2003 Fiscal Year Final Research Report Summary
Fixation of functional Molecules Confined to One-dimentional Porous Crystal with Nanometer-scale Quantum Channels
| Project/Area Number |
13440201
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Inorganic chemistry
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| Research Institution | Osaka City University |
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Principal Investigator |
TADOKORO Makoto Osaka City University, Graduate School of Science, Professor, 大学院・理学研究科, 助教授 (60249951)
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| Project Period (FY) |
2001 – 2003
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| Keywords | Hydrogen Bond / Ziolite / Crystal Engineering / Supra-molecular Chemistry / Nanosience / Ruthenium Complex / Molecular Crystal / Electrochemistry |
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| Research Abstract |
Research on microporous solids has focused largely on inorganic materials such as zeolites. Although syntheses of fragments of these prototypes have been achieved, extensions to three-dimensional networks by conventional synthesis have been difficult to realize. One approach to rational design of such networks with these fragments has been achieved by using the coordinating and intermolecular hydrogen-bonding properties, the geometly, and the composition of transition metal complexes which are naturally predisposed to form a certain array of several well categorized solid networks. A goal of this research has been the design of new functional materials without restraint at the properties of zeolite such as selective adsorption and catalytic activity. The tools of molecular synthesis of hydrogen-bonded coordination compounds would be useful to engineer new types of microporous solids constructed by transition metal ions and hydrogen bonding. A design based on a modular approach using bu
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ilding blocks [M^<III>(Hbim)_3] (M = Co) and trimesic acids forms a crystal structure with extended honeycomb sheets (diameter of porosity ca. 16Å). The whole structure with 1-D channels results from stacking of the layers along the c axis. In this study we have placed nanometer-scale water clusters within the porous crystal formed from molecular blocks specifically designed to investigate the molecular dynamics of confined water molecules. X-ray crystallography of a crystal filled with water has demonstrated that water clusters found in a one-dimensional nanochannel consist of multi-layered water structure with hydrogen bonding networks. The water-tubes exhibit continuous dynamics resembling a water-ice transition, which produces a "three-layered ice" state below Ca. -38℃. In the ice state, we have observed novel fragments of water clusters in a cubic ice phase I_c of similar structure. The fragment was recognized as a distinct structural model of the crystal embryo in heterogeneous nucleation on an ice I_c. Furthermore, they demonstrated the existence of a unique water tetramer containing water molecules with three nearest neighbouring hydrogen bonds without normal tetrahedral ones. Less
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