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Enhancement of Atmospheric H2So4/H2O Nucleation: Organic Oxidation Products Versus Amines : Volume 13, Issue 6 (18/06/2013)

By Berndt, T.

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Book Id: WPLBN0003990770
Format Type: PDF Article :
File Size: Pages 35
Reproduction Date: 2015

Title: Enhancement of Atmospheric H2So4/H2O Nucleation: Organic Oxidation Products Versus Amines : Volume 13, Issue 6 (18/06/2013)  
Author: Berndt, T.
Volume: Vol. 13, Issue 6
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Historic
Publication Date:
2013
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

Citation

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Sipilä, M., Stratmann, F., Vanhanen, J., Patokoski, J., Berndt, T., Kulmala, M.,...Mikkilä, J. (2013). Enhancement of Atmospheric H2So4/H2O Nucleation: Organic Oxidation Products Versus Amines : Volume 13, Issue 6 (18/06/2013). Retrieved from http://worldebooklibrary.com/


Description
Description: Leibniz-Institut für Troposphärenforschung e.V., Permoserstr. 15, 04318 Leipzig, Germany. Atmospheric H2SO4/H2O nucleation influencing effects have been studied in the flow tube IfT-LFT (Institute for Tropospheric Research – Laminar Flow Tube) at 293 ± 0.5 K and a pressure of 1 bar using synthetic air as the carrier gas. The presence of a possible background amine concentration in the order of 107–108 molecule cm−3 throughout the experiments has to be taken into account. In a first set of investigations, ozonolysis of olefins (tetramethylethylene, 1-methyl-cyclohexene, α-pinene and limonene) for close to atmospheric concentrations, served as the source of OH radicals and possibly other oxidants initiating H2SO4 formation starting from SO2. The oxidant generation is inevitably associated with the formation of a series of organic oxidation products arising from the parent olefins. These products (first generation mainly) showed no clear effect on the number of nucleated particles within a wide range of experimental conditions for H2SO4 concentrations higher than ~107 molecule cm−3. A comparison of the results of two different particle counters (50% cut-off size: about 1.5 nm or 2.5–3 nm) suggested that the early growth process of the nucleated particles was not significantly influenced by the organic oxidation products. An additional, H2SO4-independent process of particle (nano-CN) formation was observed in the case of α-pinene and limonene ozonolysis for H2SO4 concentrations smaller than ~10 7 molecule cm−3. Furthermore, the findings confirm the existence of an additional oxidant for SO2 beside OH radicals, very likely stabilized Criegee Intermediate (sCI). In the case of the ozonolysis of tetramethylethylene, the H2SO4 measurements in the absence and presence of an OH radical scavenger were well described by modelling using recently obtained kinetic data for the sCI reactivity in this system. A second set of experiments has been performed in the presence of added amines (trimethylamine, dimethylamine, aniline and pyridine) in the concentration range of a few 107–1010 molecule cm−3. Here, photolytic OH radical generation was applied for H2SO4 production with no addition of other organics. All amines showed a significant nucleation enhancement with increasing efficiency in the order pyridine < aniline < dimethylamine < trimethylamine. This result supports the idea of H2SO4 cluster stabilization by amines due to strong H2SO4 ↔ amine interactions. On the other hand, this study reveals that for organic oxidation products (in presence of the possible amine background as stated) a distinct H2SO4/H2O nucleation enhancement can be due to increased H2SO4 formation caused by additional organic oxidant production (sCI) rather than by stabilization of H2SO4 clusters due to H2SO4 ↔ organics in

Summary
Enhancement of atmospheric H2SO4/H2O nucleation: organic oxidation products versus amines

Excerpt
Anglada, J. M., Aplincourt, P., Bofill, J. M., and Cremer, D.: Atmospheric formation of OH radicals and H2O2 from alkene ozonolysis under humid conditions, Chem. Phys. Chem., 2, 215–221, 2002.; Atkinson, R.: Kinetics and mechanisms of the gas-phase reactions of the hydroxyl radical with organic compounds under atmospheric conditions, Chem. Rev., 86, 69–201, 1986.; Atkinson, R., Aschmann, S. M., and Pitts Jr., J. N.: Rate constants for the gas-phase reactions of the OH radical with a~series of monoterpenes at 294 ± 1 K, Int.~J. Chem. Kinet., 18, 287–299, 1986.; Atkinson, R., Aschmann, S. M., Arey, J., and Shorees, B.: Formation of OH radicals in the gas-phase reactions of O3 with a~series of terpenes,~J. Geophys. Res., 97, 6065–6073, 1992.; Atkinson, R., Tuazon, E. C., and Aschmann, S. M.: Products of the gas-phase reaction of O3 with alkenes, Environ. Sci. Technol., 29, 1674–1680, 1995.; Berndt, T. and Böge, O.: Formation of phenol and carbonyls from the atmospheric reaction of OH radicals with benzene, Phys. Chem. Chem. Phys., 8, 1205–1214, 2006.; Berndt, T., Böge, O., and Stratmann, F.: Atmospheric particle formation from the ozonolysis of alkenes in the presence of SO2, Atmos. Environ., 38, 2145–2153, 2004.; Berndt, T., Stratmann, F., Sipilä, M., Vanhanen, J., Petäjä, T., Mikkilä, J., Grüner, A., Spindler, G., Lee Mauldin III, R., Curtius, J., Kulmala, M., and Heintzenberg, J.: Laboratory study on new particle formation from the reaction $OH + SO2$: influence of experimental conditions, \chem{H_{2}O} vapour, NH3 and the amine tert-butylamine on the overall process, Atmos. Chem. Phys., 10, 7101–7116, doi:10.5194/acp-10-7101-2010, 2010.; Berndt, T., Jokinen, J., Mauldin III, R. L., Petäjä, T., Herrmann, H., Junninen, H., Paasonen, P., Worsnop, D. R., and Sipila, M.: Gas-phase ozonolysis of selected olefins: the yield of stabilized criegee intermediate and the reactivity toward SO2,~J. Phys. Chem. Lett., 3, 2892–2896, 2012.; Coffman, D. J. and Hegg, D. A.: A~preliminary study of the effect of ammonia on particle nucleation in the boundary layer,~J. Geophys. Res., 100, 7147–7160, 1995.; Grönberg, L., Lövkvist, P., and Jönsson, J. A.: Measurement of aliphatic amines in ambient air and rainwater, Chemosphere, 24, 1533–1540, 1992.; Cornell, S. E., Jickells, T. D., Cape, J. N., Rowland, A. P., and Duce, R. A.: Organic nitrogen deposition on land and coastal environments: a~review of methods and data, Atmos. Environ., 37, 2173–2191, 2003.; Darnall, K. R., Winer, A. M., Lloyd, A. C., and Pitts Jr., J. N.: Relative rate constants for the reaction of OH radicals with selected C6 and C7 alkanes and alkenes at 305 ± 2 K, Chem. Phys. Lett., 44, 415–418, 1976.; DeMore, W. B., Sander, S. P., Golden, D. M., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E., and Molina, M. J.: Chemical kinetics and photochemical data for use in stratospheric modelling, Evaluation number 12, JPL

 

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