Showing papers by "Robert J. Yokelson published in 2011"

Emission factors for open and domestic biomass burning for use in atmospheric models

Abstract: . Biomass burning (BB) is the second largest source of trace gases and the largest source of primary fine carbonaceous particles in the global troposphere. Many recent BB studies have provided new emission factor (EF) measurements. This is especially true for non-methane organic compounds (NMOC), which influence secondary organic aerosol (SOA) and ozone formation. New EF should improve regional to global BB emissions estimates and therefore, the input for atmospheric models. In this work we present an up-to-date, comprehensive tabulation of EF for known pyrogenic species based on measurements made in smoke that has cooled to ambient temperature, but not yet undergone significant photochemical processing. All EFs are converted to one standard form (g compound emitted per kg dry biomass burned) using the carbon mass balance method and they are categorized into 14 fuel or vegetation types. Biomass burning terminology is defined to promote consistency. We compile a large number of measurements of biomass consumption per unit area for important fire types and summarize several recent estimates of global biomass consumption by the major types of biomass burning. Post emission processes are discussed to provide a context for the emission factor concept within overall atmospheric chemistry and also highlight the potential for rapid changes relative to the scale of some models or remote sensing products. Recent work shows that individual biomass fires emit significantly more gas-phase NMOC than previously thought and that including additional NMOC can improve photochemical model performance. A detailed global estimate suggests that BB emits at least 400 Tg yr−1 of gas-phase NMOC, which is almost 3 times larger than most previous estimates. Selected recent results (e.g. measurements of HONO and the BB tracers HCN and CH3CN) are highlighted and key areas requiring future research are briefly discussed.

The Fire INventory from NCAR (FINN): a high resolution global model to estimate the emissions from open burning

Abstract: . The Fire INventory from NCAR version 1.0 (FINNv1) provides daily, 1 km resolution, global estimates of the trace gas and particle emissions from open burning of biomass, which includes wildfire, agricultural fires, and prescribed burning and does not include biofuel use and trash burning. Emission factors used in the calculations have been updated with recent data, particularly for the non-methane organic compounds (NMOC). The resulting global annual NMOC emission estimates are as much as a factor of 5 greater than some prior estimates. Chemical speciation profiles, necessary to allocate the total NMOC emission estimates to lumped species for use by chemical transport models, are provided for three widely used chemical mechanisms: SAPRC99, GEOS-CHEM, and MOZART-4. Using these profiles, FINNv1 also provides global estimates of key organic compounds, including formaldehyde and methanol. Uncertainties in the emissions estimates arise from several of the method steps. The use of fire hot spots, assumed area burned, land cover maps, biomass consumption estimates, and emission factors all introduce error into the model estimates. The uncertainty in the FINNv1 emission estimates are about a factor of two; but, the global estimates agree reasonably well with other global inventories of biomass burning emissions for CO, CO2, and other species with less variable emission factors. FINNv1 emission estimates have been developed specifically for modeling atmospheric chemistry and air quality in a consistent framework at scales from local to global. The product is unique because of the high temporal and spatial resolution, global coverage, and the number of species estimated. FINNv1 can be used for both hindcast and forecast or near-real time model applications and the results are being critically evaluated with models and observations whenever possible.

Boreal forest fire emissions in fresh Canadian smoke plumes: C 1 -C 10 volatile organic compounds (VOCs), CO 2 , CO, NO 2 , NO, HCN and CH 3 CN

Abstract: . Boreal regions comprise about 17 % of the global land area, and they both affect and are influenced by climate change. To better understand boreal forest fire emissions and plume evolution, 947 whole air samples were collected aboard the NASA DC-8 research aircraft in summer 2008 as part of the ARCTAS-B field mission, and analyzed for 79 non-methane volatile organic compounds (NMVOCs) using gas chromatography. Together with simultaneous measurements of CO2, CO, CH4, CH2O, NO2, NO, HCN and CH3CN, these measurements represent the most comprehensive assessment of trace gas emissions from boreal forest fires to date. Based on 105 air samples collected in fresh Canadian smoke plumes, 57 of the 80 measured NMVOCs (including CH2O) were emitted from the fires, including 45 species that were quantified from boreal forest fires for the first time. After CO2, CO and CH4, the largest emission factors (EFs) for individual species were formaldehyde (2.1 ± 0.2 g kg−1), followed by methanol, NO2, HCN, ethene, α-pinene, β-pinene, ethane, benzene, propene, acetone and CH3CN. Globally, we estimate that boreal forest fires release 2.4 ± 0.6 Tg C yr−1 in the form of NMVOCs, with approximately 41 % of the carbon released as C1-C2 NMVOCs and 21 % as pinenes. These are the first reported field measurements of monoterpene emissions from boreal forest fires, and we speculate that the pinenes, which are relatively heavy molecules, were detected in the fire plumes as the result of distillation of stored terpenes as the vegetation is heated. Their inclusion in smoke chemistry models is expected to improve model predictions of secondary organic aerosol (SOA) formation. The fire-averaged EF of dichloromethane or CH2Cl2, (6.9 ± 8.6) × 10−4 g kg−1, was not significantly different from zero and supports recent findings that its global biomass burning source appears to have been overestimated. Similarly, we found no evidence for emissions of chloroform (CHCl3) or methyl chloroform (CH3CCl3) from boreal forest fires. The speciated hydrocarbon measurements presented here show the importance of carbon released by short-chain NMVOCs, the strong contribution of pinene emissions from boreal forest fires, and the wide range of compound classes in the most abundantly emitted NMVOCs, all of which can be used to improve biomass burning inventories in local/global models and reduce uncertainties in model estimates of trace gas emissions and their impact on the atmosphere.

