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Requlation and Cotolysis of Strong Solid Acid Generated on Extra-Framework Aluminum

Research Project

Project/Area Number 11650809
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 InstitutionTottori University

Principal Investigator

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

Co-Investigator(Kenkyū-buntansha) OKUMURA Kazu  Tottori Univ., Faculty of Engineering Research Associate, 工学部, 助手 (30294341)
KATADA Naonobu  Tottori Univ., Faculty of Engineering Assistant Professor, 工学部, 助教授 (00243379)
Project Period (FY) 1999 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥3,000,000 (Direct Cost: ¥3,000,000)
Fiscal Year 2000: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 1999: ¥1,900,000 (Direct Cost: ¥1,900,000)
KeywordsZeolite / Ocid property / extro framework aluminum / ZSM-5 / USY / ammona TPD / EDTA / croking reaction / ZSN-5 / クラッチング反応 / 固体酸性質
Research Abstract

The relationship between the acidic property and the composition of a zeolite was precisely measured using Y-and mordenite-type samples with high aluminum contents. The number of the desorbed ammonia, showing the acid amount, was approximately same to the number of [Al]-[Na] atoms over the experimental range. This is quite different from the conventionally observed relationship where the secondary-neighboring aluminum species is formed. It is pointed out that the isomorphously substituted aluminum in zeolite generates the acid site according to the stoichiometry even when the aluminum atoms locate the secondary-neighboring sites.
Very strong acid site was observed on the zeolite ZSM-5 in measurements of temperature programmed desorption of ammonia. The site was ascribable to the non-framework aluminum, which interacted with the usual framework acid site. By impregnation of aluminum cation, the strong acid site was created at the expense of the acid site in a zeolite framework.
Conditions of a step for template molecule removal affected strongly the concentration of very strong acid site in HZSM-5. Treatment with ammonia with water at ca 373 K was also studied as a procedure to affect the solid acidity, and a similarity of acid sites created by both methods was identified. From the quantitative measurements of acid sites, it was found that the very strong acid site consisted of two Al cations. Catalytic activity for octane cracking was enhanced by the presence of very strong acid site.
Strong Bronsted acid site with a narrow distribution of acid strength and large amount, which was active for alkane cracking, was formed by Na_2H_2-ethylenediaminetetraacetic acid treatment of ultra stable Y zeolite.

Report

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

    (18 results)

All Other

All Publications (18 results)

  • [Publications] T.Kunieda, et al: "Strong Acid Sites Formed by a Combination of Framework Acid Site and Extra-Framework Cation in Porous Materials"Proceedings, 12^<th> IZC, MRS. IV. 2549-2556 (1999)

    • 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: "Acid Property of Y-and Mordenite-Type Zeolites with High Aluminum Concentration under Dry Condition"J.Phys Chem.B. 104. 7561-7564 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Y.Miyamoto, et al: "Acidity of Zeolite β with Different Si/Al_2 Ratio as Measured by Temperature Programmed Desorption of Ammonia"Micropor.Mesopor.Mater. 40. 271-281 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] 片田 ら: "アンモニア昇温脱離法による固体酸性質測定"触媒. 42. 218-222 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] 丹羽 ら: "アンモニアの昇温脱離法によるゼオライト固体酸性質の研究"表面. 37. 371-382 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Kunieda, N.Katada, and M.Niwa: "Strong Acid Sites Formed by a Combination of Framework Acid Site and Extra-framework Cation in Porous Materials as Measured by Temperature Programmed Desorption of Ammonia"Proceedings, 12^<th> International Zeolite Conference, Materials Research Society. IV-2549. (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] N.Katada, T.Miyamoto, H.A.Begum, N.Naito, M.Niwa, A.Matsumoto, and K.Tsutsumi: "Strong Acidity of MFI Type Ferrisilicate Determined by Temperature-Programmed Desorption of Ammonia"J.Phys.Chem., B. 104. 5511-5518 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Y.Miyamoto, N.Katada, and M.Niwa: "Acidity of Zeolite β with Different Si/Al_2 Ratio as Measured by Temperature Programmed Desorption of Ammonia"Microporous and Mesoporous Materials. 40. 271-281 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] N.Katada, Y.Kageyama, and M.Niwa: "Acidic Property of Y-and Mordenite-Type Zeolites with High Aluminum Concentration under Dry Conditions"J.Phys.Chem.B. 104. 7561-7564 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] S.Kohara, N.Katada, and M.Niwa: "Very Strong Acid Site in HZSM-5 Formed during the Template Removal Step ; Its Control, Structure and Catalytic Activity"13^<th> International Zeolite Congress. (in Press.).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Y.Kageyama, N.Katada, and M.Niwa: "Strong Bronsted Acidity and High Catalytic Activity for Alkane Cracking over Na_2H_2-EDTA Treated Ultra Stable Y Zeolite"Chem.Commun.. (submitted).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] T.Kunieda, et al.: "Strong Acid Sites Formed by a Combination of Framework Acid Site and Extra-Framework Calion in Porous Materials as Measured by Temperature Programmed Desorption of Ammonia"Proceedings, 12^<th> IZC, MRS. IV. 2549-2556 (1999)

    • Related Report
      2000 Annual Research Report
  • [Publications] N.Katada, et al: "Acid Property of Y- and Mordenite-Type Zeolites with High Aluminum Concentration under Dry Conditions"J.Phys.Chem.B. 104. 7561-7564 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Miyamoto, et al.: "Acidity of Zeolite β with Different Si/Al_2 Ratio as Measured by Temperature Programmed Desorption of Ammonia."Micropor, Mesopor. Mater.. 40. 271-281 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 片田 ら: "アンモニア昇温脱離法による固体酸性質測定"触媒. 42. 218-222 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 丹羽 ら: "アンモニアの昇温脱離法によるゼオライト固体酸性質の研究"表面. 37. 371-382 (1999)

    • Related Report
      2000 Annual Research Report
  • [Publications] Kunieda ら: "Source of selectivity of p-xylene Formation・・・"J.Catal. 188(2). 231-233 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Kunieda ら: "String Acid Sites Formed by a Combination of・・・"Proceedings,12th IZC,MRS. IV. 2549-2556 (1999)

    • Related Report
      1999 Annual Research Report

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

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