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Discussion papers
https://doi.org/10.5194/acp-2019-423
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-423
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 07 May 2019

Submitted as: research article | 07 May 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Single-particle experiments measuring humidity and inorganic salt effects on gas-particle partitioning of butenedial

Adam W. Birdsall1, Jack C. Hensley2, Paige S. Kotowitz3,a, Andrew J. Huisman3,b, and Frank N. Keutsch1,2,4 Adam W. Birdsall et al.
  • 1Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA, USA
  • 2School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA
  • 3Chemistry Department, Union College, Schenectady, NY, USA
  • 4Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA, USA
  • anow at: nanoComposix, San Diego, CA, USA
  • bnow at: Gentex Corporation, Zeeland, MI, USA

Abstract. An improved understanding of the fate and properties of atmospheric aerosol particles requires a detailed process-level understanding of fundamental factors influencing the aerosol, including partitioning of aerosol components between the gas and particle phases. Laboratory experiments with levitated particles provide a way to study fundamental aerosol processes over timescales relevant to the multiday lifetime of atmospheric aerosol particles, in a controlled environment in which various characteristics relevant to atmospheric aerosol can be prepared (e.g., high surface-to-volume ratio, highly concentrated or supersaturated solutions, changes to relative humidity). In this study, the four-carbon unsaturated compound butenedial, a dialdehyde produced by oxidation of aromatic compounds that undergoes hydration in the presence of water, was used as a model organic aerosol component to investigate different factors affecting gas–particle partitioning, including the role of lower-volatility reservoir species such as hydrates, time scales involved in equilibration between higher- and lower-volatility forms, and the effect of inorganic salts. The experimental approach was to use a laboratory system coupling particle levitation in an electrodynamic balance (EDB) with particle composition measurement via mass spectrometry (MS). In particular, by fitting measured evaporation rates to a kinetic model, the effective vapor pressure was determined for butenedial and compared under different experimental conditions, including as a function of ambient relative humidity and presence of high concentrations of inorganic salts. Even under dry (RH < 5 %) conditions, the evaporation rate of butenedial is orders of magnitude lower than what would be expected if butenedial existed purely as a dialdehyde in the particle, implying an equilibrium strongly favoring hydrated forms and the strong preference of certain dialdehyde compounds to remain in a hydrated form even under lower water content conditions. Butenedial exhibits a salting-out effect in the presence of sodium chloride and sodium sulfate, in contrast to glyoxal. The outcomes of these experiments are also helpful in guiding the design of future EDB-MS experiments.

Adam W. Birdsall et al.
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Short summary
We have measured the evaporation rates of butenedial, a four-carbon dialdehyde produced in the atmosphere, from individual levitated particles. Effective vapor pressures and Henry's law constants, which characterize the compound's gas-particle partitioning behavior, were determined. The important role of hydration reactions was observed under both dry and humid conditions, as well as a salting-out effect in the presence of sodium chloride or sodium sulfate.
We have measured the evaporation rates of butenedial, a four-carbon dialdehyde produced in the...
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