Fate of Springtime Atmospheric Reactive Mercury: Concentrations and Deposition at Zeppelin, Svalbard

Fate of Springtime Atmospheric Reactive Mercury: Concentrations and Deposition at Zeppelin, Svalbard
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春季大气活性汞的命运:斯瓦尔巴齐柏林飞艇的浓度和沉积

DOI:
10.1021/acsearthspacechem.1c00299
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发表时间:
2021
影响因子:
3.4
通讯作者:
Huang, Jiaoyan
Huang, Jiaoyan
中科院分区:
化学3区
文献类型:
--
作者:
Osterwalder, Stefan;Dunham-Cheatham, Sarrah M.;Ferreira Araujo, Beatriz;Magand, Olivier;Thomas, Jennie L.;Baladima, Foteini;Pfaffhuber, Katrine Aspmo;Berg, Torunn;Zhang, Lei;Huang, Jiaoyan

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在北极日出期间,中纬度大气中元素汞(Hg)的排放被广泛氧化为活性汞(RM)化合物,导致大气沉积增强,影响北极海洋野生动物和人类。很难估计RM干沉积,因为RM浓度、化合物和它们的沉积速度是不明确的。在这里,我们研究了用基于膜的方法采样的RM浓度,发现在斯瓦尔巴群岛的齐柏林天文台(2019年3月26日至7月24日),这些浓度超过了基于珠光体的RM检测的5倍。测量到的气态氧化汞的干沉积约占模型RM沉积的一半,表明颗粒结合的汞是干沉积的重要组成部分。通过热膜解吸,发现RM化学以Hg-Cl /Br(51%)和Hg-N(45%)化合物为主。反轨迹分析表明,Hg-Br /Cl化合物主要来自海洋边界层(海冰暴露)内的平流,而Hg-N主要来自自由对流层。周平均RM化合物特定干沉降速度范围为0.12至0.49 cm s-1,净RM干沉降为1.9 μg m-2 (1.5-2.5 μg m-2; 95%置信区间),超过斯瓦尔巴群岛Hg年平均湿沉降通量。总体而言,我们发现春季大气RM沉积在北极海洋环境中被低估了。
Mid-latitude atmospheric elemental mercury (Hg) emissions undergo extensive oxidation to reactive Hg (RM) compounds during Arctic polar sunrise, resulting in enhanced atmospheric deposition that impacts Arctic marine wildlife and humans. It has been difficult to estimate RM dry deposition, because RM concentrations, compounds, and their deposition velocities are ill-defined. Here, we investigate RM concentrations sampled with membrane-based methods and find these to exceed denuder-based RM detection by 5 times at the Zeppelin Observatory on Svalbard (March 26–July 24, 2019). Measured dry deposition of gaseous oxidized Hg was about half of the modeled RM deposition, demonstrating that particulate-bound Hg was an important component of dry deposition. Using thermal membrane desorption, RM chemistry was found to be dominated by Hg–Cl/Br (51%) and Hg–N (45%) compounds. Back-trajectory analysis indicated that Hg–Br/Cl compounds were predominantly advected from within the marine boundary layer (sea ice exposure), while Hg–N originated from the free troposphere. Weekly average RM compound-specific dry deposition velocities ranged from 0.12 to 0.49 cm s–1, with a net RM dry deposition of 1.9 μg m–2(1.5–2.5 μg m–2; 95% confidence interval) that exceeds the mean annual Hg wet deposition flux in Svalbard. Overall, we find that springtime atmospheric RM deposition has been underestimated in the Arctic marine environment.
2003 年春季新奥勒松不同海拔高度的大气汞行为
DOI: --
发表时间: 2005
期刊:
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期刊: BIOGEOSCIENCES
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