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Ubiquitous atmospheric production of organic acids mediated by cloud droplets

机译:云液滴介导的有机酸无处不在的大气生产

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摘要

The oxidation of hydrated formaldehyde from cloud droplets is the dominant source of atmospheric formic acid, increasing atmospheric acidity by reducing cloud and rainwater pH.Atmospheric acidity is increasingly determined by carbon dioxide and organic acids(1-3). Among the latter, formic acid facilitates the nucleation of cloud droplets(4) and contributes to the acidity of clouds and rainwater(1,5). At present, chemistry-climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood(2,6-9). Here we present atmospheric chamber experiments that show that formaldehyde is efficiently converted to gaseous formic acid via a multiphase pathway that involves its hydrated form, methanediol. In warm cloud droplets, methanediol undergoes fast outgassing but slow dehydration. Using a chemistry-climate model, we estimate that the gas-phase oxidation of methanediol produces up to four times more formic acid than all other known chemical sources combined. Our findings reconcile model predictions and measurements of formic acid abundance. The additional formic acid burden increases atmospheric acidity by reducing the pH of clouds and rainwater by up to 0.3. The diol mechanism presented here probably applies to other aldehydes and may help to explain the high atmospheric levels of other organic acids that affect aerosol growth and cloud evolution.
机译:来自云液滴的水合甲醛的氧化是大气甲酸的主要来源,通过还原云和雨水pH,较大的酸性酸度增加了大气酸度越来越多地通过二氧化碳和有机酸(1-3)确定。在后者中,甲酸有助于云液滴(4)的成核,并有助于云和雨水的酸度(1,5)。目前,化学 - 气候模型极大地低估了甲酸的大气负担,因为与其来源和水槽有关的关键过程仍然很清楚(2,6-9)。在这里,我们提供了大气室实验,表明甲醛通过涉及其水合形式的多相途径有效地转化为气态甲酸。在暖云液滴中,甲磺酸越野快速排出,但脱水缓慢。使用化学气候模型,我们估计甲醇的气相氧化产生多达四倍的甲酸比所有其他已知的化学源相结合。我们的研究结果和甲酸丰度的模型预测和测量。通过将云和雨水的pH减少至0.3,额外的甲酸负荷增加了大气酸度。这里呈现的二醇机制可能适用于其他醛,并有助于解释影响气溶胶生长和云演化的其他有机酸的高大气水平。

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  • 来源
    《Nature》 |2021年第7858期|233-237|共5页
  • 作者单位

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany|Univ Libre Bruxelles ULB Spect Quantum Chem & Atmospher Remote Sensing Brussels Belgium;

    Karlsruhe Inst Technol Inst Meteorol & Climate Res Karlsruhe Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Univ Libre Bruxelles ULB Spect Quantum Chem & Atmospher Remote Sensing Brussels Belgium;

    Univ Libre Bruxelles ULB Spect Quantum Chem & Atmospher Remote Sensing Brussels Belgium|Sorbonne Univ CNRS UVSQ LATMOS IPSL Paris France;

    Univ Libre Bruxelles ULB Spect Quantum Chem & Atmospher Remote Sensing Brussels Belgium;

    Royal Belgian Inst Space Aeron Brussels Belgium;

    Royal Belgian Inst Space Aeron Brussels Belgium;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Univ Wollongong Sch Earth Atmospher & Life Sci Ctr Atmospher Chem Wollongong NSW Australia;

    Max Planck Inst Chem Mainz Germany|Roshydromet & RAS Inst Global Climate & Ecol Moscow Russia;

    Natl Ctr Atmospher Res POB 3000 Boulder CO 80307 USA;

    Karlsruhe Inst Technol Inst Meteorol & Climate Res Karlsruhe Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Univ Wollongong Sch Earth Atmospher & Life Sci Ctr Atmospher Chem Wollongong NSW Australia;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Univ Toronto Dept Phys Toronto ON Canada;

    Univ Liege Inst Astrophys & Geophys Liege Belgium;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Natl Ctr Atmospher Res POB 3000 Boulder CO 80307 USA;

    Univ Wollongong Sch Earth Atmospher & Life Sci Ctr Atmospher Chem Wollongong NSW Australia;

    Sorbonne Univ CNRS UVSQ LATMOS IPSL Paris France|Ricardo Energy & Environm Harwell Berks England;

    Max Planck Inst Chem Mainz Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Max Planck Inst Chem Mainz Germany;

    Karlsruhe Inst Technol Inst Meteorol & Climate Res Karlsruhe Germany;

    Univ Toronto Dept Phys Toronto ON Canada;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Royal Belgian Inst Space Aeron Brussels Belgium;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Royal Belgian Inst Space Aeron Brussels Belgium;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

    Forschungszentrum Julich Inst Energy & Climate Res IEK Troposphere 8 Julich Germany;

  • 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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  • 正文语种 eng
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