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Self-limited Uptake of Α-pinene-oxide to Acidic Aerosol: the Effects of Liquid-liquid Phase Separation and Implications for the Formation of Secondary Organic Aerosol and Organosulfates from Epoxides : Volume 13, Issue 3 (18/03/2013)

By Drozd, G. T.

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Book Id: WPLBN0003996716
Format Type: PDF Article :
File Size: Pages 24
Reproduction Date: 2015

Title: Self-limited Uptake of Α-pinene-oxide to Acidic Aerosol: the Effects of Liquid-liquid Phase Separation and Implications for the Formation of Secondary Organic Aerosol and Organosulfates from Epoxides : Volume 13, Issue 3 (18/03/2013)  
Author: Drozd, G. T.
Volume: Vol. 13, Issue 3
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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Woo, J. L., Mcneill, V. F., & Drozd, G. T. (2013). Self-limited Uptake of Α-pinene-oxide to Acidic Aerosol: the Effects of Liquid-liquid Phase Separation and Implications for the Formation of Secondary Organic Aerosol and Organosulfates from Epoxides : Volume 13, Issue 3 (18/03/2013). Retrieved from http://www.ebooklibrary.org/


Description
Description: Department of Chemical Engineering, Columbia University, New York, NY, 10027, USA. The reactive uptake of Α-pinene oxide (ΑPO) to acidic sulfate aerosol was studied under humid conditions in order to gain insight into the effects of liquid-liquid phase separation on aerosol heterogeneous chemistry and further elucidate the formation of secondary organic aerosol and organosulfates from epoxides. A continuous flow environmental chamber was used to monitor changes in diameter of monodisperse, deliquesced, acidic sulfate particles exposed to ΑPO at 30 and 50% RH. In order to induce phase separation and probe potential limits to particle growth from acidic uptake, ΑPO was introduced over a wide range of concentrations, from 200 ppb to 5 ppm. Uptake was observed to be highly dependent on initial aerosol pH. Significant uptake of ΑPO to aerosol was observed with initial pH < 0. When exposed to 200 ppb ΑPO, aerosol with pH = −1 doubled in volume, and 6% volume growth was observed at pH = 0. Aerosol with pH = 1 showed no growth. The extreme acidity required for efficient ΑPO uptake suggests that this chemistry is typically not a major route to formation of aerosol mass or organosulfates in the atmosphere. Partition coefficients (Kp) ranged from 0.2–1.6 × 10−4 m3 Μg−1 and were correlated to initial particle acidity and particle organic content; particles with higher organic content had lower partition coefficients. Effective uptake coefficients (Γ) ranged from 0.4 to 4.7 × 10−5 and are much lower than recently reported for uptake to bulk solutions. In experiments in which ΑPO was added to bulk H2SO4 solutions, phase separation was observed for mass loadings similar to those observed with particles, and product distributions were dependent on acid concentration. Liquid-liquid phase separation in bulk experiments, along with our observations of decreased uptake to particles with the largest growth factors, suggest an organic coating forms upon uptake to particles, limiting reactive uptake.

Summary
Self-limited uptake of Α-pinene-oxide to acidic aerosol: the effects of liquid-liquid phase separation and implications for the formation of secondary organic aerosol and organosulfates from epoxides

Excerpt
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, doi:10.5194/acp-11-10995-2011, 2011.; Coelho, J. V., de Meireles, A. L. P., da Silva Rocha, K. A., Pereira, M. C., Oliveira, L. C. A., and Gusevskaya, E. V.: Isomerization of ±-pinene oxide catalyzed by iron-modified mesoporous silicates, Appl. Catal. A-Gen., 443–444, 125–132, doi:10.1016/j.apcata.2012.07.030, 2012.; Darer, A. I., Cole-Filipiak, N. C., O'Connor, A. E., and Elrod, M. J.: Formation and stability of atmospherically relevant isoprene-derived organosulfates and organonitrates, Environ. Sci. Technol., 45, 1895–1902, doi:10.1021/es103797z, 2011.; Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, doi:10.5194/acp-11-11069-2011, 2011.; Galloway, M. M., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Flagan, R. C., Seinfeld, J. H., and Keutsch, F. N.: Glyoxal uptake on ammonium sulphate seed aerosol: reaction products and reversibility of uptake under dark and irradiated conditions, Atmos. Chem. Phys., 9, 3331–3345, doi:10.5194/acp-9-3331-2009, 2009.; Gladden, J. K. and Dole, M.: Diffusion in supersaturated solutions. I I. Glucose solutions, J. Am. Chem. Soc., 75, 3900–3904, doi:10.1021/ja01112a008, 1953.; Hatch, L. E., Creamean, J. M., Ault, A. P., Surratt, J. D., Chan, M. N., Seinfeld, J. H., Edgerton, E. S., Su, Y., and Prather, K. A.: Measurements of isoprene-derived organosulfates in ambient aerosols by aerosol time-of-flight mass spectrometry – Part 2: Temporal variability and formation mechanisms, Environ. Sci. Technol., 45, 8648–8655, doi:10.1021/es2011836, 2011.; Hu, K. S., Darer, A. I., and Elrod, M. J.: Thermodynamics and kinetics of the hydrolysis of atmospherically relevant organonitrates and organosulfates, Atmos. Chem. Phys., 11, 8307–8320, doi:10.5194/acp-11-8307-2011, 2011.; Iinuma, Y., Boge, O., Kahnt, A., and Herrmann, H.: Laboratory chamber studies on the formation of organosulfates from reactive uptake of monoterpene oxides, Phys. Chem. Chem. Phys., 11, 7985–7997, doi:10.1039/b904025k, 2009.; Kroll,&am

 

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