Secondary organic aerosol formation from smoldering and flaming combustion of biomass: a box model parametrization based on volatility basis set
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Published:2019-09-12
Issue:17
Volume:19
Page:11461-11484
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Stefenelli Giulia, Jiang JianhuiORCID, Bertrand Amelie, Bruns Emily A., Pieber Simone M.ORCID, Baltensperger Urs, Marchand NicolasORCID, Aksoyoglu SebnemORCID, Prévôt André S. H., Slowik Jay G., El Haddad Imad
Abstract
Abstract. Residential wood combustion remains one of the most important sources of
primary organic aerosols (POA) and secondary organic aerosol (SOA)
precursors during winter. The overwhelming majority of these precursors have not been traditionally considered in regional models, and only recently were lignin pyrolysis products and polycyclic aromatics identified as the
principal SOA precursors from flaming wood combustion. The SOA yields of
these components in the complex matrix of biomass smoke remain unknown and
may not be inferred from smog chamber data based on single-compound systems.
Here, we studied the ageing of emissions from flaming and
smoldering-dominated wood fires in three different residential stoves,
across a wide range of ageing temperatures (−10, 2
and 15 ∘C) and emission loads. Organic gases (OGs) acting as SOA
precursors were monitored by a proton-transfer-reaction time-of-flight mass
spectrometer (PTR-ToF-MS), while the evolution of the aerosol properties
during ageing in the smog chamber was monitored by a high-resolution
time-of-flight aerosol mass spectrometer (HR-ToF-AMS). We developed a novel
box model based on the volatility basis set (VBS) to determine the
volatility distributions of the oxidation products from different precursor
classes found in the emissions, grouped according to their emission pathways
and SOA production rates. We show for the first time that SOA yields in
complex emissions are consistent with those reported in literature from
single-compound systems. We identify the main SOA precursors in both flaming
and smoldering wood combustion emissions at different temperatures. While
single-ring and polycyclic aromatics are significant precursors in flaming
emissions, furans generated from cellulose pyrolysis appear to be important
for SOA production in the case of smoldering fires. This is especially the
case at high loads and low temperatures, given the higher volatility of
furan oxidation products predicted by the model. We show that the oxidation
products of oxygenated aromatics from lignin pyrolysis are expected to
dominate SOA formation, independent of the combustion or ageing conditions,
and therefore can be used as promising markers to trace ageing of biomass
smoke in the field. The model framework developed herein may be
generalizable for other complex emission sources, allowing determination of
the contributions of different precursor classes to SOA, at a level of
complexity suitable for implementation in regional air quality models.
Funder
Seventh Framework Programme Horizon 2020
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference85 articles.
1. Aiken, A. C., DeCarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A.,
Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun,
Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M.
R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy,
J., Metzger, A., Baltensperger, U., and Jimenez, J. L.: O∕C and OM∕OC ratios
of primary, secondary, and ambient organic aerosols with high-resolution
time-of-flight aerosol mass spectrometry, Anviron. Sci. Technol., 42, 4478–4485, https://doi.org/10.1021/es703009q, 2008. 2. Atkinson, R. and Arey, J.: Atmospheric degradation of volatile organic
compounds, Chem. Rev., 103, 4605–4638, https://doi.org/10.1021/cr0206420,
2003. 3. Barmet, P., Dommen, J., DeCarlo, P. F., Tritscher, T., Praplan, A. P., Platt, S. M., Prévôt, A. S. H., Donahue, N. M., and Baltensperger, U.: OH clock determination by proton transfer reaction mass spectrometry at an environmental chamber, Atmos. Meas. Tech., 5, 647–656, https://doi.org/10.5194/amt-5-647-2012, 2012. 4. Bertrand, A., Stefenelli, G., Bruns, E. A., Pieber, S. M., Temime-Roussel,
B., Slowik, J. G., Prévôt, A. S. H., Wortham, H., El Haddad, I., and Marchand, N.: Primary emissions and secondary aerosol production potential
from woodstoves for residential heating: Influence of the stove technology
and combustion efficiency, Atmos. Environ., 169, 65–79,
https://doi.org/10.1016/j.atmosenv.2017.09.005, 2017. 5. Bertrand, A., Stefenelli, G., Jen, C. N., Pieber, S. M., Bruns, E. A., Ni, H., Temime-Roussel, B., Slowik, J. G., Goldstein, A. H., El Haddad, I., Baltensperger, U., Prévôt, A. S. H., Wortham, H., and Marchand, N.: Evolution of the chemical fingerprint of biomass burning organic aerosol during aging, Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, 2018a.
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