On the role of particle inorganic mixing state in the reactive uptake of N2O5 to ambient aerosol particles

Olivia S. Ryder, Andrew P. Ault, John F. Cahill, Timothy L. Guasco, Theran P. Riedel, Luis A. Cuadra-Rodriguez, Cassandra J. Gaston, Elizabeth Fitzgerald, Christopher Lee, Kimberly A. Prather, Timothy H. Bertram

Research output: Contribution to journalArticle

37 Scopus citations

Abstract

The rates of heterogeneous reactions of trace gases with aerosol particles are complex functions of particle chemical composition, morphology, and phase state. Currently, the majority of model parametrizations of heterogeneous reaction kinetics focus on the population average of aerosol particle mass, assuming that individual particles have the same chemical composition as the average state. Here we assess the impact of particle mixing state on heterogeneous reaction kinetics using the N2O5 reactive uptake coefficient, γ(N2O5), and dependence on the particulate chloride-to-nitrate ratio (nCl-/nNO3 -). We describe the first simultaneous ambient observations of single particle chemical composition and in situ determinations of γ(N 2O5). When accounting for particulate nCl -/nNO3- mixing state, model parametrizations of γ(N2O5) continue to overpredict γ(N 2O5) by more than a factor of 2 in polluted coastal regions, suggesting that chemical composition and physical phase state of particulate organics likely control γ(N2O5) in these air masses. In contrast, direct measurement of γ(N2O 5) in air masses of marine origin are well captured by model parametrizations and reveal limited suppression of γ(N2O 5), indicating that the organic mass fraction of fresh sea spray aerosol at this location does not suppress γ(N2O5). We provide an observation-based framework for assessing the impact of particle mixing state on gas-particle interactions.

Original languageEnglish (US)
Pages (from-to)1618-1627
Number of pages10
JournalEnvironmental Science and Technology
Volume48
Issue number3
DOIs
StatePublished - Feb 4 2014
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry

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    Ryder, O. S., Ault, A. P., Cahill, J. F., Guasco, T. L., Riedel, T. P., Cuadra-Rodriguez, L. A., Gaston, C. J., Fitzgerald, E., Lee, C., Prather, K. A., & Bertram, T. H. (2014). On the role of particle inorganic mixing state in the reactive uptake of N2O5 to ambient aerosol particles. Environmental Science and Technology, 48(3), 1618-1627. https://doi.org/10.1021/es4042622