Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>

Atmospheric radiocarbon (<sup>14</sup>C) represents an important observational constraint on emissions of fossil-fuel derived carbon into the atmosphere due to the absence of <sup>14</sup>C in fossil fuel reservoirs. The high sensitivity and precision that accelerator mass sp...

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Main Authors: B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, T. P. Guilderson
Format: Article
Language:English
Published: Copernicus Publications 2013-11-01
Series:Atmospheric Chemistry and Physics
Online Access:http://www.atmos-chem-phys.net/13/11101/2013/acp-13-11101-2013.pdf
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author B. W. LaFranchi
G. Pétron
J. B. Miller
S. J. Lehman
A. E. Andrews
E. J. Dlugokencky
B. Hall
B. R. Miller
S. A. Montzka
W. Neff
P. C. Novelli
C. Sweeney
J. C. Turnbull
D. E. Wolfe
P. P. Tans
K. R. Gurney
T. P. Guilderson
author_facet B. W. LaFranchi
G. Pétron
J. B. Miller
S. J. Lehman
A. E. Andrews
E. J. Dlugokencky
B. Hall
B. R. Miller
S. A. Montzka
W. Neff
P. C. Novelli
C. Sweeney
J. C. Turnbull
D. E. Wolfe
P. P. Tans
K. R. Gurney
T. P. Guilderson
author_sort B. W. LaFranchi
collection DOAJ
description Atmospheric radiocarbon (<sup>14</sup>C) represents an important observational constraint on emissions of fossil-fuel derived carbon into the atmosphere due to the absence of <sup>14</sup>C in fossil fuel reservoirs. The high sensitivity and precision that accelerator mass spectrometry (AMS) affords in atmospheric <sup>14</sup>C analysis has greatly increased the potential for using such measurements to evaluate bottom-up emissions inventories of fossil fuel CO<sub>2</sub> (CO<sub>2</sub>ff), as well as those for other co-emitted species. Here we use observations of <sup>14</sup>CO<sub>2</sub> and a series of primary hydrocarbons and combustion tracers from discrete air samples collected between June 2009 and September 2010 at the National Oceanic and Atmospheric Administration Boulder Atmospheric Observatory (BAO; Lat: 40.050° N, Lon: 105.004° W) to derive emission ratios of each species with respect to CO<sub>2</sub>ff. The BAO tower is situated at the boundary of the Denver metropolitan area to the south and a large industrial and agricultural region to the north and east, making it an ideal location to study the contrasting mix of emissions from the activities in each region. The species considered in this analysis are carbon monoxide (CO), methane (CH<sub>4</sub>), acetylene (C<sub>2</sub>H<sub>2</sub>), benzene (C<sub>6</sub>H<sub>6</sub>), and C<sub>3</sub>–C<sub>5</sub> alkanes. We estimate emissions for a subset of these species by using the Vulcan high resolution CO<sub>2</sub>ff emission data product as a reference. We find that CO is overestimated in the 2008 National Emissions Inventory (NEI08) by a factor of ~2. A close evaluation of the inventory suggests that the ratio of CO emitted per unit fuel burned from on-road gasoline vehicles is likely over-estimated by a factor of 2.5. Using a wind-directional analysis of the data, we find enhanced concentrations of CH<sub>4</sub>, relative to CO<sub>2</sub>ff, in air influenced by emissions to the north and east of the BAO tower when compared to air influenced by emissions in the Denver metro region to the south. Along with enhanced CH<sub>4</sub>, the strongest enhancements of the C<sub>3</sub>–C<sub>5</sub> alkanes are also found in the north and east wind sector, suggesting that both the alkane and CH<sub>4</sub> enhancements are sourced from oil and gas fields located to the northeast, though it was not possible to rule out the contribution of non oil and gas CH<sub>4</sub> sources.
