2,269 research outputs found

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

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    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-offlight 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 onedimensional gas chromatography-mass spectrometry (GCMS) 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

    A dual‐chamber method for quantifying the effects of atmospheric perturbations on secondary organic aerosol formation from biomass burning emissions

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    Biomass burning (BB) is a major source of atmospheric pollutants. Field and laboratory studies indicate that secondary organic aerosol (SOA) formation from BB emissions is highly variable. We investigated sources of this variability using a novel dual-smog-chamber method that directly compares the SOA formation from the same BB emissions under two different atmospheric conditions. During each experiment, we filled two identical Teflon smog chambers simultaneously with BB emissions from the same fire. We then perturbed the smoke with UV lights, UV lights plus nitrous acid (HONO), or dark ozone in one or both chambers. These perturbations caused SOA formation in nearly every experiment with an average organic aerosol (OA) mass enhancement ratio of 1.78 ± 0.91 (mean ± 1σ). However, the effects of the perturbations were highly variable ranging with OA mass enhancement ratios ranging from 0.7 (30% loss of OA mass) to 4.4 across the set of perturbation experiments. There was no apparent relationship between OA enhancement and perturbation type, fuel type, and modified combustion efficiency. To better isolate the effects of different perturbations, we report dual-chamber enhancement (DUCE), which is the quantity of the effects of a perturbation relative to a reference condition. DUCE values were also highly variable, even for the same perturbation and fuel type. Gas measurements indicate substantial burn-to-burn variability in the magnitude and composition of SOA precursor emissions, even in repeated burns of the same fuel under nominally identical conditions. Therefore, the effects of different atmospheric perturbations on SOA formation from BB emissions appear to be less important than burn-to-burn variability

    Fine-scale simulation of ammonium and nitrate over the South Coast Air Basin and San Joaquin Valley of California during CalNex-2010

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    National ambient air quality standards (NAAQS) have been set for PM_2.5 due to its association with adverse health effects. PM_2.5 design values in the South Coast Air Basin (SoCAB) and San Joaquin Valley of California exceed NAAQS levels, and NH^(+)_(4) and NO^(-)_(3) make up the largest fraction of total PM2.5 mass on polluted days. Here we evaluate fine-scale simulations of PM_(2.5) NH^(+)_(4) and NO^(-)_(3) with the Community Multiscale Air Quality model using measurements from routine networks and the California Research at the Nexus of Air Quality and Climate Change 2010 campaign. The model correctly simulates broad spatial patterns of NH^(+)_(4) and NO^(-)_(3) including the elevated concentrations in eastern SoCAB. However, areas for model improvement have been identified. NH_3 emissions from livestock and dairy facilities appear to be too low, while those related to waste disposal in western SoCAB may be too high. Analyses using measurements from flights over SoCAB suggest that problems with NH3 predictions can influence NO^(-)_(3) predictions there. Offline ISORROPIA II calculations suggest that overpredictions of NH_x in Pasadena cause excessive partitioning of total nitrate to the particle phase overnight, while underpredictions of Na^+ cause too much partitioning to the gas phase during the day. Also, the model seems to underestimate mixing during the evening boundary layer transition leading to excessive nitrate formation on some nights. Overall, the analyses demonstrate fine-scale variations in model performance within and across the air basins. Improvements in inventories and spatial allocations of NH_3 emissions and in parameterizations of sea spray emissions, evening mixing processes, and heterogeneous ClNO_2 chemistry could improve model performance

    Emissions of nitrogen-containing organic compounds from the burning of herbaceous and arboraceous biomass: Fuel composition dependence and the variability of commonly used nitrile tracers

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    Volatile organic compounds (VOCs) emitted from residential wood and crop residue burning were measured in Colorado, U.S. When compared to the emissions from crop burning, residential wood burning exhibited markedly lower concentrations of acetonitrile, a commonly used biomass burning tracer. For both herbaceous and arboraceous fuels, the emissions of nitrogen-containing VOCs (NVOCs) strongly depend on the fuel nitrogen content; therefore, low NVOC emissions from residential wood burning result from the combustion of low-nitrogen fuel. Consequently, the emissions of compounds hazardous to human health, such as HNCO and HCN, and the formation of secondary pollutants, such as ozone generated by NOx, are likely to depend on fuel nitrogen. These results also demonstrate that acetonitrile may not be a suitable tracer for domestic burning in urban areas. Wood burning emissions may be best identified through analysis of the emissions profile rather than reliance on a single tracer species
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