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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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Volume 17, issue 15 | Copyright
Atmos. Chem. Phys., 17, 9399-9415, 2017
https://doi.org/10.5194/acp-17-9399-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 07 Aug 2017

Research article | 07 Aug 2017

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

Francisco Mena1, Tami C. Bond1, and Nicole Riemer2 Francisco Mena et al.
  • 1Department of Civil and Environmental Engineering, University of Illinois Urbana-Champaign, Urbana, IL 61801, USA
  • 2Department of Atmospheric Sciences, University of Illinois Urbana-Champaign, Urbana, IL 61801, USA

Abstract. Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCN activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 1016 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation (ssat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20% if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume processes. This homogenizing effect requires the components to be truly co-emitted, rather than sequentially emitted.

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We estimate how biofuel burning may contribute to cloud droplet numbers by modeling the evolution of the size and composition of each particle in a biofuel burning plume from emission until it reaches ambient temperature and humidity. Condensation of semi-volatile gases homogenizes composition so that particles without water affinity can form cloud droplets. Coagulation barely changes properties relevant to clouds, except for limiting the number of emitted particles or enhancing homogenization.
We estimate how biofuel burning may contribute to cloud droplet numbers by modeling the...
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