Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

Pair your accounts.

Export articles to Mendeley

Get article recommendations from ACS based on references in your Mendeley library.

You’ve supercharged your research process with ACS and Mendeley!

STEP 1:
Click to create an ACS ID

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

MENDELEY PAIRING EXPIRED
Your Mendeley pairing has expired. Please reconnect
ACS Publications. Most Trusted. Most Cited. Most Read
My Activity
CONTENT TYPES

Figure 1Loading Img

Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions

Cite this: ACS Earth Space Chem. 2023, 7, 4, 788–799
Publication Date (Web):March 29, 2023
https://doi.org/10.1021/acsearthspacechem.2c00358
Copyright © 2023 American Chemical Society

    Article Views

    840

    Altmetric

    -

    Citations

    LEARN ABOUT THESE METRICS
    Other access options
    Supporting Info (1)»

    Abstract

    Abstract Image

    Isoprene is the nonmethane volatile organic compound (VOC) emitted in the largest amounts to the atmosphere, and it is a significant source of secondary organic aerosol (SOA) mass. The uptake of isoprene oxidation products followed by multiphase chemistry in fine particles is the key pathway to form isoprene epoxydiol-derived SOA (IEPOX-SOA). However, many parameters that relate to the diffusion and reaction of IEPOX in the particle phase remain uncertain since reaction kinetics previously measured in bulk aqueous-phase solutions might be different from atmospheric aerosols. Here, we use simultaneous environmental chamber measurements of multiple parameters governing IEPOX-SOA formation at timescales of ∼hours: particle size distribution, composition, and volatility of IEPOX-SOA to constrain the key parameters governing IEPOX-SOA formation under humid (i.e., 50% relative humidity, RH) and varying seed aerosol acidity conditions. Reducing the 2-methyltetrol (tetrol) reaction rate constants by a factor of 4 brings the model predictions in agreement with the IEPOX-SOA measurements with acidified ammonium bisulfate seed aerosols. For less acidic ammonium sulfate aerosols, we find that both the organosulfate (OS) and tetrol reaction rate constants need to be reduced to bring model predictions closer to chamber observations. Using the measured nonvolatile content of IEPOX-SOA, we constrain the oligomerization timescale of tetrols. We find that the oligomerization timescale is 4 h with acidified seed aerosols, but a much longer timescale of 24 h is needed for nonacidified aerosols, indicating that the aerosol acidity greatly affects the oligomerization rate of tetrols. We show that the actual kinetics of IEPOX-SOA formation rate on aerosols consisting of both ammonium bisulfate and ammonium sulfate is a factor of 4–5 slower under 50–60% RH conditions compared to their application in previous models, which were mostly based on bulk aqueous solution measurements.

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. You can change your affiliated institution below.

    Supporting Information

    ARTICLE SECTIONS
    Jump To

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsearthspacechem.2c00358.

    • Size-dependent particle wall loss (Section S1), gas-phase chamber wall loss (Section S2), time evolution of organosulfate branching ratio (Figure S2), model predicted resistance to mass transfer (Figure S3), time series concentrations of aerosol components in the chamber (Figure S4), time evolution of IEPOX uptake coefficient (Figure S5), size distribution evolution of aerosol number concentration for AS aerosols (Figure S6), time evolution of number mean diameter and aerosol size distribution with different oligomerization timescales (Figure S7), sensitivity of relative mass fractions on tetrol oligomerization time scale (Figure S8), and references (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 2 publications.

    1. Yuzhi Chen, Alexandra E. Ng, Jaime Green, Yue Zhang, Matthieu Riva, Theran P. Riedel, Havala O. T. Pye, Ziying Lei, Nicole E. Olson, Madeline E. Cooke, Zhenfa Zhang, William Vizuete, Avram Gold, Barbara J. Turpin, Andrew P. Ault, Jason D. Surratt. Applying a Phase-Separation Parameterization in Modeling Secondary Organic Aerosol Formation from Acid-Driven Reactive Uptake of Isoprene Epoxydiols under Humid Conditions. ACS ES&T Air 2024, 1 (6) , 511-524. https://doi.org/10.1021/acsestair.4c00002
    2. Jie Zhang, Manish Shrivastava, Lan Ma, Wenqing Jiang, Cort Anastasio, Qi Zhang, Alla Zelenyuk. Modeling Novel Aqueous Particle and Cloud Chemistry Processes of Biomass Burning Phenols and Their Potential to Form Secondary Organic Aerosols. Environmental Science & Technology 2024, 58 (8) , 3776-3786. https://doi.org/10.1021/acs.est.3c07762