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Prodical Application of Environmental Catalysis through the Chemical Vapor Deposition of Silica

Research Project

Project/Area Number 10555278
Research Category

Grant-in-Aid for Scientific Research (B).

Allocation TypeSingle-year Grants
Section展開研究
Research Field 触媒・化学プロセス
Research InstitutionTottori University

Principal Investigator

NIWA Miki  Tottori Univ., Faculty of Engineering Professor, 工学部, 教授 (10023334)

Co-Investigator(Kenkyū-buntansha) KAZU Okumura  Tottori Univ., Faculty of Engineering Research Associate, 工学部, 助手 (30294341)
NAONOBU Katada  Tottori Univ., Faculty of Engineering Assistant Professor, 工学部, 助教授 (00243379)
Project Period (FY) 1998 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥11,700,000 (Direct Cost: ¥11,700,000)
Fiscal Year 2000: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 1999: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 1998: ¥9,700,000 (Direct Cost: ¥9,700,000)
KeywordsEnvironmental Catalyst / Hydrohobicity / Silica CVD / pallodium / Zeolite / Alumina / NO Removal / Catalytic Combastion
Research Abstract

The improvement of the catalytic activity and durability of Pd/zeolite catalyst for the NO-CH_4-O_2 reaction in the presence of water vapor is an important subject. We found that the much improvement in the durability was attained by the modification of the external surface of zeolite with SiO_2 monolayer through the chemical vapor deposition (CVD) due to the generation of the hydrophobic character in the external surface of zeolite. The initial activity for NO reduction was increased by the addition of the Ag, Mn into the Pd/zeolite. The combination of the addition effect of and CVD of SiO_2 layer over ZSM-5 external surface resulted in the improvement in both activity and durability of Pd for NO-CH_4-O_2 reaction.
A continuous-flow method of chemical vapor deposition of tetramethoxysilane on γ-alumina was developed for industrial utilization of silica monolayer solid-acid catalyst. The flow method caused relatively heterogeneous coverage of silicon compared to static reactor especially in the low silicon concentration region. However, the difference in the structure was small in the high silicon concentration region where the coverage arrived at almost 100%. The catalytic activity for double-bond isomerization of 1-butene and thermal stability obtained by the two methods were similar, showing that the continuous flow method was sufficient to prepare the silica monolayer catalyst industrially.
Chemical vapor deposition of Si(OCH_3)_4 was carried out on silicalite crystals in order to control the pore-opening size. Adsorption of alkanes on silicalite an CVD-silicalite was performed gravimetrically and chromatographically. It was found that the linear and branched paraffins could be separated by choosing the extent of silica deposition on silicalite.

Report

(4 results)
  • 2000 Annual Research Report   Final Research Report Summary
  • 1999 Annual Research Report
  • 1998 Annual Research Report
  • Research Products

    (27 results)

All Other

All Publications (27 results)

