Institut UTINAM-UMR 6213, CNRS/Université de Franche-Comté, 16 route de Gray, F-25030 Besancon Cedex, France.
Chemphyschem. 2010 Dec 17;11(18):4088-96. doi: 10.1002/cphc.201000364.
Quantum calculations are used to study the interaction of water molecules with carbonaceous clusters containing one single carbon atom vacancy. This is a simple but realistic way to model the active surfaces found in soot emitted by aircrafts. Prior to water adsorption, the atomic vacancy is oxidised by an approaching oxygen molecule, which is also likely to occur behind planes. The results of the calculations show that this oxidation process results in the formation of one ketone-like site and one epoxide-like site around the atomic vacancy. These sites may act as nucleation centers for water molecules, which are, however, physisorbed on the oxidized surface, leading to very weak charge transfer with the surface. Although less attractive for water than, for instance, a carboxyl-like site, the ketone-like site can also participate in the hydrophilic behavior of soot primary particles. In contrast, the epoxide-like site formed around the vacancy shows a very low affinity for water molecules.
量子计算被用于研究含有单个碳原子空位的碳质团簇与水分子的相互作用。这是一种简单但现实的方法，可以模拟飞机排放的烟尘中发现的活性表面。在水吸附之前，原子空位被一个接近的氧分子氧化，这种情况也可能发生在飞机的机翼后面。计算结果表明，这个氧化过程导致在原子空位周围形成一个酮似位点和一个环氧化物似位点。这些位点可能充当水分子的成核中心，但由于它们是物理吸附在氧化表面上，与表面的电荷转移非常微弱。尽管与羧基类位点相比，酮似位点对水分子的吸引力较小，但它也可以参与烟尘初级粒子的亲水性行为。相比之下，在空位周围形成的环氧化物似位点对水分子的亲和力非常低。
