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New VIII group metal alloy catalysts - preparation and catalytic functions

Research Project

Project/Area Number 10650766
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 InstitutionGraduate School of Engineering, HOKKAIDO UNIVERSITY

Principal Investigator

TAKEZAWA Nobutsune  Hokkaido Univ., Grad. School of Eng., Prof., 大学院・工学研究科, 教授 (60001715)

Co-Investigator(Kenkyū-buntansha) IWASA Nobuhiro  Hokkaido Univ., Grad. School of Eng., Inst., 大学院・工学研究科, 助手 (30223374)
FUJITA Shinichiro  Hokkaido Univ., Grad. School of Eng., Inst., 大学院・工学研究科, 助手 (80156869)
SHIMOKAWABE Masahide  Hokkaido Univ., Grad. School of Eng., Asso. Prof., 大学院・工学研究科, 助教授 (40125323)
Project Period (FY) 1998 – 1999
Project Status Completed (Fiscal Year 1999)
Budget Amount *help
¥3,500,000 (Direct Cost: ¥3,500,000)
Fiscal Year 1999: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 1998: ¥2,800,000 (Direct Cost: ¥2,800,000)
KeywordsPd alloys / Pt alloys / Dehydrogenation of alcohols / Methyl formate / Ethyl acetate / Formaldehyde / Acetaldehyde / Hydrogenolysis / 水酸化分解 / 脱カルボニル / Pd / ZnO触媒 / Zn / メタノール水蒸気改質 / 昇温還元
Research Abstract

Pd supported on ZnO, GaィイD22ィエD2OィイD23ィエD2, InィイD22ィエD2OィイD23ィエD2, or CdO, Pt supported on ZnO, GaィイD22ィエD2OィイD23ィエD2, or InィイD22ィエD2OィイD23ィエD2, or Ru supported on InィイD22ィエD2OィイD23ィエD2 exhibited anomalously high selectivity for (a) dehydrogenation of CHィイD23ィエD2OH to HCOOCHィイD23ィエD2 and (b) of CHィイD23ィエD2CHィイD22ィエD2OH to CHィイD23ィエD2COOCィイD22ィエD2HィイD25ィエD2, c the steam reforming of methanol, and (d) hydrogenolysis of ester (HCOOCHィイD23ィエD2 or CHィイD23ィエD2COOCィイD22ィエD2HィイD25ィエD2) to alcohol (CHィイD23ィエD2OH and CHィイD23ィエD2CHィイD22ィエD2OH ) among various supported VIII group metal catalysts. The selectivity for the reaction (a), (b), c or (d) was greatly improved upon the formation of bimetallic alloys (Pd-Zn, Pd-Ga, Pd-Ga, Pt-Zn, Pt-Ga, and Pt-In ). Over the alloyed catalysts aldehyde species (HCHO or CHィイD23ィエD2CHO) formed in the reactions were stabilized, and (1) effectively attacked by CHィイD23ィエD2O- (or, CHィイD23ィエD2CHィイD22ィエD2O-) , -OH and hydrogen, being transformed into HCOOCHィイD23ィエD2 … More (or CHィイD23ィエD2COOCィイD22ィエD2HィイD25ィエD2) and COィイD22ィエD2/HィイD22ィエD2 respectively in the dehydrogenation of CHィイD23ィエD2OH (or CHィイD23ィエD2CHィイD22ィエD2OH ) and the steam reforming of CHィイD23ィエD2OH or (2) attacked by hydrogen, being selectively converted into CHィイD23ィエD2OH ( or CHィイD23ィエD2CHィイD22ィエD2OH ) in the hydrogenolysis of HCOOCHィイD23ィエD2 (or CHィイD23ィエD2COOCィイD22ィエD2HィイD25ィエD2). Over the other catalysts containing unalloyed Pd or Pt, HCHO or CHィイD23ィエD2CHO species were readily decarbonylated to COィイD22ィエD2/HィイD22ィエD2 or CO/CHィイD24ィエD2 in dehydrogenation of CHィイD23ィエD2 or CHィイD23ィエD2CHィイD22ィエD2OH, steam reforming of CHィイD23ィエD2OH and hydrogenolysis of HCOOCHィイD23ィエD2 or CHィイD23ィエD2COOCィイD22ィエD2HィイD25ィエD2.
Mechanism of the Pd-Zn alloy formation was also studied in the reduction of Pd/ZnO catalysts. It was found that hydrogen initially retained in Pd spilled rapidly over to ZnO. The ZnO was then reduced to metallic Zn, being transformed into PdZn. Once the alloy produced, the spillover hydrogen atoms on the alloys to ZnO was greatly suppressed, resulting in the selective formation of PdZn in the course of the reduction of Pd/ZnO. Less

Report

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

    (26 results)

All Other

All Publications (26 results)

