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Phase Partitioning and Volatility of Secondary Organic Aerosol Components Formed from Α-pinene Ozonolysis and Oh Oxidation: the Importance of Accretion Products and Other Low Volatility Compounds : Volume 15, Issue 14 (16/07/2015)

By Lopez-hilfiker, F. D.

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Book Id: WPLBN0003984839
Format Type: PDF Article :
File Size: Pages 12
Reproduction Date: 2015

Title: Phase Partitioning and Volatility of Secondary Organic Aerosol Components Formed from Α-pinene Ozonolysis and Oh Oxidation: the Importance of Accretion Products and Other Low Volatility Compounds : Volume 15, Issue 14 (16/07/2015)  
Author: Lopez-hilfiker, F. D.
Volume: Vol. 15, Issue 14
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection (Contemporary), Copernicus GmbH
Historic
Publication Date:
2015
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

Citation

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Thornton, J. A., Lopez-Hilfiker, F. D., Rubach, F., Daumit, K. E., Hunter, J. F., Mohr, C.,...Kleist, E. (2015). Phase Partitioning and Volatility of Secondary Organic Aerosol Components Formed from Α-pinene Ozonolysis and Oh Oxidation: the Importance of Accretion Products and Other Low Volatility Compounds : Volume 15, Issue 14 (16/07/2015). Retrieved from http://www.ebooklibrary.org/


Description
Description: Department of Atmospheric Sciences, University of Washington, Seattle, WA, 98195, USA. We measured a large suite of gas- and particle-phase multi-functional organic compounds with a Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) developed at the University of Washington. The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We focus here on results from experiments utilizing an ionization method most selective towards acids (acetate negative ion proton transfer), but our conclusions are based on more general physical and chemical properties of the SOA. Hundreds of compounds were observed in both gas and particle phases, the latter being detected by temperature-programmed thermal desorption of collected particles. Particulate organic compounds detected by the FIGAERO–HR-ToF-CIMS are highly correlated with, and explain at least 25–50 % of, the organic aerosol mass measured by an Aerodyne aerosol mass spectrometer (AMS). Reproducible multi-modal structures in the thermograms for individual compounds of a given elemental composition reveal a significant SOA mass contribution from high molecular weight organics and/or oligomers (i.e., multi-phase accretion reaction products). Approximately 50 % of the HR-ToF-CIMS particle-phase mass is associated with compounds having effective vapor pressures 4 or more orders of magnitude lower than commonly measured monoterpene oxidation products. The relative importance of these accretion-type and other extremely low volatility products appears to vary with photochemical conditions. We present a desorption-temperature-based framework for apportionment of thermogram signals into volatility bins. The volatility-based apportionment greatly improves agreement between measured and modeled gas-particle partitioning for select major and minor components of the SOA, consistent with thermal decomposition during desorption causing the conversion of lower volatility components into the detected higher volatility compounds.

Summary
Phase partitioning and volatility of secondary organic aerosol components formed from α-pinene ozonolysis and OH oxidation: the importance of accretion products and other low volatility compounds

Excerpt
An, W. J., Pathak, R. K., Lee, B.-H., and Pandis, S. N.: Aerosol volatility measurement using an improved thermodenuder: Application to secondary organic aerosol, J. Aerosol Sci., 38, 305–314, doi:10.1016/j.jaerosci.2006.12.002, 2007.; Blanksby, S. J. and Ellison, G. B.: Bond Dissociation Energies of Organic Molecules, Acc. Chem. Res., 36, 255–263, doi:10.1021/ar020230d, 2003.; Capouet, M. and Müller, J.-F.: A group contribution method for estimating the vapour pressures of α-pinene oxidation products, Atmos. Chem. Phys., 6, 1455–1467, doi:10.5194/acp-6-1455-2006, 2006.; Cappa, C. D.: A model of aerosol evaporation kinetics in a thermodenuder, Atmos. Meas. Tech., 3, 579–592, doi:10.5194/amt-3-579-2010, 2010.; Cappa, C. D. and Jimenez, J. L.: Quantitative estimates of the volatility of ambient organic aerosol, Atmos. Chem. Phys., 10, 5409–5424, doi:10.5194/acp-10-5409-2010, 2010.; DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop, D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, doi:10.1021/ac061249n, 2006.; DePalma, J. W., Horan, A. J., Hall IV, W. A., and Johnston, M. V.: Thermodynamics of oligomer formation: implications for secondary organic aerosol formation and reactivity, Phys. Chem. Chem. Phys., 15, 6935, doi:10.1039/c3cp44586k, 2013.; Docherty, K. S., Wu, W., Lim, Y. B., and Ziemann, P. J.: Contributions of Organic Peroxides to Secondary Aerosol Formed from Reactions of Monoterpenes with O3, Environ. Sci. Technol., 39, 4049–4059, doi:10.1021/es050228s, 2005.; Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, doi:10.5194/acp-11-3303-2011, 2011.; Dougherty, R. C.: Temperature and pressure dependence of hydrogen bond strength: A perturbation molecular orbital approach, J. Chem. Phys., 109, 7372, doi:10.1063/1.477343, 1998.; Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurtén, T., Nielsen, L. B., Jørgensen, S., Kjaergaard, H. G., Canagaratna, M., Maso, M. D., Berndt, T., Petäjä, T., Wahner, A., Kerminen, V.-M., Kulmala, M., Worsnop, D. R., Wildt, J., and Mentel, T. F.: A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, doi:10.1038/nature13032, 2014.; Epstein, S. A., Riipinen, I., and Donahue, N. M.: A Semiempirical Correlation between Enthalpy of Vaporization and Saturation Concentration for Organic Aerosol, Environ. Sci. Technol., 44, 743–748, doi:10.1021/es902497z, 2010.; Gao, S., Keywood, M., Ng, N. L., Surratt, J., Varutbangkul, V., Bahreini, R., Flagan, R. C., and Seinfeld, J. H.: Low-Molecular-Weight and Oligomeric Components in Secondary Organic Aerosol from the Ozonolysis of Cycloalkenes and α-Pinene, J. Phys. Chem. A, 108, 10147–10164, do

 

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