Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups
Abstract
The albedo and microphysical properties of clouds are controlled in part by the hygroscopicity of particles serving as cloud condensation nuclei (CCN). Hygroscopicity of complex organic mixtures in the atmosphere varies widely and remains challenging to predict. Here we present new measurements characterizing the CCN activity of pure compounds in which carbon chain length and the number of hydroperoxy, carboxyl, and carbonyl functional groups were systematically varied to establish the contributions of these groups to organic aerosol apparent hygroscopicity. Apparent hygroscopicity decreased with carbon chain length and increased with polar functional groups in the order carboxyl > hydroperoxy > carbonyl. Activation diameters at different supersaturations deviated from the -3/2 slope in log-log space predicted by Köhler theory, suggesting that water solubility limits CCN activity of particles composed of weakly functionalized organic compounds. Results are compared to a functional group contribution model that predicts CCN activity of organic compounds. The model performed well for most compounds but under-predicted the CCN activity of hydroperoxy groups. New best-fit hydroperoxy group/water interaction parameters were derived from the available CCN data. Lastly, these results may help improve estimates of the CCN activity of ambient organic aerosols from composition data.
- Authors:
-
- Colorado State Univ., Fort Collins, CO (United States); Univ. of North Carolina, Chapel Hill, NC (United States)
- Univ. of Colorado, Boulder, CO (United States)
- Colorado State Univ., Fort Collins, CO (United States)
- North Carolina State Univ., Raleigh, NC (United States)
- Publication Date:
- Research Org.:
- Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Biological and Environmental Research (BER)
- OSTI Identifier:
- 1364101
- Grant/Contract Number:
- SC0012043
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 27; Journal ID: ISSN 1089-5639
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; organic aerosol; cloud condensation nuclei (CCN); aerosol hygroscopicity; Köhler theory; hydroperoxides; solubility; carboxylic acids; multifunctional carbonyls; group contribution method; UNIFAC
Citation Formats
Petters, Sarah Suda, Pagonis, Demetrios, Claflin, Megan Suzanne, Levin, Ezra J. T., Petters, Markus D., Ziemann, Paul J., and Kreidenweis, Sonia M. Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups. United States: N. p., 2017.
Web. doi:10.1021/acs.jpca.7b04114.
Petters, Sarah Suda, Pagonis, Demetrios, Claflin, Megan Suzanne, Levin, Ezra J. T., Petters, Markus D., Ziemann, Paul J., & Kreidenweis, Sonia M. Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups. United States. https://doi.org/10.1021/acs.jpca.7b04114
Petters, Sarah Suda, Pagonis, Demetrios, Claflin, Megan Suzanne, Levin, Ezra J. T., Petters, Markus D., Ziemann, Paul J., and Kreidenweis, Sonia M. Fri .
"Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups". United States. https://doi.org/10.1021/acs.jpca.7b04114. https://www.osti.gov/servlets/purl/1364101.
@article{osti_1364101,
title = {Hygroscopicity of organic compounds as a function of carbon chain length, carboxyl, hydroperoxy, and carbonyl functional groups},
author = {Petters, Sarah Suda and Pagonis, Demetrios and Claflin, Megan Suzanne and Levin, Ezra J. T. and Petters, Markus D. and Ziemann, Paul J. and Kreidenweis, Sonia M.},
abstractNote = {The albedo and microphysical properties of clouds are controlled in part by the hygroscopicity of particles serving as cloud condensation nuclei (CCN). Hygroscopicity of complex organic mixtures in the atmosphere varies widely and remains challenging to predict. Here we present new measurements characterizing the CCN activity of pure compounds in which carbon chain length and the number of hydroperoxy, carboxyl, and carbonyl functional groups were systematically varied to establish the contributions of these groups to organic aerosol apparent hygroscopicity. Apparent hygroscopicity decreased with carbon chain length and increased with polar functional groups in the order carboxyl > hydroperoxy > carbonyl. Activation diameters at different supersaturations deviated from the -3/2 slope in log-log space predicted by Köhler theory, suggesting that water solubility limits CCN activity of particles composed of weakly functionalized organic compounds. Results are compared to a functional group contribution model that predicts CCN activity of organic compounds. The model performed well for most compounds but under-predicted the CCN activity of hydroperoxy groups. New best-fit hydroperoxy group/water interaction parameters were derived from the available CCN data. Lastly, these results may help improve estimates of the CCN activity of ambient organic aerosols from composition data.},
doi = {10.1021/acs.jpca.7b04114},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 27,
volume = 121,
place = {United States},
year = {Fri Jun 16 00:00:00 EDT 2017},
month = {Fri Jun 16 00:00:00 EDT 2017}
}
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Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition
journal, January 2018
- DeRieux, Wing-Sy Wong; Li, Ying; Lin, Peng
- Atmospheric Chemistry and Physics, Vol. 18, Issue 9
An investigation on hygroscopic properties of 15 black carbon (BC)-containing particles from different carbon sources: roles of organic and inorganic components
journal, July 2020
- Wang, Minli; Chen, Yiqun; Fu, Heyun
- Atmospheric Chemistry and Physics, Vol. 20, Issue 13