Impact of chamber wall loss of gaseous organic compounds on secondary organic aerosol formation: Explicit modeling of SOA formation from alkane and alkene oxidation

La, Y. S.; Camredon, M.; Ziemann, P. J.; Valorso, R.; Matsunaga, A.; Lannuque, V.; Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.

doi:10.5194/acp-16-1417-2016

Title: Impact of chamber wall loss of gaseous organic compounds on secondary organic aerosol formation: Explicit modeling of SOA formation from alkane and alkene oxidation

Journal Article · Mon Feb 08 04:00:00 UTC 2016 · Atmospheric Chemistry and Physics (Online)

DOI: https://doi.org/10.5194/acp-16-1417-2016 · OSTI ID:1253626

La, Y. S. ^[1]; Camredon, M. ^[2]; Ziemann, P. J. ^[3]; Valorso, R. ^[2]; Matsunaga, A. ^[4]; Lannuque, V. ^[2]; Lee-Taylor, J. ^[5]; Hodzic, A. ^[6]; Madronich, S. ^[6]; Aumont, B. ^[2]

Univ. Paris Est Creteil et Univ. Paris Diderot, Creteil (France); Université Paris Est Créteil et Université Paris, France
Univ. Paris Est Creteil et Univ. Paris Diderot, Creteil (France)
Univ. of Colorado, Boulder, CO (United States)
Univ. of California, Riverside, CA (United States)
Univ. of Colorado, Boulder, CO (United States); National Center for Atmospheric Research, Boulder, CO (United States)
National Center for Atmospheric Research, Boulder, CO (United States)

Recent studies have shown that low volatility gas-phase species can be lost onto the smog chamber wall surfaces. Although this loss of organic vapors to walls could be substantial during experiments, its effect on secondary organic aerosol (SOA) formation has not been well characterized and quantified yet. Here the potential impact of chamber walls on the loss of gaseous organic species and SOA formation has been explored using the Generator for Explicit Chemistry and Kinetics of the Organics in the Atmosphere (GECKO-A) modeling tool, which explicitly represents SOA formation and gas–wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene series (linear, cyclic and C₁₂-branched alkanes and terminal, internal and 2-methyl alkenes with 7 to 17 carbon atoms) under high NO_x conditions. Simulated trends match observed trends within and between homologous series. The loss of organic vapors to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phases. Simulated distributions of the species in various phases suggest that nitrates, hydroxynitrates and carbonylesters could substantially be lost onto walls. The extent of this process depends on the rate of gas–wall mass transfer, the vapor pressure of the species and the duration of the experiments. Furthermore, this work suggests that SOA yields inferred from chamber experiments could be underestimated up a factor of 2 due to the loss of organic vapors to chamber walls.

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Research Organization:: University Corporation for Atmospheric Research, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: SC0006780

OSTI ID:: 1253626

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 3 Vol. 16; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime Hodzic, A.; Kasibhatla, P. S.; Jo, D. S. Atmospheric Chemistry and Physics Discussions, Vol. 15, Issue 22 https://doi.org/10.5194/acpd-15-32413-2015	journal	January 2015
Challenges in determining atmospheric organic aerosol volatility distributions using thermal evaporation techniques Cain, Kerrigan P.; Karnezi, Eleni; Pandis, Spyros N. Taylor & Francis https://doi.org/10.6084/m9.figshare.12047115.v1	text	January 2020
Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013 Thompson, Samantha L.; Yatavelli, Reddy L. N.; Stark, Harald Taylor & Francis https://doi.org/10.6084/m9.figshare.4165656	text	January 2016
Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013 Thompson, Samantha L.; Yatavelli, Reddy L. N.; Stark, Harald Taylor & Francis https://doi.org/10.6084/m9.figshare.4165656.v1	text	January 2016
Dynamic method to measure partition coefficient and mass accommodation coefficient for gas‒particle interaction of phthalates Cao, Jianping; Eichler, Clara M. A.; Wu, Yaoxing Taylor & Francis https://doi.org/10.6084/m9.figshare.8316500	text	January 2019

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Title: Impact of chamber wall loss of gaseous organic compounds on secondary organic aerosol formation: Explicit modeling of SOA formation from alkane and alkene oxidation

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