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DEVELOPMENT OF OXIDATION CATALYSTS UTILIZING CHARACTERISTICS OF HETEROPOLY COMPOUNDS

Research Project

Project/Area Number 09650856
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionTHE UNIVERSITY OF TOKYO

Principal Investigator

MIZUNO Noritaka  THE UNIVERSITY OF TOKYO,GRADUATE SCHOOL OF ENGINEERING,ASSOCIATE PROFESSOR, 大学院・工学系研究科, 助教授 (50181904)

Project Period (FY) 1997 – 1998
Project Status Completed (Fiscal Year 1998)
Budget Amount *help
¥3,400,000 (Direct Cost: ¥3,400,000)
Fiscal Year 1998: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 1997: ¥2,400,000 (Direct Cost: ¥2,400,000)
KeywordsHETEROPOLY COMPOUNDS / ALKANES / SELECTIVE OXIDATION / ヘチロポリ化合物
Research Abstract

1. Mono-, di-, and tri-iron-substituted polyoxometalates were synthesized and
characterized. The efficiency and activity for the utilization of hydrogen peroxide greatly depended on the iron centers and the di-iron-substituted polyoxometalate, gamma-SiW_<10>{Fe(0H_2)}_20_<38>^<6->, showed the highest efficiency of hydrogen peroxide utilization and conversion based on substrates used. It is remarkable that the efficiency of hydrogen peroxide utilization to oxygenated products reached up to ca. 100% for the oxygenation of cyclohexane catalyzed by dr-iron-substituted polyoxometalate. Such a high efficiency has never been reported. Not only cyclohexane but also n-hexane, n-pentane, and adamantane were catalytically oxygenated with high efficiency of hydrogen peroxide utilization.Methane was also oxygenated to methanol by using gamma-SiW_<10>{Fe(OH_2)}_2O_<38>^<6->. It was also suggested that di-iron-substituted polyoxometalate was stable under the conditions used and in the presence of hydrogen peroxide.
2. Keggin-type heteropolymolybdates have been found to catalyze the selective oxidation of isobutane with molecular oxygen. The preferable contents of Cs and V are 2.5 and 1, respectively, and the addition of Ni enhanced the catalytic activity for the oxidation of isobutane. The preferred content of Ni was 0.08. It was shown that isobutane oxidation is a surface-type reaction and the catalytic activity is controlled by the oxidizing ability of the catalyst surface. Cs2.5Ni0.08H1.34PVMo11O4O also catalyzed the oxidation of propane.

Report

(3 results)
  • 1998 Annual Research Report   Final Research Report Summary
  • 1997 Annual Research Report
  • Research Products

    (26 results)

All Other

All Publications (26 results)

