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Development of environmentlly benign chemical processes using specific catalytic functions of zeolites

Research Project

Project/Area Number 09305054
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionTokyo Institute of Technology

Principal Investigator

YASHIMA Tatsuaki  Tokyo Institute of Technology, Graduate School of Science and Engineering, Professor, 大学院・理工学研究科, 教授 (60016409)

Co-Investigator(Kenkyū-buntansha) KOMATSU Takayuki  Tokyo Institute of Technology, Graduate School of Science and Engineering, Associate Professor, 大学院・理工学研究科, 助教授 (40186797)
OGUNI Masaharu  Tokyo Institute of Technology, Graduate School of Science and Engineering, Professor, 大学院・理工学研究科, 教授 (50144423)
Project Period (FY) 1997 – 1999
Project Status Completed (Fiscal Year 1999)
Budget Amount *help
¥37,300,000 (Direct Cost: ¥37,300,000)
Fiscal Year 1999: ¥3,800,000 (Direct Cost: ¥3,800,000)
Fiscal Year 1998: ¥12,700,000 (Direct Cost: ¥12,700,000)
Fiscal Year 1997: ¥20,800,000 (Direct Cost: ¥20,800,000)
KeywordsZeloite / Metallosilicate / Catalyst / Beckmann rearrangement / Ammoximation / Aromatization / Isobutenol / Environmentally benign process / シクロヘキサノンオキシム / ε-カプロラクタム / チタノシリケート / モルデナイト / シリカライト / ヘプタン / 異性化 / 白金 / オキシム化
Research Abstract

In order to achieve environmentally benign chemical processes, specific functions of zeolite catalysts have been utilized in some synthesis reactions, which have significant environmental problems in industry.
1. Titanosilicates with mordenite and MCM-22 structure were prepared to use as catalysts for the liquid-phase ammoximation of cyclohexanone. Characterization by UV, IR, XRD and CィイD116ィエD1OィイD22ィエD2-CィイD118ィエD1OィイD22ィエD2 exchange revealed that TiィイD14+ィエD1 was introduced into the framework of zeolite structure. These titanosilicates showed high activity and selectivity for the formation of cyclohexanone oxime.
2. Ferrierite and Ca-A zeolite were found to have high selectivity to ε-caprolactam in the Beckmann rearrangement of cyclohexanone oxime. Based on the kinetic results, the reaction scheme and the effect of solvent were discussed.
3. Zeolites having various acidity and structure were used as a bi-functional catalyst for the isomerization of heptane combined with Pt particles loaded on the surface of zeolites. Pt-β showed the highest activity for the isomerization into monomethyl hexane and dimethyl heptane.
4. Pt-Ge intermetallic compounds were supported on H-ZSM-5 by chemical vapor deposition of GeClィイD22ィエD2(acac)ィイD22ィエD2 onto Pt loaded H-ZSM-5. This catalyst gave high activity, selectivity and stability for the formation of aromatic hydrocarbons from butane because of high dehydrogenation activity and low hydrogenolysis activity.
5. Titanosilicate with MCM-22 structure was revealed to have high activity and selectivity for the formation of isobutenol from isobutene and formaldehyde. Its low acidity resulted in the long catalyst life compared with MCM-22 aluminosilicate zeolite.
From the above results, the possibility to realize the environmentally benign chemical process was discussed.

Report

(4 results)
  • 1999 Annual Research Report   Final Research Report Summary
  • 1998 Annual Research Report
  • 1997 Annual Research Report
  • Research Products

    (36 results)

All Other

All Publications (36 results)

