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ELECTROCATALYTIC ACTIVITY OF METALS IN ELECTRO-CHEMICAL REACTION

Research Project

Project/Area Number 09450313
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 工業物理化学
Research InstitutionChiba University

Principal Investigator

HORI Yoshio  CHIBA UNIVERSITY, FACULTY OF ENGINEERING, PROFESSOR, 工学部, 教授 (20114324)

Co-Investigator(Kenkyū-buntansha) HOSHI Nagahiro  CHIBA UNIVERSITY, GRADUATE SCHOOL OF NATURAL SCIENCES, ASSISTANT PROFESSOR, 大学院・自然科学研究科, 講師 (30238729)
KOGA Osamu  CHIBA UNIVERSITY, FACULTY OF ENGINEERING, ASSOCIATE PROFESSOR, 工学部, 助教授 (60110293)
Project Period (FY) 1997 – 1999
Project Status Completed (Fiscal Year 1999)
Budget Amount *help
¥11,400,000 (Direct Cost: ¥11,400,000)
Fiscal Year 1999: ¥1,700,000 (Direct Cost: ¥1,700,000)
Fiscal Year 1998: ¥3,800,000 (Direct Cost: ¥3,800,000)
Fiscal Year 1997: ¥5,900,000 (Direct Cost: ¥5,900,000)
KeywordsCOィイD22ィエD2 / Electrochemical reduction / Metal / Electrode / Single crystal / Crystal orientation / Atomic configuration / Copper / 二酸化炭素 / エチレン / エタノール / 白金 / アセトニトリル / 電極触媒 / ニ酸化炭素 / 電極触媒活性
Research Abstract

COィイD22ィエD2 is electrochemically reduced to various products, depending on the electrode metals. Pt can reduce COィイD22ィエD2 to CO strongly adsorbed on the electrode by hydrogen atoms preadsorbed on the electrode. We studied this reaction using high index platinum single crystal electrodes. The activity of the electrodes for the electrochemical reduction of COィイD22ィエD2 depends highly on atomic configuration of the electrode. The activity order is (111) < (997) < (332) < (221) < (110) < (331) < (110). This order agrees with the step atom density of the electrode surface. We presumed that the hydrogen atoms active for the reaction are the adsorbed hydrogen atoms at the 4-fold sites of the stepped atoms.
The electrochemical reduction of COィイD22ィエD2 was also conducted with platinum electrodes in the electrolyte solution of acetonitrile-water mixtures. The main products are oxalic acid in water free acetonitrile, and formic acid in the electrolyte which contains some concentrations of water. They were obtained continuously from the platinum electrode in spite of the presence of strongly adsorbed CO on the surface. The product selectivity resembles that of Pb and Hg. The machanism was ratinalized in terms of prevention of the adsorption of the COィイD22ィエD2 anion radical on the electrode surface owing to the strongly adsorbed CO.
High index plane single crystals of copper were also studied for the electrochemical reduction of COィイD22ィエD2. The product selectivity is remarkably affected by the crystal orientation of the electrode. (111) surface is favorable for methane formation, and (100) yields more ethylene. We employed some electrodes composed mainly of (100) and small fraction of (111) steps. (711) orientation, composed of 4 atomic rows of (100) surface and (111) step gave high ethylene selectivity. The ethylene formation may be activated by the presence of (111) step in (100) atomic configuration.

Report

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

    (32 results)

All Other

All Publications (32 results)

