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Ozonolysis of Mixed Oleic-Acid/Stearic-Acid Particles:  Reaction Kinetics and Chemical Morphology

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Division of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138; Department of Geological Sciences and Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287; Chemistry Department, Boston College, Chestnut Hill, Massachusetts 02467; Aerodyne Research, Inc., Billerica, Massachusetts 08121; and Institute of Low-Temperature Science, Hokkaido University, Sapporo, 060-0819, Japan
Cite this: J. Phys. Chem. A 2005, 109, 48, 10910–10919
Publication Date (Web):November 10, 2005
https://doi.org/10.1021/jp054714d
Copyright © 2005 American Chemical Society
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    Abstract

    The ozonolysis of mixed oleic-acid/stearic-acid (OL/SA) aerosol particles from 0/100 to 100/0 wt % composition is studied. The magnitude of the divergence of the particle beam inside an aerosol mass spectrometer shows that, in the concentration range 100/0 to 60/40, the mixed OL/SA particles are liquid prior to reaction. Upon ozonolysis, particles having compositions of 75/25 and 60/40 change shape, indicating that they have solidified during reaction. Transmission electron micrographs show that SA(s) forms needles. For particles having compositions of 75/25, 60/40, and greater SA content, the reaction kinetics exhibit an initial fast decay of OL for low O3 exposure with no further loss of OL at higher O3 exposures. For compositions from 50/50 to 10/90, the residual OL concentration remains at 28 ± 2% of its initial value. The initial reactive uptake coefficient for O3, as determined by OL loss, decreases linearly from 1.25 (±0.2) × 10-3 to 0.60 (±0.15) × 10-3 for composition changes of 100/0 to 60/40. At 50/50 composition, the uptake coefficient drops abruptly to 0.15 (±0.1) × 10-3, and there are no further changes with increased SA content. These observations can be explained with a combination of three postulates:  (1) Unreacted mixed particles remain as supersaturated liquids up to 60/40 composition, and the OL in this form rapidly reacts with O3. (2) SA, as it solidifies, locks into its crystal structure a significant amount of OL, and this OL is completely inaccessible to O3. (3) Accompanying crystallization, some stearic acid molecules connect as a filamentous network to form a semipermeable gel containing liquid OL but with a reduced uptake coefficient because of the decrease in molecular diffusivity in the gel. An individual particle of 50/50 to 90/10 is hypothesized as a combination of SA crystals having OL impurities (postulate 2) that are partially enveloped by an SA/OL gel (postulate 3) to explain (a) the abrupt drop in the uptake coefficient from 60/40 to 50/50 and (b) the residual OL content even after high ozone exposure. The results of this study, pointing out the important effects of particle phase, composition, and morphology on chemical reactivity, contribute to an improved understanding of the aging processes of atmospheric aerosol particles.

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    †

     Harvard University.

    ‡

     Arizona State University.

    §

     Boston College.

    ‖

     Aerodyne Research, Inc.

    ⊥

     Institute of Low-Temperature Science.

    *

     To whom correspondence should be addressed. E-mail:  [email protected]. Web:  www.deas.harvard.edu/environmental-chemistry.

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