Aerosol optical properties and trace gas emissions by PAX and OP-FTIR for laboratory-simulated western US wildfires during FIREX

摘要

Western wildfires have a major impact on air quality in the US. In the fall of 2016, 107 test fires were burned in the large-scale combustion facility at the US Forest Service Missoula Fire Sciences Laboratory as part of the Fire Influence on Regional and Global Environments Experiment (FIREX). Canopy, litter, duff, dead wood, and other fuel components were burned in combinations that represented realistic fuel complexes for several important western US coniferous and chaparral ecosystems including ponderosa pine, Douglas fir, Engelmann spruce, lodgepole pine, subalpine fir, chamise, and manzanita. In addition, dung, Indonesian peat, and individual coniferous ecosystem fuel components were burned alone to investigate the effects of individual components (e.g., duff) and fuel chemistry on emissions. The smoke emissions were characterized by a large suite of state-of-the-art instruments. In this study we report emission factor (EF, grams of compound emitted per kilogram of fuel burned) measurements in fresh smoke of a diverse suite of critically important trace gases measured using open-path Fourier transform infrared spectroscopy (OP-FTIR). We also report aerosol optical properties (absorption EF; single-scattering albedo, SSA; and ?ngstr?m absorption exponent, AAE) as well as black carbon (BC) EF measured by photoacoustic extinctiometers (PAXs) at 870 and 401?nm. The average trace gas emissions were similar across the coniferous ecosystems tested and most of the variability observed in emissions could be attributed to differences in the consumption of components such as duff and litter, rather than the dominant tree species. Chaparral fuels produced lower EFs than mixed coniferous fuels for most trace gases except for NOsubx/sub and acetylene. A careful comparison with available field measurements of wildfires confirms that several methods can be used to extract data representative of real wildfires from the FIREX laboratory fire data. This is especially valuable for species rarely or not yet measured in the field. For instance, the OP-FTIR data alone show that ammonia (1.62?g?kgsup?1/sup), acetic acid (2.41?g?kgsup?1/sup), nitrous acid (HONO, 0.61?g?kgsup?1/sup), and other trace gases such as glycolaldehyde (0.90?g?kgsup?1/sup) and formic acid (0.36?g?kgsup?1/sup) are significant emissions that were poorly characterized or not characterized for US wildfires in previous work. The PAX measurements show that the ratio of brown carbon (BrC) absorption to BC absorption is strongly dependent on modified combustion efficiency (MCE) and that BrC absorption is most dominant for combustion of duff (AAE 7.13) and rotten wood (AAE 4.60): fuels that are consumed in greater amounts during wildfires than prescribed fires. Coupling our laboratory data with field data suggests that fresh wildfire smoke typically has an EF for BC near 0.2?g?kgsup?1/sup, an SSA of ～ 0.91, and an AAE of ～ 3.50, with the latter implying that about 86?% of the aerosol absorption at 401?nm is due to BrC.