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Volume 17, issue 2
Atmos. Chem. Phys., 17, 1471-1489, 2017
https://doi.org/10.5194/acp-17-1471-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 17, 1471-1489, 2017
https://doi.org/10.5194/acp-17-1471-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 31 Jan 2017

Research article | 31 Jan 2017

Multi-instrument comparison and compilation of non-methane organic gas emissions from biomass burning and implications for smoke-derived secondary organic aerosol precursors

Lindsay E. Hatch1,a, Robert J. Yokelson2, Chelsea E. Stockwell2,b, Patrick R. Veres3,4, Isobel J. Simpson5, Donald R. Blake5, John J. Orlando6, and Kelley C. Barsanti1,a Lindsay E. Hatch et al.
  • 1Department of Civil and Environmental Engineering, Portland State University, Portland, OR, USA
  • 2Department of Chemistry, University of Montana, Missoula, MT, USA
  • 3Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 4Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
  • 5Department of Chemistry, University of California, Irvine, Irvine, CA, USA
  • 6National Center for Atmospheric Research, Boulder, CO, USA
  • acurrent address: Department of Chemical and Environmental Engineering and College of Engineering – Center for Environmental Research and Technology (CE-CERT), University of California, Riverside, Riverside, CA, USA
  • bcurrent address: Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA

Abstract. Multiple trace-gas instruments were deployed during the fourth Fire Lab at Missoula Experiment (FLAME-4), including the first application of proton-transfer-reaction time-of-flight mass spectrometry (PTR-TOFMS) and comprehensive two-dimensional gas chromatography–time-of-flight mass spectrometry (GC × GC-TOFMS) for laboratory biomass burning (BB) measurements. Open-path Fourier transform infrared spectroscopy (OP-FTIR) was also deployed, as well as whole-air sampling (WAS) with one-dimensional gas chromatography–mass spectrometry (GC-MS) analysis. This combination of instruments provided an unprecedented level of detection and chemical speciation. The chemical composition and emission factors (EFs) determined by these four analytical techniques were compared for four representative fuels. The results demonstrate that the instruments are highly complementary, with each covering some unique and important ranges of compositional space, thus demonstrating the need for multi-instrument approaches to adequately characterize BB smoke emissions. Emission factors for overlapping compounds generally compared within experimental uncertainty, despite some outliers, including monoterpenes.

Data from all measurements were synthesized into a single EF database that includes over 500 non-methane organic gases (NMOGs) to provide a comprehensive picture of speciated, gaseous BB emissions. The identified compounds were assessed as a function of volatility; 6–11% of the total NMOG EF was associated with intermediate-volatility organic compounds (IVOCs). These atmospherically relevant compounds historically have been unresolved in BB smoke measurements and thus are largely missing from emission inventories. Additionally, the identified compounds were screened for published secondary organic aerosol (SOA) yields. Of the total reactive carbon (defined as EF scaled by the OH rate constant and carbon number of each compound) in the BB emissions, 55–77% was associated with compounds for which SOA yields are unknown or understudied. The best candidates for future smog chamber experiments were identified based on the relative abundance and ubiquity of the understudied compounds, and they included furfural, 2-methyl furan, 2-furan methanol, and 1,3-cyclopentadiene. Laboratory study of these compounds will facilitate future modeling efforts.

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The most comprehensive database of gaseous biomass burning emissions to date was compiled. Four complementary instruments were deployed together during laboratory fires. The results generally compared within experimental uncertainty and highlighted that a range of measurement approaches are required for adequate characterization of smoke composition. Observed compounds were binned based on volatility, and priority recommendations were made to improve secondary organic aerosol predictions.
The most comprehensive database of gaseous biomass burning emissions to date was compiled. Four...
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