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Development of Novel Methods for Synthesizing Hydrophobic Metallosilicates

Research Project

Project/Area Number 11555212
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 InstitutionYokohama National University

Principal Investigator

TATSUMI Takashi  Faculty of Engineering, Yokohama National University, Professor, 工学部, 教授 (30101108)

Co-Investigator(Kenkyū-buntansha) TSUNEKI Hideaki  Materials & Functions Research Laboratory, Nippon Shokubai Co.Ltd. Manager, No.1 Research Section, 第1研究室長
YOSHITAKE Hideaki  Institute of Environmental Science and Technology, Yokohama National University, Associate Professor, 環境科学研究センター, 助教授 (20230716)
Project Period (FY) 1999 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥12,400,000 (Direct Cost: ¥12,400,000)
Fiscal Year 2000: ¥2,700,000 (Direct Cost: ¥2,700,000)
Fiscal Year 1999: ¥9,700,000 (Direct Cost: ¥9,700,000)
KeywordsZeolites / Hydrogen peroxide oxidation / Titanosilicate / Hydrophobicity / MFI structure / BEA structure / MWW structure / エポキシ化 / 過酸化水素 / 水熱合成 / 固相合成 / 修飾
Research Abstract

By increasing hydrophobicity, zeolite catalysts showing high activity and selectivity for the oxidation of organic compounds with aqueous hydrogen peroxide were synthesized. The relationship between catalytic performance and either hydrophobicity or acidity was investigated for TS-1, Ti-β and Ti-MWW.Ti-β, which has 3D-12 MR channel, was able to epoxidize bulky cyclic compounds ; however, epoxides were cleaved by water to give diols, which should be due to the acidity of Ti-β. By ion-exchanging calcined Ti-β with quaternary ammonium ions, Ti-β showing high activity and selectivity for epoxidation was successfully prepared. Ammonium ion-exchanged catalyst was not selective for epoxidation because of the oxidation of ammonium ion during the reaction while ion-exchange with alkali metal ions resulted in suppression of oxidation activity. With the coexistence of boric acid, Ti-MWW was successfully crystallized to show pure phase by using either piperidine or hexamethyleneimine as a structure directing agent. Ti-MWW always contained a part of octahedral Ti species which aggregated upon the calcination to form anatase. Nevertheless, these extraframework Ti species together with a part of framework boron was removed readily by treating the as-synthesized samples with acid solutions. Ti-MWW thus pretreated was characterized as containing mainly tetrahedral Ti species in the framework sites by various spectroscopic techniques. Ti-MWW was more active for the epoxidation reactions with hydrogen peroxide than TS-1. Piperidine-directed Ti-MWW was more active than hexamethyleneimine-directed Ti-MWW.The former was hexagonal plate with small crystallite size in shape and the latter consisted of a coagulation of needle-like particles. Thus we have developed a method of obtaining titanosilicate catalysts having small crystallite size, high hydrophobicity and low acidity, which show high activity in liquid-phase oxidations.

Report

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

    (31 results)

All Other

All Publications (31 results)

  • [Publications] Takashi Tatsumi: "Intramolecular Rearrangement of Epoxides Generated In-situ over Titanium Silicate Molecular Sieves"J.Catal.,182. 349-356 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] 辰巳敬: "メタロシリケート触媒の設計と触媒反応"化学総説,41. 120-130 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Tatsumi: "UTM-1 : A Eight-Membered Ring Zeolite with the Basic Building Chains of the MFI topology"J.Phys.Chem.,B,103. 8647-8649 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Synthesis of Pure Silica NU-1 and Na-and Al-Free Ti-NU-1 Synthesized by Dry Gel Conversion Method"Microporous Mesporous Mater.,34. 1-7 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Importance of Hydrophobicity in the Liquid Phase Oxidation Catalyzed by Titanosilicate"Res.Chem.Interm.,26. 7-12 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Hydrothermal Synthesis of a Novel Titanosilicate with MWW Topology"Chem.Lett.. 774-775 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Effect of Potassium on the Catalytic Activity of TS-1"Appl.Catal.,200. 125-134 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Singularities of Ti-MWW catalysts in the oxidation of alkenes"Stud.Surf.Sci.Catal.. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "A Novel Titanosilicate with MWW Structure : I.Hyrothermal Synthesis, Elimination of Extraframework Titanium and Characterizations"J.Phys.Chem.,B,. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takaslai Tatsumi: "Intramolecular Rearrangement of Epoxides Generated In-situ over Titanium Silicate Molecular Sieves"J.Catal.. 182.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Tatsumi: "Design and Catalysis of Metallosilicates"Kikan Kagaku Sosetsu. 41.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Tatsumi: "UTM-1 : A Eight-Membered Ring Zeolite with the Basic Building Chains of the MFI topology"J.Phys.Chem., B. 103.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Synthesis of Pure Silica NU-1 and Na-and Al-Free Ti-NU-1 Synthesized by Dry Gel Conversion Method"Microporous Mesporous Mater.. 34.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Importance of Hydrophobicity in the Liquid Phase Oxidation Catalyzed by Titanosilicate"Res.Chem.Interm.. 26.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Hydrothermal Synthesis of a Novel Titanosilicate with MWW Topology"Chem.Lett..

