Atmospheric Carbon Tetrachloride: Mysterious Emissions Gap Almost Closed

Carbon tetrachloride (CCl4) is a major ozone-depleting substance and its production and consumption is controlled under the Montreal Protocol for emissive uses. The most recent WMO/UNEP Scientific Assessment of Ozone Depletion [WMO, 2014] estimated a 2007-2012 CCl4 bottom-up emission of 1-4 Gg yr-1, based on country-by-country reports to UNEP, vs. a global top-down emissions estimate of 57 Gg yr-1, based on atmospheric measurements. To understand the gap between the top-down and bottom-up emissions estimates, a CCl4 activity was formed under the auspices of the Stratosphere-Troposphere Processes And their Role in Climate (SPARC) project. Several new findings were brought forward by the SPARC CCl4 activity.

CCl4 is destroyed in the stratosphere, oceans, and soils. The total lifetime estimate has been increased from 26 to 33 years. The new 33-year total lifetime lowers the top-down emissions estimate to 40 (25-55) Gg yr-1. In addition, a persistent hemispheric difference implies substantial ongoing Northern Hemisphere emissions, yielding an independent emissions estimate of 30 Gg yr-1. The combination of these two yields an emissions estimate of 35 Gg yr-1. Regional estimates have been made for Australia, North America, East Asia, and Western Europe. The sum of these estimates results in emissions of 21 Gg yr-1, albeit this does not include all regions of the world. Four bottom-up CCl4 emissions pathways have been identified, i.e., fugitive, unreported non-feedstock, unreported inadvertent, and legacy emissions. The new industrial bottom-up emissions estimate includes emissions from chloromethanes plants (13 Gg yr-1) and feedstock fugitive emissions (2 Gg yr-1). When combined with legacy emissions and unreported inadvertent emissions ( 10 Gg yr-1), the total global emissions are 20±5 Gg yr-1. While the new bottom-up value is still less than the aggregated top-down values, these estimates reconcile the CCl4 budget discrepancy when considered at the edges of their uncertainties.