  • [Publications] N.Iwasa: "Selective PhZn Alloy Formation in the Reduction of Pd/ZnO Catalysts"Bull. Chem.Soc.Japan. 71. 1451-1455 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N.Iwasa: "New Catalytic Functions of Pd-Zn,Pd-Ga,Pd-In,Pt-Zn,Pt-Ga and Pt-In Alloys in the Conversion of Methanol"Catal.Letters. 54. 119-123 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S.Fujita: "Methanol Synthesis from CO_2 over Cu/ZnO Catalysts Prepared from Various Coppercipitated Precursors"Catal.Today. 45. 241-244 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S.Fujita: "Vapor Phase Methylation of Pyridine with CO-H_2 and CO_2-H_2 over a Ni Catalyst"React.Kinet.Catal.Letters. 67. 9-12 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 竹澤暢恒: "二酸化炭素からのメタノール合成一反応機構と触媒"季刊 化学総説. No.41. 189-194 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S.Fujita: "Vapor Phase Methylation of Pyridine with CO-H_2 over Metal Catalysts"Appl.Catal.,A General. 185. 323-327 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N.Iwasa: "Difference in the Reactivity of Acetaldehyde Intermediates in Dehydrogenation of Ethanol over Supported Pd Catalysts"Catal.Letters. 62. 179-184 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 岩佐信弘: "担持PdおよびPt触媒の合金化による触媒特性の変化(解説)"触媒. (印刷中). (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Iwasa, N. Ogawa, S. Masuda, and N. Takezawa: "Selective PdZn Alloy Formation in the Reduction of Pd/Zn Catalysts"Bull. Chem. Soc. Japan.. 71. 1451-1455 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Iwasa, T. Mayanagi, N. Ogawa, K. Sakatai, N. Takezawa: "New Catalytic Functions of Pd-Zn, Pd-Ga, Pd-In, Pt-Zn, Pt-Ga, and Pt-In Alloys in the Conversion of Methanol"Catal. Letters. 54. 119-123 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S. Fujita, Y. Kanamori, A. M. Agus, and N. Takezawa: "Methanol Synthesis from COィイD22ィエD2 over Cu/ZnO Catalysts Prepared from Various Coprecipitated Precursors"Catal. Today. 45. 241-244 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S. Fujita, N. Hiyoshi, and N. Takezawa: "Vapor Phase Methylation of Pyridine with CO-HィイD22ィエD2 and COィイD22ィエD2-HィイD22ィエD2 over a Ni Catalyst"React. Kinet. Catal. Letters. 67. 9-12 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Takezawa, S. Fujita: "Methanol Synthesis from COィイD22ィエD2 -Mechanism and Catalysts ( in Japanese)"Kikan Kagaku Sosetsu ( Chemical Review ) No. 41, Chemical Society of Japan. (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S. Fujita, N. Hiyoshi, N. Takezawa: "Vapor Phase Methylation of Pyridine with CO-HィイD22ィエD2 over Metal Catalysts"Appl. Catal. A General. 185. 323-327 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Iwasa, O. Yamamoto, R. Tamura, M. Nishikubo, and N. Takezawa: "Difference in the Reactivity of Acetaldehyde Intermediates in Dehydrogenation of Ethanol over Supported Pd Catalysts"Catal. Letters. 62. 179-184 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Iwasa and N. Takezawa: "Changes in Catalytic Performances Supported Pd and Pd upon the Formation of Alloys ( Review in Japanese )"Shokubai (Catalysts & Catalysis ). (in press). (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] S.Fujita: "Vopor Phase Methylation of Pyridine with CO-H_2 over a Ni Catalyst"React. Kinet. Catal. Letters. 67. 9-12 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 竹澤 暢恒: "二酸化炭素からのメタノール合成―反応機構と触媒"季刊 化学総説. No.41. 189-194 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] S.Fujita: "Vapor Phase Methylation of Pyridine with CO-H_2 over a Metal Catalysts"Appl. Catal., A General. 185. 323-327 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] N.Iwasa: "Difference in the Reactivity of Acetaldehyde Intermediates in Dehydrogenation of Ethanol over Supported Pd Catalysts"Catal. Letters. 62. 179-184 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 岩佐 信弘: "担持PtおよびPt触媒の合金化による触媒特性の変化(解説)"触媒、印刷中. (2000)

    • Related Report
      1999 Annual Research Report
  • [Publications] N.Iwasa,N.Ogawa,S.Masuda,and N.Takezawa: "Selective PdZn Alloy Formation in the Reduction of Pd/ZnO Catalysts" Bull.Chem.Soc.Japan. 71. 1451-1455 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Iwasa,T.Mayanagi,N.Ogawa,K.Sakata,and N.Takezawa: "New Catalytic Functions of Pd-Zn, Pd-Ga, Pd-In, Pt-Ga, and Pt-In Alloys in the Conversion of Methanol" Catal.Letters. 54. 119-123 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] S.Fujita,Y.Kanamori,A.M.Agus,and N.Takezawa: "Methanol Synthesis from CO_2 over Cu/ZnO Catalysts Prepared from Various Coprecipitated Precursors" Catal.Today. 45. 241-244 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] S.Fujita,N.Hiyoshi and N.Takezawa: "Vapor Phase Methylation of Pyridine with CO-H_2 and CO_2-H_2 over a Ni Catalyst" React.Kinet.Catal.Letters, in press.(1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] 竹澤暢恒、藤田進一郎: "二酸化炭素らのメタノール合成 -反応機構と触媒-" 化学総説. (1999)

    • Related Report
      1998 Annual Research Report

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Published: 1998-04-01   Modified: 2016-04-21  

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