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Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

Roldin, Pontus LU ; Eriksson, Axel LU ; Nordin, Erik LU ; Öström, Emilie LU ; Mogensen, D.; Rusanen, A.; Boy, M.; Swietlicki, Erik LU ; Svenningsson, Birgitta LU and Zelenyuk, A., et al. (2014) In Atmospheric Chemistry and Physics 14(15). p.7953-7993
Abstract
We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost... (More)
We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of alpha-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), and (4) the influence of chamber wall effects on the observed SOA formation in smog chambers. ADCHAM is able to capture the observed alpha-pinene SOA mass increase in the presence of NH3(g). Organic salts of ammonium and carboxylic acids predominantly form during the early stage of SOA formation. In the smog chamber experiments, these salts contribute substantially to the initial growth of the homogeneously nucleated particles. The model simulations of evaporating alpha-pinene SOA particles support the recent experimental findings that these particles have a semi-solid tar-like amorphous-phase state. ADCHAM is able to reproduce the main features of the observed slow evaporation rates if the concentration of low-volatility and viscous oligomerized SOA material at the particle surface increases upon evaporation. The evaporation rate is mainly governed by the reversible decomposition of oligomers back to monomers. Finally, we demonstrate that the mass-transfer-limited uptake of condensable organic compounds onto wall-deposited particles or directly onto the Teflon chamber walls of smog chambers can have a profound influence on the observed SOA formation. During the early stage of the SOA formation the wall-deposited particles and walls themselves serve as an SOA sink from the air to the walls. However, at the end of smog chamber experiments the semi-volatile SOA material may start to evaporate from the chamber walls. With these four model applications, we demonstrate that several poorly quantified processes (i.e. mass transport limitations within the particle phase, oligomerization, heterogeneous oxidation, organic salt formation, and chamber wall effects) can have a substantial influence on the SOA formation, lifetime, chemical and physical particle properties, and their evolution. In order to constrain the uncertainties related to these processes, future experiments are needed in which as many of the influential variables as possible are varied. ADCHAM can be a valuable model tool in the design and analysis of such experiments. (Less)
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Atmospheric Chemistry and Physics
volume
14
issue
15
pages
7953 - 7993
publisher
Copernicus Gesellschaft Mbh
external identifiers
  • wos:000341103600020
  • scopus:84905970243
ISSN
1680-7324
DOI
10.5194/acp-14-7953-2014
project
MERGE
language
English
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yes
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443e5c67-4659-45d9-875a-6a277e3c1eaa (old id 4728859)
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2014-10-27 09:33:34
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2017-10-08 03:23:22
@article{443e5c67-4659-45d9-875a-6a277e3c1eaa,
  abstract     = {We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of alpha-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), and (4) the influence of chamber wall effects on the observed SOA formation in smog chambers. ADCHAM is able to capture the observed alpha-pinene SOA mass increase in the presence of NH3(g). Organic salts of ammonium and carboxylic acids predominantly form during the early stage of SOA formation. In the smog chamber experiments, these salts contribute substantially to the initial growth of the homogeneously nucleated particles. The model simulations of evaporating alpha-pinene SOA particles support the recent experimental findings that these particles have a semi-solid tar-like amorphous-phase state. ADCHAM is able to reproduce the main features of the observed slow evaporation rates if the concentration of low-volatility and viscous oligomerized SOA material at the particle surface increases upon evaporation. The evaporation rate is mainly governed by the reversible decomposition of oligomers back to monomers. Finally, we demonstrate that the mass-transfer-limited uptake of condensable organic compounds onto wall-deposited particles or directly onto the Teflon chamber walls of smog chambers can have a profound influence on the observed SOA formation. During the early stage of the SOA formation the wall-deposited particles and walls themselves serve as an SOA sink from the air to the walls. However, at the end of smog chamber experiments the semi-volatile SOA material may start to evaporate from the chamber walls. With these four model applications, we demonstrate that several poorly quantified processes (i.e. mass transport limitations within the particle phase, oligomerization, heterogeneous oxidation, organic salt formation, and chamber wall effects) can have a substantial influence on the SOA formation, lifetime, chemical and physical particle properties, and their evolution. In order to constrain the uncertainties related to these processes, future experiments are needed in which as many of the influential variables as possible are varied. ADCHAM can be a valuable model tool in the design and analysis of such experiments.},
  author       = {Roldin, Pontus and Eriksson, Axel and Nordin, Erik and Öström, Emilie and Mogensen, D. and Rusanen, A. and Boy, M. and Swietlicki, Erik and Svenningsson, Birgitta and Zelenyuk, A. and Pagels, Joakim},
  issn         = {1680-7324},
  language     = {eng},
  number       = {15},
  pages        = {7953--7993},
  publisher    = {Copernicus Gesellschaft Mbh},
  series       = {Atmospheric Chemistry and Physics},
  title        = {Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM},
  url          = {http://dx.doi.org/10.5194/acp-14-7953-2014},
  volume       = {14},
  year         = {2014},
}