  • [Publications] 堀、高橋、吉浪、村田: "Electrochemical Reduction of CO at a Copper Electrode"J. Phys. Chem. B. 101(36). 7075-7081 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 星、鈴木、堀: "Catalytic activity of CO_2 reduction rate on Pt single crystal electrodes Pt(S)-[n(111)x(111)], Pt(S)-[n(111)x(100)] and Pt(S)-[n(100)x(111)]"J. Phys. Chem. B. 101(42). 8520-8524 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 星、加藤、堀: "Electrochemical Reduction of CO_2 on Single Crystal Electrodes of Silver Ag(111), Ag(100) and Ag(110)"J. Electroanal. Chem.. 440(1). 283-286 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 古賀、松尾、山崎、堀: "Infrared Spectroscopic Observation of Intermediate Species on an Ni and an Fe Electrode in the Electrochemical Reduction of CO_2 and CO to Hydrocarbons"Bull. Chem. Soc. Jpn.. 71(2). 315-320 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 古賀、松尾、星、堀: "Charge Displacement Adsorption of Carbon Monoxide on [110] Zone Copper Single Crystal Electrodes in Relation with PZC"Electrochim. Acta. 44(6-7). 903-907 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 堀、古賀、渡辺、松尾: "FTIR Measurements of Charge Displacement Adsorption of CO on Polyand Single Crystal (100) of Cu Electrodes"Electrochim. Acta. 44(8-9). 1389-1395 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 星、川谷、工藤、堀: "Significant Enhancement of the Electrochemical Reduction of CO_2 at the Kink Sites on Pt(S)-[n(110)x(100)] and Pt(S)-[n(100)x(110)]"J. Electroanal. Chem.. 467(1). 67-73 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 星、村上、富田、堀: "Electrochemical reduction of CO_2 on the low index planes of platinum in acetonitrile"Electrochemistry. 67(12). 1144-1146 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, M. Noma T. Suzuki, and Y. Hori: "Structural Effect on the Rate of COィイD22ィエD2 Reduction on Single Crystal Electrodes of Palladium."J. Electroanal. Chem.. 421(1). 15-18 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Y. Hori, R. Takahashi, Y. Yoshinami, A. Murata: "Electrochemical Reduction of CO at a Copper Electrode."J. Phys. Chem. B. 101(36). 7075-7081 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, T. Suzuki, and Y. Hori: "Catalytic activity of COィイD22ィエD2 reduction rate on Pt single crystal electrodes Pt(S)-[n(111)x(111)], Pt(S)-[n(111)x(100)] and Pt(S)-[n(100)x(111)]."J. Phys. Chem. B. 101(42). 8520-8524 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, M. Kato, and Y. Hori: "Electrochemical Reduction of COィイD22ィエD2 on Single Crystal Electrodes of Silver Ag(111), Ag(100) and Ag(110)."J. Electroanal. Chem.. 440(1). 283-286 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] O. Koga, T. Matsuo, H. Yamazaki, and Y. Hori: "Infrared Spectroscopic Observation of Intermediate Species on an Ni and an Fe Electrode in the Electrochemical Reduction of COィイD22ィエD2 and CO to Hydrocarbons."Bull. Chem. Soc. Jpn.. 71(2). 315-320 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] O. Koga, T. Matsuo, N. Hoshi, and Y. Hori: "Charge Displacement Adsorption of Carbon Monoxide on [110] Zone Copper Single Crystal Electrodes in Relation with PZC."Electrochim. Acta. 44(6-7). 903-907 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Y. Hori, O. Koga, Y. Watanabe, and T. Matsuo: "FTIR Measurements of Charge Displacement Adsorption of CO on Poly- and Single Crystal (100) of Cu Electrodes."Electrochim. Acta. 44(8-9). 1389-1395 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, S. Kawatani, M. Kudo, and Y. Hori: "Significant Enhancement of the Electrochemical Reduction of COィイD22ィエD2 at the Kink Sites on Pt(S)-[n(110)x(100)] and Pt(S)-[n(100)x(110)]."J. Electroanal. Chem.. 467(1). 67-73 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, T, Murakami, Y. Tomita, and Y. Hori: "Electrochemical reduction of COィイD22ィエD2 on the low index planes of platinum in acetonitrile."Electrochemistry. 67(12). 1144-1146 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] Nagahiro Hoshi, Kyoko Kagaya and Yoshio Hori: "Voltammograms of the single crystal electrodes of palladium in aqueous sulfuric acid electrolyte : Pd(S)-[n(111)×(111)] and Pd(S)-[n(100)×(111)]"J. Electroanal. Chem.. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] N. Hoshi, and Y. Hori: "Electrochemical reduction of carbon dioxide at a series of platinum single crystal electrodes."Electrochim. Acta. (in press).

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1999 Final Research Report Summary
  • [Publications] 星、川谷、工藤、堀: "Significant Enhancement of the Electrochemical Reduction of CO_2 at the Kink Sites on Pt(S)-[n(110)x(100)]and Pt(S)-[n(100)x(110)]"J. Electroanal. Chem.. 467(1). 67-73 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 星、村上、富田、堀: "Electrochemical reduction of CO_2 on the low index planes of platinum in acetonitrile"Electrochemistry. 67(12). 1144-1146 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 星、加賀谷、堀: "Voltammograms of the single crystal electrodes of palladium in aqueous sulfuric acid electrolyte: Pd(S)-[n(111)×(111)] and Pd(S)-[n(100)×(111)]"J. Electroanal. Chem.. (印刷中).

    • Related Report
      1999 Annual Research Report
  • [Publications] 古賀,松尾,山崎,堀: "Infrared Spectroscopic Observation of Intermediate Species on an Ni and an Fe Electrode in the Electrochemical Reduction of CO2 and CO to Hydrocarbons." Bull.Chem.Soc.Jpn.71(2). 315-320 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 古賀,松尾,星,堀: "Charge Displacement Adsorption of Carbon Monoxide on[110]Zone Copper Single Crystal Electrodes in Relation with PZC." Electrochim.Acta. 44(6). 903-907 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 堀,古賀,渡辺,松尾: "FTIR Measurements of Charge Displacement Adsorption of CO on Poly- and Single Crystal(100)of Cu Electrodes" Electrochim.Acta. 44(8). 1389-1395 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 星,川谷,工藤,堀: "Significant Enhancement of the Electrochemical Reduction of CO_2 at the Kink Sites on Pt(S)-[n(110)x(100)]and Pt(S)-[n(100)x(110)]." J.Electroanal.Chem.(印刷中).

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Hoshi: "Structural effect on the Rate of CO_2 Reduction on Single Crystal Electrodes of Palladium." J.Electroanal.Chem.,. 421. 15-18 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Y.Hori: "Electrochemical reduction of CO at a Copper Electrode." J.Phys.Chem.B. 101(36). 7075-7081 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Hoshi: "Catalytic activity of C0_2 reduction rate on Pt single crystal electrodes;Pt(S)-[n(111)x(111)],Pt(S)-[n(111)x(100)]and Pt(S)-[n(100)x(111)]." J.Phys.Chem.B. 101(42). 8520-8524 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] N.Hoshi: "Electrochemical Reduction of CO_2 on Single Crystal Electrodes of Silver;Ag(111),Ag(100)and Ag(110)." J.Electroanal.Chem.,. 440. 283-286 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] O.Koga: "Infrared Spectroscopic Observation of Intermediate Species on Ni and Fe Electrodes in the Electrochemical Reduction of CO_2 and CO to Hydrocarbons." Bull.Chem.Soc.Jpn.71. 315-320 (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] O.Koga: "Charge Displacement Adsorption of Carbon Monoxide on[110]Zone Copper Single Crystal Electrodes in Relation with PZC." Electrochim.Acta.,in press. (1998)

    • Related Report
      1997 Annual Research Report

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

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