Heterogeneous Reactivity of Nitric Acid with Nascent Sea Spray Aerosol: Large Differences Observed between and within Individual Particles.
Current climate and atmospheric chemistry models assume that all sea spray particles react as if they are pure NaCl. However, recent studies of sea spray aerosol particles have shown that distinct particle types exist (including sea salt, organic carbon, and biological particles) as well as mixtures of these and, within each particle type, there is a range of single-particle chemical compositions. Because of these differences, individual particles should display a range of reactivities with trace atmospheric gases. Herein, to address this, we study the composition of individual sea spray aerosol particles after heterogeneous reaction with nitric acid. As expected, a replacement reaction of chloride with nitrate is observed; however, there is a large range of reactivities spanning from no reaction to complete reaction between and within individual sea spray aerosol particles. These data clearly support the need for laboratory studies of individual, environmentally relevant particles to improve our fundamental understanding as to the properties that determine reactivity.
†Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.
Andrew P
AP
Ault
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.
Timothy L
TL
Guasco
†Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.
Jonas
J
Baltrusaitis
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.
Olivia S
OS
Ryder
†Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.
Jonathan V
JV
Trueblood
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.
Douglas B
DB
Collins
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.
Matthew J
MJ
Ruppel
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.
Luis A
LA
Cuadra-Rodriguez
‡Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92037, United States.|§Scripps Institution of Oceanography, University of California, San Diego, La Jolla, California 92093, United States.
Kimberly A
KA
Prather
†Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, United States.
Vicki H
VH
Grassian
X-ray photoelectron spectroscopy; atmospheric aerosol; heterogeneous reactions; micro-Raman spectroscopy; sea spray aerosol; single-particle analysis; surface chemistry