Laboratory study on new particle formation from the reaction OH + SO2: influence of experimental conditions, H2O vapour, NH3 and the amine tert-butylamine on the overall process

Nucleation experiments starting from the reaction of OH radicals with SO2 have been performed in the IfT-LFT flow tube under atmospheric conditions at 293±0.5 K for a relative humidity of 13–61%. The presence of differen
Nucleation experiments starting from the reaction of OH radicals with SO2 have been performed in the IfT-LFT flow tube under atmospheric conditions at 293±0.5 K for a relative humidity of 13–61%. The presence of different additives (H2, CO, 1,3,5-trimethylbenzene) for adjusting the OH radical concentration and resulting OH levels in the range (4–300) ×105 molecule cm -3 did not influence the nucleation process itself. The number of detected particles as well as the threshold H2SO4 concentration needed for nucleation was found to be strongly dependent on the counting efficiency of the used counting devices. High-sensitivity particle counters allowed the measurement of freshly nucleated particles with diameters down to about 1.5 nm. A parameterization of the experimental data was developed using power law equations for H2SO4 and H2O vapour. The exponent for H2SO4 from different measurement series was in the range of 1.7–2.1 being in good agreement with those arising from analysis of nucleation events in the atmosphere. For increasing relative humidity, an increase of the particle number was observed. The exponent for H2O vapour was found to be 3.1 representing an upper limit. Addition of 1.2×1011 molecule cm -3 or 1.2×1012 molecule cm -3 of NH3 (range of atmospheric NH3 peak concentrations) revealed that NH3 has a measureable, promoting effect on the nucleation rate under these conditions. The promoting effect was found to be more pronounced for relatively dry conditions, i.e. a rise of the particle number by 1–2 orders of magnitude at RH = 13% and only by a factor of 2–5 at RH = 47% (NH3 addition: 1.2×1012 molecule cm -3). Using the amine tert-butylamine instead of NH3, the enhancing impact of the base for nucleation and particle growth appears to be stronger. Tert-butylamine addition of about 1010 molecule cm -3 at RH = 13% enhances particle formation by about two orders of magnitude, while for NH3 only a small or negligible effect on nucleation in this range of concentration appeared. This suggests that amines can strongly influence atmospheric H2SO4-H2O nucleation and are probably promising candidates for explaining existing discrepancies between theory and observations.
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Metadaten
Author:Torsten Berndt, Frank Stratmann, Mikko Sipilä, Joonas Vanhanen, Tuukka Petäjä, Jyri Mikkilä, Achim Grüner, Gerald Spindler, R. Lee Mauldin III., Joachim Curtius, Markku Kulmala, Jost Heintzenberg
URN:urn:nbn:de:hebis:30-78049
DOI:http://dx.doi.org/10.5194/acp-10-7101-2010
ISSN:1680-7316
ISSN:1680-7324
Parent Title (English):Atmospheric chemistry and physics
Publisher:European Geosciences Union
Place of publication:Katlenburg-Lindau
Document Type:Article
Language:English
Date of Publication (online):2010/08/03
Date of first Publication:2010/08/03
Publishing Institution:Univ.-Bibliothek Frankfurt am Main
Release Date:2010/09/03
Volume:10
Pagenumber:16
First Page:7101
Last Page:7116
Note:
© Author(s) 2010. This work is distributed under the Creative Commons Attribution 3.0 License.
HeBIS PPN:226847675
Institutes:Geowissenschaften
Dewey Decimal Classification:550 Geowissenschaften
Sammlungen:Universitätspublikationen
Licence (German):License LogoCreative Commons - Namensnennung 3.0

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