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

  • Author(s): Hu, L
  • Montzka, SA
  • Miller, BR
  • Andrews, AE
  • Miller, JB
  • Lehman, SJ
  • Sweeney, C
  • Miller, SM
  • Thoning, K
  • Siso, C
  • Atlas, EL
  • Blake, DR
  • De Gouw, J
  • Gilman, JB
  • Dutton, G
  • Elkins, JW
  • Hall, B
  • Chen, H
  • Fischer, ML
  • Mountain, ME
  • Nehrkorn, T
  • Biraud, SC
  • Moore, FL
  • Tans, P
  • et al.

Published Web Location

http://dx.doi.org/10.1073/pnas.1522284113
No data is associated with this publication.
Abstract

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 CCl4y-1during 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 CCl4emissions 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 CCl4emission 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 CCl4throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl4sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).

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