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In-Situ Infrared Spectroscopic Study of the Dynamics of Protons in the Cages of Zeolites

Research Project

Project/Area Number 06640760
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field 機能・物性・材料
Research InstitutionNational Science Museum

Principal Investigator

WAKABAYASHI Fumitaka  National Science Museum, Department of Science and Engineering, Curator, 理工学研究部, 研究官 (30158589)

Project Period (FY) 1994 – 1996
Project Status Completed (Fiscal Year 1996)
Budget Amount *help
¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 1996: ¥400,000 (Direct Cost: ¥400,000)
Fiscal Year 1995: ¥400,000 (Direct Cost: ¥400,000)
Fiscal Year 1994: ¥1,400,000 (Direct Cost: ¥1,400,000)
Keywordszeolite / acid site / acid hydroxy group / infrared spectroscopy / hydrogen bond / MTG reaction / dynamic process / probe molecule / メタノール / メトキシ種 / 水 / 動的挙動 / 酸性度 / 窒素 / 希ガス / プロトン移動 / ジメチルエーテル
Research Abstract

The interaction between small molecules and hydroxyl groups in the cages of H-form zeolites was systematically investigated by means of in-situ transmission infrared spectroscopy. The main purpose of this research is to clarify the fundamental processes taking place in zeolite catalysis, which would give the fundamental understanding of the acidity of zeolites at molecular level.
(1) The Interaction between small and weakly basic molecules : The interaction of diatomic molecules such as H_2, O_2, and N_2, and rare gases such as He, Ar, Kr and Xe with the representative H-form zeolites, H-MOR,H-Y and H-ZSM-5 were investigated. These molecules except for He form hydrogen bonding with the acidic OH groups. It was revealed out that we can characterize the acidity of the zeolites using the IR data of the interaction.
(2) The characteristics of N_2 as a probe molecules of the acid sites in zeolites : We have revealed out that N_2 can be used as the probe of acid sites. The characteristic of N_2 as the probe was examined in detail. Since N_2 is very weak base and unreactive, it serves as an excellent new type of the probe molecule that probes only the strong acid sites without changing the intrinsic nature of the acid sites. Its nature was compared with that of CO that has been widely used as the probe recent years.
(3) The absorption and reaction of the reactive molecules on the acid sites of zeolites : By using H_2, ^<18>O as absorbate, the main feature of the IR bands observed for the water adsorption was conclusively attributed to the H-bonded adsorption. The dynamic processes of the methanol conversion to dimethyl ether and the H/D exchange reaction between water and the acidic hydroxy groups were followed by means of rapid-scanning FT-IR spectroscopy.

Report

(4 results)
  • 1996 Annual Research Report   Final Research Report Summary
  • 1995 Annual Research Report
  • 1994 Annual Research Report
  • Research Products

    (29 results)

All Other

All Publications (29 results)

