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Massive volcanic SO_2 oxidation and sulphate aerosol deposition in Cenozoic North America

机译：北美新生代的大规模火山SO_2氧化和硫酸盐气溶胶沉积

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Volcanic eruptions release a large amount of sulphur dioxide (SO_2) into the atmosphere. SO_2 is oxidized to sulphate and can subsequently form sulphate aerosol, which can affect the Earth's radiation balance, biologic productivity and high-altitude ozone concentrations, as is evident from recent volcanic eruptions. SO_2 oxidation can occur via several different pathways that depend on its flux and the atmospheric conditions. An investigation into how SO_2 is oxidized to sulphate-the oxidation product preserved in the rock record-can therefore shed light on past volcanic eruptions and atmospheric conditions. Here we use sulphur and triple oxygen isotope measurements of atmospheric sulphate extracted from tuffaceous deposits to investigate the specific oxidation pathways from which the sulphate was formed. We find that seven eruption-related sulphate aerosol deposition events have occurred during the mid-Cenozoic era (34 to 7 million years ago) in the northern High Plains, North America. Two extensively sampled ash beds display a similar sulphate mixing pattern that has two distinct atmospheric secondary sulphates. A three-dimensional atmospheric sulphur chemistry and transport model study reveals that the observed, isotopically discrete sulphates in sediments can be produced only in initially alkaline doudwater that favours an ozone-dominated SO_2 oxidation pathway in the troposphere. Our finding suggests that, in contrast to the weakly acidic conditions today, doudwater in the northern High Plains may frequently have been alkaline during the mid-Cenozoic era. We propose that atmospheric secondary sulphate preserved in continental deposits represents an unexploited geological archive for atmospheric SO_2 oxidation chemistry linked to volcanism and atmospheric conditions in the past.
机译：火山喷发将大量的二氧化硫（SO_2）释放到大气中。 SO_2被氧化成硫酸盐并随后形成硫酸盐气溶胶，这可以影响地球的辐射平衡，生物生产力和高海拔臭氧浓度，最近的火山喷发就是明显的证据。 SO_2氧化可以通过几种不同的途径发生，这取决于其通量和大气条件。因此，对SO_2如何被氧化成硫酸盐（岩石记录中保存的氧化产物）的研究可以揭示过去的火山喷发和大气条件。在这里，我们使用从凝灰岩矿床中提取的大气硫酸盐的硫和三重氧同位素测量方法，来研究形成硫酸盐的特定氧化途径。我们发现在北美北部高平原地区的新生代中期（34至700万年前）发生了7次与喷发有关的硫酸盐气溶胶沉积事件。两个经过大量采样的灰床显示出相似的硫酸盐混合模式，其中包含两种不同的大气二次硫酸盐。一项三维大气硫化学和迁移模型研究表明，沉积物中观察到的，同位素分立的硫酸盐只能在有利于对流层中以臭氧为主的SO_2氧化途径的初始碱性淡水中产生。我们的发现表明，与今天的弱酸性条件相比，北部高平原地区的淡水在新生代中期可能经常是碱性的。我们认为，保留在大陆沉积物中的大气二次硫酸盐代表了过去与火山作用和大气条件相关的大气SO_2氧化化学的未开发地质档案。

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  • 来源
    《Nature》 |2010年第7300期|P.iii909-912|共5页
  • 作者

    Huiming Bao; Shaocai Yu; Daniel Q. Tong;

  • 作者单位

    Department of Geology and Geophysics, Louisiana State University, Baton Rouge, Louisiana 70803-4101, USA;

    Atmospheric Modeling and Analysis Division (E243-03), National Exposure Research Laboratory, United States Environmental Protection Agency, Research Triangle Park, North Carolina 27711, USA;

    Air Resources Laboratory, National Oceanic and Atmospheric Administration, Silver Springs, Maryland 20910, USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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