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
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309; Global Monitoring Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305;
Global Monitoring Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305;
Proc Natl Acad Sci U S A. 2016 Mar 15;113(11):2880-5. doi: 10.1073/pnas.1522284113. Epub 2016 Feb 29.
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).
基于美国国家海洋和大气管理局(National Oceanic and Atmospheric Administration)的气袋空气采样网络在全美多个站点的大气观测数据进行反演建模,得出了全国范围内四氯化碳(CCl4)的排放量。我们估计在2008 - 2012年期间,美国四氯化碳的年平均排放量为4.0(2.0 - 6.5)Gg CCl4 y(-1),这比向美国环境保护局(EPA)有毒物质排放清单(TRI)报告的排放量(平均0.06 Gg y(-1))高出近两个数量级,但仅占这些年全球四氯化碳排放量的8%(3 - 22%)。观测确定并在所有反演结果中一致显示的排放区域包括墨西哥湾沿岸各州、加利福尼亚州的旧金山湾区以及科罗拉多州的丹佛地区。观测得出的排放量和美国EPA TRI均表明,得克萨斯州和路易斯安那州是最大的排放源,在2008 - 2012年期间占美国全国四氯化碳排放总量的三分之一到三分之二。这些结果在定性上与早年进行的多次飞机和船舶调查一致,这些调查表明在休斯顿及其周边地区测得的大气摩尔分数有显著增加。此外,美国四氯化碳排放分布与TRI中包含的工业活动分布比与其他潜在四氯化碳源(如未封闭的垃圾填埋场或与人口密度相关的活动,例如使用含氯漂白剂)的分布更为一致。