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Effect of Potassium on the Catalytic Activity of TS-1"Appl.Catal.. 200.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "Singularities of Ti-MWW catalysts in the oxidation of alkenes"Stud.Surf.Sci.Catal.. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takashi Tatsumi: "A Novel Titanosilicate with MWW Structure : I.Hyrothermal Synthesis, Elimination of Extraframework Titanium and Characterizations"J.Phys.Chem., B. (in press.).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Takshi Tatsumi: "Intramolecular Rearrangement of Epoxides Generated In-situ over Titanium Silicate Molecular Sieves "J.Catal.. 182. 349-356 (1999)

    • Related Report
      2000 Annual Research Report
  • [Publications] 辰巳敬: "メタロシリケート触媒の設計と触媒反応"化学総説. 41. 120-130 (1999)

    • Related Report
      2000 Annual Research Report
  • [Publications] T.Tatsumi: "UTM-1 : A Eight-Membered Ring Zeolite with the Basic Building Chains of the MFI topology"J.Phys.Chem.,B. 103. 8647-8649 (1999)

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "Synthesis of Pure Silica NU-1 and Na-and Al-Free Ti-NU-1 Synthesized by Dry Gel Conversion Method"Microporous Mesporous Mater.. 34. 1-7 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "Importance of Hydrophobicity in the Liquid Phase Oxidation Catalyzed by Titanosilicate"Res.Chem.Interm.. 26. 7-12 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "Hydrothermal Synthesis of a Novel Titanosilicate with MWW Topology"Chem.Lett.. 774-775 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "Effect of Potassium on the Catalytic Activity of TS-1"Appl.Catal.. 200. 125-134 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "Singularities of Ti-MWW catalysts in the oxidation of alkenes"Stud.Surf.Sci.Catal.. (in press).

    • Related Report
      2000 Annual Research Report
  • [Publications] Takashi Tatsumi: "A Novel Titanosilicate with MWW Structure : I.Hyrothermal Synthesis, Elimination of Extraframework Titanium and Characterizations"J.Phys.Chem.,B,. (in press).

    • Related Report
      2000 Annual Research Report
  • [Publications] T.Tatsumi,K.A.Koyano,N.Igarashi: "Acticity Enhancement by Trimethylsilylation of Ti-containing Mesoporous Molecular Sieve Catalysts for Oxidation of Alkenes and Alkanes with H_2O_2"Stud. Surf. Sci. Catal. 121. 221-226 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Tatsumi,Q.Xia,Nizamidin Jappar: "Characteristics of Liquid Phase Oxidation over Ti-Beta Zeolite Synthesized by a Dry gel Conversion Method"Proceedings of the 12th International Zeolite Conference. 1391-1398 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] A.Bhaumik,T.Tatsumi: "Synthesis of Pure Silica NU-1 and Na- and Al-Free Ti-NU-1 Synthesized by Dry Gel Conversion Method"Microporous Mesoporous Mater.. 34. 1-7 (2000)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Tatsumi: "Importance of Hydrophobicity in the Liquid Phase Oxidation Catalyzed by Titanosilicate"Res. Chem. Interm.. 26. 7-12 (2000)

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2016-04-21  

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