  • [Publications] K.Okumura, et al: "X-ray Absorption Fine Structure Study of the Formation of the Highly Dispersed PdO over ZSM-5 and the Structural change of Pd Induced by Absorption of NO"J.Phys.Chem.B. 104. 1050-1057 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] K.Okumura. et al: "Regulation of the Dispersion of PdO through the Interaction with Acid Sites of Zeolites Studied by Extended X-ray Absorption Fine Structure"J.Phys.Chem.B. 104. 9670-9675 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] J.Amano et al: "Water Vapor Tolerance of the Pd/HZSM-5 in the NO-Methane-O_2 Reaction : Its Relation with Very Strong Solid Acidity of Zeolite Support"Stud.Surf.Sci.and Catal. 130. 905-910 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] N.Katada. et al: "A Continuous-Flow Method for Chemical Vapor Deposition of Tetramethoxysilane on gamma-Alumina to Prepare Silica Monolayer"J.Chem.Eng.Jpn.. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.A.Begum. et al: "Chemical Vapor Deposition of Silica on Silicalite Crystals and shope Selective Adsorption of Paraffins"Micropor.Mesopor.mater.. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Masaki Suzuki, Jiro Amano and Miki Niwa: "CVD of Silica on Palladium-Loaded Zeolite ; A Method to Cancel the Activity Retardation by Water Vapor in the Reduction of NO"Micro.-Mesoporous Mater.. 21. 541-547 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Naonobu Katada and Miki Niwa: "Microstructure of Silica Monolayer Solid Acid Catalyst Determined by ^<29>Si NMR Spectroscopy"Res.Chem.Intermed.. 24. 481-494 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Naonobu Katada, Toshiyuki Fujii, Koji Iwata, Yasushi Hibino and Miki Niwa: "Concentration of Hydroxyl Groups on Silica Monolayer Solid Acid Catalyst"J.Catal.. 186. 478-480 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Jong-Ho Kim, Yoji Ikoma, and Miki Niwa: "Control of HY zeolite Pore-opening size by CVD of Silicon Alkoxide"Micro.- Mesoporous Mater.. 32. 37-44 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Kazu Okumura, Hideaki Tanaka and Miki Niwa: "Influence of Acid-Base Property of Support on the Toluene Combustion Activity of Palladium"Catal. Lett.. 58. 43-48 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Kazu Okumura, Jiro Amano and Miki Niwa: "EXAFS study of Pd-loaded on ZSM-5 for the Reduction of NO with Methane in the Presence of Oxygen"Chem Lett.. 997-998 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Kazu Okumura, Jiro Amano, Naoko Yasunobu and Miki Niwa: "X-ray Absorption Fine Structure Study of the Formation of the Highly Dispersed PdO over ZSM-5 and the Structural Change of Pd Induced by Adsorption of NO"J.Phys.Chem., B.. 104. 1050-1057 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Kazu Okumura and Miki Niwa: "Regulation of the Dispersion of PdO through the Interaction with Acid Sites of Zeolites Studied by Extended X-ray Absorption Fine Structure"J.Phys.Chem., B.. 104. 9670-9675 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Jiro Amano, Osamu Shoji, Kazu Okumura and Miki Niwa: "Water Vapor Tolerance of the Pd/HZSM-5 in the NO-methane-O_2 Reaction : Its Relation with Very Strong Acidity of Zeolite Support"Stud.Surf.Sci.Catal.. 130. 905-910 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Naonobu Katada, Hitoshi Fukui and Miki Niwa: "A Continuous-Flow Method for Chemical Vapor Deposition of Tetramethoxysilane on gamma-Alumina to Prepare Silica Monolayer Solid Acid Catalyst"J.Chem.Eng.Jpn..

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Hosne Ara Begum, Naonobu Katada and Miki Niwa: "Chemical Vapor Deposition of Silica on Silicalite Crystals and Shape Selective Adsorption of Paraffins"Micro.-Mesoporous Mater.. in press..

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] K.Okumura, et al.: "X-ray Absorption Fine Structure Study of the Formation of the Highly Dispersed PdO over ZSM-5 and the Structural Change of Pd Induced by Adsorption of NO"J.Phys.Chem.B. 104. 1050-1057 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] K.Okumura, et al: "Regulation of the Dispersion of PdO through the Interaction with Acid Sites of Zeolites Studied by Extended X-ray Absorption Fine Structure"J.Phys.Chem.B. 104. 9670-9675 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] J.Amano et al.: "Water Vapor Tolerance of the Pd/HZSM-5 in the NO-Methane-O_2 Reaction : Its Relation with Very Strong Solid Acidity of Zeolite Support"Stud.Surf.Sci.and Catal.. 130. 905-910 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] N.Katada, et al.: "A Continuous-Flow Method for Chemical Vapor Deposition of Tetramethoxysilane on gamma-Alumina to Prepare Silica Monolayer"J.Chem.Eng.Jpn.. (in press).

    • Related Report
      2000 Annual Research Report
  • [Publications] H.A.Begun, et al.: "Chemical Vapor Deposition of silica on Silicalite Crystals and Shape Selective Adsorption of Paraffins"Micropol.Mesopor.Mater.. (in press).

    • Related Report
      2000 Annual Research Report
  • [Publications] N.Katadaら: "Concentration of Flydroxyl Groups on Silica Monolayer"Journal of Catalysis. 186. 478-480 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] J.ーH.Kim,M.Niwaら: "Control of HYZeolite Pore-opening size by CVD of Silicon"Microporons and Mesoporous Material. 32. 37-44 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Okumuraら: "EXAFS study of Pol-loaded ZSM-5 for the Reduction of NO"Chemistry Letters. 1999. 997-998 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] K.Okumuraら: "Influence of Acid-Base Property of Support on the Toluene"Catalysis Letters. 58. 43-48 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] M.Suzuki, J.Amano, M.Niwa: "CVD of Silica on Palladium-loaded Zeolite ; A Method to Cancel the Activity Retardation by Water Vapor in the Reduction of NO" Microporous and Mesoporous Materials. 21. 541-547 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Katada, M.Niwa: "Microstructure of Silica Monolayer Solid Acid Catalyst Determined by 29S ; NMR Spectroscopy" Research on Chemical Intermediates. 24. 481-494 (1998)

    • Related Report
      1998 Annual Research Report

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Published: 1998-04-01   Modified: 2016-04-21  

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