Development of Novel Liquidphase Oxidation System by Utilizing Characteristic of Oxide Clusters

利用氧化物团簇特性开发新型液相氧化体系

基本信息

  • 批准号:
    11450303
  • 负责人:
  • 金额:
    $ 8.7万
  • 依托单位:
  • 依托单位国家:
    日本
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
  • 财政年份:
    1999
  • 资助国家:
    日本
  • 起止时间:
    1999 至 2001
  • 项目状态:
    已结题

项目摘要

The Keggin-type di-iron-substituted silicotungstate, γ-SiW_10 {Fe(OH_2)}_2O_<38>^<6-> (I), was synthesized by the reaction of the lacunary [γ-SiW_<10>O_<36>]^<8-> with Fe(NO_3)_3 in an acidic aqueous solution and isolated as the tetra-n-butyl ammonium salt (TBA-I). It was characterized by various analyzes and the structure with the oxo-bridged di-iron site was clarified. TBA-I was stable and catalyzed selective oxidation of various alkenes and alkenes with hydrogen peroxide : Cyclohexane, adamantane, n-hexane, and n-pentane were catalytically oxidized. Even lower alkenes such as methane, ethane, propane, and n-butane were catalytically oxidized. It was remarkable that the efficiency of hydrogen peroxide utilization to oxygenated products reached up to ca. 100 % for the" oxidation of cyclopean and adamantine. Alkenes were mainly deoxidized with hydrogen peroxide. It was demonstrated that the TBA-I showed high turnover number of 135-147 for the oxidation of cyctohexane with 1 atm oxygen. The catalytic activity greatly depended on structures of iron centers and TBA-I showed the highest turnover number of 135-147 for the oxidation of cyclopean with 1 atm oxygen among iron and tri-transition-metal-substituted silicotungstates.
短句来源在酸性水溶液中,由[γ-SiW_<10>O_<36>]^<8->与Fe(NO_3)_3反应合成keggin型二铁取代钨酸硅γ-SiW_10 {Fe(OH_2)}_2O_<38>^<6-> (I),分离得到四正丁基铵盐(TBA-I)。通过各种分析对其进行表征,明确了含氧桥接双铁位点的结构。tba - 1稳定,催化多种烯烃和烯烃与过氧化氢选择性氧化:环己烷、金刚烷、正己烷和正戊烷被催化氧化。甚至更低的烯烃,如甲烷、乙烷、丙烷和正丁烷也被催化氧化。值得一提的是,双氧水对氧化产物的利用效率可达100%左右,用于环己烷和金刚烷的氧化。烯烃主要用过氧化氢脱氧。结果表明,tba -1在1atm氧条件下氧化环己烷时具有较高的周转率(135 ~ 147)。催化活性很大程度上取决于铁中心的结构,tba -1在铁和三过渡金属取代的钨酸硅中以1atm氧氧化环己烷的转化率最高,为135 ~ 147。

