurements and is likely related to environmental factors favouring the formation of surface wetness. Methanol may adsorb to or dissolve in this surface water and eventually be chemically or biologically removed from it. Management activities in agriculture and forestry are shown to increase local methanol emission by orders of magnitude; however, they are neglected at present in global budgets. While contemporary net land methanol budgets are overall consistent with the grand mean of the micrometeorological methanol flux measurements, we caution that the present approach of simulating methanol emission and deposition separately is prone to opposing systematic errors and does not allow for full advantage to be taken of the rich information content of micrometeorological flux measurements.},
doi = {10.5194/acp-15-7413-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 13,
volume = 15,
place = {United States},
year = {Thu Jul 09 00:00:00 EDT 2015},
month = {Thu Jul 09 00:00:00 EDT 2015}
}

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Qualitative and Quantitative Characterization of Volatile Organic Compound Emissions from Cut Grass
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Methanol oxidation by temperate soils and environmental determinants of associated methylotrophs
journal, December 2012

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  • The ISME Journal, Vol. 7, Issue 5
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Simultaneous growth and emission measurements demonstrate an interactive control of methanol release by leaf expansion and stomata
journal, March 2007

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  • Journal of Experimental Botany, Vol. 58, Issue 7
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Net primary production of forests: a constant fraction of gross primary production?
journal, February 1998


Interannual and seasonal changes in the soil exchange rates of monoterpenes and other VOCs in a Mediterranean shrubland
journal, October 2008


Leaf and root pectin methylesterase activity and 13C/12C stable isotopic ratio measurements of methanol emissions give insight into methanol production in Lycopersicon esculentum
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Aerobic methanol-oxidizing Bacteria  in soil
journal, November 2009


Terrestrial Gross Carbon Dioxide Uptake: Global Distribution and Covariation with Climate
journal, July 2010


Active Atmosphere-Ecosystem Exchange of the Vast Majority of Detected Volatile Organic Compounds
journal, August 2013


Cataloguing Soil Carbon Stocks
journal, December 2010


Soil microorganisms as controllers of atmospheric trace gases (H2, CO, CH4, OCS, N2O, and NO).
journal, January 1996


Methanol and acetaldehyde fluxes over ryegrass
journal, September 2007


Fluxes and concentrations of volatile organic compounds from a South-East Asian tropical rainforest
journal, January 2010

  • Langford, B.; Misztal, P. K.; Nemitz, E.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 17
  • DOI: 10.5194/acp-10-8391-2010

Emissions of isoprenoids and oxygenated biogenic volatile organic compounds from a New England mixed forest
journal, January 2011

  • McKinney, K. A.; Lee, B. H.; Vasta, A.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 10
  • DOI: 10.5194/acp-11-4807-2011

Abiotic and biotic control of methanol exchanges in a temperate mixed forest
journal, January 2012

  • Laffineur, Q.; Aubinet, M.; Schoon, N.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 1
  • DOI: 10.5194/acp-12-577-2012

Seasonal cycles of biogenic volatile organic compound fluxes and concentrations in a California citrus orchard
journal, January 2012

  • Fares, S.; Park, J. -H.; Gentner, D. R.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 20
  • DOI: 10.5194/acp-12-9865-2012

Virtual disjunct eddy covariance measurements of organic compound fluxes from a subalpine forest using proton transfer reaction mass spectrometry
journal, January 2002

  • Karl, T. G.; Spirig, C.; Rinne, J.
  • Atmospheric Chemistry and Physics, Vol. 2, Issue 4
  • DOI: 10.5194/acp-2-279-2002

Eddy covariance flux measurements of biogenic VOCs during ECHO 2003 using proton transfer reaction mass spectrometry
journal, January 2005

  • Spirig, C.; Neftel, A.; Ammann, C.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 2
  • DOI: 10.5194/acp-5-465-2005

Eddy covariance VOC emission and deposition fluxes above grassland using PTR-TOF
posted_content, September 2010


Direct ecosystem fluxes of volatile organic compounds from oil palms in South-East Asia
posted_content, August 2011


First space-based derivation of the global atmospheric methanol emission fluxes
journal, January 2011

  • Stavrakou, T.; Guenther, A.; Razavi, A.
  • Atmospheric Chemistry and Physics Discussions, Vol. 11, Issue 2
  • DOI: 10.5194/acpd-11-5217-2011

Hydrocarbon fluxes above a Scots pine forest canopy: Measurements and modeling
journal, February 2007


BVOC ecosystem flux measurements at a high latitude wetland site
posted_content, December 2008


Fluxes and concentrations of volatile organic compounds above central London, UK
posted_content, August 2009


Environmental controls over methanol emission from leaves
journal, January 2007


Modelling the dynamic chemical interactions of atmospheric ammonia with leaf surface wetness in a managed grassland canopy
journal, January 2009

  • Burkhardt, J.; Flechard, C. R.; Gresens, F.
  • Biogeosciences, Vol. 6, Issue 1
  • DOI: 10.5194/bg-6-67-2009

Methanol exchange between grassland and the atmosphere
journal, January 2007


Is forest management a significant source of monoterpenes into the boreal atmosphere?
posted_content, August 2011


Works referencing / citing this record:

Ecosystem-scale volatile organic compound fluxes during an extreme drought in a broadleaf temperate forest of the Missouri Ozarks (central USA)
journal, July 2015

  • Seco, Roger; Karl, Thomas; Guenther, Alex
  • Global Change Biology, Vol. 21, Issue 10
  • DOI: 10.1111/gcb.12980

Acidotolerant Bacteria and Fungi as a Sink of Methanol-Derived Carbon in a Deciduous Forest Soil
journal, July 2017


Modelling bidirectional fluxes of methanol and acetaldehyde with the FORCAsT canopy exchange model
journal, January 2016

  • Ashworth, Kirsti; Chung, Serena H.; McKinney, Karena A.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 24
  • DOI: 10.5194/acp-16-15461-2016

Canopy-scale flux measurements and bottom-up emission estimates of volatile organic compounds from a mixed oak and hornbeam forest in northern Italy
journal, January 2016

  • Acton, W. Joe F.; Schallhart, Simon; Langford, Ben
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 11
  • DOI: 10.5194/acp-16-7149-2016

Anthropogenic and biogenic influence on VOC fluxes at an urban background site in Helsinki, Finland
journal, January 2016

  • Rantala, Pekka; Järvi, Leena; Taipale, Risto
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 12
  • DOI: 10.5194/acp-16-7981-2016

Temporal variation of VOC fluxes measured with PTR-TOF above a boreal forest
journal, January 2018

  • Schallhart, Simon; Rantala, Pekka; Kajos, Maija K.
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 2
  • DOI: 10.5194/acp-18-815-2018

Annual cycle of volatile organic compound exchange between a boreal pine forest and the atmosphere
journal, January 2015


Canopy-scale flux measurements and bottom-up emission estimates of volatile organic compounds from a mixed oak and hornbeam forest in northern Italy
posted_content, October 2015


Annual cycle of volatile organic compound exchange between a boreal pine forest and the atmosphere
posted_content, June 2015


Temporal variation of VOC fluxes measured with PTR-TOF above a boreal forest
journal, June 2017

  • Schallhart, Simon; Rantala, Pekka; Kajos, Maija K.
  • Atmospheric Chemistry and Physics Discussions
  • DOI: 10.5194/acp-2017-394

Acidotolerant Bacteria and Fungi as a Sink of Methanol-Derived Carbon in a Deciduous Forest Soil
journal, July 2017