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首页> 外文期刊>Atmospheric chemistry and physics >Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements
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Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

机译：来自气溶胶质谱仪测量的异戊二烯环氧二醇衍生的二次有机气溶胶（IEPOX-SOA）的实时示踪剂的表征

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摘要

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78% of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC(5)H(6)O (fC(5)H(6)O = C5H6O+ / OA) across multiple field, chamber, and source data sets. A background of similar to 1.7 +/- 0.1 parts per thousand (parts per thousand = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 +/- 0.6 parts per thousand are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 +/- 2.0 parts per thousand) is 4 times lower than the average for IEPOX-SOA (22 +/- 7 parts per thousand), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC(5)H(6)O (similar to 6.5 +/- 2.2 parts per thousand on average) than other sites, consistent with the expected IEPOX- SOA formation in those studies. fC(5)H(6)O in IEPOX- SOA is always elevated (12-40 parts per thousand) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC(5)H(6)O (< 3 parts per thousand) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX- SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX- SOA as a triangle plot of f(CO2) vs. fC(5)H(6)O. Finally, we develop a simplified method to estimate ambient IEPOX- SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of similar to 2, if the fC(5)H(6)O of the local IEPOX- SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX- SOA and will enable improved characterization of this OA component.
机译：大量的二次有机气溶胶（SOA）可以由异戊二烯环氧二醇（IePox）形成，其主要是异戊二烯的氧化产物，主要是低无条件。通过将阳性基质分子分解（PMF）施加到气溶胶质谱仪（AMS）测量，通过将来自其他平行异戊二烯氧化途径形成的SOA的总IePox-SOA量化。这里总结了几种大陆的多场研究中的有机气溶胶（OA）的IePox-SOA级分，并展示了由Geos-Chem化学传输模型模拟的气相Iepox浓度的一致图案。在南方氧化剂和气溶胶研究（SOA）期间，78％的PMF分离的IEPOX-SOA由测定的IePox-SOA分子示踪剂（2-甲基四核，C5-三醇和IePox衍生的有机硫酸盐及其二聚体）占据占据综述它是我们知识的环境SOA组件的最高水平鉴定。在PMF解析的IEPOX-SOA光谱中发现C5H6O +（M / Z 82）的增强信号。为了研究这种离子作为Iepox-SOA的示踪剂的适用性，我们在多场，腔室和源数据上检查Fc（5）H（6）O（Fc（5）H（6）o = C5H60 + / OA）套。在城市，生物量燃烧和其他人为原发性有机气溶胶（POA）强烈影响的研究中，观察到类似于1.7 +/- 0.1份每千（千分之一）的0.1份（千分之一）。在蒙脱烯排放受强烈影响的研究中发现了较高的3.1 +/- 0.6份‰的背景值。平均实验室单萜类SOA值（5.5 +/- 2.0份）比IEPOX-SOA（22 +/- 7份）的平均值低4倍，这使一些空间将两者分开给OA。低水平下的异戊二烯排放的位置具有更高的Fc（5）小时（6）o（6）o（平均相似的6.5 +/- 2.2份），与其他网站一致，与那些预期的Iepox-SOA形成一致学习。 IePox-SOA中的Fc（5）H（6）o总是升高（每千份12-40份），但在位置之间的不同变化，其显示在其详细分子组合物中反射大的变化。在腔室研究中，在非IePox衍生的异戊二烯-SOA中报道的低Fc（5）H（6）O（<3份/份）表明该示踪离子由IePox-SOA特别提高，并且不是示踪剂所有SOA来自异戊二烯。我们介绍了一种图形诊断，研究IePox-SOA作为F（CO2）与Fc（5）H（6）O的三角形图的存在和老化。最后，我们开发了一种简化的方法来估计环境IEPOx-SOA质量浓度，其显示与完整PMF方法相比表现良好。如果局部Iepox-SOA的FC（5）H（6）O不可用，则示踪方法的不确定性高达2。当只有单位质量分辨率数据可用时，与气溶胶化学物质监测（ACSM）一样，由于M / Z 82的其他离子的干扰增加，所有方法可能会更少。该研究阐明了不同的强度和限制AMS检测IEPOx-SOA的方法，并将实现该OA组件的改进表征。

