Prinn R, Cunnold D, Rasmussen R, Simmonds P, Alyea F, Crawford A, Fraser P, Rosen R
Science. 1987 Nov 13;238(4829):945-50. doi: 10.1126/science.238.4829.945.
Frequent atmospheric measurements of the anthropogenic compound methylchloroform that were made between 1978 and 1985 indicate that this species is continuing to increase significantly around the world. Reaction with the major atmospheric oxidant, the hydroxyl radical (OH), is the principal sink for this species. The observed mean trends for methylchloroform are 4.8, 5.4, 6.4, and 6.9 percent per year at Aldrigole (Ireland) and Cape Meares (Oregon), Ragged Point (Barbados), Point Matatula (American Samoa), and Cape Grim (Tasmania), respectively, from July 1978 to June 1985. These measured trends, combined with knowledge of industrial emissions, were used in an optimal estimation inversion scheme to deduce a globally averaged methylchloroform atmospheric lifetime of 6.3 (+ 1.2, -0.9) years (1sigma uncertainty) and a globally averaged tropospheric hydroxyl radical concentration of (7.7 +/- 1.4) x 10(5) radicals per cubic centimeter (1sigma uncertainty). These 7 years of gas chromatographic measurements, which comprise about 60,000 individual calibrated real-time air analyses, provide the most accurate estimates yet of the trends and lifetime of methylchloroform and of the global average for tropospheric hydroxyl radical levels. Accurate determination of hydroxyl radical levels is crucial to understanding global atmospheric chemical cycles and trends in the levels of trace gases such as methane.
1978年至1985年间对人为化合物甲基氯仿进行的频繁大气测量表明,该物质在全球范围内仍在显著增加。与主要大气氧化剂羟基自由基(OH)的反应是该物质的主要汇。1978年7月至1985年6月期间,在爱尔兰的奥尔德里戈尔、俄勒冈州的梅尔斯角、巴巴多斯的拉格点、美属萨摩亚的马塔图拉角和塔斯马尼亚的格里姆角,甲基氯仿的观测平均年增长率分别为4.8%、5.4%、6.4%和6.9%。这些测量趋势与工业排放知识相结合,用于最优估计反演方案,以推断甲基氯仿在全球平均大气中的寿命为6.3(+1.2,-0.9)年(1σ不确定性),以及全球平均对流层羟基自由基浓度为(7.7±1.4)×10⁵个/立方厘米(1σ不确定性)。这7年的气相色谱测量包括约60000次单独校准的实时空气分析,提供了迄今为止对甲基氯仿趋势和寿命以及对流层羟基自由基水平全球平均值的最准确估计。准确测定羟基自由基水平对于理解全球大气化学循环以及甲烷等痕量气体水平的趋势至关重要。