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1996 Fiscal Year Final Research Report Summary

Novel functions of composite catalysts derived from Pd and support metal oxides-mechanism and utilization

Research Project

Project/Area Number 07650932
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 InstitutionHokkaido University

Principal Investigator

TAKEZAWA Nobutsune  Hokkaido University, Faculty of Engineering, Professor, 工学部, 教授 (60001715)

Co-Investigator(Kenkyū-buntansha) IWASA Nobuhiro  Instructor, Faculty of Engineering, Hokkaido University, 工学部, 助手 (30223374)
FUJITA Shinichiro  Instructor, Faculty of Engineering, Hokkaido University, 工学部, 助手 (80156869)
SHIMOKAWABE Masahide  Associate Professor, Faculty of Engineering, Hokkaido University, 工学部, 助教授 (40125323)
Project Period (FY) 1995 – 1996
KeywordsPd / ZnO / Steam reforming of methanol / Dehydrogenation of methaniol / Methyl formate / Pd-Zn alloy / PtZn alloy / Novel alloy catalysts
Research Abstract

Pd/ZnO exhibited anomalously high catalytic performance for the steam reforming of methanol and the dehydrogenation to HCOOCH_3 among various supported Pd ctalysts. The selectivities for the steam reforming and the dehydrogenation to HCOOCH_3 were achieved at 99.5% and 80%, respectively. In contraast, the other supported Pd catalysts showed the selectivities of 0-40% and 0%, respectively for the steam reforming and the dehydrogenation to HCOOCH_3. The catalytic performance of Pd/ZnO for the steam reforming and the dehydrogenation was greatly improved by previously reducing the catalyst at higher temperatures. The increased catalytic performace was attributed to PdZn alloys formed in the previous reduction of the catalyst. By XP spectroscopy, it was revealed that electron transfer took place from Pd to Zn in the formation of PdZn alloys. Over the alloyed catalysts, formaldehyde species formed in the reactions were effectively attacked by -OH or CH_3O-, being transformed into CO_2 and H_ … More 2 or HCOOCH_3. Over the other catalysts containing unalloyed Pd, the formaldehyde species decomposed selectively to CO and H_2 in the steam steam reforming and the dehydrogenation of methanol. It was suggested that formaldehyde species were stabilized on positively charged Pd sites in eta^1 (O) -form in the reactions over PdZn alloys, and subjected to the nucleophilic addition of -OH or CH_3O-. On the basis of the proposed mechanism of the generation of new catalytic function of Pd, novel Pd_<3.1>Zn_<6.9> and PtZn alloy catalysts were developed. These alloys showed high selectivity for the dehydrogenation of methanol to HCOOCH_3 as well as the steam reeforming. Experimemts were carried out over Pd/ZnO catalysts prepared by various preparation methods. Pd/ZnO (10wt% Pd) obtained by precipitation of Pd (II) and Zn (II) with a Na_2CO_3 solution exhibited best performance for the steam reforming among the Pd catalysts so far studied. The activity of Pd/ZnO was twice that for Cu/SiO_2 (30wt% Cu) previously studied. Less

  • Research Products

    (24 results)

All Other

All Publications (24 results)

