| Project/Area Number |
62470069
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| Research Category |
Grant-in-Aid for General Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Research Field |
工業物理化学
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| Research Institution | Hokkaido University |
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Principal Investigator |
ICHIKAWA Masaru Catalysis Research Center, Hokkaido University, Professor, 解媒化学研究センター, 教授 (70176288)
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| Co-Investigator(Kenkyū-buntansha) |
FUKUOKA Atsushi Catalysis Research Center, Hokkaido University, Research Associate, 助手 (80189927)
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| Project Period (FY) |
1987 – 1989
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| Project Status |
Completed (Fiscal Year 1990)
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| Budget Amount *help |
¥6,000,000 (Direct Cost: ¥6,000,000)
Fiscal Year 1989: ¥500,000 (Direct Cost: ¥500,000)
Fiscal Year 1988: ¥1,200,000 (Direct Cost: ¥1,200,000)
Fiscal Year 1987: ¥4,300,000 (Direct Cost: ¥4,300,000)
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| Keywords | Cluster / Zeolite / Alkane Activation / Bimetal Catalysts / Multisite Effect / Ensemble Effect / Ligand Effect / Hydrogenolysis / クラスター / バイメタルクラスター / ゼオライト担持触媒 / 合成ガス反応 / 含酸素化合物合成 / ヒドロホルミル化反応 / 直鎖状アルコール合成 / 超強酸点の化学設計 |
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| Research Abstract |
A series of metal/bimetal catalysts have been prepared from the carbonyl clusters such as Rh_<6-X>Ir_X(CO)_<16> (X=0-6) and [Fe_2Rh_4(CO)_<16>]^<2-> which were synthesized inside NaY zeolite supercages. NaY-entrapped Rh_6, Ir_6, Rh_4Ir_2, Rh_3Ir_3, and Rh_2Ir_4 crystallites derived from the carbonyl clusters have been well characterized by FTIR, ^<129>Xe NMR, and CO/H chemisorption on their metallic structure and electronic states. The results suggested that the reduced crystallites inside NaY zeolite consisted of the cluster ensemble with the controlled metal compositions and fairly stabilized through several sequence of oxidation, reduction, and alkane hydrogenolysis. As the test reactions, hydrogenlysis of n-butane and ethane, and benzene hydrogenation were conducted. It is of interest to observe the dramatic decrease of hydrogenolysis activity by four order of magnitude across the series of clusters by increasing the number of modest Ir atoms in the active Rh ensembles, while a slight enhanacement activity for the benzene hydrogenation. For butane hydrogenolysis, the smaller Rh ensembles in the bimetallic clusters gave the maximum selectivities towards the central C-C bond scission to give C_2H_6.
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