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  • 来源
    《Atmospheric chemistry and physics》 |2015年第20期|共27页
  • 作者

    Hu W. W.; Campuzano-Jost P.; Palm B. B.; Day D. A.; Ortega A. M.; Hayes P. L.; Krechmer J. E.; Chen Q.; Kuwata M.; Liu Y. J.; de Sa S. S.; McKinney K.; Martin S. T.; Hu M.; Budisulistiorini S. H.; Riva M.; Surratt J. D.; St Clair J. M.; Isaacman-Van Wertz G.; Yee L. D.; Goldstein A. H.; Carbone S.; Brito J.; Artaxo P.; de Gouw J. A.; Koss A.; Wisthaler A.; Mikoviny T.; Karl T.; Kaser L.; Jud W.; Hansel A.; Docherty K. S.; Alexander M. L.; Robinson N. H.; Coe H.; Allan J. D.; Canagaratna M. R.; Paulot F.; Jimenez J. L.;

  • 作者单位

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Harvard Univ Sch Engn &

    Appl Sci Cambridge MA 02138 USA;

    Peking Univ Coll Environm Sci &

    Engn State Key Joint Lab Environm Simulat &

    Pollut Con Beijing 100871 Peoples R China;

    Univ N Carolina Dept Environm Sci &

    Engn Gillings Sch Global Publ Hlth Chapel Hill NC USA;

    Univ N Carolina Dept Environm Sci &

    Engn Gillings Sch Global Publ Hlth Chapel Hill NC USA;

    Univ N Carolina Dept Environm Sci &

    Engn Gillings Sch Global Publ Hlth Chapel Hill NC USA;

    CALTECH Div Geol &

    Planetary Sci Pasadena CA 91125 USA;

    Univ Calif Berkeley Dept Environm Sci Policy &

    Management Berkeley CA 94720 USA;

    Univ Calif Berkeley Dept Environm Sci Policy &

    Management Berkeley CA 94720 USA;

    Univ Calif Berkeley Dept Environm Sci Policy &

    Management Berkeley CA 94720 USA;

    Univ Sao Paulo Dept Appl Phys Sao Paulo Brazil;

    Univ Sao Paulo Dept Appl Phys Sao Paulo Brazil;

    Univ Sao Paulo Dept Appl Phys Sao Paulo Brazil;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

    Univ Colorado Dept Chem &

    Biochem Boulder CO 80309 USA;

    Univ Oslo Dept Chem Oslo Norway;

    Univ Oslo Dept Chem Oslo Norway;

    Univ Innsbruck Inst Atmospher &

    Cryospher Sci A-6020 Innsbruck Austria;

    Univ Innsbruck Inst Ion Phys &

    Appl Phys A-6020 Innsbruck Austria;

    Univ Innsbruck Inst Ion Phys &

    Appl Phys A-6020 Innsbruck Austria;

    Univ Innsbruck Inst Ion Phys &

    Appl Phys A-6020 Innsbruck Austria;

    Alion Sci &

    Technol Res Triangle Pk NC USA;

    Pacific NW Natl Lab Environm Mol Sci Lab Richland WA 99352 USA;

    Univ Manchester Sch Earth Atmospher &

    Environm Sci Manchester Lancs England;

    Univ Manchester Sch Earth Atmospher &

    Environm Sci Manchester Lancs England;

    Univ Manchester Sch Earth Atmospher &

    Environm Sci Manchester Lancs England;

    Aerodyne Res Inc Billerica MA USA;

    NOAA Geophys Fluid Dynam Lab Princeton NJ USA;

    Univ Colorado Cooperat Inst Res Environm Sci Boulder CO 80309 USA;

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  • 正文语种 eng
  • 中图分类 大气科学（气象学）;
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