2005 Fiscal Year Final Research Report Summary
Synthesis of Unsaturated Alcohols Catalyzed by Metal Oxide Nano Particles Incorporated in Mesoporous Materials
| Project/Area Number |
16560677
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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 | Kobe University |
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Principal Investigator |
NISHIYAMA Satoru Kobe University, Center for Environmental Management, Associate Professor, 環境管理センター, 助教授 (00156126)
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| Co-Investigator(Kenkyū-buntansha) |
TSURUYA Shigeru Kobe University, Department of Chemical Science and Engineering, Faculty of Engineering, Professor, 工学部, 教授 (00031120)
ICHIHASHI Yuichi Kobe University, Department of Chemical Science and Engineering, Faculty of Engineering, Research Associate, 工学部, 助手 (20362759)
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| Project Period (FY) |
2004 – 2005
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| Keywords | Tin / zirconium / MCM-41 / grafting method / reduction of acetophenone / MPV reduction / ammonia titration / high turn over frequency |
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| Research Abstract |
Well-dispersed Sn and Zr oxide catalysts in mesopores of MCM-41 have been studied. Conventional impregnation method usually brings about aggregation of metal oxide particles on porous materials. Template ion exchange method was applied for introducing Sn or Zr component in to the mesopores of MCM-41. The template ion exchange was carried out by dipping MCM-41 as synthesized, which includes micelle rods of the template molecules, in the corresponding aqueous or alcoholic solution of Sn or Zr. The template ions, organic ternary ammonium ions, are cations and can be exchanged by Sn^<2+> or Zr^<4+> ions. Homogeneous introduction of the metal cations was expected in the mesopores of MCM-41. The residual template ions were removed by calcination in a flowing air. During the calcination, unexpected superheating was observed. This was ascribed to combustion of the residual templates. The obtained Sn or Zr oxide supported MCM-41 indicated that the particles of Sn or Zr oxide were aggregated to
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large particles. In some cases, degradation of pore structure was also observed. To avoid superheating of the catalysts, an alternative method to remove the residual template molecules from the catalysts was investigated. The treatment of HCl was effective for removal of the residual template molecules. The obtained catalysts after the HCl treatment were able to be calcined without superheating. The dispersion of Sn and Zr was evaluated by ammonia-benzaldehyde titration. The HCl-treated catalysts indicated high dispersion of Sn or Zr in the mesopores of MCM-41. The catalytic activity of the catalysts synthesized here was evaluated by MPV reduction of acetophenone (AP) to 1-phenylethyl alcohol (1-PEA). The HCl-treated catalysts showed higher turnover frequency than the conventionally prepared MCM-41-supported Sn or Zr catalysts. The template ion exchange method and the appropriate post treatment, HCl treatment, brought about the high activity for the MPV reduction. Grafting method was also studied for preparation of Zr supported on MCM-41. Zirconium n-propoxide molecules were reacted with hydroxyl groups on the surface of MCM-41. The Zr cations were expected to be fixed tightly on MCM-41. The obtained Zr/MCM-41 indicated the high turnover frequency for the MPV reduction of AC to 1PEA.
The effective methods were developed to obtain the highly dispersed Sn and Zr oxide on MCM-41 support in this study Less
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