Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol
Abstract
The diffusivity of semivolatile organic compounds (SVOCs) in the bulk particle phase of a viscous atmospheric secondary organic aerosol (SOA) can have a profound impact on aerosol growth and size distribution dynamics. Here, we investigate the bulk diffusivity of SVOCs formed from photo-oxidation of isoprene as they partition to a bimodal aerosol consisting of an Aitken (potassium sulfate) and accumulation mode (aged α-pinene SOA) particles as a function of relative humidity (RH). The model analysis of the observed size distribution evolution shows that liquid-like diffusion coefficient values of Db > 10–10 cm2 s–1 fail to explain the growth of the Aitken mode. Instead, much lower values of Db between 2.5 × 10–15 cm2 s–1 at 32% RH and 8 × 10–15 cm2 s–1 at 82% RH were needed to successfully reproduce the growth of both modes. The diffusivity within the aged α-pinene SOA remains appreciably slow even at 80% RH, resulting in hindered partitioning of SVOCs to large viscous particles and allowing smaller and relatively less viscous particles to effectively absorb the available SVOCs and grow much faster than would be possible otherwise. Our results have important implications for modeling SOA formation and growth in the ambient atmosphere.
- Authors:
-
[1];
[1];
[2];
[3]
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Atmospheric Science and Global Change Div. (ASGC)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). William R. Wiley Environmental Molecular Sciences Lab.
- Purdue Univ., West Lafayette, IN (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1599607
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 54; Journal Issue: 5; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; Transport properties; Diffusion; Oligomers; Evaporation; Aerosols
Citation Formats
Zaveri, Rahul A., Shilling, John E., Zelenyuk, Alla, Zawadowicz, Maria A., Suski, Kaitlyn, China, Swarup, Bell, David M., Veghte, Daniel, and Laskin, Alexander. Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol. United States: N. p., 2020.
Web. doi:10.1021/acs.est.9b05514.
Zaveri, Rahul A., Shilling, John E., Zelenyuk, Alla, Zawadowicz, Maria A., Suski, Kaitlyn, China, Swarup, Bell, David M., Veghte, Daniel, & Laskin, Alexander. Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol. United States. https://doi.org/10.1021/acs.est.9b05514
Zaveri, Rahul A., Shilling, John E., Zelenyuk, Alla, Zawadowicz, Maria A., Suski, Kaitlyn, China, Swarup, Bell, David M., Veghte, Daniel, and Laskin, Alexander. Wed .
"Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol". United States. https://doi.org/10.1021/acs.est.9b05514. https://www.osti.gov/servlets/purl/1599607.
@article{osti_1599607,
title = {Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol},
author = {Zaveri, Rahul A. and Shilling, John E. and Zelenyuk, Alla and Zawadowicz, Maria A. and Suski, Kaitlyn and China, Swarup and Bell, David M. and Veghte, Daniel and Laskin, Alexander},
abstractNote = {The diffusivity of semivolatile organic compounds (SVOCs) in the bulk particle phase of a viscous atmospheric secondary organic aerosol (SOA) can have a profound impact on aerosol growth and size distribution dynamics. Here, we investigate the bulk diffusivity of SVOCs formed from photo-oxidation of isoprene as they partition to a bimodal aerosol consisting of an Aitken (potassium sulfate) and accumulation mode (aged α-pinene SOA) particles as a function of relative humidity (RH). The model analysis of the observed size distribution evolution shows that liquid-like diffusion coefficient values of Db > 10–10 cm2 s–1 fail to explain the growth of the Aitken mode. Instead, much lower values of Db between 2.5 × 10–15 cm2 s–1 at 32% RH and 8 × 10–15 cm2 s–1 at 82% RH were needed to successfully reproduce the growth of both modes. The diffusivity within the aged α-pinene SOA remains appreciably slow even at 80% RH, resulting in hindered partitioning of SVOCs to large viscous particles and allowing smaller and relatively less viscous particles to effectively absorb the available SVOCs and grow much faster than would be possible otherwise. Our results have important implications for modeling SOA formation and growth in the ambient atmosphere.},
doi = {10.1021/acs.est.9b05514},
journal = {Environmental Science and Technology},
number = 5,
volume = 54,
place = {United States},
year = {Wed Jan 29 00:00:00 EST 2020},
month = {Wed Jan 29 00:00:00 EST 2020}
}
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Works referencing / citing this record:
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