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  Uptake of gaseous formaldehyde by soil surfaces: a combination of adsorption/desorption equilibrium and chemical reactions

Li, G., Su, H., Li, X., Kuhn, U., Meusel, H., Hoffmann, T., et al. (2016). Uptake of gaseous formaldehyde by soil surfaces: a combination of adsorption/desorption equilibrium and chemical reactions. Atmospheric Chemistry and Physics, 16(15), 10299-10311. doi:10.5194/acp-16-10299-2016.

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 Creators:
Li, G.1, Author              
Su, H.1, Author              
Li, Xin2, Author
Kuhn, U.1, Author              
Meusel, H.1, Author              
Hoffmann, Thorsten2, Author
Ammann, Markus2, Author
Pöschl, U.1, Author              
Shao, Min2, Author
Cheng, Y.1, Author              
Affiliations:
1Multiphase Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826290              
2external, ou_persistent22              

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 Abstract: Gaseous formaldehyde (HCHO) is an important precursor of OH radicals and a key intermediate molecule in the oxidation of atmospheric volatile organic compounds (VOCs). Budget analyses reveal large discrepancies between modeled and observed HCHO concentrations in the atmosphere. Here, we investigate the interactions of gaseous HCHO with soil surfaces through coated-wall flow tube experiments applying atmospherically relevant HCHO concentrations of similar to 10 to 40 ppbv. For the determination of uptake coefficients (gamma), we provide a Matlab code to account for the diffusion correction under laminar flow conditions. Under dry conditions (relative humidity = 0 %), an initial gamma of (1.1 +/- 0.05) x 10(4) is determined, which gradually drops to (5.5 +/- 0.4) x 10(5) after 8 h experiments. Experiments under wet conditions show a smaller gamma that drops faster over time until reaching a plateau. The drop of gamma with increasing relative humidity as well as the drop over time can be explained by the adsorption theory in which high surface coverage leads to a reduced uptake rate. The fact that gamma stabilizes at a non-zero plateau suggests the involvement of irreversible chemical reactions. Further back-flushing experiments show that two-thirds of the adsorbed HCHO can be re-emitted into the gas phase while the residual is retained by the soil. This partial reversibility confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions which must be considered in trace gas exchange (emission or deposition) at the atmosphere-soil interface. Our results suggest that soil and soil-derived airborne particles can either act as a source or a sink for HCHO, depending on ambient conditions and HCHO concentrations.

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Language(s): eng - English
 Dates: 2016
 Publication Status: Published in print
 Pages: -
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 Rev. Type: -
 Identifiers: ISI: 000383230600001
DOI: 10.5194/acp-16-10299-2016
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Title: Atmospheric Chemistry and Physics
Source Genre: Journal
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Publ. Info: Katlenburg-Lindau, Germany : European Geosciences Union
Pages: - Volume / Issue: 16 (15) Sequence Number: - Start / End Page: 10299 - 10311 Identifier: ISSN: 1680-7316
CoNE: https://pure.mpg.de/cone/journals/resource/111030403014016