2016 Fiscal Year Research-status Report
特異的ヘテロ原子サイトを有する革新的ゼオライトの計算機支援合成
| Project/Area Number |
16K18284
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| Research Institution | The University of Tokyo |
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Principal Investigator |
CHAIKITTISILP W. 東京大学, 大学院工学系研究科(工学部), 助教 (70732048)
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| Project Period (FY) |
2016-04-01 – 2018-03-31
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| Keywords | ゼオライト / ナノ多孔性材料 / 触媒 |
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| Outline of Annual Research Achievements |
The objective of this research project is to synthesize zeolite possessing controlled locations of heteroatoms such as aluminum, boron, gallium, and zinc inside the zeolite frameworks with the aids of computations. Efficient uses of organic structure-directing agents (OSDAs) together with the unique characteristics of different heteroatoms are thought to alter the locations of framework heteroatoms. In the first year (平成28年度), the effects of OSDAs structures on the formation of MFI-type zeolites were intensively studied. The results suggested that only small difference in OSDA structures can remarkably affects the physico-chemical properties, including crystalline phases and morphology, of the resulting zeolites.
The effects of OSDA structures on the locations of aluminum were then studied by selecting an IFR-type zeolite as a model structure because IFR has a moderate number of crystallographic tetrahedral sites, allowing the aluminum locations to be distinguished by 27Al 3Q MAS NMR. The computational calculations suggested that the OSDAs are likely to be well fitted inside the zeolite cavities and slightly change the relative stability of aluminum sites. IFR-type zeolites synthesized with different OSDAs under an identical condition were characterized by 27Al NMR with the aid of DFT calculations. The results showed that aluminum locations of IFR-type zeolites can be tuned on a basis of energies derived from zeolite-OSDA complexes. This combined experimental and computational approach would lead to rational synthesis of zeolites with controlled aluminum locations.
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| Current Status of Research Progress |
Current Status of Research Progress
2: Research has progressed on the whole more than it was originally planned.
Reason
In the first year (平成28年度), efficient OSDAs were computationally designed. The combined computational and experimental investigations revealed the massive impacts of OSDA structures, which is a critical component for the designed synthesis of zeolites with controlled locations of heteroatoms.
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| Strategy for Future Research Activity |
In the second year (平成29年度), the works have been extended to different heteroatoms other than aluminum. In particular, the intrinsic effects of boron, gallium, and zinc on the structural chemistry of zeolites will be intensively studied with the well designed OSDAs.
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