A 60 yr record of atmospheric carbon monoxide reconstructed from Greenland firn air
A 60 yr record of atmospheric carbon monoxide reconstructed from Greenland firn air
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DOI：
10.5194/acp-13-7567-2013
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发表时间：
2013-01-01
影响因子：
6.3
通讯作者：
White, J. W. C.
中科院分区：
文献类型：
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作者：
Petrenko, V. V.;Martinerie, P.;White, J. W. C.
我们提出了第一个重建的北方半球（NH）高纬度大气中一氧化碳（CO）的摩尔分数从格陵兰的积雪空气。在格陵兰岛的三个深冰芯点（NGRIP于2001年，Summit于2006年，NEEM于2008年）收集了Firn空气样本。CO记录从三个网站同意彼此以及最近的大气测量，表明CO保存在这些网站的积雪。CO大气的历史重建回到1950年的测量使用的组合的两个前向模型的气体输运在积雪和逆模型。重建的历史表明，北极CO在1950年为140-150 nmol mol（-1），这是高于今天的值。从1950年到1970年代，CO摩尔分数上升了10-15 nmol mol（-1），并在1970年代或1980年代初达到峰值，随后下降了约30 nmol mol（-1），降至今天的水平。我们比较了CO的历史与大气历史的甲烷，轻烃，分子氢，CO稳定同位素和羟基自由基（OH），以及与已公布的CO排放清单和结果的历史运行的化学运输模型。我们发现，重建格陵兰CO的历史不能与现有的排放清单，除非不切实际的大的变化，OH的假设。我们认为，现有的CO排放清单严重低估了历史NH排放量，并未能捕捉到排放量下降开始于20世纪70年代末，这是最有可能是由于减少排放量的道路运输在北美和欧洲。
We present the first reconstruction of the Northern Hemisphere (NH) high latitude atmospheric carbon monoxide (CO) mole fraction from Greenland firn air. Firn air samples were collected at three deep ice core sites in Greenland (NGRIP in 2001, Summit in 2006 and NEEM in 2008). CO records from the three sites agree well with each other as well as with recent atmospheric measurements, indicating that CO is well preserved in the firn at these sites. CO atmospheric history was reconstructed back to the year 1950 from the measurements using a combination of two forward models of gas transport in firn and an inverse model. The reconstructed history suggests that Arctic CO in 1950 was 140-150 nmol mol(-1), which is higher than today's values. CO mole fractions rose by 10-15 nmol mol(-1) from 1950 to the 1970s and peaked in the 1970s or early 1980s, followed by a approximate to 30 nmol mol(-1) decline to today's levels. We compare the CO history with the atmospheric histories of methane, light hydrocarbons, molecular hydrogen, CO stable isotopes and hydroxyl radicals (OH), as well as with published CO emission inventories and results of a historical run from a chemistry-transport model. We find that the reconstructed Greenland CO history cannot be reconciled with available emission inventories unless unrealistically large changes in OH are assumed. We argue that the available CO emission inventories strongly underestimate historical NH emissions, and fail to capture the emission decline starting in the late 1970s, which was most likely due to reduced emissions from road transportation in North America and Europe.