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  • 1
    Publication Date: 2017-01-04
    Description: Author Posting. © The Author(s), 2011. This is the author's version of the work. It is posted here by permission of National Academy of Sciences for personal use, not for redistribution. The definitive version was published in Proceedings of the National Academy of Sciences of the United States of America (2012), doi:10.1073/pnas.1110564109.
    Description: Detailed airborne, surface, and subsurface chemical measurements, primarily obtained in May and June 2010, are used to quantify initial hydrocarbon compositions along different transport pathways – in deep subsurface plumes, in the initial surface slick, and in the atmosphere – during the Deepwater Horizon (DWH) oil spill. Atmospheric measurements are consistent with a limited area of surfacing oil, with implications for leaked hydrocarbon mass transport and oil drop size distributions. The chemical data further suggest relatively little variation in leaking hydrocarbon composition over time. While readily soluble hydrocarbons made up ~25% of the leaking mixture by mass, subsurface chemical data show these compounds made up ~69% of the deep plume mass; only ~31% of deep plume mass was initially transported in the form of trapped oil droplets. Mass flows along individual transport pathways are also derived from atmospheric and subsurface chemical data. Subsurface hydrocarbon composition, dissolved oxygen, and dispersant data are used to provide a new assessment of release of hydrocarbons from the leaking well. We use the chemical measurements to estimate that (7.8±1.9) x106 kg of hydrocarbons leaked on June 10, 2010, directly accounting for roughly three-quarters of the total leaked mass on that day. The average environmental release rate of (10.1 ± 2.0) x106 kg/day derived using atmospheric and subsurface chemical data agrees within uncertainties with the official average leak rate of (10.2 ± 1.0) x106 kg/day derived using physical and optical methods.
    Description: This research was supported by the National Science Foundation through grants to D. Blake (AGS-1049952), J. Kessler (OCE-1042650 and OCE-0849246), D. Valentine (OCE-1042097 and OCE-0961725), E. Kujawinski (OCE-1045811), and R. Camilli (OCE-1043976), by U.S. Coast Guard contract to R. Camilli (Contract HSCG3210CR0020), and by U.S. Department of Energy grant to D. Valentine (DE- NT0005667). The August, September, and October research cruises were funded by NOAA through a contract with Consolidated Safety Services, Incorporated. The NOAA P-3 oil spill survey flights were funded in part by NOAA and in part by a U.S. Coast Guard Pollution Removal Funding Authorization to NOAA.
    Repository Name: Woods Hole Open Access Server
    Type: Preprint
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  • 2
    Publication Date: 2019-07-13
    Description: Wildfires emit significant amounts of pollutants that degrade air quality. Plumes from three wildfires in the western U.S. were measured from aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Biomass Burning Observation Project (BBOP), both in summer 2013. This study reports an extensive set of emission factors (EFs) for over 80 gases and 5 components of submicron particulate matter (PM1) from these temperate wildfires. These include rarely, or never before, measured oxygenated volatile organic compounds and multifunctional organic nitrates. The observed EFs are compared with previous measurements of temperate wildfires, boreal forest fires, and temperate prescribed fires. The wildfires emitted high amounts of PM1 (with organic aerosol (OA) dominating the mass) with an average EF that is more than 2 times the EFs for prescribed fires. The measured EFs were used to estimate the annual wildfire emissions of carbon monoxide, nitrogen oxides, total non methane organic compounds, and PM1 from 11 western U.S. states. The estimated gas emissions are generally comparable with the 2011 National Emissions Inventory (NEI). However, our PM1 emission estimate (1530 +/- 570 Gg/yr) is over 3 times that of the NEI PM2.5 estimate and is also higher than the PM2.5 emitted from all other sources in these states in the NEI. This study indicates that the source of OA from biomass burning in the western states is significantly underestimated. In addition, our results indicate that prescribed burning may be an effective method to reduce fine particle emissions.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN44715 , Journal of Geophysical Research (ISSN 2169-897X); 122; 11; 6108-6129
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  • 3
    Publication Date: 2019-07-13
