| 研究実績の概要 |
The goal of this research is to understand the reaction mechanism of solid-state catalytic metathesis reaction that takes place on the surface of the MTO on ZnCl2//meso-Al2O3 catalyst, and to apply the obtained knowledge for the development of novel catalytic system. To achieve this goal, the applicant conducted the mechanistic studies in a following stepwise manner.
Mechanistic study consists of (1) preparation of MTO catalyst supported by the ZnCl2-modified γ-alumina (γ-Al2O3), (2) solid-state NMR experiment using 13C-labeled MTO on ZnCl2//γ-Al2O3, which will be carried out with a (3) comparison with the analysis of newly developed 13C-labeled MTO on ZnCl2//meso-Al2O3 to understand the factors involved in the high efficiency toward olefin metathesis. Then, the obtained information on the active species will be subjected to (4) the application to develop novel heterogeneous catalytic system using porous materials.
This investigation was carried out to complete the synthesis of 13C-labeled MTO, followed by the measurement of 13C-labeled MTO on γ-Al2O3 via solid-state NMR. Moreover, the preparation of 13C-labeled MTO on meso-Al2O3 has also been achieved; yet, the effect of ZnCl2 additive to the meso-Al2O3 catalyst for high efficiency in metathesis reaction could not be clearly explained. Facing this difficulty, completely new approach was designed. To develop the novel catalytic reactions using porous materials, trapping unstable hemiaminals inside the widely available zeolite has currently been studied to search for their further application in organic reactions.
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