项目成果

期刊论文数量(50)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
N. Mizuno: "Development of Selective Oxidation Catalyzed by Metal-Substituted Polyoxometalates"PETROTECH. 24. 931-936 (2001)
N. Mizuno:“金属取代的多金属氧酸盐催化选择性氧化的发展”PETROTECH。
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N.Mizuno et al.: "Comparison of Catalytic Activity and Efficiency of Hydrogen Peroxide Utilization of Di-Iron-Containing Silicotungstate with Iron Containing Complexes and The Oxidation of Methane and Ethane"Res.Chem.Interm.. 26. 193-199 (2000)
N.Mizuno 等人:“含二铁硅钨酸盐与含铁配合物的过氧化氢利用的催化活性和效率以及甲烷和乙烷的氧化的比较”Res.Chem.Interm.. 26. 193-199 (
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Y.Seki et al.: "Reaction Mechanism of Oxidation of Methane with Hydrogen Peroxide Catalyzed by 11-Molybdo-1-vanadophosphoric Acid Catalyst Precursor"J.Phys.Chem.B. 104. 5940-5944 (2000)
Y.Seki等:“11-钼-1-钒磷酸催化剂前体催化过氧化氢氧化甲烷的反应机理”J.Phys.Chem.B。
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N.Mizuno et al.: "Aqueous Phase Oxygenation of Methane with Hydrogen Peroxide Catalyzed by Di-iron-substituted Sillicotungstate"J.Catal.. 184. 550-552 (1999)
N.Mizuno 等:“二铁取代的硅钨酸盐催化的甲烷与过氧化氢的水相氧化”J.Catal.. 184. 550-552 (1999)
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    0
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N.Mizuno: "Synthesis of Di-Iron-Containing Inorganic Synzyme, γ-SiW_<10>{Fe(OH_2)}_2O^<6->_<38'> and the Liquid-Phase Oxidation Catalysis"Catal. Surv. Jpn.. 4. 149-154 (2001)
N.Mizuno:“含二铁无机合成酶,γ-SiW_<10>{Fe(OH_2)}_2O^<6->_<38> 的合成和液相氧化催化”Surv。日本.. 4. 149-154 (2001)
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MIZUNO Noritaka其他文献

New Strategy for Precise Synthesis of Polyoxometalate Catalysts with Designed Active Sites
具有设计活性位点的多金属氧酸盐催化剂的精确合成新策略
Rational Design of Efficient Fluorophores Serving as High Concentration Dopant for Liquid Crystals
合理设计高效荧光团作为液晶高浓度掺杂剂
  • DOI:
  • 发表时间:
    2023
  • 期刊:
  • 影响因子:
    0
  • 作者:
    SUZUKI Kosuke;MIZUNO Noritaka;YAMAGUCHI Kazuya;Tsuneaki Sakurai
  • 通讯作者:
    Tsuneaki Sakurai

MIZUNO Noritaka的其他文献

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{{ truncateString('MIZUNO Noritaka', 18)}}的其他基金

Development of High Performance Polyoxometalate-Based Catalysts‒From Molecular Catalysts to Nano-Structured Catalysts ‒
高性能多金属氧酸盐基催化剂的开发——从分子催化剂到纳米结构催化剂——
  • 批准号:
    24350026
  • 财政年份:
    2012
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Development of efficient supported catalysts using novel metal hydroxide precursors
使用新型金属氢氧化物前体开发高效负载催化剂
  • 批准号:
    21360391
  • 财政年份:
    2009
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Development of Selective Oxidation Catalyst by Control of Multi-Nuclear Active Site of Transition Metal and Reaction Field
控制过渡金属多核活性位点和反应场的选择性氧化催化剂的研制
  • 批准号:
    18065002
  • 财政年份:
    2006
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research on Priority Areas
Development of polyoxometalate-based selective oxidation catalysts
多金属氧酸盐选择性氧化催化剂的开发
  • 批准号:
    16206077
  • 财政年份:
    2004
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research (A)
Development of Epoxidation of Alkenes with Molecular Oxygen Catalyzed by Metal-substituted Polyoxometalates
金属取代多金属氧酸盐催化分子氧环氧化烯烃的研究进展
  • 批准号:
    14350423
  • 财政年份:
    2002
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Development of Catalytic Reaction Fiekl From Nano-to Subnano-Scale by Utilizing Properties of Large Oxide Cluster
利用大氧化物团簇的性质发展从纳米到亚纳米尺度的催化反应
  • 批准号:
    14078207
  • 财政年份:
    2002
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research on Priority Areas
DEVELOPMENT OF OXIDATION CATALYSTS UTILIZING CHARACTERISTICS OF HETEROPOLY COMPOUNDS
利用杂多化合物的特性开发氧化催化剂
  • 批准号:
    09650856
  • 财政年份:
    1997
  • 资助金额:
    $ 8.7万
  • 项目类别:
    Grant-in-Aid for Scientific Research (C)

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