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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

Journal Article · · Atmospheric Chemistry and Physics (Online)
 [1];  [1];  [2];  [1];  [3];  [1];  [4];  [5];  [5];  [1]
  1. Univ. Paris Est Creteil et Univ. Paris Diderot, Creteil (France)
  2. Univ. of Colorado, Boulder, CO (United States)
  3. Univ. of California, Riverside, CA (United States)
  4. Univ. of Colorado, Boulder, CO (United States); National Center for Atmospheric Research, Boulder, CO (United States)
  5. 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 NOx 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.

Research Organization:
University Corporation for Atmospheric Research, Boulder, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0006780
OSTI ID:
1253626
Journal Information:
Atmospheric Chemistry and Physics (Online), Vol. 16, Issue 3; ISSN 1680-7324
Publisher:
European Geosciences UnionCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 68 works
Citation information provided by
Web of Science

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The role of low volatile organics on secondary organic aerosol formation posted_content June 2013
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Multiday production of condensing organic aerosol mass in urban and forest outflow posted_content July 2014
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Cited By (31)

Chemical evolution of atmospheric organic carbon over multiple generations of oxidation journal February 2018
Dynamic method to measure partition coefficient and mass accommodation coefficient for gas‒particle interaction of phthalates journal July 2019
Challenges in determining atmospheric organic aerosol volatility distributions using thermal evaporation techniques journal April 2020
How aging process changes characteristics of vehicle emissions? A review journal September 2019
SOA formation from the photooxidation of  α -pinene: systematic exploration of the simulation of chamber data journal January 2016
Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime journal January 2016
Model–measurement comparison of functional group abundance in α -pinene and 1,3,5-trimethylbenzene secondary organic aerosol formation journal January 2016
Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α -pinene ozonolysis journal January 2016
Constraining uncertainties in particle-wall deposition correction during SOA formation in chamber experiments journal January 2017
Observations of sesquiterpenes and their oxidation products in central Amazonia during the wet and dry seasons journal January 2018
Influence of the vapor wall loss on the degradation rate constants in chamber experiments of levoglucosan and other biomass burning markers journal January 2018
Exploration of the influence of environmental conditions on secondary organic aerosol formation and organic species properties using explicit simulations: development of the VBS-GECKO parameterization journal January 2018
Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia journal January 2018
Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea journal January 2018
Evolution of the chemical fingerprint of biomass burning organic aerosol during aging journal January 2018
Different roles of water in secondary organic aerosol formation from toluene and isoprene journal January 2018
Gas-phase composition and secondary organic aerosol formation from standard and particle filter-retrofitted gasoline direct injection vehicles investigated in a batch and flow reactor journal January 2018
Chemical composition and hydrolysis of organic nitrate aerosol formed from hydroxyl and nitrate radical oxidation of α-pinene and β-pinene journal January 2019
Development of a protocol for the auto-generation of explicit aqueous-phase oxidation schemes of organic compounds journal January 2019
Gas-phase composition and secondary organic aerosol formation from standard and particle filter-retrofitted gasoline direct injection vehicles investigated in a batch and flow reactor interactiveresource January 2018
Challenges in determining atmospheric organic aerosol volatility distributions using thermal evaporation techniques text January 2020
Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013 text January 2016
Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol journal January 2017
Model-measurement comparison of functional group abundance in α-pinene and 1,3,5-trimethylbenzene secondary organic aerosol formation posted_content February 2016
Development of a protocol for the auto-generation of explicit aqueous-phase oxidation schemes of organic compounds posted_content January 2019
Influence of the vapor wall loss on the degradation rate constants in chamber experiments of levoglucosan and other biomass burning markers posted_content January 2018
Rethinking the global secondary organic aerosol (SOA) budget: stronger production, faster removal, shorter lifetime journal January 2015
Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013 text January 2016
Dynamic method to measure partition coefficient and mass accommodation coefficient for gas‒particle interaction of phthalates text January 2019
Field intercomparison of the gas/particle partitioning of oxygenated organics during the Southern Oxidant and Aerosol Study (SOAS) in 2013 journal September 2016
Photosensitized Formation of Secondary Organic Aerosols above the Air/Water Interface journal August 2016

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