Investigating the Synergistic Interactions Between Anthropogenic Gas-phase Hydrophobic Organics and Biogenic SOA Particles
EMSL Project ID
48913
Abstract
We propose to investigate the molecular-level processes responsible for anthropogenic-biogenic interactions that enhance production and atmospheric lifetime of biogenic secondary organic aerosol (BSOA). The proposed work will focus on the synergistic interactions between hydrophobic organic molecules of anthropogenic origin emitted as incomplete combustion byproducts of fossil and biomass fuels and biogenic precursors that oxidize to form BSOA particles. We will utilize the EMSL’s Single Particle Mass Spectrometer (SPLAT II) to comprehensively characterize the physical and chemical properties of BSOA particles (phase, viscosity, morphology, composition, and volatility) formed in the presence of these hydrophobic molecules of anthropogenic origin. In addition, we will use the high-resolution Orbitrap-MS to characterize the molecular composition of these particles and the Proton Transfer Reaction Mass Spectrometer (PTR-MS) to monitor gas-phase concentrations of hydrophobic organics, BSOA precursor, and other relevant species as a function of reaction time. We will quantify how particle formation yields from dominant BSOA precursors, like isoprene, limonene and monoterpenes change due to interactions with different hydrophobic organics of anthropogenic origin, such as polycyclic aromatic hydrocarbons (PAHs) with different molecular structures and volatilities, dioctyl phthalate (DOP), and dioctyl sebacate (DOS). These findings will then be incorporated in our 3D regional and global chemical transport models to investigate the global impacts of these observations. We will conduct present-day and pre-industrial climate simulations to understand the role that these processes play in human influences on climate change. These climate models will utilize the advanced supercomputing resources at EMSL. This state-of-the-art combined model-measurement approach is expected to transform how we think about the synergistic interactions between anthropogenic and biogenic emissions.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2015-10-01
End Date
2017-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Kramer A.L., K.J. Suski, D.M. Bell, A. Zelenyuk-Imre, and S.L. Massey Simonich. 2019. "Formation of Polycyclic Aromatic Hydrocarbon Oxidation Products in alpha-Pinene Secondary Organic Aerosol Particles Formed through Ozonolysis." Environmental Science & Technology 53, no. 12:6669-6677. PNNL-SA-144860. doi:10.1021/acs.est.9b01732
Shrivastava MKB, S Lou, A Zelenyuk-Imre, RC Easter, Jr, RA Corley, BD Thrall, PJ Rasch, JD Fast, SL Massey Simonich, H Shen, and S Tao. 2017. "Global Long-Range Transport and Lung Cancer Risk from Polycyclic Aromatic Hydrocarbons Shielded by Coatings of Organic Aerosol." Proceedings of the National Academy of Sciences of the United States of America 114(6):1246-1251. doi:10.1073/pnas.1618475114
Zelenyuk-Imre A, D Imre, JM Wilson, DM Bell, KJ Suski, MKB Shrivastava, J Beranek, ML Alexander, AL Kramer, and SL Massey Simonich. 2017. "The Effect of Gas-phase Polycyclic Aromatic Hydrocarbons on the Formation and Properties of Biogenic Secondary Organic Aerosol Particles." Faraday Discussions 200:143-164. doi:10.1039/C7FD00032D