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Geoscientific Model Development An interactive open-access journal of the European Geosciences Union
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Volume 10, issue 6 | Copyright
Geosci. Model Dev., 10, 2303-2320, 2017
https://doi.org/10.5194/gmd-10-2303-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Development and technical paper 23 Jun 2017

Development and technical paper | 23 Jun 2017

Constraining a hybrid volatility basis-set model for aging of wood-burning emissions using smog chamber experiments: a box-model study based on the VBS scheme of the CAMx model (v5.40)

Giancarlo Ciarelli1,a, Imad El Haddad1, Emily Bruns1, Sebnem Aksoyoglu1, Ottmar Möhler2, Urs Baltensperger1, and André S. H. Prévôt1 Giancarlo Ciarelli et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
  • 2Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
  • anow at: Laboratoire Inter-Universitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583, Université Paris Est Créteil et Université Paris Diderot, Institut Pierre Simon Laplace, Créteil, France

Abstract. In this study, novel wood combustion aging experiments performed at different temperatures (263 and 288K) in a ∼7m3 smog chamber were modelled using a hybrid volatility basis set (VBS) box model, representing the emission partitioning and their oxidation against OH. We combine aerosol–chemistry box-model simulations with unprecedented measurements of non-traditional volatile organic compounds (NTVOCs) from a high-resolution proton transfer reaction mass spectrometer (PTR-MS) and with organic aerosol measurements from an aerosol mass spectrometer (AMS). Due to this, we are able to observationally constrain the amounts of different NTVOC aerosol precursors (in the model) relative to low volatility and semi-volatile primary organic material (OMsv), which is partitioned based on current published volatility distribution data. By comparing the NTVOCOMsv ratios at different temperatures, we determine the enthalpies of vaporization of primary biomass-burning organic aerosols. Further, the developed model allows for evaluating the evolution of oxidation products of the semi-volatile and volatile precursors with aging. More than 30000 box-model simulations were performed to retrieve the combination of parameters that best fit the observed organic aerosol mass and O:C ratios. The parameters investigated include the NTVOC reaction rates and yields as well as enthalpies of vaporization and the O:C of secondary organic aerosol surrogates. Our results suggest an average ratio of NTVOCs to the sum of non-volatile and semi-volatile organic compounds of ∼4.75. The mass yields of these compounds determined for a wide range of atmospherically relevant temperatures and organic aerosol (OA) concentrations were predicted to vary between 8 and 30% after 5h of continuous aging. Based on the reaction scheme used, reaction rates of the NTVOC mixture range from 3.0 × 10−11 to 4. 0 × 10−11cm3molec−1s−1. The average enthalpy of vaporization of secondary organic aerosol (SOA) surrogates was determined to be between 55000 and 35000Jmol−1, which implies a yield increase of 0.03–0.06%K−1 with decreasing temperature. The improved VBS scheme is suitable for implementation into chemical transport models to predict the burden and oxidation state of primary and secondary biomass-burning aerosols.

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In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources of air pollution. Novel wood-burning experiments performed in a state-of-the-art smog chamber provide valuable information on the chemical properties of wood-burning emissions and the transformation in the atmosphere. In this study, these new data were used in a box model to constrain a parameterization suitable for predicting the contribution of wood burning to air pollution with large-scale models.
In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources...
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