Northern Hemisphere atmospheric history of carbon monoxide since preindustrial times reconstructed from multiple Greenland ice cores
Northern Hemisphere atmospheric history of carbon monoxide since preindustrial times reconstructed from multiple Greenland ice cores
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从多个格陵兰冰芯重建的北半球自前工业时代以来一氧化碳的大气历史
DOI：
10.5194/cp-2021-28
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发表时间：
2021
影响因子：
4.3
通讯作者：
J. Chappellaz
中科院分区：
文献类型：
--
作者：
X. Faïn;R. Rhodes;Place Philip;V. Petrenko;Kévin Fourteau;N. Chellman;E. Crosier;J. McConnell;E. Brook;T. Blunier;M. Legrand;J. Chappellaz
抽象的。一氧化碳（CO）是一种受管制的污染物，也是决定大气氧化能力的关键成分之一。获得一个可靠的记录的大气CO混合比，因为前工业时代是必要的，以评估气候化学模型的条件不同，从今天和约束过去的CO源。我们提出了高分辨率的测量CO混合比从冰芯钻在格陵兰冰盖上的五个不同的网站，经历了一系列的雪积累率，平均表面温度，和不同的化学成分。将光反馈腔增强吸收光谱仪（OF-CEAS）耦合到连续熔化器系统，并在2013年至2019年期间进行的四次分析活动中运行。总体而言，连续流分析（CFA）的CO进行了超过700米的冰。基于CFA的CO测量具有出色的外部精度（范围为3.3-6.6 ppbv，1 sigma），并实现了一致的低空白（范围为4.1+/-1.2至12.6+/-4.4 ppbv），使古大气解释成为可能。然而，五个CO记录都表现出变化太大，太快，以反映过去的大气混合比的变化。对离散冰样品进行的补充试验表明，这些变化不是分析方法的人为因素（即，在融化期间从冰中的有机物产生CO），但很可能与分析前冰内原位产生CO有关。CO和TOC的高分辨率记录的信号分辨率和共同调查的评价表明，过去的大气CO变化可以提取记录的基线在四个站点的积累率高于20厘米水当量每年（weq yr-1）。然而，这些基线应作为过去大气CO负荷的上限。基线CO记录从四个站点相结合，以产生一个多站点平均冰芯重建过去的大气CO的北方半球高纬度地区，覆盖期间从1700年至1957 CE。从1700年到1875年，记录显示在100-115 ppbv范围内稳定或略有增加。从1875年到1957年，记录显示从114+/-4 ppbv单调增加到147+/-6 ppbv。冰芯多站点CO记录表现出良好的重叠与大气CO记录从格陵兰的积雪空气跨越1950-2010年的时间段。结合冰芯和积雪的空气CO的历史，跨越1700-2010 CE提供了有用的限制，为未来的模式研究的大气变化，因为前工业化时期。
Abstract. Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. Obtaining a reliable record of atmospheric CO mixing ratios since pre-industrial times is necessary to evaluate climate-chemistry models in conditions different from today and to constrain past CO sources. We present high-resolution measurements of CO mixing ratios from ice cores drilled at five different sites on the Greenland ice sheet which experience a range of snow accumulation rates, mean surface temperatures, and different chemical compositions. An optical-feedback cavity-enhanced absorption spectrometer (OF-CEAS) was coupled to continuous melter systems and operated during four analytical campaigns conducted between 2013 and 2019. Overall, continuous flow analyses (CFA) of CO were carried out on over 700 m of ice. The CFA-based CO measurements exhibit excellent external precision (ranging 3.3-6.6 ppbv, 1sigma), and achieve consistently low blanks (ranging from 4.1+/-1.2 to 12.6+/-4.4 ppbv), enabling paleo-atmospheric interpretations. However the five CO records all exhibit variability too large and rapid to reflect past atmospheric mixing ratio changes. Complementary tests conducted on discrete ice samples demonstrate that these variations are not artifacts of the analytical method (i.e., production of CO from organics in the ice during melting), but very likely are related to in situ CO production within the ice before analysis. Evaluation of signal resolution and co-investigation of high-resolution records of CO and TOC show that past atmospheric CO variations can be extracted from the records’ baselines at four sites with accumulation rates higher than 20 cm water equivalent per year (weq yr-1). However, such baselines should be taken as upper bounds of past atmospheric CO burden. Baseline CO records from four sites are combined to produce a multisite average ice core reconstruction of past atmospheric CO for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE. From 1700 to 1875 CE, the record reveals stable or slightly increasing values in the 100-115 ppbv range. From 1875 to 1957 CE, the record indicates a monotonic increase from 114+/-4 ppbv to 147+/-6 ppbv. The ice-core multisite CO record exhibits an excellent overlap with the atmospheric CO record from Greenland firn air which spans the 1950-2010 time period. The combined ice-core and firn air CO history, spanning 1700-2010 CE provides useful constraints for future model studies of atmospheric changes since the preindustrial period.
影响因子：
5.1
作者：
Lamarque, J. -F.;Shindell, D. T.;Zeng, G.
通讯作者：
Zeng, G.