DOI: 10.1073/pnas.1209071109. Phase of atmospheric secondary organic material affects its reactivity

Phase of atmospheric secondary organic material affects its reactivity

10.1073/pnas.1209071109

Crossref journal-article

Proceedings of the National Academy of Sciences

Proceedings of the National Academy of Sciences (341)

Abstract

The interconversion of atmospheric organic particles among solid, semisolid, and liquid phases is of keen current scientific interest, especially for particles of secondary organic material (SOM). Herein, the influence of phase on ammonia uptake and subsequent particle-phase reactions was investigated for aerosol particles of adipic acid and α-pinene ozonolysis SOM. The nitrogen content of the particles was monitored by online mass spectrometry for increasing ammonia exposure. Solid and semisolid adipic acid particles were inert to the ammonia uptake for low RH (< 5%). For the solid particles, ammonia exposure at high relative humidity (RH; > 94%) induced a first-order deliquescence phase transition into aqueous particles. Solid particles exposed to supersaturated (RH > 100%) conditions and cycled back to high RH (> 94%), thereby becoming acidic metastable particles, underwent a gradual second-order transition upon ammonia exposure to form aqueous, partially neutralized particles. For α-pinene SOM, ammonia exposure at low RH increased the particle-phase ammonium content by a small amount. Mass spectrometric observations suggest a mechanism of neutralization and co-condensation of acidic gas-phase species, consistent with a highly viscous semisolid upon which adsorption occurs. At high RH the ammonium content increased greatly, indicative of rapid diffusion and absorption in a liquid environment. The mass spectra indicated the production of organonitrogen compounds, possibly by particle-phase reactive chemistry. The present results demonstrate that phase can be a key regulator of the reactivity of atmospheric SOM particles.

Bibliography

Kuwata, M., & Martin, S. T. (2012). Phase of atmospheric secondary organic material affects its reactivity. Proceedings of the National Academy of Sciences, 109(43), 17354â17359.

Authors 2

Mikinori Kuwata (first)
Scot T. Martin (additional)

References 48 Referenced 195

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Dates

Type	When
Created	12 years, 10 months ago (Oct. 9, 2012, 12:26 a.m.)
Deposited	2 years, 1 month ago (June 26, 2023, 12:33 a.m.)
Indexed	4 days, 20 hours ago (Aug. 20, 2025, 9:15 a.m.)
Issued	12 years, 10 months ago (Oct. 8, 2012)
Published	12 years, 10 months ago (Oct. 8, 2012)
Published Online	12 years, 10 months ago (Oct. 8, 2012)
Published Print	12 years, 10 months ago (Oct. 23, 2012)

Funders 0

None

BibTeX

@article{Kuwata_2012, title={Phase of atmospheric secondary organic material affects its reactivity}, volume={109}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.1209071109}, DOI={10.1073/pnas.1209071109}, number={43}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Kuwata, Mikinori and Martin, Scot T.}, year={2012}, month=oct, pages={17354–17359} }

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