Catalytic Performance of Active Species Prepared in Hydrophobic Mesoporous Materials
| Project/Area Number |
16560675
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| Research Category |
Grant-in-Aid for Scientific Research (C)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Catalyst/Resource chemical process
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| Research Institution | Tokyo Institute of Technology |
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Principal Investigator |
BABA Toshihide Tokyo Institute of Technology, Interdisciplinary Graduate School of Science and Engineering, Professor, 大学院・総合理工学研究科, 教授 (50165057)
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| Project Period (FY) |
2004 – 2005
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| Project Status |
Completed (Fiscal Year 2005)
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| Budget Amount *help |
¥3,200,000 (Direct Cost: ¥3,200,000)
Fiscal Year 2005: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2004: ¥2,500,000 (Direct Cost: ¥2,500,000)
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| Keywords | methane / ethene / propene / Zeolite / silver cations / カルベニウムイオン / 銀イオンクラスター / メチル化反応 / ベンゼン / トルエン / メソポーラス物質 / 疎水性 / 有機ー無幾ハイブリッド / ブレンステッド酸 / ルイス酸 / スルホ基 |
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| Research Abstract |
The heterolytic dissociation of methane over silver cationic clusters (Ag_n^+) in Ag^+-exchanged zeolites, leading to the formation of silver hydride (Ag_n-H) and CH_3^<δ+> species, which reacts with ethene to form propene around 673 K. Methane conversion of 13.2% is achieved at 673 K over Ag-ZSM-5 catalyst to form higher hydrocarbons, such as propene and toluene. Under these reaction conditions, H-ZSM-5 does not catalyze the methane conversion, only ethene being converted into higher hydrocarbons. The reaction of methane with benzene also proceeded to form toluene and xylenes over Ag-ZSM-5 at 673 K. Zeolites exchanged with metal cations such as In and Ga also activate methane in the presence of ethene. Using ^<13>C-labeled methane as a reactant, propene is shown to be a primary product from by methane and ethene. Thus, a significant proportion of propene was singly ^<13>C-labeled (^<13>CC_2H_6). When In-ZSM-5 was used as a catalyst, not only propene, but also benzene and toluene were formed. ^<13>C atoms were not found in benzene molecules produced, indicating that benzene is entirely originated from ethene. On the other hand, in toluene, ^<13>C atoms are found in toluene, and singly ^<13>C-labeled toluene (^<13>CC_6H_8) was formed. This implies that toluene is formed by the reaction of benzene with methane, though there is a possibility that it is formed by the reaction of propene with n-butenes formed by the dimerization of ethene. The former the reaction path was confirmed by direct reaction of ^<13> _CH_4 with benzene.
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Report
(3 results)
Research Products
(13 results)
