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Title: Understanding the Applicability of Gas/Particle Partitioning Theory to SOA using Novel Chemically-Speciated Partitioning Measurements (Final Report)

Technical Report ·
DOI:https://doi.org/10.2172/1725658· OSTI ID:1725658
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Colorado, Boulder, CO (United States)
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The main objective of this research grant project was to investigate the physical-chemical processes and properties of particles and partitioning gases that influence gas/particle (G/P) partitioning and timescales for equilibration, to directly determine the conditions under which equilibrium G/P partitioning theory can be applied to secondary organic aerosol (SOA). SOA constitutes a major component of submicron particles in the atmosphere, which have important implications for air quality, human and ecosystem health, radiation balance, and climate; however SOA formation, evolution and losses are not well understood. Use of novel on-line measurements of chemically-speciated partitioning measurements of both gas-phase and particle-phase components was a central component to advancing these scientific goals. The key approach was to conduct environmental chamber studies with systems of increasing complexity to determine G/P partitioning rates and equilibrium states for chemically-speciated SOA components. The project builds on our previous work on gas-wall partitioning that must be understood in order to study G/P partitioning in chambers, and to help extrapolate the results to be atmospherically relevant. The goal was to employ measurements and modeling to systematically determine when G/P partitioning theory accurately describes the distribution of oxidized organic compounds in the gas and aerosol phases, and when and why it does not (e.g., aerosol phase-state kinetic limitations, non-ideal mixing, phase separation, oligomer formation,), for chemical and physical conditions typically found throughout the continental boundary layer.

Research Organization:
University of Colorado, Boulder
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER). Earth and Environmental Systems Science Division
DOE Contract Number:
SC0016559
OSTI ID:
1725658
Report Number(s):
DOE-CU-16559
Resource Relation:
Related Information: See the "Related Identifiers/DOIs" field for references/DOI of published papers supported by and acknowledging this grant and related to this final report. More details on publications, conference presentations, and other products are documented in the uploaded pdf with the full technical report narrative in the "Upload/Link" section.Additional papers that are in review and expected to be published soon and thus do not have a DOI at the time of submission of this report include:B.A. Nault, P. Campuzano-Jost, D.A. Day, D.S. Jo, J.C. Schroder, H.M. Allen, R. Bahreini, H. Bian, D.R. Blake, M. Chin, S.L. Clegg, P.R. Colarco, J.D. Crounse, M.J. Cubison, P.F. DeCarlo, J.E. Dibb, G.S. Diskin, A. Hodzic, W. Hu, J.M. Katich, M.J. Kim, J.K. Kodros, A. Kupc, F.D. Lopez-Hilfiker, E.A. Marais, A.M. Middlebrook, J.A. Neuman, J.B. Nowak, B.B. Palm, F. Paulot, J.R. Pierce, G.P. Schill, E. Scheuer, J.A. Thornton, K. Tsigaridis, P.O. Wennberg, C.J. Williamson, J.L. Jimenez. Models underestimate the increase of acidity with remoteness biasing radiative impact calculations. Submitted, Sep. 2020.X. Liu, D.A. Day, J.E. Krechmer, P.J. Ziemann, J.L. Jimenez. Determining Activity Coefficients of SOA from Isothermal Evaporation in a Laboratory Chamber. Environ. Sci. Technol. Lett., in review, 2020.
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
54 ENVIRONMENTAL SCIENCES
58 GEOSCIENCES
partitioning
gas-particle partitioning
gas-wall interactions
particle phase
secondary organic aerosol
SOA
accommodation coefficient
activity coefficient
environmental chambers
smog chambers
Teflon chamber
volatility
tubing interactions
IEPOX
atmosphere
air quality
climate
modeling
vapor pressure
global modeling
chemical modeling
atmospheric chemistry
atmospheric science
pollution
structural activity relationships