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  • 1
    Publication Date: 2019-08-09
    Description: We report enhancements of glyoxal relative to carbon monoxide and formaldehyde from biomass burning plumes intercepted from the NOAA WP-3D aircraft during the 2013 Southeast Nexus and 2015 Shale Oil and Natural Gas Nexus field campaigns. The intercepted biomass burning plumes were from small agricultural fires. Since the plume ages were not known, these values are normalized excess mixing ratios, instead of the more common emission ratio, which is used only for fresh emissions. Glyoxal was measured using broadband cavity enhanced spectroscopy, which provides a sensitive and highly selective measurement of glyoxal. Emissions of other species such as methane, formaldehyde, and nitrous acid agreed with previous laboratory and field measurements, but the glyoxal emissions relative to CO were on average a factor of 4 lower than previously reported. Several glyoxal loss processes such as aerosol uptake were examined to determine if they could affect the observed glyoxal concentrations, but they were insufficient to explain the lower measured values of glyoxal relative to other biomass burning trace gases, indicating that glyoxal emissions from biomass burning may be significantly overestimated.
    Keywords: Environment Pollution
    Type: NF1676L-27262 , GSFC-E-DAA-TN47723 , Environmental Science and Technology (ISSN 0013-936X) (e-ISSN 1520-5851); 51; 20; 11761-11770
    Format: application/pdf
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  • 2
    Publication Date: 2017-01-02
    Description: Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20–30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C=C bonds (e.g., terpenes) to form SOA, but won’t react appreciably with many of their oxidation products or any species in the gas phase that lacks a C=C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C=C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C=C bonds. O3 and NO3 oxidation produced SOA with elemental O:C and H:C similar to the least oxidized OA observed in local ambient air, and neither oxidant led to net mass loss at the highest exposures, in contrast with OH oxidation. An OH exposure in the OFR equivalent to several hours of atmospheric aging also produced SOA with O:C and H:C values similar to ambient OA, while higher aging (days–weeks) led to formation of SOA with progressively higher O:C and lower H:C (and net mass loss at the highest exposures). NO3 oxidation led to the production of particulate organic nitrates (pRONO2), while OH and O3 oxidation (under low NO) did not, as expected. These measurements of SOA formation provide the first direct comparison of SOA formation potential and chemical evolution from OH, O3 and NO3 oxidation in the real atmosphere, and help to clarify the oxidation processes that lead to SOA formation from biogenic hydrocarbons.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 3
    Publication Date: 2018-06-13
    Description: We report the emissions of glyoxal and methylglyoxal from the open burning of biomass during the NOAA-led 2016 FIREX intensive at the Fire Sciences Laboratory in Missoula, MT. Both compounds were measured using cavity enhanced spectroscopy, which is both more sensitive and more selective than methods previously used to determine emissions of these two compounds. A total of 75 burns were conducted, using 33 different fuels in 8 different categories, providing a far more comprehensive dataset for emissions than was previously available. Measurements of methylglyoxal using our instrument suffer from spectral interferences from several other species, but methylglyoxal emissions could be constrained within roughly a factor of 2. Methylglyoxal emissions were 2–3 times higher than glyoxal emissions on a molar basis, in contrast to previous studies that report methylglyoxal emissions lower than glyoxal emissions. Methylglyoxal emission ratios for all fuels averaged 3.6±2.4ppbv methylglyoxal/ppmv CO, while emission factors averaged 0.66±0.50g methylglyoxal/kg fuel burned. Primary emissions of glyoxal from biomass burning were much lower than previous laboratory measurements, but consistent with recent measurements from aircraft. Glyoxal emission ratios for all fuels averaged 1.4±0.7ppbv glyoxal/ppmv CO, while emission factors averaged 0.20±0.12g glyoxal/kg fuel burned, values that are at least a factor of 4 lower than assumed in previous estimates of the global glyoxal budget. While there was significant variability in the glyoxal emission ratios and factors between the different fuel groups, glyoxal and formaldehyde were highly correlated during the course of any given fire, and the ratio of glyoxal to formaldehyde, RGF, was consistent across many different fuel types, with an average value of 0.068±0.018. While RGF values for fresh emissions were consistent across many fuel types, further work is required to determine how this value changes as the emissions age.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 4
