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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Exploration of the Mechanism of the Hydrolysis of Chlorine Nitrate in Small Water Clusters Using Electronic Structure Methods
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Exploration of the Mechanism of the Hydrolysis of Chlorine Nitrate in Small Water Clusters Using Electronic Structure Methods

机译：用电子结构方法探索小水团簇中硝酸氯的水解机理

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High-level electronic structure calculations have been used to study the mechanism of hydrolysis of chlorine nitrate in neutral water clusters containing three to eight solvating water molecules. The calculations clarify some of the current uncertainties in the hydrolysis mechanism. As the size of the water cluster is increased, ClONO_2 shows increasing ionization along the O_2NO-Cl bond consistent with the proposed predissociation in which the electrophilicity of the chlorine atom is enhanced, thus making it more susceptible to nucleophilic attack from a surface water molecule. A species akin to the experimentally observed intermediate, H_2OCl~+ is found to be stable in a cluster containing eight water molecules. The hydrolysis products, ionized nitric (H_3O~+/NO_3~-) and molecular hypochlorous (HOCl) acids, are found to be stable in two different types of structures, containing six and eight water molecules. For the water cluster containing six water molecules, which has a structure related to ordinary hexagonal ice, ClONO_2 is hydrolyzed to yield H_3O~+/NO_3~-/HOCl, with essentially no barrier. The calculations thus predict that hydrolysis of ClONO_2 on PSC ice aerosols can proceed spontaneously in small neutral water clusters.
机译：高级电子结构计算已用于研究中性水簇（包含三到八个溶剂化水分子）中硝酸氯的水解机理。该计算澄清了水解机理中当前的一些不确定性。随着水簇尺寸的增加，ClONO_2沿O_2NO-Cl键显示出越来越强的电离，这与拟议的预离解相符，氯原子的亲电性得到了增强，从而使其更易于受到表面水分子的亲核攻击。发现类似于实验观察到的中间体H_2OCl〜+在包含八个水分子的簇中稳定。发现水解产物离子化的硝酸（H_3O〜+ / NO_3〜-）和分子次氯酸（HOCl）在两种不同类型的结构中稳定，分别包含六个和八个水分子。对于含有六个水分子的水簇，其结构与普通的六角形冰有关，ClONO_2水解后可生成H_3O〜+ / NO_3〜-/ HOCl，基本没有阻挡层。因此，计算结果预测，PSC冰气溶胶上ClONO_2的水解可在小型中性水团簇中自发进行。

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