  • [Publications] N. Iwasa, S. Masuda, N. Ogawa, and N. Takezawa: "The Steam Reforming of Methanol over Pd/ZnO-Effect of the Formation of PdZn Alloys upon the Reaction" Appl. Catal.125. 145-157 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] N. Iwasa, S. Masuda, and N. Takezawa,: "Steam Reforming of Methanol over Ni, Co, Pd, and Pt Supported on ZnO" React. Kinet. Catal. Letters,. 55,. 349-353 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] N. Iwasa, T. Akazawa, S. Ohyama, K. Fujikawa, and N. Takezawa: "Dehydrogenation of Methanol to Methy Formate over Supported Ni, Pd, and Pt Catalysts-Anomalous Catalytic Functions of PdZn and PtZn Alloys" React. Kinet. Catal. Letters. 55. 245-250 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] S. Fujita, H.Ito, and N. Taskezawa: "Remarks on the Assignments of Temperature Programmed Desorption Peaks for Surface Species Formed on Cu/ZnO in the Methanol Synthesis from CO" Catal. Letters,. 33. 67-74 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] S. Fujita, A. M. Satriyo, G. C. Shen, and N. Takezawa,: "Mechanism of the Formation of the Precursors for the Cu/ ZnO Methanol Synthesis Catalysts by a Coprecipitation Method" Catal. Letters,. 33,. 85-92 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] S. Fujita, M. Usui, T. Hanada, and N. Taskezawa: "Methanol Synthesis from CO_2-H_2 under atomospheric pressure over Pd and Cu catalysts" React. Kinet. Catal. Letters. 56. 15-19 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] S. Fujita, M. Usui, H. Ito. and N. Takezawa: "Mechanisms of Methanol Synthesis from Carbon Dioxide and from Carbon Monoxide at Atmosheric Presslure over Cu/ZnO" J. Catal.157. 403-413 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] 岩佐信弘、増田稔、小川訓聡、竹澤暢恒: "Pd/ZnO触媒のメタノール改質に対する特異な触媒特性(予稿)" 触媒,. 486-489 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] 竹澤暢恒: "メタノール水蒸気改質触媒(特集)" 触媒. 37,. 320-326 (1995)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] 藤田進一郎、アグスサトリヨ、沈国成、金森圭徳、竹澤暢恒: "共沈法によるCu/ZnO触媒の調製-前駆体生成の機構とCO_2からのメタノール合成に対する前駆体の構造の影響(予稿)" 触媒. 38. 390-393 (1996)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] 藤田進一郎、竹澤暢恒: "気相および液相メタノール合成の機構(特集)" 触媒. 39(印刷中). (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] N.Takezawa and N. Iwasa: "Steam Reforming and Dehydrogenation of Methanol - Difference in the Catalytic Functions of Copper and Group VIII Metals" Catal. Today. (in press). (1997)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Iwasa, S.Masuda, N.Ogawa, and N.Takezawa: "The steam reforming of methanol over Pd/ZnO-Effect of the Formation of PdZn alloys upon the Reaction" Appl.Catal.125-157 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] N.Iwasa, S.Masuda, and N.Takezawa: "Steam reforming of methanol over Ni, Co, Pd, and Pt supported on ZnO" React.Kinet.Catal.Letters. 55. 349-353 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] N.Iwada, T.Akazawa, S.Ohyama, K..Fujikawa, and N.Takezawa: "Dehydrogenation of methanol to methyl formate over supported Ni, Pd, and Pt catalysts-anomalous catalytic functions of PdZn and PtZn alloys" React.Kinet.catal.Letters. 55. 245-250 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita, H.Ito, and N.Takezawa: "Remarks on the assignments of Temperature programd de-sorption peaks for surface species formed on Cu/ZuO and ZnO in the methanol synthesis from CO" Catal.Letters. 33. 67-74 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita, A.M..Satriyo, G.C.Shen and N.Takezawa: "Mechanism of the formation of the the precursors for the Cu/ZnO methanol synthesis catalysts by a coprecipitation method" Catal.Letters. 33. 85-92 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita, M.Usui, T.Hanada, and N.Takezawa: "Methanol Synthesis from CO_2-H_2 and CO-H_2 under atmospheric pressure over Pd and Cu catalysts" React.Kinet.Catal.Letters. 56. 15-19 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita, M.Usui, H.Ito, and T.Takezawa: "Mechanisms of methanol synthesis from carbon dioxide and from carbon monoxide at atmospheric pressure over Cu/ZnO" J.Catal.157. 403-413 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] N.Iwasa, S.Masuda, N.Ogawa, and N.Takezawa: "Anomalous Catalytic performance of Pd/ZnO for reforming of methanol (in Japanese)" Shokubai (Catalyst). 486-489 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] N.Takezawa: "Methanol steam reforming catalysts (review, in Japanese)" Shokubai (Catalyst). 37. 320-326 (1995)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita, A.M..Sarriyo, G.C..Shen G.C.Shen, Y.Kanamori, and N.Takezawa: "Preparatiuon of precursers for Cu/ZnO catalysts-mechanism of the formation of the precursors and effect of the structure of the precursors upon the methanol synthesis from CO_2" Shokubai (Catalyst). 38. 390-93 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] S.Fujita and N.Takezawa: "Recent mechanistic studies on the methanol synthesis in gas phase and in liquid phase (review, in Japanese)" Shokubai (Catalyst). 39 (in press). (1997)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] N.Takezawa and N.Iwasa: "Steam reforming and dehydrogenation of methanol -difference in the catalytic functions of copper and group VIII metals" Catal.Today. (in press). (1996)

    • Description
      「研究成果報告書概要(欧文)」より

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Published: 1999-03-09  

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