Chong Esther, Marak Katherine E, Li Yang, Freedman Miriam Arak
Department of Chemistry, The Pennsylvania State University, University Park, PA 16802, USA.
Phys Chem Chem Phys. 2021 Feb 7;23(5):3565-3573. doi: 10.1039/d0cp04220j. Epub 2021 Jan 29.
Heterogeneous ice nucleation is a common process in the atmosphere, but relatively little is known about the role of different surface characteristics on the promotion of ice nucleation. We have used a series of iron oxides as a model system to study the role of lattice mismatch and defects induced by milling on ice nucleation activity. The iron oxides include wüstite (FeO), hematite (FeO), magnetite (FeO), and goethite (FeOOH). The iron oxides were characterized by X-ray diffraction (XRD) and Brunauer-Emmett-Teller (BET) surface area measurements. The immersion freezing experiments were performed using an environmental chamber. Wüstite (FeO) had the highest ice nucleation activity, which we attribute to its low lattice mismatch with hexagonal ice and the exposure of Fe-OH after milling. A comparison study of MnO and wüstite (FeO) with milled and sieved samples for each suggests that physical defects alone result in only a slight increase in ice nucleation activity. Despite differences in the molecular formula and surface groups, hematite (FeO), magnetite (FeO), and goethite (FeOOH) had similar ice nucleation activities, which may be attributed to their high lattice mismatch to hexagonal ice. This study provides further insight into the characteristics of a good heterogeneous ice nucleus and, more generally, helps to elucidate the interactions between aerosol particles and ice particles in clouds.
非均相冰核形成是大气中的常见过程,但对于不同表面特征在促进冰核形成方面的作用,人们了解相对较少。我们使用了一系列铁氧化物作为模型系统,来研究研磨引起的晶格失配和缺陷对冰核形成活性的作用。这些铁氧化物包括方铁矿(FeO)、赤铁矿(Fe₂O₃)、磁铁矿(Fe₃O₄)和针铁矿(FeOOH)。通过X射线衍射(XRD)和布鲁诺尔-埃米特-泰勒(BET)比表面积测量对这些铁氧化物进行了表征。使用环境舱进行了浸入式冻结实验。方铁矿(FeO)具有最高的冰核形成活性,我们将其归因于它与六方冰的低晶格失配以及研磨后Fe-OH的暴露。对MnO和方铁矿(FeO)分别进行研磨和筛分样品的比较研究表明,仅物理缺陷只会导致冰核形成活性略有增加。尽管分子式和表面基团存在差异,但赤铁矿(Fe₂O₃)、磁铁矿(Fe₃O₄)和针铁矿(FeOOH)具有相似的冰核形成活性,这可能归因于它们与六方冰的高晶格失配。这项研究进一步深入了解了良好的非均相冰核的特征,更广泛地说,有助于阐明气溶胶颗粒与云中冰颗粒之间的相互作用。