PNNL

Abstract

Vegetative fuels commonly consumed in prescribed fires were collected from five locations in the southeastern and southwestern U.S. and burned in a series of 77 fires at the U.S. Forest Service Fire Sciences Laboratory in Missoula, Montana. The particulate matter (PM2.5) emissions were measured by gravimetric filter sampling with subsequent analysis for elemental carbon (EC), organic carbon (OC), and 38 elements. The trace gas emissions were measured with a large suite of state-of-the-art instrumentation including an open-path Fourier transform infrared (OP FTIR) spectrometer, proton-transfer-reaction mass spectrometry (PTR-MS), proton-transfer ion-trap mass spectrometry (PIT-MS), negative-ion proton-transfer chemical-ionization mass spectrometry (NI-PT-CIMS), and gas chromatography with MS detection (GC-MS). 204 trace gas species (mostly non-methane organic compounds (NMOC)) were identified and quantified with the above instruments. An additional 152 significant peaks in the unit mass resolution mass spectra were quantified, but either could not be identified or most of the signal at that molecular mass was unaccounted for by identifiable species. As phase II of this study, we conducted airborne and ground-based sampling of the emissions from real prescribed fires mostly in the same land management units where the fuels for the lab fires were collected. A broad variety, but smaller number of species (21 trace gas species and PM2.5) was measured on 14 fires in chaparral and oak savanna in the southwestern US, as well as pine forest understory in the southeastern US and Sierra Nevada mountains of California. These extensive field measurements of emission factors (EF) for temperate biomass burning are useful both for modeling and to examine the representativeness of our lab fire EF. The lab/field EF ratio for the pine understory fuels was not statistically different from one, on average. However, our lab EF for “smoldering compounds” emitted by burning the semi-arid SW fuels should likely be increased by about a factor of 2.7 to better represent field fires. Based on the lab/field comparison, we present a table with emission factors for 365 pyrogenic species (including unidentified species) for 4 broad fuel types: pine understory, semi-arid shrublands, evergreen canopy, and duff. To our knowledge this is the most complete measurement of biomass burning emissions to date and it should enable improved representation of smoke in atmospheric models. The results provide important insights into the nature of smoke. For example, ~35% (range from 16-71%) of the mass of gas-phase NMOC species was attributed to the species that we could not identify. These unidentified species are likely not represented in most models, but some provision should be made for the fact that they will react in the atmosphere. In addition, the total mass of gas-phase NMOC divided by the mass of co-emitted PM2.5 averaged ~2.6 for the main fire types with a range from ~1.8-8.8. About 36-63% of the NMOC were likely semivolatile or of intermediate volatility. Thus, the gas-phase NMOC represent a large reservoir of potential precursors for secondary formation of organic aerosol. For the one fire in organic soil (Alaskan duff) about 28% of the emitted carbon was present as gas-phase NMOC in contrast to the other fuels for which NMOC accounted for only ~1-3% of emitted carbon. 71% of the mass of NMOC emitted by the smoldering duff was un-identified. The duff results highlight the need to learn more about the emissions from smoldering organic soils. The ?NMOC/“NOx-as-NO” ratio was consistently about ten for the main fire types when accounting for all NMOC, indicating strongly NOx-limited O3 production conditions. Finally, the fuel consumption per unit area was measured on 6 of the 14 prescribed fires and averaged 7.08 ± 2.09 (1?) Mg ha-1.