    Publication Date: 2017-10-17
    Description: Volatile and intermediate-volatility non-methane organic gases (NMOGs) released from biomass burning were measured during laboratory-simulated wildfires by proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF). We identified NMOG contributors to more than 150 PTR ion masses using gas chromatography (GC) pre-separation with electron ionization, H3O+ chemical ionization, and NO+ chemical ionziation, an extensive literature review, and time-series correlation, providing higher certainty for ion identifications than has been previously available. Our interpretation of the PTR-ToF mass spectrum accounts for nearly 90 % of NMOG mass detected by PTR-ToF across all fuel types. The relative contributions of different NMOGs to individual exact ion masses are mostly similar across many fires and fuel types. The PTR-ToF measurements are compared to corresponding measurements from open-path Fourier transform infrared spectroscopy (OP-FTIR), broadband cavity enhanced spectroscopy (ACES), and iodide ion chemical ionization mass spectrometry (I-CIMS) where possible. The majority of comparisons have slopes near 1 and values of the linear correlation coefficient, R2, of 〉 0.8, including compounds that are not frequently reported by PTR-MS such as ammonia, hydrogen cyanide (HCN), nitrous acid (HONO), and propene. The exceptions include methylglyoxal and compounds that are known to be difficult to measure with one or more of the deployed instruments. The fire-integrated emission ratios to CO and emission factors of NMOGs from 18 fuel types are provided. Finally, we provide an overview of the chemical characteristics of detected species. Non-aromatic oxygenated compounds are the most abundant. Furans and aromatics, while less abundant, comprise a large portion of the OH reactivity. The OH reactivity, its major contributors, and the volatility distribution of emissions can change considerably over the course of a fire.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 5
    Publication Date: 2016-12-20
    Description: The sum of all reactive nitrogen species (NOy) includes NOx (NO2 + NO) and all of its oxidized forms, and the accurate detection of NOy is critical to understanding atmospheric nitrogen chemistry. Thermal dissociation (TD) inlets, which convert NOy to NO2 followed by NO2 detection, are frequently used in conjunction with techniques such as laser induced fluorescence (LIF) and cavity ringdown spectroscopy (CRDS) to measure total NOy when set at 〉 600 °C, or speciated NOy when set at intermediate temperatures. We report the conversion efficiency of known amounts of several representative NOy species to NO2 in our TD-CRDS instrument, under a variety of experimental conditions. We find that the conversion efficiency of HNO3 is highly sensitive to the flow rate and the residence time through the TD inlet, as well as the presence of other species that may be present during ambient sampling, such as ozone (O3). Conversion of HNO3 at 400 °C, nominally the set point used to selectively convert organic nitrates, can range from 2–6 % and may represent an interference in measurement of organic nitrates under some conditions. The conversion efficiency is strongly dependent on the operating characteristics of individual quartz ovens, and should be well calibrated prior to use in field sampling. We demonstrate quantitative conversion of both gas phase N2O5 and particulate ammonium nitrate in the TD inlet at 650 °C, the temperature normally used for conversion of HNO3. N2O5 has two thermal dissociation steps, one at low temperature representing dissociation to NO2 and NO3, and one at high temperature representing dissociation of NO3, which produces exclusively NO2 and not NO. We also find a significant interference from partial conversion (5–10 %) of NH3 to NO at 650 °C in the presence of representative (50 ppbv) levels of O3 in dry zero air. Although this interference appears to be suppressed when sampling ambient air, we nevertheless recommend regular characterization of this interference using standard additions of NH3 to TD instruments that convert reactive nitrogen to NO or NO2.
