Oxidation of a model alkane aerosol by OH radical: the emergent nature of reactive uptake

Houle, F. A.; Hinsberg, W. D.; Wilson, K. R.

doi:10.1039/c4cp05093b

Title: Oxidation of a model alkane aerosol by OH radical: the emergent nature of reactive uptake

Journal Article · Tue Jan 06 00:00:00 EST 2015 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c4cp05093b· OSTI ID:1512167

Houle, F. A. ^[1]; Hinsberg, W. D. ^[2]; Wilson, K. R. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Columbia Hill Technical Consulting, Fremont, CA (United States)

An accurate description of the evolution of organic aerosol in the Earth’s atmosphere is essential for climate models. However, the complexity of multiphase chemical and physical transformations has been challenging to describe at the level required to predict aerosol lifetimes and changes in chemical composition. In this work a model is presented that reproduces experimental data for the early stages of oxidative aging of squalane aerosol by hydroxyl radical (OH), a process governed by reactive uptake of gas phase species onto the particle surface. Simulations coupling free radical reactions and Fickian diffusion are used to elucidate how the measured uptake coefficient reflects the elementary steps of sticking of OH to the aerosol as a result of a gas-surface collision, followed by very rapid abstraction of hydrogen and subsequent free radical reactions. It is found that the uptake coefficient is not equivalent to a sticking coefficient or an accommodation coefficient: it is an intrinsically emergent process that depends upon particle size, viscosity, and OH concentration. An expression is derived to examine how these factors control reactive uptake over a broad range of atmospheric and laboratory conditions, and is shown to be consistent with simulation results. Well-mixed, liquid behavior is found to depend on the reaction conditions in addition to the nature of the organic species in the aerosol particle.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1512167

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 17, Issue 6; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 58 works

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