Peroxy radical and related trace gas measurements in the boundary layer above the Atlantic Ocean

Peroxy radical and related trace gas measurements in the boundary layer above the Atlantic Ocean
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DOI:
10.1029/2000jd900613
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发表时间:
2001-03-27
影响因子:
4.4
通讯作者:
Kraus, A
Kraus, A
中科院分区:
地球科学2区
文献类型:
--
作者:
Burkert, J;Andrés-Hernández, MD;Kraus, A

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过氧自由基(RO2*=HO2+Sigma RO2,其中 HO2 是氢过氧自由基,R 是有机基团)的测量是在德国科考船 Polarstern(ANT XIV/1 号巡航,1996 年)上对大西洋对流层和平流层物种进行空气化学和激光雷达研究(ALBATROSS)期间使用化学放大器技术(PERCA)进行的。获得的数据与 1991 年早期巡航 (ANT X/1) 的先前结果进行了比较。观察到两个数据集之间的合理一致性,表明这些测量的可靠性。两个数据集都考虑了自由基放大器对环境水蒸气存在的敏感性。中午前后测量了 40 至 80 pptv 之间的最大 RO2* 混合比。许多天都观察到夜间信号。北大西洋和南大西洋不同纬度地区的气团可以使用反向轨迹来表征。尽管 RO2* 的寿命相对较短,但其混合比似乎受到与污染源相关的空气团行进路径的影响,而较高水平的空气团则与此有关。基于 CH4 和 CO 氧化化学的盒模型相当好地描述了 RO2*,但无法解释持续的夜间信号和观察到的 HCHO。需要额外的 HCHO 灵魂,这表明非甲烷碳氢化合物 (NMHC) 化学在遥远的大西洋边界层中的重要性。向后轨迹和痕量气体浓度的变化都表明生物质燃烧、船舶和自然排放可能是造成观察到的与假设化学成分偏差的原因。
Measurements of peroxy radicals (RO2*=HO2+Sigma RO2, where HO2 is the hydroperoxyl radical and R is an organic group) were made using the chemical amplifier technique (PERCA) during the Air chemistry and Lidar studies of tropospheric and stratospheric species on the Atlantic Ocean (ALBATROSS) campaign on board the German research vessel Polarstern (cruise ANT XIV/1, 1996). The data obtained are compared to previous results from an earlier cruise in 1991 (ANT X/1). Reasonable agreement between the two data sets was observed, indicating the reliability of these measurements. Both data sets take into account the sensitivity of the radical amplifier to the presence of ambient water vapor. Maximum RO2* mixing ratios around noon between 40 and 80 pptv were measured. Nighttime signals were observed on many days. Air masses in different latitude regions in the North and South Atlantic could be characterized using back trajectories. In spite of the fact that the RO2* is relatively short lived, its mixing ratio appears to be influenced by the path traveled by the air mass somewhat higher levels being associated with sources of pollution. A box model based on CH4 and CO oxidation chemistry describes RO2* reasonably well but could not explain the persistent nighttime signals and the HCHO observed. An additional soul ce of HCHO is required, indicating the importance of nonmethane hydrocarbon (NMHC) chemistry in the remote Atlantic boundary layer. Both back trajectories and variations of trace gas concentrations indicate that biomass burning, ship, and natural emissions are likely responsible for the observed deviations from the assumed chemistry.