Department of Environmental Science, Policy, and Management, University of California, 147 Mulford Hall, Berkeley, CA 94720, USA.
Proc Natl Acad Sci U S A. 2010 Apr 13;107(15):6676-81. doi: 10.1073/pnas.0911858107. Epub 2010 Feb 8.
An understanding of the gas/particle-phase partitioning of semivolatile compounds is critical in determining atmospheric aerosol formation processes and growth rates, which in turn affect global climate and human health. The Study of Organic Aerosol at Riverside 2005 campaign was performed to gain a better understanding of the factors responsible for aerosol formation and growth in Riverside, CA, a region with high concentrations of secondary organic aerosol formed through the phase transfer of low-volatility reaction products from the oxidation of precursor gases. We explore the ability of the thermal desorption aerosol gas chromatograph (TAG) to measure gas-to-particle-phase transitioning for several organic compound classes (polar and nonpolar) found in the ambient Riverside atmosphere by using in situ observations of several hundred semivolatile organic compounds. Here we compare TAG measurements to modeled partitioning of select semivolatile organic compounds. Although TAG was not designed to quantify the vapor phase of semivolatile organics, TAG measurements do distinguish when specific compounds are dominantly in the vapor phase, are dominantly in the particle phase, or have both phases present. Because the TAG data are both speciated and time-resolved, this distinction is sufficient to see the transition from vapor to particle phase as a function of carbon number and compound class. Laboratory studies typically measure the phase partitioning of semivolatile organic compounds by using pure compounds or simple mixtures, whereas hourly TAG phase partitioning measurements can be made in the complex mixture of thousands of polar/nonpolar and organic/inorganic compounds found in the atmosphere.
了解半挥发性化合物的气/粒相间分配对于确定大气气溶胶的形成过程和增长率至关重要,而这反过来又会影响全球气候和人类健康。2005 年河滨有机气溶胶研究(Study of Organic Aerosol at Riverside 2005 campaign)旨在更好地了解导致加利福尼亚州河滨地区气溶胶形成和增长的因素,该地区由于前体气体氧化产生的低挥发性反应产物通过相转移形成了高浓度的二次有机气溶胶。我们通过原位观测数百种半挥发性有机化合物,探讨了热解吸气溶胶气相色谱仪(thermal desorption aerosol gas chromatograph,TAG)测量环境中几种有机化合物(极性和非极性)从气相到颗粒相转变能力。在这里,我们将 TAG 测量结果与选定半挥发性有机化合物的模型分配进行了比较。尽管 TAG 并非专为量化半挥发性有机物的气相而设计,但 TAG 测量确实可以区分特定化合物主要处于气相、主要处于颗粒相还是两者均存在。由于 TAG 数据既具有特异性又具有时间分辨率,因此这种区分足以根据碳数和化合物类别观察从气相到颗粒相的转变。实验室研究通常使用纯化合物或简单混合物来测量半挥发性有机化合物的相分配,而在大气中存在的数千种极性/非极性和有机/无机化合物的复杂混合物中,每小时都可以进行 TAG 相分配测量。