  • [Publications] N.Mizuno: "Oxidation of Isobutane Catalyzed by Partially Salified Cesium Molybdovanadophospboric Acids" Journal of Physical Chemistry. 102. 437-443 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Liquid-phase Oxygenation of Hydrocarbons with Molecular Oxygen Catalyzed by Fe_2Ni-substituted Keggin-type Heteropolyanion" Journal of Molecular Catalysis. 117. 159-168 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Copper as an Effective Additive for Enhancemont of catalytic Activity of Cs_<2.5>H_<1.5>PVMo_<11>O_<40> for selective Oxidation of Lower Alkanes" Chemistry Letters. 621-622 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Selective Oxidation of Ephame, Propane, and Isobutane Catalyzed by Copper-containing Cs_<2.5>H_<1.5>PVMo_<11>O_<40> under Oxygen-poor Conditions" Journal of Catalysis. 178. 391-394 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Highly Efficient Utilization of Hydrogen Peroxide for Oxygenation of Alkanes Catalyzed by Di-Iron-Containing Polyoxometalate" Journal of The American Chemical Society. 120. 9267-9272 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Heterogeneous Catalysis" Chemical Reviews. 98. 199-217 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Copper as an Effective Additive for Enhancement of Catalytic Activity of Cs_<2.5>H_<1.5>PVMo_<11>O_<40> for Selective Oxidation of Lower Alkanes" Chem.Lett.621-622 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Selective Oxidation of Ethane, Propane, and Isobutane Catalyzed by Copper-containing Cs_<2.5>H_<1.5>PVMo_<11>O_<40> under Oxygen-poor Conditions" J.Catal.178. 391-394 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Highly Efficient Utilization of Hydrogen Peroxide for Oxygenation of Alkanes Catalyzed by Di-Iron-Containing Polyoxometalate Catalyst Precursor" J.Am.Chem.Soc.120. 9267-9272 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Heterogeneous Catalysis" Chem.Rev.98. 199-217 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Oxidation of Isobutane Catalyzed by Partially Salified Cesium Molybdovanadophosphoric Acids" J.Phys.Chem.102. 437-443 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Liquid-phase Oxygenation of Hydrocarbons with Molecular Oxygen Catalyzed by Fe_2Ni-substituted Keggin-type Heteropolyanion" J.Mol.Catal.117. 159-168 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] W.Randall: "Metal Complexes of the Lacunary Heteropolytungstates, PW_9O_<34>^<9-> and P_2W_<15>O_<56>^<12->" Inorg.Synth.31. 167-185 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] K.Nomiya: "Polyoxoanion-supported Atomically Dispersed Iridium (I) and Rhodium (I)" Inorg.Synth.31. 186-201 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Low-temperature Oxygenation of Methane into Formic Acid with Molecular Oxygen in the Presence of Hydrogen Catalyzed by Pd_<0.08>Cs_<2.5>H_<1.34>PVMo_<11>O_<40>" Chem.Commun.1295-1296 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] Y.Seki: "High-yield Liquid-phase Oxygenation of Methane with Hydrogen Peroxide Catalyzed by 12-Molybdovanadophosphoric Acid Catalyst Precursor" Appl.Catal.157. L47-L51 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Mizuno: "Copper as an Effective Additive for Enhancement of Catalytic Activity of Cs_<2.5>H_<1.5>PVMo_<11>O_<40> for Selective Oxidation of Lower Alkanes" Chemistry Letters. 621-622 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Mizuno: "Selective Oxidation of Ethane,Propane,and Isobutane Catalyzed by Copper-containing Cs_<2.5>H_<1.5>PVMo_<11>O_<40> under Oxygen-poor Conditions" Journal of Catalysis. 178. 391-394 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Mizuno: "Highly Efficient Utilization of Hydrogen Peroxide for Oxygenation of Alkanes Catalyzed by Di-Iron-Containing Polyoxometalate" Journal of The American Chemical Society. 120. 9267-9272 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Mizuno: "Heterogeneous Catalysis" Chemical Reviews. 98. 199-217 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Mizuno: "Oxidation of Isobutame Catalyzed by Partially Salifed Cesium Molybdovanadophosphoric Acids" Journal of Physical Chemistry. 102. 437-443 (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Mizuno: "Liquid-phase Oxygenation of Hydrocarbons with Molecular Oxygen Catalyzed by Fe_2Ni-substituted Keggin-type Heteropolyanion" Journal of Molecular Catalysis. 117. 159-168 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] W.Randall: "Metal Complexes of the Lacunary Heteropoly tungstates,PW_9O_<34>^<9-> and p_2W_<15>O_<56>^<12->" Inorganic Syntheses. 31. 167-185 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] K.Nomiya: "Polyoxoanion-supported Atomically Dispersed Iridium(I)and Rhodium(I)" Inorganic Syntheses. 31. 186-201 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Mizuno: "Low-temperature Oxygenation of Methane into Formic Acid with Molecular Oxygen in the Presence of Hydrogen Catalyzed by Pd_<0.08>Cs_<2.5>H_<1.34>PVMo_<11>O_<40>" Chemical Communications. 1997. 1295-1296 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Y.Seki: "High-yield Liquid-Phase Oxygenation of Methane with Hydrogen Peroxide Catalyzed by 12-Molybdovanadophosphoric Acid Catalyst Precusor" Applied Catalysis. 157. L47-L51 (1997)

    • Related Report
      1997 Annual Research Report

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Published: 1997-04-01   Modified: 2016-04-21  

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