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Volume 18, issue 10 | Copyright
Atmos. Chem. Phys., 18, 6985-7000, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 18 May 2018

Research article | 18 May 2018

Particle-bound reactive oxygen species (PB-ROS) emissions and formation pathways in residential wood smoke under different combustion and aging conditions

Jun Zhou1,a, Peter Zotter2, Emily A. Bruns1, Giulia Stefenelli1, Deepika Bhattu1, Samuel Brown1,3, Amelie Bertrand1,4, Nicolas Marchand4, Houssni Lamkaddam1, Jay G. Slowik1, André S. H. Prévôt1, Urs Baltensperger1, Thomas Nussbaumer2, Imad El-Haddad1, and Josef Dommen1 Jun Zhou et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
  • 2Lucerne University of Applied Sciences and Arts, Engineering and Architecture, Bioenergy Research, 6048 Horw, Switzerland
  • 3Institute for Atmospheric and Climate Science, ETH, Zurich, Switzerland
  • 4Aix Marseille Univ, CNRS, LCE, Marseille, France
  • anow at: Graduate School of Global Environmental Studies, Kyoto University, Kyoto, 606-8501, Japan

Abstract. Wood combustion emissions can induce oxidative stress in the human respiratory tract by reactive oxygen species (ROS) in the aerosol particles, which are emitted either directly or formed through oxidation in the atmosphere. To improve our understanding of the particle-bound ROS (PB-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 PB-ROS content and the chemical properties of the aerosols were quantified by a novel ROS analyzer using the DCFH (2′,7′-dichlorofluorescin) assay and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). For all eight combustion devices tested, primary PB-ROS concentrations substantially increased upon aging. The level of primary and aged PB-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 1 order of magnitude lower than those from manually operated devices, which indicates that automatic combustion devices operated at optimum conditions to achieve near-complete combustion should be employed to minimize PB-ROS emissions. The use of an electrostatic precipitator decreased the primary and aged ROS emissions by a factor of  ∼ 1.5 which is however still within the burn-to-burn variability. The parameters controlling the PB-ROS formation in secondary organic aerosol were investigated by employing a regression model, including the fractions of the mass-to-charge ratios mz 44 and 43 in secondary organic aerosol (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 PB-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 PB-ROS content at higher OA concentrations, while further aging seems to result in a decay of PB-ROS. The results and the special data analysis methods deployed in this study could provide a model for PB-ROS analysis of further wood or other combustion studies investigating different combustion conditions and aging methods.

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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...