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首页> 外文期刊>Atmospheric chemistry and physics >Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis
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Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis

机译：温度对α-甲酸臭氧溶解高含氧有机分子（HOMS）形成的影响

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摘要

Highly oxygenated organic molecules (HOMs) are important contributors to secondary organic aerosol (SOA) and new-particle formation (NPF) in the boreal atmosphere. This newly discovered class of molecules is efficiently formed from atmospheric oxidation of biogenic volatile organic compounds (VOCs), such as monoterpenes, through a process called autoxidation. This process, in which peroxyradical intermediates isomerize to allow addition of molecular oxygen, is expected to be highly temperature-dependent. Here, we studied the dynamics of HOM formation during -pinene ozonolysis experiments performed at three different temperatures, 20, 0 and -15°C, in the Aarhus University Research on Aerosol (AURA) chamber. We found that the HOM formation, under our experimental conditions (50 ppb -pinene and 100 ppb ozone), decreased considerably at lower temperature, with molar yields dropping by around a factor of 50 when experiments were performed at 0°C, compared to 20°C. At -15°C, the HOM signals were already close to the detection limit of the nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer used for measuring gasphase HOMs. Surprisingly, comparing spectra measured at 0 and 20°C, ratios between HOMs of different oxidation levels, e.g., the typical HOM products C_(10)H_(14)O_7, C_(10)H_(14)O_9, and C_(10)H_(14)O_(11), changed considerably less than the total HOM yields. More oxidized species have undergone more isomerization steps; yet, at lower temperature, they did not decrease more than the less oxidized species. One possible explanation is that the primary rate-limiting steps forming these HOMs occur before the products become oxygenated enough to be detected by our CI-APi-TOF (i.e., typically seven or more oxygen atoms). The strong temperature dependence of HOM formation was observed under temperatures highly relevant to the boreal forest, but the exact magnitude of this effect in the atmosphere will be mu
机译：高含氧有机分子（HOMS）是北方气氛中二次有机气溶胶（SOA）和新颗粒形成（NPF）的重要贡献。通过称为自氧化的方法，该新发现的分子是有效的从生物挥发性有机化合物（VOC）的大气氧化，例如单萜溶解。该方法，其中过氧化的中间体异构化以允许添加分子氧，预期高温依赖性。在这里，我们研究了在奥胡斯大学气溶胶（光环）室的三种不同温度，20,0和-15°C中进行的 - 中臭氧臭氧溶解实验期间HOM形成的动态。我们发现，在我们的实验条件下（50ppb-丁烯和100ppb臭氧）下的母母形成在较低温度下显着降低，当在0℃下进行实验时，摩尔产量滴加约50倍，与20相比°C。在-15°C下，HOM信号已经接近硝酸盐的化学电离大气压接口飞行时间（CI-API-TOF）质谱仪的检测极限，用于测量Gasphase HOMS。令人惊讶的是，比较在0和20℃下测量的光谱，在不同氧化水平的HOM之间测量，例如，典型的HOM产物C_（10）H_（14）O_7，C_（10）H_（14）O_9和C_（10 ）H_（14）O_（11），变化远低于总HOM产量。更多氧化物种经历了更多的异构化步骤;然而，在较低的温度下，它们没有减少超过较少的氧化物种。一种可能的解释是，在产品变为足以由我们的CI-API-TOF检测的氧化之前，形成这些霍姆的主要速率限制步骤（即，通常是七种或更多种氧原子）。在与北方森林高度相关的温度下观察HOM形成的强烈温度依赖性，但大气中这种效果的确切程度将是MU

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  • 来源
    《Atmospheric chemistry and physics》 |2019年第2期|共17页
  • 作者

    Lauriane L. J. Quéléver; Kasper Kristensen; Louise Normann Jensen; Bernadette Rosati; Ricky Teiwes; Kaspar R. Daellenbach; Otso Per?kyl?; Pontus Roldin; Rossana Bossi; Henrik B. Pedersen; Marianne Glasius; Merete Bilde; Mikael Ehn;

  • 作者单位

    Institute for Atmospheric and Earth System Research (INAR/Physics) P.O. Box 64 00014 University of Helsinki Finland;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Institute for Atmospheric and Earth System Research (INAR/Physics) P.O. Box 64 00014 University of Helsinki Finland;

    Institute for Atmospheric and Earth System Research (INAR/Physics) P.O. Box 64 00014 University of Helsinki Finland;

    Division of Nuclear Physics Lund University P.O. Box 118 22100 Lund Sweden;

    Department of Environmental Science Aarhus University Frederiksborgvej 399 4000 Roskilde Denmark;

    Department of Physics and Astronomy Aarhus University Ny Munkegade 120 8000 Aarhus C Denmark;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Department of Chemistry Aarhus University Langelandsgade 140 8000 Aarhus C Denmark;

    Institute for Atmospheric and Earth System Research (INAR/Physics) P.O. Box 64 00014 University of Helsinki Finland;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 大气科学（气象学）;
  • 关键词

    the boreal atmosphere; atmospheric oxidation; the dynamics;

    机译：北方气氛;大气氧化;动态;

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