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二元羧酸包覆对炭黑颗粒质量-迁移率关系的影响

Effects of coating of dicarboxylic acids on the mass-mobility relationship of soot particles.

作者信息

Xue Huaxin, Khalizov Alexei F, Wang Lin, Zheng Jun, Zhang Renyi

机构信息

Department of Atmospheric Sciences, Texas A&M University, College Station, Texas 77843, USA.

出版信息

Environ Sci Technol. 2009 Apr 15;43(8):2787-92. doi: 10.1021/es803287v.

Abstract

Atandem differential mobility analyzer (TDMA) and a differential mobility analyzer-aerosol particle mass analyzer (DMA-APM) have been employed to study morphology and hygroscopicity of soot aerosol internally mixed with dicarboxylic acids. The effective densities, fractal dimensions, and dynamic shape factors of soot particles before and after coating with succinic and glutaric acids are determined. Coating of soot with succinic acid results in a significant increase in the particle mobility diameter, mass, and effective density, but these properties recover to their initial values once succinic acid is removed by heating, suggesting that no restructuring of the soot core occurs. This conclusion is also supported from the observation of similar fractal dimensions and dynamic shape factors for fresh and coated/heated soot aggregates. Also, no change is observed when succinic acid-coated aggregates are cycled through elevated relative humidity (5% to 90% to 5% RH) below the succinic acid deliquescence point. When soot is coated with glutaric acid, the particle mass increases, but the mobility diameter shrinks by 10-40%. Cycling the soot aerosol coated with glutaric acid through elevated relative humidity leads to an additional mass increase, indicating that condensed water remains within the coating even at low RH. The fractal dimension of soot particles increases after coating and remains high when glutaric acid is removed by heating. The dynamic shape factor of glutaric acid-coated and heated soot is significantly lower than that of fresh soot, suggesting a significant restructuring of the soot agglomerates by glutaric acid. The results imply that internal mixing of soot aerosol during atmospheric aging leads to changes in hygroscopicity, morphology, and effective density, which likely modify their effects on direct and indirect climate forcing and deposition in the human respiratory system.

摘要

串联差分迁移率分析仪(TDMA)和差分迁移率分析仪-气溶胶颗粒质量分析仪(DMA-APM)已被用于研究与二元羧酸内混合的烟灰气溶胶的形态和吸湿性。测定了用琥珀酸和戊二酸包覆前后烟灰颗粒的有效密度、分形维数和动态形状因子。用琥珀酸包覆烟灰会导致颗粒迁移直径、质量和有效密度显著增加,但一旦通过加热去除琥珀酸,这些性质就会恢复到初始值,这表明烟灰核心没有发生结构重组。这一结论也得到了新鲜烟灰聚集体与包覆/加热后烟灰聚集体具有相似分形维数和动态形状因子的观察结果的支持。此外,当琥珀酸包覆的聚集体在低于琥珀酸潮解点的相对湿度升高(5%至90%至5%RH)下循环时,未观察到变化。当用戊二酸包覆烟灰时,颗粒质量增加,但迁移直径缩小10%-40%。使包覆有戊二酸的烟灰气溶胶在相对湿度升高的条件下循环会导致额外的质量增加,这表明即使在低相对湿度下,凝结水仍保留在包覆层内。包覆后烟灰颗粒的分形维数增加,并且在通过加热去除戊二酸后仍保持较高水平。戊二酸包覆并加热后的烟灰的动态形状因子明显低于新鲜烟灰,这表明戊二酸使烟灰团聚体发生了显著的结构重组。结果表明,大气老化过程中烟灰气溶胶的内混合会导致吸湿性、形态和有效密度发生变化,这可能会改变它们对直接和间接气候强迫以及在人类呼吸系统中沉积的影响。

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