Elucidation of Aqueous Solution Surface Structure and Its Role in AtomosphericChemical Reaction Process

水溶液表面结构及其在大气化学反应过程中的作用的阐明

• 批准号: 20750003
• 负责人: ISHIYAMA Tatsuya
• 金额: $ 2.41万
• 依托单位: Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Young Scientists (B)
• 财政年份: 2008
• 资助国家: 日本
• 起止时间: 2008 至 2009
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-20750003/
• 关键词: 表面; 界面; 気液界面; 不均質大気化学; 分子動力学シミュレーション; 和周波発生スペクトル; 硫酸水溶液; 電気二重層

Structure of air/aqueous sulfuric acid solution interface, which plays an important role in atomospheric chemical reaction processes, was analyzed by molecular dynamics simulations. Our simulations suggest that the aqueous sulfuric acid solution surface at low concentration condition (0.02x, x : mole fraction) has cation at topmost surface layer region and anion at submonolayer region, which forms relatively strong electric double layer structure induced by the dissociating ions. On the other hand, ions in the surface region at high concentration condition (0.3x), which is a similar concentration to the atomospheric sulfuric acid aerosols, are completely in the first dissociation process of sulfuric acid, as well as the low concentration condition. However the electric double layer structure disappears at the surface, contrary to the low concentration condition. These findings provide a physicochemical basis for the construction of the atmospheric chemical reaction model.

采用分子动力学模拟方法对大气化学反应过程中起重要作用的空气/硫酸水溶液界面结构进行了分析。模拟结果表明，在低浓度条件下（0.02x，x：摩尔分数），硫酸水溶液表面在最上层区域为阳离子，在亚单层区域为阴离子，在解离离子的诱导下形成较强的双电层结构。另一方面，在与大气硫酸气溶胶浓度相近的高浓度条件（0.3x）下，表面区域的离子完全处于硫酸的第一解离过程，以及低浓度条件。然而，双电层结构在表面消失，与低浓度条件相反。这些结果为建立大气化学反应模式提供了物理化学基础。

项目成果

水表面における分子間配向相関の振動スペクトル応答

水面分子间取向关系的振动光谱响应

• 发表时间: 2009
• 作者: 石山達也;森田明弘
• 通讯作者: 森田明弘

硫酸水溶液表面構造と和周波発生スペクトルの分子動力学計算

硫酸水溶液表面结构及和频发生谱的分子动力学计算

• 发表时间: 2009
• 作者: K. Takahashi;T. Kaneko;R. Hatakeyama;越智義浩;石山達也
• 通讯作者: 石山達也

Vibrational Spectroscopic Response of Intermolecular Orientational Correlation at the Water Surface

• DOI: 10.1021/jp9060957
• 发表时间: 2009-09-17
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY C
• 影响因子: 3.7
• 作者: Ishiyama, Tatsuya;Morita, Akihiro
• 通讯作者: Morita, Akihiro

Analysis of anisotropic local field in sum frequency generation spectroscopy with the charge response kernel water model

• DOI: 10.1063/1.3279126
• 发表时间: 2009-12-28
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Ishiyama, Tatsuya;Morita, Akihiro
• 通讯作者: Morita, Akihiro

Recent progress in theoretical analysis of vibrational sum frequency generation spectroscopy.

• DOI: 10.1039/b808110g
• 发表时间: 2008-09
• 期刊: Physical chemistry chemical physics : PCCP
• 作者: A. Morita;T. Ishiyama