    Electronic ISSN: 1867-8610
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 6
    Publication Date: 2017-05-31
    Description: The sum of all reactive nitrogen species (NOy) includes NOx (NO2+NO) and all of its oxidized forms, and the accurate detection of NOy is critical to understanding atmospheric nitrogen chemistry. Thermal dissociation (TD) inlets, which convert NOy to NO2 followed by NO2 detection, are frequently used in conjunction with techniques such as laser-induced fluorescence (LIF) and cavity ring-down spectroscopy (CRDS) to measure total NOy when set at 〉600°C or speciated NOy when set at intermediate temperatures. We report the conversion efficiency of known amounts of several representative NOy species to NO2 in our TD-CRDS instrument, under a variety of experimental conditions. We find that the conversion efficiency of HNO3 is highly sensitive to the flow rate and the residence time through the TD inlet as well as the presence of other species that may be present during ambient sampling, such as ozone (O3). Conversion of HNO3 at 400°C, nominally the set point used to selectively convert organic nitrates, can range from 2 to 6% and may represent an interference in measurement of organic nitrates under some conditions. The conversion efficiency is strongly dependent on the operating characteristics of individual quartz ovens and should be well calibrated prior to use in field sampling. We demonstrate quantitative conversion of both gas-phase N2O5 and particulate ammonium nitrate in the TD inlet at 650°C, which is the temperature normally used for conversion of HNO3. N2O5 has two thermal dissociation steps, one at low temperature representing dissociation to NO2 and NO3 and one at high temperature representing dissociation of NO3, which produces exclusively NO2 and not NO. We also find a significant interference from partial conversion (5–10%) of NH3 to NO at 650°C in the presence of representative (50ppbv) levels of O3 in dry zero air. Although this interference appears to be suppressed when sampling ambient air, we nevertheless recommend regular characterization of this interference using standard additions of NH3 to TD instruments that convert reactive nitrogen to NO or NO2.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 7
    Publication Date: 2018-10-26
    Description: We report the emissions of glyoxal and methylglyoxal from the open burning of biomass during the NOAA-led 2016 FIREX intensive at the Fire Sciences Laboratory in Missoula, MT. Both compounds were measured using cavity-enhanced spectroscopy, which is both more sensitive and more selective than methods previously used to determine emissions of these two compounds. A total of 75 burns were conducted, using 33 different fuels in 8 different categories, providing a far more comprehensive dataset for emissions than was previously available. Measurements of methylglyoxal using our instrument suffer from spectral interferences from several other species, and the values reported here are likely underestimates, possibly by as much as 70%. Methylglyoxal emissions were 2–3 times higher than glyoxal emissions on a molar basis, in contrast to previous studies that report methylglyoxal emissions lower than glyoxal emissions. Methylglyoxal emission ratios for all fuels averaged 3.6±2.4ppbv methylglyoxal(ppmv CO)−1, while emission factors averaged 0.66±0.50g methylglyoxal(kg fuel burned)−1. Primary emissions of glyoxal from biomass burning were much lower than previous laboratory measurements but consistent with recent measurements from aircraft. Glyoxal emission ratios for all fuels averaged 1.4±0.7ppbv glyoxal(ppmv CO)−1, while emission factors averaged 0.20±0.12g glyoxal(kg fuel burned)−1, values that are at least a factor of 4 lower than assumed in previous estimates of the global glyoxal budget. While there was significant variability in the glyoxal emission ratios and factors between the different fuel groups, glyoxal and formaldehyde were highly correlated during the course of any given fire, and the ratio of glyoxal to formaldehyde, RGF, was consistent across many different fuel types, with an average value of 0.068±0.018. While RGF values for fresh emissions were consistent across many fuel types, further work is required to determine how this value changes as the emissions age.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 8
    Publication Date: 2019-07-10
    Description: New techniques have recently been developed to capture reactive nitrogen species for accurate measurement of their isotopic composition. Reactive nitrogen species play important roles in atmospheric oxidation capacity (hydroxyl radical and ozone formation) and may have impacts on air quality and climate. Tracking reactive nitrogen species and their chemistry in the atmosphere based upon concentration alone is challenging. Isotopic analysis provides a potential tool for tracking the sources and chemistry of species such as nitrogen oxides (NOx = NO + NO2), nitrous acid (HONO), nitric acid (HNO3) and particulate nitrate (NO3−(p)). Here we study direct biomass burning (BB) emissions during the