  • [Publications] Fumitaka Wakabayashi et al.: "Direct comparison of N_2 and CO as IR-spectroscopic probes of acid sites in H-ZSM-5 zeolite" The Journal of Physical Chemistry. 99. 10573-10580 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 2. Adsorption oxygen,hydrogen,and rare gases on H-mordenite at low temperatures" The Journal of Physical Chemistry. 99. 14805-14812 (1995)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR study of H_2^<18>O adsorption on H-ZSM-5 : direct evidence for the hydrogen-bonded adsorption of water" The Journal of Physical Chemistry. 100. 1442-1444 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 3. Adsorption of oxygen,argon,nitrogen and xenon on H-ZSM-5 at low temperatures" The Journal of Physical Chemistry. 100. 4154-4159 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "An attempt to a semi-quantitative analysis of Lewis acid sites in H-ZSM-5 zeolite using water as an IR-spectroscopic titrant" Catalysis Letters. 38. 15-19 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] T.Fujino et al.: "FT-IR and quantum chemical studies of the interaction between dimethyl ether and H-ZSM-5 zeolite" The Journal of Physical Chemistry. 100. 11649-11653 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "Rapid-scanning FT-IR study on the adsorptions of methanol and water on H-ZSM-5 zeolite" Studies in Surface Science and Catalysis. 105. 1739-1746 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR study of the interaction between oxygen,argon,helium,nitrogen,and xenon with hydroxyl groups in H-Y zeolite at low temperatures" Microporous Materials. 8. 29-37 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "A new method for characterizing solid surface acidity-An infrared spectroscopic method using probe molecules such as N_2 and rare gases" Catalysis Surveys from Japan. 1(印刷中). (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "Direct comparison of N_2 and CO as IR-spectroscopic probes of acid sites in H-ZSM-5 zeolite" The Journal of Physical Chemistry. 99. 10573-10580 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 2. Adsorption of oxygen, hydrogen, and rare gases on H-mordenite at low temperatures." The Journal of Physical Chemistry. 99. 14805-14812 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR study of H_2^<18>O adcorption on H-ZSM-5 : direct evidence for the hydrogen-bonded adsorption of water." The Journal of Physical Chemistry. 100. 1442-1444 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 3. Adsorption of oxygen, argon, nitorogen, and xenon on H-ZSM-5 at low temperatures." The Journal of Physical Chemistry. 100. 4154-4159 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "An attempt to a semi-quantiative analysis of Lewis acid sites in H-ZSM-5 zeolite using water as an IR-spectroscopic titrant." Catalysis Letters. 38. 15-19 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] T.Fujino et al.: "Ft-IR and quantum chemical studies of the interaction between dimethyl ether and H-ZSM-5 zeolite." The Journal of Physical Chemistry. 100. 11649-11653 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "Rapid-scanning FT-IR study on the adsorptions of methanol and water on H-ZSM-5 zeolite." Studies in Surface Science and Catalysis. 105. 1739-1746 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "FT-IR study of the interaction between oxygen, argon, helium, nitrogen, and xenon with hydroxyl groups in H-Y zeolite at low temperatures." Microporous Materials. 8. 29-37 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Fumitaka Wakabayashi et al.: "A new method for characterizing solid surface acidity-An infrared spectroscopic method using probe molecules such as N_2 and rare gases." Catalysis Surveys from Japan. Vol.1, No.2 (in press.). (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] F.Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 3.Adsorption of oxygen,argon,nitrogen,and xenon on H-ZSM-5 at low temperatures." The Journal of Physical Chemistry. 100. 4154-4159 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "An attempt to a semi-quantitative analysis of Lewis acid sites in H-ZSM-5 zeolite using water as an IR-spectroscopic titrant." Catalysis Letters. 38. 15-19 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] T.Fujino et al.: "FT-IR and quantum chemical studies of the interaction between dimethyl ether and H-ZSM-5 zeolite." The Journal of Physical Chemistry. 100. 11649-11653 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "Comments on “N_2 asorption at 77 K on H-mordenite and alkali-metal exchanged mordenites : an IR study"" The Journal of Physical Chemistry. 100. 18882-18882 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "Rapid-scanning FT-IR study on the adsorptions of methanol and water on H-ZSM-5 zeolite." Studies in Surface Science and Catalysis. 105. 1739-1746 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "FT-IR study of the interaction between oxygen,argon,helium,nitrogen,and xenon with hydroxyl groups in H-Y zeolite at low temperatures." Microporous Materials. 8. 29-37 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "Direct comparison of N_2 and CO as IR-spectroscopic probes of acid sites in H-ZSM-5 zeolite." The Journal of Physical Chemistry. 99. 10573-10580 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 2.Adsorption of oxygen,hydrogen,and rare gases on H-mordenite at low temperatures." The Journal of Physical Chemistry. 99. 14805-14812 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "FT-IR study of H_2^<18>O adsorption on H-ZSM-5 : a direct evidence for the hydrogen-bonded adsorption of water." The Journal of Physical Chemistry. 100. 1442-1444 (1996)

    • Related Report
      1995 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "FT-IR studies of the interaction between zeolitic hydroxyl groups and small molecules 3.Adsorption of oxygen,argon,nitrogen,and xenon on H-ZSM-5 at low temperatures." The Journal of Physical Chemistry. 100(印刷中). (1996)

    • Related Report
      1995 Annual Research Report
  • [Publications] F.Wakabayashi et al.: "Re-examination of band deconvolutwn of the ν(OH) bands obsened for bare and Nz.adsorbed H-mardenite" Bull.Natn.Sci.Mus.,Tokyo,Ser.E. 17. 19-26 (1994)

    • Related Report
      1994 Annual Research Report

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Published: 1994-04-01   Modified: 2016-04-21  

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