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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
https://doi.org/10.5194/acp-2017-1068
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article
21 Nov 2017
Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).
Reactive oxygen species (ROS) emissions and formation pathways in residential wood smoke under different combustion and aging conditions
Jun Zhou1, Peter Zotter2, Emily A. Bruns1, Giulia Stefenelli1, Deepika Bhattu1, Samuel Brown1,3, Amelie Bertrand4, Nicolas Marchand4, Houssni Lamkaddam1, Jay G. Slowik1, André S. H. Prévôt1, Urs Baltensperger1, Thomas Nussbaumer2, Imad El Haddad1, and Josef Dommen1 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
2Lucerne University of Applied Sciences and Arts, School of Engineering and Architecture, Bioenergy Research, 6048 Horw, Switzerland
3Institute for Atmospheric and Climate Science, ETH, Zurich, Switzerland
4Aix Marseille Univ, CNRS, LCE, Marseille, France
Abstract. Wood combustion emissions can induce oxidative stress in the human respiratory tract caused by reactive oxygen species (ROS), either directly or after oxidation in the atmosphere. To improve our understanding of the ROS generation potential of wood combustion emissions, a suite of smog chamber (SC) and potential aerosol mass (PAM) chamber experiments were conducted under well determined conditions for different combustion devices and technologies, different fuel types, operation methods, combustion regimes, combustion phases and aging conditions. The ROS content as well as the chemical properties of the aerosols were quantified by a novel ROS analyzer and a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS). For all eight tested combustion devices, primary ROS concentrations substantially increased upon aging. The level of primary and aged ROS emission factors (EFROS) were dominated by the combustion device (within different combustion technologies) and to a greater extent by the combustion regimes: the variability within one device was much higher than the variability of EFROS from different devices. Aged EFROS under bad combustion conditions were ~ 2–80 times higher than under optimum combustion conditions. EFROS from automatically operated combustion devices were on average one order of magnitude lower than those from manually operated appliances, which indicates that automatic combustion devices operated at optimum conditions to achieve near-complete combustion should be employed to minimize ROS emissions. The parameters controlling the ROS formation in secondary organic aerosol were investigated by employing a regression model, including the fractions of the mass spectrometric signatures m/z 44 and 43 in SOA (f44-SOA and f43-SOA), the OH exposure, and the total organic aerosol mass. The regression model results of the SC and PAM chamber aging experiments indicate that the ROS content in SOA seems to increase with the SOA oxidation state, which initially increases with OH exposure and decreases with the additional partitioning of semi-volatile components with lower ROS content at higher OA concentrations, while further aging seems to result in a decay of ROS. The results and the special data analysis methods deployed in this study could provide a role model for ROS analysis of further wood or any other combustion studies investigating different combustion conditions and aging methods.

Citation: Zhou, J., Zotter, P., Bruns, E. A., Stefenelli, G., Bhattu, D., Brown, S., Bertrand, A., Marchand, N., Lamkaddam, H., Slowik, J. G., Prévôt, A. S. H., Baltensperger, U., Nussbaumer, T., El Haddad, I., and Dommen, J.: Reactive oxygen species (ROS) emissions and formation pathways in residential wood smoke under different combustion and aging conditions, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-1068, in review, 2017.
Jun Zhou et al.
Jun Zhou et al.

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Short summary
We thoroughly studied the Reactive oxygen species (ROS) generation potential of particulate wood combustion emissions, from different combustion technologies, fuel types, operation methods, combustion regimes and phases. ROS from automatically operated combustion devices under optimal conditions were much lower than those from manually operated appliances. We examined the impact of atmospheric aging on ROS content in SOA and determined the controlling parameters, by using an online ROS analyzer.
We thoroughly studied the Reactive oxygen species (ROS) generation potential of particulate wood...
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