skip to main content

DOE PAGESDOE PAGES

Title: Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses

National-scale emissions of carbon tetrachloride (CCl 4) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration's flask air sampling network. We estimate an annual average US emission of 4.0 (2.0-6.5) Gg CCl 4 y -1 during 2008- 2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y -1) but only 8% (3-22%) of global CCl 4 emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl 4 emission during 2008-2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl 4 throughout the United States is more consistent with themore » distribution of industrial activities included in the TRI than with the distribution of other potential CCl 4 sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).« less
Authors:
 [1] ;  [2] ;  [1] ;  [2] ;  [1] ;  [3] ;  [1] ;  [4] ;  [2] ;  [1] ;  [5] ;  [6] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [7] ;  [8] ;  [9] more »;  [9] ;  [8] ;  [1] ;  [2] « less
  1. Univ. of Colorado, Boulder, CO (United States); National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
  2. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
  4. Stanford Univ., CA (United States)
  5. Univ. of Miami, FL (United States)
  6. Univ. of California, Irvine, CA (United States)
  7. Univ. of Colorado, Boulder, CO (United States); Univ. of Groningen (Netherlands)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  9. Atmosperic and Environmental Research, Lexington, MA (Untied States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 113; Journal Issue: 11; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES
OSTI Identifier:
1471010

Hu, Lei, Montzka, Stephen A., Miller, Ben R., Andrews, Arlyn E., Miller, John B., Lehman, Scott J., Sweeney, Colm, Miller, Scot M., Thoning, Kirk, Siso, Carolina, Atlas, Elliot L., Blake, Donald R., de Gouw, Joost, Gilman, Jessica B., Dutton, Geoff, Elkins, James W., Hall, Bradley, Chen, Huilin, Fischer, Marc L., Mountain, Marikate E., Nehrkorn, Thomas, Biraud, Sebastien C., Moore, Fred L., and Tans, Pieter. Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses. United States: N. p., Web. doi:10.1073/pnas.1522284113.
Hu, Lei, Montzka, Stephen A., Miller, Ben R., Andrews, Arlyn E., Miller, John B., Lehman, Scott J., Sweeney, Colm, Miller, Scot M., Thoning, Kirk, Siso, Carolina, Atlas, Elliot L., Blake, Donald R., de Gouw, Joost, Gilman, Jessica B., Dutton, Geoff, Elkins, James W., Hall, Bradley, Chen, Huilin, Fischer, Marc L., Mountain, Marikate E., Nehrkorn, Thomas, Biraud, Sebastien C., Moore, Fred L., & Tans, Pieter. Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses. United States. doi:10.1073/pnas.1522284113.
Hu, Lei, Montzka, Stephen A., Miller, Ben R., Andrews, Arlyn E., Miller, John B., Lehman, Scott J., Sweeney, Colm, Miller, Scot M., Thoning, Kirk, Siso, Carolina, Atlas, Elliot L., Blake, Donald R., de Gouw, Joost, Gilman, Jessica B., Dutton, Geoff, Elkins, James W., Hall, Bradley, Chen, Huilin, Fischer, Marc L., Mountain, Marikate E., Nehrkorn, Thomas, Biraud, Sebastien C., Moore, Fred L., and Tans, Pieter. 2016. "Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses". United States. doi:10.1073/pnas.1522284113. https://www.osti.gov/servlets/purl/1471010.
@article{osti_1471010,
title = {Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses},
author = {Hu, Lei and Montzka, Stephen A. and Miller, Ben R. and Andrews, Arlyn E. and Miller, John B. and Lehman, Scott J. and Sweeney, Colm and Miller, Scot M. and Thoning, Kirk and Siso, Carolina and Atlas, Elliot L. and Blake, Donald R. and de Gouw, Joost and Gilman, Jessica B. and Dutton, Geoff and Elkins, James W. and Hall, Bradley and Chen, Huilin and Fischer, Marc L. and Mountain, Marikate E. and Nehrkorn, Thomas and Biraud, Sebastien C. and Moore, Fred L. and Tans, Pieter},
abstractNote = {National-scale emissions of carbon tetrachloride (CCl4) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration's flask air sampling network. We estimate an annual average US emission of 4.0 (2.0-6.5) Gg CCl4 y-1 during 2008- 2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y-1) but only 8% (3-22%) of global CCl4 emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl4 emission during 2008-2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl4 throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl4 sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).},
doi = {10.1073/pnas.1522284113},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 11,
volume = 113,
place = {United States},
year = {2016},
month = {2}
}