Shipborne measurements of Antarctic submicron organic aerosols: an NMR perspective linking multiple sources and bioregions

Shipborne measurements of Antarctic submicron organic aerosols: an NMR perspective linking multiple sources and bioregions
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南极亚微米有机气溶胶的船载测量:连接多个来源和生物区域的核磁共振视角

DOI:
10.5194/acp-2019-888
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发表时间:
2019
影响因子:
6.3
通讯作者:
D. Gentner
D. Gentner
中科院分区:
地球科学1区
文献类型:
--
作者:
R. Sheu;Aurelie R. Marcotte;Peeyush Khare;S. Charan;Jenna C. Ditto;D. Gentner

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抽象的。近海海域亚微米级气溶胶粒子的浓度 南极洲受海冰范围的影响。这种效果有两种方式: 一方面,海冰通过海雾调节颗粒的产生。 (初级气溶胶);另一方面,它拥有复杂的 释放二次粒子前体的生物体。过去的研究 记录南极洲细小气溶胶的化学成分表明 活跃在沿海地区的各种潜在的一次和二次来源, 近海海洋区域,以及海冰本身。特别是, 除了众所周知的有机和硫磺物质来源之外 由微藻产生的二甲基硫化物(DMS)的氧化,最近 在2015年的PEGASO邮轮上获得的发现表明 微生物区系也会产生含氮的有机化合物。 在边缘冰区殖民。以补充气溶胶来源 使用在线质谱学技术进行的分配,在这里我们 讨论核执行离线光谱分析的结果 核磁共振光谱学。在这项研究中,我们(I)介绍了 跨越生物区域的公海水域上空的环境气溶胶的组成, 并将其与(Ii)海水样本和(Iii)在船上海喷室中产生的气泡破裂气雾剂的成分进行比较。我们的 结果表明,储罐内的气溶胶过程对初级浓缩物有一定的强化作用。 含有脂肪和糖的海洋颗粒,同时耗尽它们的游离态 氨基酸,解释了为什么氨基酸只在 分析了海洋气溶胶样品中的痕量浓度。分析了几个问题 环境亚微米气溶胶样品中的水溶性有机碳 显示了三个生物区的不同的核磁共振指纹:(1)开放的Southern 海洋中上层环境,其中气溶胶富含初级 含有脂类和糖类的海洋颗粒;(2) 韦德尔海,次生有机化合物,包括甲烷磺酸 气溶胶成分中富含酸性和半挥发胺;以及(3) 陆地沿海地区,由陆地排放的蔗糖等糖类追踪 植物。最后,一种新的生物化学标记肌酸被发现 在韦德尔海的样本中发现,提供了另一种 确认含氮代谢物在人体内的重要性 南极极地气溶胶。
Abstract. The concentrations of submicron aerosol particles in maritime regions around Antarctica are influenced by the extent of sea ice. This effect is two ways: on one side, sea ice regulates the production of particles by sea spray (primary aerosols); on the other side, it hosts complex communities of organisms emitting precursors for secondary particles. Past studies documenting the chemical composition of fine aerosols in Antarctica indicate various potential primary and secondary sources active in coastal areas, in offshore marine regions, and in the sea ice itself. In particular, beside the well-known sources of organic and sulfur material originating from the oxidation of dimethylsulfide (DMS) produced by microalgae, recent findings obtained during the 2015 PEGASO cruise suggest that nitrogen-containing organic compounds are also produced by the microbiota colonizing the marginal ice zone. To complement the aerosol source apportionment performed using online mass spectrometric techniques, here we discuss the outcomes of offline spectroscopic analysis performed by nuclear magnetic resonance (NMR) spectroscopy. In this study we (i) present the composition of ambient aerosols over open-ocean waters across bioregions, and compare it to the composition of (ii) seawater samples and (iii) bubble-bursting aerosols produced in a sea-spray chamber onboard the ship. Our results show that the process of aerosolization in the tank enriches primary marine particles with lipids and sugars while depleting them of free amino acids, providing an explanation for why amino acids occurred only at trace concentrations in the marine aerosol samples analyzed. The analysis of water-soluble organic carbon (WSOC) in ambient submicron aerosol samples shows distinct NMR fingerprints for three bioregions: (1) the open Southern Ocean pelagic environments, in which aerosols are enriched with primary marine particles containing lipids and sugars; (2) sympagic areas in the Weddell Sea, where secondary organic compounds, including methanesulfonic acid and semivolatile amines abound in the aerosol composition; and (3) terrestrial coastal areas, traced by sugars such as sucrose, emitted by land vegetation. Finally, a new biogenic chemical marker, creatinine, was identified in the samples from the Weddell Sea, providing another confirmation of the importance of nitrogen-containing metabolites in Antarctic polar aerosols.