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

Abstract

We present field observations made in June 2011 downwind of Dallas-Fort Worth, TX, and evaluate the role of stabilized Criegee radicals (sCIs) in gaseous sulfuric acid (H2SO4) production. Zero-dimensional model calculations show that sCI from BVOCs composed the majority of the sCIs. The main uncertainty associated with an evaluation of H2SO4 production from the sCI reaction channel is the lack of experimentally determined reaction rates for sCIs formed from isoprene ozonolysis with SO2. In general, the maximum of H2SO4 production from the sCI channel is found in the late afternoon as ozone increases towards the late afternoon. The sCI channel, however, contributes minor H2SO4 production compared with the conventional OH channel. Finally, The production and the loss rates of H2SO4 are compared. The application of the recommended mass accommodation coefficient causes significant overestimation of H2SO4 loss rates compared with H2SO4 production rates. On the other hand, the application of a lower experimental value for the mass accommodation coefficient provides good agreement between the loss and production rates of H2SO4. The results suggest that the recommended coefficient for the H2O surface may not be suitable for this relatively dry environment.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1221492
Report Number(s):
PNNL-SA-108336
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Atmospheric Chemistry and Physics, 15(13):7413-7427
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics, 15(13):7413-7427
Country of Publication:
United States
Language:
English

Citation Formats

Wohlfahrt, G., Amelynck, C., Ammann, Christof, Arneth, A., Bamberger, Ines, Goldstein, Allen H., Gu, Lianhong, Guenther, Alex B., Hansel, A., Heinesch, B., Holst, Thomas, Hortnagl, Lukas, Karl, T., Laffineur, Q., Neftel, Albrecht, McKinney, Karena, Munger, William, Pallardy, Stephen G., Schade, Gunner W., Seco, Roger, 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, Christof, Arneth, A., Bamberger, Ines, Goldstein, Allen H., Gu, Lianhong, Guenther, Alex B., Hansel, A., Heinesch, B., Holst, Thomas, Hortnagl, Lukas, Karl, T., Laffineur, Q., Neftel, Albrecht, McKinney, Karena, Munger, William, Pallardy, Stephen G., Schade, Gunner W., Seco, Roger, & Schoon, N. An ecosystem-scale perspective of the net land methanol flux: synthesis of micrometeorological flux measurements. United States. doi:10.5194/acp-15-7413-2015.
Wohlfahrt, G., Amelynck, C., Ammann, Christof, Arneth, A., Bamberger, Ines, Goldstein, Allen H., Gu, Lianhong, Guenther, Alex B., Hansel, A., Heinesch, B., Holst, Thomas, Hortnagl, Lukas, Karl, T., Laffineur, Q., Neftel, Albrecht, McKinney, Karena, Munger, William, Pallardy, Stephen G., Schade, Gunner W., Seco, Roger, and Schoon, N. Thu . "An ecosystem-scale perspective of the net land methanol flux: synthesis of micrometeorological flux measurements". United States. doi:10.5194/acp-15-7413-2015.
@article{osti_1221492,
title = {An ecosystem-scale perspective of the net land methanol flux: synthesis of micrometeorological flux measurements},
author = {Wohlfahrt, G. and Amelynck, C. and Ammann, Christof and Arneth, A. and Bamberger, Ines and Goldstein, Allen H. and Gu, Lianhong and Guenther, Alex B. and Hansel, A. and Heinesch, B. and Holst, Thomas and Hortnagl, Lukas and Karl, T. and Laffineur, Q. and Neftel, Albrecht and McKinney, Karena and Munger, William and Pallardy, Stephen G. and Schade, Gunner W. and Seco, Roger and Schoon, N.},
abstractNote = {We present field observations made in June 2011 downwind of Dallas-Fort Worth, TX, and evaluate the role of stabilized Criegee radicals (sCIs) in gaseous sulfuric acid (H2SO4) production. Zero-dimensional model calculations show that sCI from BVOCs composed the majority of the sCIs. The main uncertainty associated with an evaluation of H2SO4 production from the sCI reaction channel is the lack of experimentally determined reaction rates for sCIs formed from isoprene ozonolysis with SO2. In general, the maximum of H2SO4 production from the sCI channel is found in the late afternoon as ozone increases towards the late afternoon. The sCI channel, however, contributes minor H2SO4 production compared with the conventional OH channel. Finally, The production and the loss rates of H2SO4 are compared. The application of the recommended mass accommodation coefficient causes significant overestimation of H2SO4 loss rates compared with H2SO4 production rates. On the other hand, the application of a lower experimental value for the mass accommodation coefficient provides good agreement between the loss and production rates of H2SO4. The results suggest that the recommended coefficient for the H2O surface may not be suitable for this relatively dry environment.},
doi = {10.5194/acp-15-7413-2015},
journal = {Atmospheric Chemistry and Physics, 15(13):7413-7427},
number = ,
volume = ,
place = {United States},
year = {2015},
month = {7}
}

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    Works referencing / citing this record:

    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