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Direct Observation of the Condensed Phase Development Processes by Infrared Spectroscopy of Giant Clusters

用红外光谱直接观察巨星团凝聚相的形成过程

基本信息

批准号：
17310057
负责人：
FUJII Asuka
金额：
$ 9.66万
依托单位：
Tohoku University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2005
资助国家：
日本
起止时间：
2005 至 2006
项目状态：
已结题

项目摘要

We have studied development of hydrogen bond networks in protic solvents such as water and methanol by using molecular clusters as microscopic model systems of their condensed phases, and following results have been obtained.1.Infrared spectroscopy of size-selected protonated water H^+(H_2O)_n was carried out up to n=100. It showed that a single excess proton totally changes the hydrogen bond structure of surrounding 100 water molecules.2.Infrared spectroscopy of protonated methanol H^+(MeOH)_n was also performed up to n=15. We demonstrated that the hydrogen bond network structure of protonated methanol is very different from that of protonated water, and it has much simpler structure, of which geometrical development is terminated by formation of the bicyclic structures.3.Infrared spectra of size-selected methanol-water mixed protonated clusters H^+(MeOH)_2(H_2O)_n were observed. In the two extreme cases, nm and n<<m, were studied, and the following features of the hydrogen bond network were shown. a)In the case of m<<n, a few methanol molecules are compatible with water in the hydrogen bond network, and the same three-dimensional cage structure as that in the protonated water cluster is formed. b)When a small number of water molecules are added to the hydrogen bond network of protonated methanol, structural changes of the network occur, and the proton is transferred from the methanol site to the water site.4.We also performed infrared spectroscopy of benzene cation clusters solvated by protic solvents such as water, methanol, and ammonia. We observed the solvation structure changes correlated to the proton affinity of the solvent molecule, and we found an intermolecular covalent bond formation between the benzene cation moiety and solvent molecule moiety, which can be regarded as an intermediate in the nucleophilic substitution reaction.

我们用分子团簇作为缩合相的微观模型系统，研究了质子溶剂（如水和甲醇）中氢键网络的发展，得到了以下结果：在n=100范围内对选定尺寸的质子化水H^+(H_2O)_n进行红外光谱分析。结果表明，一个多余的质子完全改变了周围100个水分子的氢键结构。对质子化甲醇H^+(MeOH)_n进行了红外光谱分析，直至n=15。我们证明了质子化甲醇的氢键网络结构与质子化水有很大的不同，它的结构要简单得多，其几何发展被双环结构的形成所终止。研究了选定尺寸的甲醇-水混合质子化团簇H^+(MeOH)_2(H_2O)_n的红外光谱。在nm和n<<m两种极端情况下，研究了氢键网络的以下特征：a)当m<<n时，氢键网络中有少量甲醇分子与水相容，形成与质子化水团簇相同的三维笼状结构。b)当少量水分子加入到质子化甲醇的氢键网络中时，网络发生结构变化，质子从甲醇位点转移到水位点。我们还进行了红外光谱的苯阳离子簇溶剂的质子溶剂，如水，甲醇和氨。我们观察到溶剂化结构的变化与溶剂分子的质子亲和力有关，我们发现苯阳离子部分与溶剂分子部分之间形成了分子间共价键，可以看作是亲核取代反应的中间体。

项目成果

期刊论文数量（0）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Magnitude and nature of interactions in benzene- (X=ethylene, acetylene) in the gas phase : Significantly different CH/π interaction of acetylene as compared with those of ethylene and methane.

气相中苯-（X=乙烯、乙炔）相互作用的强度和性质：与乙烯和甲烷相比，乙炔的 CH/π 相互作用显着不同。

DOI：
发表时间：
2007
期刊：
J.Phys.Chem.A 111(5)
影响因子：
0
作者：
Kenta Shibasaki;Asuka Fujii;Naohiko Mikami;Seiji Tsuzuki
通讯作者：
Seiji Tsuzuki

Morphology of protonated methanol clusters : An infrared spectroscopic study of hydrogen bond networks of H^+(CH_30H)_n(n=4-15)

质子化甲醇簇的形态：H^(CH_30H)_n(n=4-15)氢键网络的红外光谱研究

DOI：
发表时间：
2005
期刊：
The Journal of Physical Chemistry A 109・1
影响因子：
0
作者：
Satoko Enomoto;Mitsuhiko Miyazaki;Asuka Fujii;Naohiko Mikami;Asuka Fujii 他3名
通讯作者：
Asuka Fujii 他3名

Infrared photodissociationn spectroscopy of ammonia cluster cations (NH3)_n^+ (n=2-4) produced by vacuum ultraviolet photoionization

真空紫外光电离产生的氨簇阳离子 (NH3)_n^ (n=2-4) 的红外光解离光谱

DOI：
发表时间：
2006
期刊：
J.Chem.Phys. 125 (16)
影响因子：
0
作者：
Yoshiyuki Matsuda;Mayumi Mori;Masaki Hachiya;Asuka Fujii;Naohiko Mikami
通讯作者：
Naohiko Mikami

Laser spectroscopic investigation of salicylic acids hydrogen bonded with water in supersonic jets : Microsolvation effects for excited state proton dislocation

超音速射流中水杨酸与水氢键的激光光谱研究：激发态质子位错的微溶剂化效应

DOI：
发表时间：
2005
期刊：
The Journal of Physical Chemistry A 109・11
影响因子：
0
作者：
Y.Matsuda;M.Mori;M.Hachiya;A.Fujii;N.Mikami;Asuka Fujii 他3名;V.Venkatesan 他3名;Eman Abd El-hakam Abou El-Nasr 他4名
通讯作者：
Eman Abd El-hakam Abou El-Nasr 他4名

Infrared and ultraviolet laser spectroscopy of jet-cooled substituted salicylic acids; substitution effects on the excited state intramolecular proton transfer in salicylic acid