    Description: Widespread efforts to abate ozone (O3) smog have significantly reduced emissions of nitrogen oxides (NOx) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NOx emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (International Consortium for Atmospheric Research on Transport and Transformation - July-August 2004), SENEX (Southeast Nexus - June-July 2013), and SEAC4RS (Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys - August-September 2013) and long-term ground measurement networks alongside a global chemistry-climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NO (sub y)) in both 2004 and 2013. Among the major RON species, nitric acid (HNO3) is dominant (approximately 42-45 percent), followed by NOx (31 percent), total peroxy nitrates (Sigma PNs; 14 percent), and total alkyl nitrates (Sigma ANs; 9-12 percent) on a regional scale. We find that most RON species, including NOx, Sigma PNs, and HNO3, decline proportionally with decreasing NOx emissions in this region, leading to a similar decline in NO (sub y). This linear response might be in part due to the nearly constant summertime supply of biogenic VOC (Volatile Organic Compounds) emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NOx emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN55277 , Atmospheric Chemistry and Physics (e-ISSN 1680-7324); 18; 3; 2341-2361
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  • 4
    Publication Date: 2019-07-13
    Description: Isoprene oxidation schemes vary greatly among gas-phase chemical mechanisms, with potentially significant ramifications for air quality modeling and interpretation of satellite observations in biogenic-rich regions. In this study, in situ observations from the 2013 SENEX mission are combined with a constrained O-D photochemical box model to evaluate isoprene chemistry among five commonly used gas-phase chemical mechanisms: CBO5, CB6r2, MCMv3.2, MCMv3.3.1, and a recent version of GEOS-Chem. Mechanisms are evaluated and inter-compared with respect to formaldehyde (HCHO), a high-yield product of isoprene oxidation. Though underestimated by all considered mechanisms, observed HCHO mixing ratios are best reproduced by MCMv3.3.1 (normalized mean bias = -15%), followed by GEOS-Chem (-17%), MCMv3.2 (-25%), CB6r2 (-32%) and CB05 (-33%). Inter-comparison of HCHO production rates reveals that major restructuring of the isoprene oxidation scheme in the Carbon Bond mechanism increases HCHO production by only approx. 5% in CB6r2 relative to CBO5, while further refinement of the complex isoprene scheme in the Master Chemical Mechanism increases HCHO production by approx. 16% in MCMv3.3.1 relative to MCMv3.2. The GEOS-Chem mechanism provides a good approximation of the explicit isoprene chemistry in MCMv3.3.1 and generally reproduces the magnitude and source distribution of HCHO production rates. We analytically derive improvements to the isoprene scheme in CB6r2 and incorporate these changes into a new mechanism called CB6r2-UMD, which is designed to preserve computational efficiency. The CB6r2-UMD mechanism mimics production of HCHO in MCMv3.3.1 and demonstrates good agreement with observed mixing ratios from SENEX (-14%). Improved simulation of HCHO also impacts modeled ozone: at approx. 0.3 ppb NO, the ozone production rate increases approx. 3% between CB6r2 and CB6r2-UMD, and rises another approx. 4% when HCHO is constrained to match observations.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN47241 , Atmospheric Environment (ISSN 1352-2310); 164; 325-336
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  • 5
    Publication Date: 2019-07-13
    Description: VOCs (Volatile Organic Compounds) related to oil and gas extraction operations in the United States were measured by H3O (sup plus) chemical ionization time-of-flight mass spectrometry (H3O (sup plus) ToFCIMS/PTR-ToF-MS (Time of Flight Chemical Ionization Mass Spectrometry/Proton Transfer Reaction-Time of Flight-Mass Spectroscopy) from aircraft during the Shale Oil and Natural Gas Nexus (SONGNEX) campaign in March-April 2015. This work presents an overview of major VOC species measured in nine oil- and gas-producing regions, and a more detailed analysis of H3O (sup plus) ToF-CIMS measurements in the Permian Basin within Texas and New Mexico. Mass spectra are dominated by small photochemically produced oxygenates and compounds typically found in crude oil: aromatics, cyclic alkanes, and alkanes. Mixing ratios of aromatics were frequently as high as those measured downwind of large urban areas. In the Permian, the H3O (sup plus) ToF-CIMS measured a number of underexplored or previously unreported species, including aromatic and cycloalkane oxidation products, nitrogen heterocycles including pyrrole (C4H5N) and pyrroline (C4H7N), H2S, and a diamondoid (adamantane) or unusual monoterpene. We additionally assess the specificity of a number of ion masses resulting from H3O (sup plus) ion chemistry previously reported in the literature, including several new or alternate interpretations.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN47232 , Atmospheric Measurement Techniques (e-ISSN 1867-8548); 10; 8; 2941-2968
