Jang Myoseon, Czoschke Nadine M, Northcross Amanda L, Cao Gang, Shaof David
Department of Environmental Sciences and Engineering, CB# 7431, Rosenau Hall, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina, 27599, USA.
Environ Sci Technol. 2006 May 1;40(9):3013-22. doi: 10.1021/es0511220.
A predictive model for secondary organic aerosol (SOA) formation by both partitioning and heterogeneous reactions was developed for SOA created from ozonolysis of alpha-pinene in the presence of preexisting inorganic seed aerosols. SOA was created in a 2 m3 polytetrafluoroethylene film indoor chamber under darkness. Extensive sets of SOA experiments were conducted varying humidity, inorganic seed compositions comprising of ammonium sulfate and sulfuric acid, and amounts of inorganic seed mass. SOA mass was decoupled into partitioning (OM(P)) and heterogeneous aerosol production (OM(H)). The reaction rate constant for OM(H) production was subdivided into three categories (fast, medium, and slow) to consider different reactivity of organic products for the particle phase heterogeneous reactions. The influence of particle acidity on reaction rates was treated in a previous semiempirical model. Model OM(H) was developed with medium and strong acidic seed aerosols, and then extrapolated to OM(H) in weak acidic conditions, which are more relevant to atmospheric aerosols. To demonstrate the effects of preexisting glyoxal derivatives (e.g., glyoxal hydrate and dimer) on OM(H), SOA was created with a seed mixture comprising of aqueous glyoxal and inorganic species. Our results show that heterogeneous SOA formation was also influenced by preexisting reactive glyoxal derivatives.
针对在预先存在的无机种子气溶胶存在下α-蒎烯臭氧分解产生的二次有机气溶胶(SOA),开发了一种通过分配和非均相反应形成SOA的预测模型。SOA在一个2立方米的聚四氟乙烯薄膜室内暗箱中生成。进行了大量的SOA实验,改变了湿度、由硫酸铵和硫酸组成的无机种子成分以及无机种子质量。SOA质量被解耦为分配(OM(P))和非均相气溶胶生成(OM(H))。将OM(H)生成的反应速率常数细分为三类(快、中、慢),以考虑有机产物在颗粒相非均相反应中的不同反应活性。颗粒酸度对反应速率的影响在先前的半经验模型中进行了处理。模型OM(H)是在中强酸性种子气溶胶条件下开发的,然后外推到与大气气溶胶更相关的弱酸性条件下的OM(H)。为了证明预先存在的乙二醛衍生物(如乙二醛水合物和二聚体)对OM(H)的影响,用包含乙二醛水溶液和无机物种的种子混合物生成了SOA。我们的结果表明,预先存在的活性乙二醛衍生物也会影响非均相SOA的形成。