Nanoparticle growth by particle-phase chemistry
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Published:2018-02-09
Issue:3
Volume:18
Page:1895-1907
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Apsokardu Michael J., Johnston Murray V.ORCID
Abstract
Abstract. The ability of particle-phase chemistry to alter the molecular composition
and enhance the growth rate of nanoparticles in the 2–100 nm diameter range
is investigated through the use of a kinetic growth model. The molecular components
included are sulfuric acid, ammonia, water, a non-volatile organic compound,
and a semi-volatile organic compound. Molecular composition and growth rate
are compared for particles that grow by partitioning alone vs. those that
grow by a combination of partitioning and an accretion reaction in the
particle phase between two organic molecules. Particle-phase chemistry causes
a change in molecular composition that is particle diameter dependent, and
when the reaction involves semi-volatile molecules, the particles grow faster
than by partitioning alone. These effects are most pronounced for particles
larger than about 20 nm in diameter. The modeling results provide a
fundamental basis for understanding recent experimental measurements of the
molecular composition of secondary organic aerosol showing that accretion
reaction product formation increases linearly with increasing aerosol
volume-to-surface-area. They also allow initial estimates of the reaction
rate constants for these systems. For secondary aerosol produced by either OH
oxidation of the cyclic dimethylsiloxane (D5) or ozonolysis of β-pinene, oligomerization rate constants on the order of 10−3 to
10−1 M−1 s−1 are needed to explain the experimental results.
These values are consistent with previously measured rate constants for
reactions of hydroperoxides and/or peroxyacids in the condensed phase.
Funder
Division of Chemistry
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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