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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
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 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 288 K) in a ∼ 7 m3 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 NTVOC ∕ OMsv 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 30 000 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 5 h of continuous aging. Based on the reaction scheme used, reaction rates of the NTVOC mixture range from 3.0 × 10−11 to 4. 0 × 10−11 cm3 molec−1 s−1. The average enthalpy of vaporization of secondary organic aerosol (SOA) surrogates was determined to be between 55 000 and 35 000 J mol−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.

Citation: Ciarelli, G., El Haddad, I., Bruns, E., Aksoyoglu, S., Möhler, O., Baltensperger, U., and Prévôt, A. S. H.: 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), Geosci. Model Dev., 10, 2303-2320, https://doi.org/10.5194/gmd-10-2303-2017, 2017.
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Short summary
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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