Generation of Supra-molecular Cluster Structure and its Binding Condition

超分子簇结构的生成及其结合条件

• 批准号: 04403002
• 负责人: NISHI Nobuyuki
• 金额: $ 22.85万
• 依托单位: KYUSHU UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for General Scientific Research (A)
• 财政年份: 1992
• 资助国家: 日本
• 起止时间: 1992 至 1994
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-04403002/
• 关键词: Cluster; Supramolecule; Ethanol; Water; X-ray diffraction; Mass spectrometry; Infrared Spectroscopy; 質量分布; 分子クラスタ; 水の構造; 疎水性水和; 溶液化学; X線回析; 分子クラスター; 酒の熟成

The structure of clusters in ethanol-water binary solutions at x_E (ethanol mole fraction) <greater than or equal>0.2 is investigated by the mass spectrometric analysis of the clusters isolated from liquid droplets and X-ray diffraction measurements of intact solution. Average numbers of water molecules (N^a) of the ethanol m-mer hydrates (5<m<15) in the mixtures at 0.2<less than or equal>x_E<less than or equal>0.8 are found to be expressed by a function of water mole fraction (x_w) : Na^a={(m/4.2) -1} ^2 (x_w+0.85), suggesting that the fundamental structure of the ethanol polymer-hydrates is invariable in thie region. An inflection point of N^a was found at x_3<approximately equal>0.2. The radial distribution functions (RDFs) fromthe X-ray measurements demonstrated a decrease of linear hydrogen bonds at 2.8 * with increasing x_E, while keeping the strongest peak at 4.8 * in 0.4<less than or equal>x_E<less than or equal>1.0. On the basis of the composition analysis of the mass spectra and the concentration dependence of RDFs, we propose the most likely model of ethanol-water binary clusters formed in the region 0.2<less than or equal>x_E<less than or equal>0.8.

通过对从液滴中分离的簇的质谱分析和完整溶液的X射线衍射测量，研究了x_E（乙醇摩尔分数）<大于或等于>0.2的乙醇-水二元溶液中簇的结构。发现0.2<小于或等于>x_E<小于或等于>0.8时混合物中乙醇m聚体水合物(5<m<15)的平均水分子数(N^a)表示为水摩尔分数 (x_w) 的函数：Na^a={(m/4.2) -1} ^2 (x_w+0.85)，表明乙醇聚合物水合物的基本结构为在该地区不变。在 x_3<约等于>0.2 处发现 N^a 的拐点。 X 射线测量的径向分布函数 (RDF) 表明，随着 x_E 的增加，线性氢键在 2.8 * 处减少，同时在 0.4 <小于或等于>x_E <小于或等于>1.0 时将最强峰值保持在 4.8 * 处。基于质谱的组成分析和RDF的浓度依赖性，我们提出了在0.2<小于或等于>x_E<小于或等于>0.8区域形成的最可能的乙醇-水二元团簇模型。

项目成果

高橋 悟: "Hydrate cluster formation of diol compounds in aqueous solution" Bulletin of Chemical Society of Japan. 68. 539-546 (1995)

高桥悟：“化合物水溶液中二醇的水合物簇形成”日本化学会通报68. 539-546（1995）。

福村 博史: "Mass Spectrometric Studies on Laser Ablation of Polystyrene" Journal of Physical Chemistry. 97. 13761-13767 (1993)

Hiroshi Fukumura：“聚苯乙烯激光烧蚀的质谱研究”物理化学杂志 97. 13761-13767 (1993)

高橋,悟: "Hydrate cluster formation of diol compounds in aqueous solution" Bulletin of Chemical Society of Japan. 68. 539-564 (1995)

Takahashi, Satoru：“化合物水溶液中二醇的水合物簇形成”日本化学会通报 68. 539-564 (1995)。

大橋 和彦: "Photodissociation Dynamics of(C_6H_6)_2^+" Journal of Chemical Physics. 98. 390-398 (1993)

Kazuhiko Ohashi：“(C_6H_6)_2^+ 的光解离动力学”化学物理杂志 98. 390-398 (1993)。

大橋和彦: "Photodissociation mechanism of benzene cluster ions on the excitation with hv=0.5-3.0eV" Laser Chemistry. (印刷中). (1995)

Kazuhiko Ohashi：“苯簇离子在 hv=0.5-3.0eV 激发下的光解离机制”激光化学（出版中）。