Isocyanic acid in the atmosphere and its possible link to smoke-related health effects.

Abstract: We measured isocyanic acid (HNCO) in laboratory biomass fires at levels up to 600 parts per billion by volume (ppbv), demonstrating that it has a significant source from pyrolysis/combustion of biomass. We also measured HNCO at mixing ratios up to 200 pptv (parts-per-trillion by volume) in ambient air in urban Los Angeles, CA, and in Boulder, CO, during the recent 2010 Fourmile Canyon fire. Further, our measurements of aqueous solubility show that HNCO is highly soluble, as it dissociates at physiological pH. Exposure levels > 1 ppbv provide a direct source of isocyanic acid and cyanate ion (NCO-) to humans at levels that have recognized health effects: atherosclerosis, cataracts, and rheumatoid arthritis, through the mechanism of protein carbamylation. In addition to the wildland fire and urban sources, we observed HNCO in tobacco smoke, HNCO has been reported from the low-temperature combustion of coal, and as a by-product of urea-selective catalytic reduction (SCR) systems that are being phased-in to control on-road diesel NOx emissions in the United States and the European Union. Given the current levels of exposure in populations that burn biomass or use tobacco, the expected growth in biomass burning emissions with warmer, drier regional climates, and planned increase in diesel SCR controls, it is imperative that we understand the extent and effects of this HNCO exposure.

Trace gas and particle emissions from open biomass burning in Mexico

Abstract: We report airborne measurements of emission fac- tors (EF) for trace gases and PM2.5 made in southern Mexico in March of 2006 on 6 crop residue fires, 3 tropical dry forest fires, 8 savanna fires, 1 garbage fire, and 7 mountain pine-oak forest fires. The savanna fire EF were measured early in the local dry season and when compared to EF measured late in the African dry season they were at least 1.7 times larger for NOx, NH3, H2, and most non-methane organic compounds. Our measurements suggest that urban deposition and high windspeed may also be associated with significantly elevated NOx EF. When considering all fires sampled, the percentage of particles containing soot increased from 15 to 60 % as the modified combustion efficiency increased from 0.88 to 0.98. We estimate that about 175 Tg of fuel was consumed by open burning of biomass and garbage and as biofuel (mainly wood cooking fires) in Mexico in 2006. Combining the fuel con- sumption estimates with our EF measurements suggests that the above combustion sources account for a large fraction of the reactive trace gases and more than 90 % of the total pri- mary, fine carbonaceous particles emitted by all combustion sources in Mexico.

Airborne and ground-based measurements of the trace gases and particles emitted by prescribed fires in the United States

Abstract: . We have measured emission factors for 19 trace gas species and particulate matter (PM2.5) from 14 prescribed fires in chaparral and oak savanna in the southwestern US, as well as conifer forest understory in the southeastern US and Sierra Nevada mountains of California. These are likely the most extensive emission factor field measurements for temperate biomass burning to date and the only published emission factors for temperate oak savanna fuels. This study helps to close the gap in emissions data available for temperate zone fires relative to tropical biomass burning. We present the first field measurements of the biomass burning emissions of glycolaldehyde, a possible precursor for aqueous phase secondary organic aerosol formation. We also measured the emissions of phenol, another aqueous phase secondary organic aerosol precursor. Our data confirm previous observations that urban deposition can impact the NOx emission factors and thus subsequent plume chemistry. For two fires, we measured both the emissions in the convective smoke plume from our airborne platform and the unlofted residual smoldering combustion emissions with our ground-based platform. The smoke from residual smoldering combustion was characterized by emission factors for hydrocarbon and oxygenated organic species that were up to ten times higher than in the lofted plume, including high 1,3-butadiene and isoprene concentrations which were not observed in the lofted plume. This should be considered in modeling the air quality impacts for smoke that disperses at ground level. We also show that the often ignored unlofted emissions can significantly impact estimates of total emissions. Preliminary evidence suggests large emissions of monoterpenes in the residual smoldering smoke. These data should lead to an improved capacity to model the impacts of biomass burning in similar temperate ecosystems.

Case study of water-soluble metal containing organic constituents of biomass burning aerosol

Abstract: Natural and prescribed biomass fires are a major source of aerosols that may persist in the atmosphere for several weeks. Biomass burning aerosols (BBA) can be associated with long-range transport of water-soluble N-, S-, P-, and metal-containing species. In this study, BBA samples were collected using a particle-into-liquid sampler (PILS) from laboratory burns of vegetation collected on military bases in the southeastern and southwestern United States. The samples were then analyzed using high resolution electrospray ionization mass spectrometry (ESI/HR-MS) that enabled accurate mass measurements for hundreds of species with m/z values between 70 and 1000 and assignment of elemental formulas. Mg, Al, Ca, Cr, Mn, Fe, Ni, Cu, Zn, and Ba-containing organometallic species were identified. The results suggest that the biomass may have accumulated metal-containing species that were re-emitted during biomass burning. Further research into the sources, dispersion, and persistence of metal-containing aerosols, as...