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

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).

Methane emissions from Alaska in 2012 from CARVE airborne observations.

We determined methane (CH4) emissions from Alaska using airborne measurements from the Carbon Arctic Reservoirs Vulnerability Experiment (CARVE). Atmospheric sampling was conducted between May and September 2012 and analyzed using a customized version of the polar weather research and forecast model linked to a Lagrangian particle dispersion model (stochastic time-inverted Lagrangian transport model). We estimated growing season CH4 fluxes of 8 ± 2 mg CH4⋅m(-2)⋅d(-1) averaged over all of Alaska, corresponding to fluxes from wetlands of 56(-13)(+22) mg CH4⋅m(-2)⋅d(-1) if we assumed that wetlands are the only source from the land surface (all uncertainties are 95% confidence intervals from a bootstrapping analysis). Fluxes roughly doubled from May to July, then decreased gradually in August and September. Integrated emissions totaled 2.1 ± 0.5 Tg CH4 for Alaska from May to September 2012, close to the average (2.3; a range of 0.7 to 6 Tg CH4) predicted by various land surface models and inversion analyses for the growing season. Methane emissions from boreal Alaska were larger than from the North Slope; the monthly regional flux estimates showed no evidence of enhanced emissions during early spring or late fall, although these bursts may be more localized in time and space than can be detected by our analysis. These results provide an important baseline to which future studies can be compared.