Ultrafine Particle Growth Rate During Biogenic Secondary Organic Matter Formation as a Function of Particle Composition, Size, and Phase

Michael S. Taylor Jr., Devon N. Higgins, Justin M. Krasnomowitz and Murray V. Johnston*, 
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Abstract

The growth rate of ultrafine seed particles by uptake of secondary organic matter (SOM) is studied with a flow tube reactor to elucidate key factors that can enhance or inhibit the rate. Through application of a time-dependent kinetic model, the molecular growth factor (GF) associated with SOM formation is determined. GF is defined as the fraction of the oxidation products from a biogenic precursor that contribute to seed particle growth. Two seed particle compositions (ammonium sulfate and ammonium bisulfate) are studied under two phase states (effloresced and deliquesced at either 10% or 60% relative humidity) for growth by two different biogenic precursors (isoprene and α-pinene). The results show: (1) ammonium sulfate seed particles give higher GFs than ammonium bisulfate seed particles, (2) increasing the water content of the seed particle increases the GF, and (3) isoprene and α-pinene show the same dependencies of GF on seed particle composition and water content. These dependencies suggest that physicochemical processes in the aqueous layer at or near the air–particle interface enhance the growth rate of particles in the 40 to 80 nm size range, which is relevant to the formation of cloud condensation nuclei.

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利用流管反应器研究了超细种子颗粒吸收次生有机物(SOM)的生长速度,以阐明提高或抑制生长速度的关键因素。通过应用随时间变化的动力学模型,确定了与 SOM 形成相关的分子生长因子 (GF)。GF 被定义为生物前体氧化产物中促进种子颗粒生长的部分。研究了两种种子颗粒成分(硫酸铵和硫酸氢铵)在两种相态(相对湿度为 10% 或 60% 的蒸发态和潮解态)下由两种不同的生物前体(异戊二烯和 α-蒎烯)生长的情况。结果表明:(1) 硫酸铵种子颗粒比硫酸氢铵种子颗粒的 GF 值更高;(2) 增加种子颗粒的含水量可提高 GF 值;(3) 异戊二烯和 α-蒎烯的 GF 值与种子颗粒成分和含水量的关系相同。这些依赖关系表明,在空气-颗粒界面或其附近的水层中的物理化学过程提高了 40 至 80 nm 粒径范围内颗粒的生长速度,这与云凝结核的形成有关。
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