 Fire Influence on Regional to Global Environments Experiment (FIREX, later evolved into FIREX-AQ) laboratory experiments at the Missoula Fire Laboratory in the fall of 2016. An annular denuder system (ADS) developed to efficiently collect HONO for isotopic composition analysis was deployed to the Fire Lab study. Concentrations of HONO recovered from the ADS collection agree well with mean concentrations averaged over each fire measured by 4 other high time resolution techniques, including mist chamber/ion chromatography (MC/IC), open-path Fourier transform infrared spectroscopy (OP-FTIR), cavity enhanced spectroscopy (CES), proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF). The concentration validation ensures complete collection of BB emitted HONO, of which the isotopic composition is preserved during the collection process. In addition, the isotopic composition of NOx and NO3−(p) from direct BB emissions were also characterized. In 20 stack fires (direct emission within ~ 5 seconds of production by the fire) that burned various biomass materials, δ15N-NOx ranges from −4.3 ‰ to +7.0 ‰, falling near the middle of the range reported in previous work. The first measurements of δ15N-HONO and δ18O-HONO in biomass burning smoke reveal a range of −5.3 – +5.8 ‰ and +5.2 – +15.2 ‰ respectively. Both HONO and NOx are sourced from N in the biomass fuel and δ15N-HONO and δ15N-NOx are strongly correlated (R2 = 0.89, p 
    Electronic ISSN: 1867-8610
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 9
    Publication Date: 2018-05-14
    Description: The chemical composition of aerosol particles is a key aspect in determining their impact on the environment. For example, nitrogen-containing particles impact atmospheric chemistry, air quality, and ecological N deposition. Instruments that measure total reactive nitrogen (Nr = all nitrogen compounds except for N2 and N2O) focus on gas-phase nitrogen and very few studies directly discuss the instrument capacity to measure the mass of Nr-containing particles. Here, we investigate the mass quantification of particle-bound nitrogen using a custom Nr system that involves total conversion to nitric oxide (NO) across platinum and molybdenum catalysts followed by NO−O3 chemiluminescence detection. We evaluate the particle conversion of the Nr instrument by comparing to mass-derived concentrations of size-selected and counted ammonium sulfate ((NH4)2SO4), ammonium nitrate (NH4NO3), ammonium chloride (NH4Cl), sodium nitrate (NaNO3), and ammonium oxalate ((NH4)2C2O4) particles determined using instruments that measure particle number and size. These measurements demonstrate Nr-particle conversion across the Nr catalysts that is independent of particle size with 98 ± 10 % efficiency for 100–600 nm particle diameters. We also show efficient conversion of particle-phase organic carbon species to CO2 across the instrument's platinum catalyst followed by a nondispersive infrared (NDIR) CO2 detector. However, the application of this method to the atmosphere presents a challenge due to the small signal above background at high ambient levels of common gas-phase carbon compounds (e.g., CO2). We show the Nr system is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation using single-component, laboratory-generated, Nr-containing particles below 2.5 µm in size. In addition we show agreement with mass measurements of an independently calibrated online particle-into-liquid sampler directly coupled to the electrospray ionization source of a quadrupole mass spectrometer (PILS–ESI/MS) sampling in the negative-ion mode. We obtain excellent correlations (R2 = 0.99) of particle mass measured as Nr with PILS–ESI/MS measurements converted to the corresponding particle anion mass (e.g., nitrate, sulfate, and chloride). The Nr and PILS–ESI/MS are shown to agree to within ∼ 6 % for particle mass loadings of up to 120 µg m−3. Consideration of all the sources of error in the PILS–ESI/MS technique yields an overall uncertainty of ±20 % for these single-component particle streams. These results demonstrate the Nr system is a reliable direct particle mass measurement technique that differs from other particle instrument calibration techniques that rely on knowledge of particle size, shape, density, and refractive index.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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  • 10
    Publication Date: 2018-07-03
    Description: Biomass burning is a large source of volatile organic compounds (VOCs) and many other trace species to the atmosphere, which can act as precursors to secondary pollutants such as ozone and fine particles. Measurements performed with a proton-transfer-reaction time-of-flight mass spectrometer during the FIREX 2016 laboratory intensive were analyzed with positive matrix factorization (PMF), in order to understand the instantaneous variability in VOC emissions from biomass burning, and to simplify the description of these types of emissions. Despite the complexity and variability of emissions, we found that a solution including just two emission profiles, which are mass spectral representations of the relative abundances of emitted VOCs, explained on average 85% of the VOC emissions across various fuels representative of the western US (including various coniferous and chaparral fuels). In addition, the profiles were remarkably similar across almost all of the fuel types tested. For example, the correlation coefficient r2 of each profile between ponderosa pine (coniferous tree) and manzanita (chaparral) is higher than 0.84. The compositional differences between the two VOC profiles appear to be related to differences in pyrolysis processes of fuel biopolymers at high and low temperatures. These pyrolysis processes are thought to be the main source of VOC emissions. “High-temperature” and “low-temperature” pyrolysis processes do not correspond exactly to the commonly used “flaming” and “smoldering” categories as described by modified combustion efficiency (MCE). The average atmospheric properties (e.g., OH reactivity, volatility, etc) of the high- and low-temperature profiles are significantly different. We also found that the two VOC profiles can describe previously reported VOC data for laboratory and field burns.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union (EGU).
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