| Project/Area Number |
13305056
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| Research Category |
Grant-in-Aid for Scientific Research (A)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
触媒・化学プロセス
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| Research Institution | YOKOHAMA NATIONAL UNIVERSITY |
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Principal Investigator |
TATSUMI Takashi YOKOHAMA NATIONAL UNIVERSITY, FACULTY OF ENGINEERING, PROFESSOR, 大学院・工学研究院, 教授 (30101108)
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| Co-Investigator(Kenkyū-buntansha) |
WU Peng YOKOHAMA NATIONAL UNIVERSITY, FACULTY OF ENGINEERING, RESEARCH ASSOCIATE, 大学院・工学研究院, 助手 (60322096)
YOSHITAKE Hideaki YOKOHAMA NATIONAL UNIVERSITY, FACULTY OF ENVIRONMENTAL AND INFORMATION SCIENCE, ASSOCIATE PROFESSOR, 大学院・環境情報研究院, 助教授 (20230716)
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| Project Period (FY) |
2001 – 2003
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| Project Status |
Completed (Fiscal Year 2003)
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| Budget Amount *help |
¥55,640,000 (Direct Cost: ¥42,800,000、Indirect Cost: ¥12,840,000)
Fiscal Year 2003: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000)
Fiscal Year 2002: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2001: ¥48,100,000 (Direct Cost: ¥37,000,000、Indirect Cost: ¥11,100,000)
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| Keywords | Titanosilicate / Zeolite / Hydrothermal Synthesis / Dry Gel Conversion Method / Fluoride Method / Liquid-Phase Oxidation / Hydrogen Peroxide / 構造可逆転換 / 層剥離 |
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| Research Abstract |
Titanosilicates containing tetrahedral Ti ions in zeolite framework prove to be attractive catalysts owing to their capability of oxidizing a variety of organic compounds with clean oxidant of hydrogen peroxide in the liquid-phase. In the last two decades, the studies have been focused on two representative titanosilicates, MFI type TS-1 and BEA type Ti-Beta. However, these two titanosilicates have a lot of difficult problems to be tackled. Medium-pore TS-a lacks the ability to oxidize bulky substrates, and there is still a large space to improve its specific activity per Ti site. Ti-Beta, on the other hand, encounters serious disadvantages of easy leaching of Ti active species probably due to its structural stacking faults. From the viewpoint of developing new heterogeneous catalytic processes for alkene epoxidation, it is urgent to prepare more efficient titanosilicates. In this study, we have succeeded in incorporating Ti into MWW zeolite of a very unique pore structure, which leads to a new generation of titanosilicate catalyst. Both hydrothermal synthesis using boric acid as a crystallization-supporting agent and postsynthesis through a reversible structural conversion result in Ti-MWW catalysts extremely active for alkene epoxidation. Ti-MWW is also converted into the catalysts with accessible reaction spaces suitable for bulky reactions by delamination or novel acid treatment.
Modification methods for developing highly active and selective catalysts from Ti-Beta have also been established. The methods involve selective poisoning of acid sites and fluorine contained within the structure of Beta zeolite, but without negative influence on the catalytic performance of framework Ti species.
Ti-containing mesoporous materials, Ti-SBA-15 and Ti-MSU-G which have higher hydrothermal stability and are stable against Ti leaching have been prepared successfully by novel postsynthesis method and direct hydrothermal synthesis, respectively.
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