  • [Publications] Zheng-Bao Wang: "Isomerization of *-heptane over Pt-loaded zeolite βcatalysts"Applied Catalysis A : General. 159. 119-132 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Tatsuaki Yashima: "Vapor phase Beckmann rearrangement of cyclohexanone oxime on the zeolite catalysts"Catalysis Today. 38. 249-253 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Peng Wu: "Synthesis of ferrisilicate with the MCM-22 structure"Chemical Communication. 663-664 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Peng Wu: "Ammoximation of ketones over titanium mordenite"Journal of Catalysis. 168. 400-411 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Tatsuaki Yashima: "Reaction scheme of aromatization of butane over Ga loaded HZSM-5 catalyst"石油学会誌. 41. 37-44 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Peng Wu: "Isomorphous substitution of Fe^<3+> in the framework of aluminosilicate mordenite by hydrothermal synthesis"Microporous and Mesoporous Matrials. 20. 139-147 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Tatsuaki Yashima: "Synthesis of 3-methyl-3-butene-1-ol from isobutene and formaldehyde on FeMCM-22 zeolites"Studies in Surface Science and Catalysis. 125. 507-514 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Takayuki Komatsu: "Shape-Selective Catalysis"American Chemical Society. 410 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Z.B. Wang, A. Kamo, T. Yoneda, T. Komatsu and T. Yashima: "Isomerization of n-heptane over Pt-loaded zeolite β catalysts"Appl. Catal. A : Genaral. 159. 119-132 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Yashima, N. Oka and T. Komatsu: "Vapor phase Beckmann rearrangement of cyclohexanone oxime on the zeolite catalysts"Catal. Today. 38. 249-253 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] P. Wu, T. Komatsu and T. Yashima: "Preparation of tianosilicate with mordenite structure by atom-planting method and its catalytic properties for hydroxylation of aromatics"Progress in Zeolite and Microporous Materials, Stud. Surf. Sci. Catal.. 105. 663-670 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] P. Wu, H. Lin, T. Komatsu and T. Yashima: "Synthesis of ferrisilicate with the MCM-22 structure"Chem. Commun.. 663-664 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] P. Wu, T. Komatsu and T. Yashima: "Ammoximation of ketones over titanium mordenite"J. Catal.. 168. 400-411 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] P. Wu, T. Komatsu, T. Yashima , S. Nakata ans H. Shouji: "Modification of mordenite acidity by isomorphous substitution of trivalent cations in the framework sites using the atom-planting method"Microporous Mater.. 12. 25-37 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Yashima, S. Fujita and T. Komatsu: "Reaction scheme of aromatization of butane over Ga loaded HZSM-5 catalyst"Sekiyu Gakkai-shi (J. Jpn. Petrol. Inst.). 41. 37-44 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] P. Wu, T. Komatsu and T. Yashima: "Isomorphous substitution of FeィイD13+ィエD1 in the framework of aluminosilicate mordenite by hydrothermal synthesis"Microporous and Mesoporous Mater.. 20. 139-147 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T. Yashima, Y. Katoh and T. Komatsu: "Synthesis of 3-methyl-3-butene-1-ol from isobutene and formaldehyde on FeMCM-22 zelites"'Porous Materials in Environmentally Friendly Processes' Stud. Surf. Sci. Catal.. 125. 507-514 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] T.Yashima: "Vapor phase Beckmann rearrangement of cyclohexanone oxime on the zeolite catalysts"Catalysis Today. 38. 249-253 (1997)

    • Related Report
      1999 Annual Research Report
  • [Publications] P.Wu: "Synthesis of ferrisilicate with the MCM-22 structure"Chemical Communications. 663-664 (1997)

    • Related Report
      1999 Annual Research Report
  • [Publications] P.Wu: "Ammoximation of ketones over titanium mordenite"Journal of Catalysis. 168. 400-411 (1997)

    • Related Report
      1999 Annual Research Report
  • [Publications] P.Wu: "Isomorphous substitution of Fe^<3+>in the framework of aluminosilicate mordenite by hydrothermal synthesis"Microporous and Mesoporous Materials. 20. 139-147 (1998)

    • Related Report
      1999 Annual Research Report
  • [Publications] M.Cheng: "Creation of acid sites on SBA-15 mesoporous silica by alumination"Chemistry Letters. 131-132 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Yashima: "Synthesis of 3-methyl-3-butene-1-ol from isobutene and formaldehyde on FeMCM-22 zeolites"Studies in Surface Science and Catalysis. 125. 507-514 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] T.Komatsu: "Shape-Selective Catalysis"American Chemical Society. 410 (2000)

    • Related Report
      1999 Annual Research Report
  • [Publications] P.Wu: "Isomorphous substitution of Fe^<3+> in the framework of aluminosilicate mordenite by hydrothermal synthesis" Microporous and Mesoporous Mater.20. 139-147 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Komatsu: "Cu^<2+>-exchanged MFI-ferrisilicate catalysts for the reduction of nitric oxide with ammonia" J.Chem.Soc.,Faraday Trans.94. 949-953 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Yashima: "Reaction scheme of aromatization of butane over Ga loaded HZSM-5 catalyst" Sekiyu Gakkai-shi(J.Jpn.Petrol.Inst.). 41. 37-44 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] P.Wu: "Selective formation of p-xylene with disproportionation of toluene over MCM-22 catalysts" Microporous and Mesoporous Mater.22. 343-356 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] P.Wu: "Hydroxylation of aromatics with hydrogen peroxide over titanosilicates with MOR and MFI structures:Effect of Ti peroxo species on the diffusion and hydroxylation activity" J.Phys.Chem.B. 102. 9297-9303 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.M.Ishaq: "Transformation of n-butane over HZSM-5 and other MFI type zeolites" Fuel Processing Technology. 56. 169-181 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Yashima: "Vapor phase Beckmann rearrangement of cyclohexanone oxime on the zeolite catalysts" Catalysis Today. 38. 249-253 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] P.Wu: "Preparation of titanosilicate with mordenite structure by atom-planting method and its catalytic properties for hydroxylation of aromatics" Stud. Surf. Sci. Catal.105. 663-670 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] P.Wu: "Ammoximation of ketones over titanium mordenite" J. Catal.168. 400-411 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] P.Wu: "Modification of Mordenite Acidity by lsomorphous Substitution of Trivalent Cations in the Framework Sites Using the Atom-Planting Method" Microporous Mater.12. 25-37 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] P.Wu: "Synthesis of ferrisilicate with the MCM-22 structure" Chem. Commun.663-664 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Z.B.Wang: "Isomerization of n-heptane over Pt-loaded zeolite β catalysts" Appl. Catal. A : General. 159. 119-132 (1997)

    • Related Report
      1997 Annual Research Report

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

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