Popovicheva Olga, Persiantseva Natalia M, Shonija Natalia K, DeMott Paul, Koehler Kirsten, Petters Markus, Kreidenweis Sonia, Tishkova Victoria, Demirdjian Benjamin, Suzanne Jean
Institute of Nuclear Physics, Moscow State University, Moscow, Russia.
Phys Chem Chem Phys. 2008 May 7;10(17):2332-44. doi: 10.1039/b718944n. Epub 2008 Mar 3.
The interaction of water with laboratory soots possessing a range of properties relevant for atmospheric studies is examined by two complementary methods: gravimetrical measurement of water uptake coupled with chemical composition and porosity analysis and HTDMA (humidified tandem differential mobility analyzer) inference of water uptake accompanied by separate TEM (transmission electron microscopy) analysis of single particles. The first method clarifies the mechanism of water uptake for bulk soot and allows the classification of soot with respect to its hygroscopicity. The second method highlights the dependence of the soot aerosol growth factor on relative humidity (RH) for quasi-monodisperse particles. Hydrophobic and hydrophilic soot are qualitatively defined by their water uptake and surface polarity: laboratory soot particles are thus classified from very hydrophobic to very hydrophilic. Thermal soot particles produced from natural gas combustion are classified as hydrophobic with a surface of low polarity since water is found to cover only half of the surface. Graphitized thermal soot particles are proposed for comparison as extremely hydrophobic and of very low surface polarity. Soot particles produced from laboratory flame of TC1 aviation kerosene are less hydrophobic, with their entire surface being available for statistical monolayer water coverage at RH approximately 10%. Porosity measurements suggest that, initially, much of this surface water resides within micropores. Consequently, the growth factor increase of these particles to 1.07 at RH > 80% is attributed to irreversible swelling that accompanies water uptake. Hysteresis of adsorption/desorption cycles strongly supports this conclusion. In contrast, aircraft engine soot, produced from burning TC1 kerosene in a gas turbine engine combustor, has an extremely hydrophilic surface of high polarity. Due to the presence of water soluble organic and inorganic material it can be covered by many water layers even below water saturation conditions. This soot demonstrates a gradual diameter growth factor (D(wet)/D(dry)) increase up to 1.22 at 93% relative humidity, most likely due to the presence of single particles with water soluble material heterogeneously distributed over their surface.
重量法测量吸水量并结合化学成分和孔隙率分析,以及通过加湿串联差分迁移率分析仪(HTDMA)推断吸水量,并对单个颗粒进行单独的透射电子显微镜(TEM)分析。第一种方法阐明了大量烟灰的吸水机制,并允许根据其吸湿性对烟灰进行分类。第二种方法突出了准单分散颗粒的烟灰气溶胶生长因子对相对湿度(RH)的依赖性。疏水性和亲水性烟灰通过其吸水量和表面极性进行定性定义:因此,实验室烟灰颗粒被分类为从非常疏水到非常亲水。由天然气燃烧产生的热烟灰颗粒被分类为疏水性,表面极性低,因为发现水仅覆盖表面的一半。提出将石墨化热烟灰颗粒作为极疏水且表面极性极低的颗粒进行比较。由TC1航空煤油的实验室火焰产生的烟灰颗粒疏水性较低,在相对湿度约为10%时,其整个表面可用于统计单层水覆盖。孔隙率测量表明,最初,大部分这种表面水存在于微孔中。因此,这些颗粒在相对湿度>80%时生长因子增加到1.07归因于吸水时伴随的不可逆膨胀。吸附/解吸循环的滞后强烈支持这一结论。相比之下,在燃气轮机发动机燃烧室中燃烧TC1煤油产生的飞机发动机烟灰具有极性极高的极亲水表面。由于存在水溶性有机和无机材料,即使在低于水饱和条件下,它也可以被许多水层覆盖。这种烟灰在93%相对湿度下显示出直径生长因子(D(湿)/D(干))逐渐增加,最高可达1.22,这很可能是由于存在表面不均匀分布有水溶性材料的单个颗粒。