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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:
Journal Article: Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
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. 2015. "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},
url = {https://www.osti.gov/biblio/1214422}, journal = {Atmospheric Chemistry and Physics (Online)},
issn = {1680-7324},
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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Cited by: 28 works
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Works referenced in this record:

Gap-filling strategies for annual VOC flux data sets
journal, January 2014


Canopy Level Fluxes of 2-Methyl-3-buten-2-ol, Acetone, and Methanol by a Portable Relaxed Eddy Accumulation System
journal, May 2001


Induced BVOCs: how to bug our models?
journal, March 2010


New constraints on terrestrial and oceanic sources of atmospheric methanol
journal, January 2008


Dealing with disjunct concentration measurements in eddy covariance applications: A comparison of available approaches
journal, May 2010


A comparison of new measurements of total monoterpene flux with improved measurements of speciated monoterpene flux
journal, January 2005


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


Methanol and acetaldehyde fluxes over ryegrass
journal, January 2007


Proton transfer reaction mass spectrometry: on-line trace gas analysis at the ppb level
journal, November 1995


Short-chain oxygenated VOCs: Emission and uptake by plants and atmospheric sources, sinks, and concentrations
journal, April 2007


The bi-directional exchange of oxygenated VOCs between a loblolly pine (Pinus taeda) plantation and the atmosphere
journal, January 2005


Aerobic methanol-oxidizing Bacteria  in soil
journal, November 2009


Biogenic volatile emissions from the soil: Biogenic volatile emissions from the soil
journal, May 2014


Methanol exchange between grassland and the atmosphere
journal, January 2007


Methanol oxidation by temperate soils and environmental determinants of associated methylotrophs
journal, December 2012


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


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


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journal, January 1995


A model for studies of tropospheric ozone and nonmethane hydrocarbons: Model description and ozone results: MATCH-MPIC DESCRIPTION AND OZONE RESULTS
journal, May 2003


Distribution and fate of selected oxygenated organic species in the troposphere and lower stratosphere over the Atlantic
journal, February 2000


Is forest management a significant source of monoterpenes into the boreal atmosphere?
journal, January 2012


Net primary production of forests: a constant fraction of gross primary production?
journal, February 1998


Methanol and other VOC fluxes from a Danish beech forest during late springtime
journal, December 2010


Biogenic methanol and its impacts on tropospheric oxidants: BIOGENIC METHANOL AND ITS IMPACTS
journal, September 2003


Mixing ratios and eddy covariance flux measurements of volatile organic compounds from an urban canopy (Manchester, UK)
journal, January 2009


Fluxes and concentrations of volatile organic compounds above central London, UK
journal, January 2010


Contribution of leaf and needle litter to whole ecosystem BVOC fluxes
journal, November 2012


Emissions of organic carbon and methane from petroleum and dairy operations in California's San Joaquin Valley
journal, January 2014


Biotic, abiotic, and management controls on methanol exchange above a temperate mountain grassland
journal, January 2011


Global budget of CO, 1988–1997: Source estimates and validation with a global model
journal, January 2007


Quantification of VOC emission rates from the biosphere
journal, July 2011


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


Atmospheric methanol budget and ocean implication: ATMOSPHERIC BUDGET OF METHANOL
journal, December 2002


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


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


Flux measurements of volatile organic compounds from an urban landscape
journal, January 2005


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


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


Hydrocarbon fluxes above a Scots pine forest canopy: measurements and modeling
journal, January 2007


First eddy covariance flux measurements by PTR-TOF
journal, January 2010


Global budget of methanol: Constraints from atmospheric observations
journal, January 2005


Measurement of isoprene fluxes at the PROPHET site
journal, October 2001


Measuring Biosphere-Atmosphere Exchanges of Biologically Related Gases with Micrometeorological Methods
journal, October 1988


BVOC ecosystem flux measurements at a high latitude wetland site
journal, January 2010


On the separation of net ecosystem exchange into assimilation and ecosystem respiration: review and improved algorithm
journal, September 2005


Leaf methanol — the simplest natural product from plants
journal, September 1996


Contributions of biogenic volatile organic compounds to net ecosystem carbon flux in a ponderosa pine plantation
journal, December 2012


Multi metric evaluation of leaf wetness models for large-area application of plant disease models
journal, September 2011


Eddy covariance measurements of oxygenated volatile organic compound fluxes from crop harvesting using a redesigned proton-transfer-reaction mass spectrometer
journal, October 2001


Qualitative and Quantitative Characterization of Volatile Organic Compound Emissions from Cut Grass
journal, March 2012


OVOC emissions from agricultural soil in northern Germany during the 2003 European heat wave
journal, November 2004


Mapping isoprene emissions over North America using formaldehyde column observations from space
journal, January 2003


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


Eddy covariance flux measurements of pollutant gases in urban Mexico City
journal, January 2009


Fluxes of oxygenated volatile organic compounds from a ponderosa pine plantation
journal, February 2001


FLUXNET: A New Tool to Study the Temporal and Spatial Variability of Ecosystem–Scale Carbon Dioxide, Water Vapor, and Energy Flux Densities
journal, November 2001


Eddy covariance VOC emission and deposition fluxes above grassland using PTR-TOF
journal, January 2011


Simultaneous leaf- and ecosystem-level fluxes of volatile organic compounds from a poplar-based SRC plantation
journal, April 2014


Environmental controls over methanol emission from leaves
journal, January 2007


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


Global human appropriation of net primary production doubled in the 20th century
journal, June 2013


High resolution PTR-TOF: Quantification and formula confirmation of VOC in real time
journal, June 2010


Simultaneous leaf- and ecosystem-level fluxes of volatile organic compounds from a poplar-based SRC plantation
journal, April 2014


OVOC emissions from agricultural soil in northern Germany during the 2003 European heat wave
journal, November 2004


High resolution PTR-TOF: Quantification and formula confirmation of VOC in real time
journal, June 2010


Canopy Level Fluxes of 2-Methyl-3-buten-2-ol, Acetone, and Methanol by a Portable Relaxed Eddy Accumulation System
journal, May 2001


Qualitative and Quantitative Characterization of Volatile Organic Compound Emissions from Cut Grass
journal, March 2012


Methanol oxidation by temperate soils and environmental determinants of associated methylotrophs
journal, December 2012


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


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


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


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


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


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


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


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


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:

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


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


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


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


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


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