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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Discovery and measurement of an isotopically distinct source of sulfate in Earth's atmosphere
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Discovery and measurement of an isotopically distinct source of sulfate in Earth's atmosphere

机译：在地球大气中发现和测量同位素不同的硫酸盐源

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Sulfate (SO_4) and its precursors are significant components of the atmosphere, with both natural and anthropogenic sources. Recently, our triple-isotope (~(16)O, ~(17)O, ~(18)O) measurements of atmospheric sulfate have provided specific insights into the oxidation pathways leading to sulfate, with important implications for models of the sulfur cycle and global climate change. Using similar isotopic measurements of aerosol sulfate in a polluted marine boundary layer (MBL) and primary sulfate (p-SO_4) sampled directly from a ship stack, we quantify the amount of p-SO_4 found in the atmosphere from ships. We find that ships contribute between 10% and 44% of the non-sea-salt sulfate found in fine [diameter (D) < 1.5 μm) particulate matter in coastal Southern California. These fractions are surprising, given that p-SO_4 constitutes ≈2-7% of total sulfur emissions from combustion sources [Seinfed JH, Pandis SN (2006) Atmospheric Chemistry and Physics (Wiley-lnter-science, New York)]. Our findings also suggest that the interaction of SO_2 from ship emissions with coarse hydrated sea salt particles may lead to the rapid removal of SO_2 in the MBL When combined with the longer residence time of p-SO_4 emissions in the MBL, these findings suggest that the importance of p-SO_4 emissions in marine environments may be underappreciated in global chemical models. Given the expected increase of international shipping in the years to come, these findings have clear implications for public health, air quality, international maritime law, and atmospheric chemistry.
机译：硫酸盐（SO_4）及其前体是大气的重要组成部分，具有自然和人为来源。最近，我们对大气硫酸盐的三同位素（〜（16）O，〜（17）O，〜（18）O）测量提供了导致硫酸盐氧化途径的特定见解，对硫循环模型具有重要意义和全球气候变化。使用对污染的海洋边界层（MBL）和直接从船堆采样的初级硫酸盐（p-SO_4）中的气溶胶硫酸盐进行的同位素测量，我们量化了从船舶大气中发现的p-SO_4的量。我们发现，在南加州沿海细颗粒物（直径（D）<1.5μm）中发现的非海盐硫酸盐中，船舶贡献了10％至44％。鉴于p-SO_4占燃烧源总硫排放的约2-7％[Seinfed JH，Pandis SN（2006）Atmospheric Chemistry and Physics（Wiley-Inter-science，New York）]，这些分数令人惊讶。我们的研究结果还表明，船舶排放物中的SO_2与粗水合海盐颗粒的相互作用可能导致MBL中SO_2的快速去除。再加上p-SO_4排放物在MBL中的停留时间更长，这些发现表明在全球化学模型中，可能无法充分理解海洋环境中p-SO_4排放的重要性。考虑到未来几年国际航运的预期增长，这些发现对公共卫生，空气质量，国际海事法和大气化学有明显的影响。

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