Department of Chemistry, University of Alberta , Edmonton, Alberta T6G 2G2, Canada.
Environ Sci Technol. 2014 Dec 16;48(24):14309-16. doi: 10.1021/es503699b. Epub 2014 Nov 26.
Restructuring of monodisperse soot aggregates due to coatings of secondary organic aerosol (SOA) derived from hydroxyl radical-initiated oxidation of toluene, p-xylene, ethylbenzene, and benzene was investigated in a series of photo-oxidation (smog) chamber experiments. Soot aggregates were generated by combustion of ethylene using a McKenna burner, treated by denuding, size-selected by a differential mobility analyzer, and injected into a smog chamber, where they were exposed to low vapor pressure products of aromatic hydrocarbon oxidation, which formed SOA coatings. Aggregate restructuring began once a threshold coating mass was reached, and the degree of the subsequent restructuring increased with mass growth factor. Although significantly compacted, fully processed aggregates were not spherical, with a mass-mobility exponent of 2.78, so additional SOA was required to fill indentations between collapsed branches of the restructured aggregates before the dynamic shape factor of coated particles approached 1. Trends in diameter growth factor, effective density, and dynamic shape factor with increasing mass growth factor indicate distinct stages in soot aggregate processing by SOA coatings. The final degree and coating mass dependence of soot restructuring were found to be the same for SOA coatings from all four aromatic precursors, indicating that the surface tensions of the SOA coatings are similar.
由于羟基引发的甲苯、对二甲苯、乙苯和苯的氧化产生的二次有机气溶胶(SOA)的涂层,单分散烟尘团聚体的结构重排已在一系列光氧化(烟雾)室实验中进行了研究。烟尘团聚体通过使用 McKenna 燃烧器燃烧乙烯来生成,通过剥落处理,通过差分迁移率分析仪进行尺寸选择,并注入烟雾室中,在那里它们暴露于芳烃氧化的低蒸气压产物中,这些产物形成 SOA 涂层。一旦达到阈值涂层质量,团聚体的结构重排就开始发生,并且随后的重排程度随着质量增长因子的增加而增加。尽管完全加工的团聚体被显著压实,但它们不是球形的,具有质量迁移指数 2.78,因此需要额外的 SOA 来填充重构团聚体塌陷分支之间的凹陷,直到涂覆颗粒的动态形状因子接近 1。随着质量增长因子的增加,直径增长因子、有效密度和动态形状因子的趋势表明,SOA 涂层对烟尘团聚体的处理存在明显的阶段。研究发现,来自所有四种芳香族前体的 SOA 涂层对烟尘重构的最终程度和涂层质量依赖性相同,这表明 SOA 涂层的表面张力相似。