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spelling doaj.art-0a64f9d27c3f48e1ad0fcf7b2d7b9ed92022-12-21T19:45:27ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242013-11-011321111011112010.5194/acp-13-11101-2013Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>B. W. LaFranchi0G. Pétron1J. B. Miller2S. J. Lehman3A. E. Andrews4E. J. Dlugokencky5B. Hall6B. R. Miller7S. A. Montzka8W. Neff9P. C. Novelli10C. Sweeney11J. C. Turnbull12D. E. Wolfe13P. P. Tans14K. R. Gurney15T. P. Guilderson16Center for Accelerator Mass Spectrometry (CAMS), Lawrence Livermore National Laboratory, Livermore, CA 94550, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAInstitute for Arctic and Alpine Research (INSTAAR), University of Colorado, Boulder 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder CO 80309, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USACooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder CO 80309, USAPhysical Sciences Division, NOAA Earth System Research Laboratory, Boulder, CO 80305, USAGlobal Monitoring Division (GMD), NOAA Earth System Research Laboratory, Boulder, CO 80305, USASchool of Life Sciences, Arizona State University, Tempe, AZ 85287, USACenter for Accelerator Mass Spectrometry (CAMS), Lawrence Livermore National Laboratory, Livermore, CA 94550, USAAtmospheric radiocarbon (<sup>14</sup>C) represents an important observational constraint on emissions of fossil-fuel derived carbon into the atmosphere due to the absence of <sup>14</sup>C in fossil fuel reservoirs. The high sensitivity and precision that accelerator mass spectrometry (AMS) affords in atmospheric <sup>14</sup>C analysis has greatly increased the potential for using such measurements to evaluate bottom-up emissions inventories of fossil fuel CO<sub>2</sub> (CO<sub>2</sub>ff), as well as those for other co-emitted species. Here we use observations of <sup>14</sup>CO<sub>2</sub> and a series of primary hydrocarbons and combustion tracers from discrete air samples collected between June 2009 and September 2010 at the National Oceanic and Atmospheric Administration Boulder Atmospheric Observatory (BAO; Lat: 40.050° N, Lon: 105.004° W) to derive emission ratios of each species with respect to CO<sub>2</sub>ff. The BAO tower is situated at the boundary of the Denver metropolitan area to the south and a large industrial and agricultural region to the north and east, making it an ideal location to study the contrasting mix of emissions from the activities in each region. The species considered in this analysis are carbon monoxide (CO), methane (CH<sub>4</sub>), acetylene (C<sub>2</sub>H<sub>2</sub>), benzene (C<sub>6</sub>H<sub>6</sub>), and C<sub>3</sub>–C<sub>5</sub> alkanes. We estimate emissions for a subset of these species by using the Vulcan high resolution CO<sub>2</sub>ff emission data product as a reference. We find that CO is overestimated in the 2008 National Emissions Inventory (NEI08) by a factor of ~2. A close evaluation of the inventory suggests that the ratio of CO emitted per unit fuel burned from on-road gasoline vehicles is likely over-estimated by a factor of 2.5. Using a wind-directional analysis of the data, we find enhanced concentrations of CH<sub>4</sub>, relative to CO<sub>2</sub>ff, in air influenced by emissions to the north and east of the BAO tower when compared to air influenced by emissions in the Denver metro region to the south. Along with enhanced CH<sub>4</sub>, the strongest enhancements of the C<sub>3</sub>–C<sub>5</sub> alkanes are also found in the north and east wind sector, suggesting that both the alkane and CH<sub>4</sub> enhancements are sourced from oil and gas fields located to the northeast, though it was not possible to rule out the contribution of non oil and gas CH<sub>4</sub> sources.http://www.atmos-chem-phys.net/13/11101/2013/acp-13-11101-2013.pdf
spellingShingle B. W. LaFranchi
G. Pétron
J. B. Miller
S. J. Lehman
A. E. Andrews
E. J. Dlugokencky
B. Hall
B. R. Miller
S. A. Montzka
W. Neff
P. C. Novelli
C. Sweeney
J. C. Turnbull
D. E. Wolfe
P. P. Tans
K. R. Gurney
T. P. Guilderson
Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
Atmospheric Chemistry and Physics
title Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
title_full Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
title_fullStr Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
title_full_unstemmed Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
title_short Constraints on emissions of carbon monoxide, methane, and a suite of hydrocarbons in the Colorado Front Range using observations of <sup>14</sup>CO<sub>2</sub>
title_sort constraints on emissions of carbon monoxide methane and a suite of hydrocarbons in the colorado front range using observations of sup 14 sup co sub 2 sub
url http://www.atmos-chem-phys.net/13/11101/2013/acp-13-11101-2013.pdf
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