Laboratory study on new particle formation from the reaction OH + SOâ: influence of experimental conditions, HâO vapour, NHâ and the amine tert-butylamine on the overall process
Nucleation experiments starting from the reaction of OH radicals with SOâ 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 (Hâ, CO, 1,3,5-trimethylbenzene) for adjusting the OH radical concentration and resulting OH levels in the range (4-300) Ã10âµ molecule cmâ»Â³ did not influence the nucleation process itself. The number of detected particles as well as the threshold HâSOâ 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 HâSOâ and HâO vapour. The exponent for HâSOâ 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 HâO vapour was found to be 3.1 representing an upper limit. Addition of 1.2Ã10¹¹ molecule cmâ»Â³ or 1.2Ã10¹² molecule cmâ»Â³ of NHâ (range of atmospheric NHâ peak concentrations) revealed that NHâ 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% (NHâ addition: 1.2Ã10¹² molecule cmâ»Â³). Using the amine tert-butylamine instead of NHâ, the enhancing impact of the base for nucleation and particle growth appears to be stronger. Tert-butylamine addition of about 10¹Ⱐmolecule cmâ»Â³ at RH = 13% enhances particle formation by about two orders of magnitude, while for NHâ only a small or negligible effect on nucleation in this range of concentration appeared. This suggests that amines can strongly influence atmospheric HâSOâ-HâO nucleation and are probably promising candidates for explaining existing discrepancies between theory and observations.
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https://n2t.org/ark:/85065/d7n58mt0
eng
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2016-01-01T00:00:00Z
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2010-08-03T00:00:00Z
Copyright Author(s) 2010. This work is distributed under the Creative Commons Attribution 3.0 License.
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