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  • 6
    Publication Date: 2019-07-13
    Description: One major goal for the NASA Atmospheric Tomography Mission (ATom) is producing an observation-based chemical climatology to represent the atmospheric heterogeneity. In this study, we use CO and O3 observations and global atmospheric model simulations to examine the spatial representativeness of the ATom-1 and -2 transects within a 4D framework provided by the NASA GEOS-5 and GMI-CTM models. Based on the probability density functions, we find that the variability of CO and O3 along the flight tracks is well hindcast by the model when sampled per ATom flights. The CO variations along the ATom-transect are likely representative of the typical CO variations over the whole Pacific basin during both the ATom-1 and -2 periods, the northern Atlantic during the ATom-1 period, and the tropical Atlantic in the ATom-2 period. Over southern Atlantic, CO along the ATom-1 transects is likely less well mixed than that of the broader region, but is still representative of the median CO concentration. CO along the ATom-2 transect is likely higher than the median CO concentration over this region. For O3, the agreements between PDFs of O3 sampled along the ATom transects and over the broader regions are fair to good over all six regions (Scores 〉 0.65) with notable discrepancies over some regions. For example, in ATom-1 over the northern Pacific and Atlantic, the transect samples air masses with higher O3 levels. During ATom-2, the transect over-represents the occurrence of O3 plumes over tropical Pacific. Over the southern Pacific and Atlantic for both ATom-1 and -2, the transects have a less uniform distribution compared to the surrounding basins, but still represent the median O3 abundance. Overall, we conclude in most cases that ATom measurements represent the statistical variations of these two species over the ocean basins at the time of measurement. Higher-order statistics, including covariance of species, has not been tested in this study.
    Keywords: Geophysics
    Type: GSFC-E-DAA-TN67698 , 2018 ATom Science Team Meeting; 13-15 Nov. 2018; Boulder, CO; United States
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  • 7
    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
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  • 8
    Publication Date: 2019-10-05
    Description: Recent studies suggest overestimates in current U.S. emission inventories of nitrogen oxides (NOx=NO+NO2). Here, we expand a previously developed Fuel-based Inventory of motor-Vehicle Emissions (FIVE) to the continental U.S. for the year 2013, and evaluate our estimates of mobile source emissions with the U.S. Environmental Protection Agency's National Emissions Inventory (NEI) interpolated to 2013. We find that mobile source emissions of NOx and carbon monoxide (CO) in the NEI are higher than FIVE by 28% and 90%, respectively. Using a chemical transport model, we model mobile source emissions from FIVE, and find consistent levels of urban NOx and CO as measured during the Southeast Nexus (SENEX) Study in 2013. Lastly, we assess the sensitivity of ozone (O3) over the Eastern U.S. to uncertainties in mobile source NOx emissions and biogenic volatile organic compound (VOC) emissions. The ground-level O3 is sensitive to reductions in mobile source NOx emissions, most notably in the Southeastern U.S. and during O3 exceedance events, under the revised standard proposed in 2015 (〉70 ppb, 8-hr maximum). This suggests that decreasing mobile source NOx emissions could help in meeting more stringent O3 standards in the future.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN61544 , Environmental Science and Technology (ISSN 0013-936X) (e-ISSN 1520-5851); 52; 13; 7360–7370
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  • 9
    Publication Date: 2019-11-30
    Description: Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.
    Keywords: Environment Pollution
    Type: GSFC-E-DAA-TN51584 , Atmospheric Chemistry and Physics (ISSN 1680-7316) (e-ISSN 1680-7324); 16; 21; 13561-13577
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  • 10
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