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高圧パルス放電による超臨界二酸化炭素の分解

Research Project

Project/Area Number 14655323
Research Category

Grant-in-Aid for Exploratory Research

Allocation TypeSingle-year Grants
Research Field 工業物理化学
Research InstitutionKumamoto University

Principal Investigator

西山 勝彦  熊本大学, 工学部, 助教授 (10202243)

Project Period (FY) 2002 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥3,400,000 (Direct Cost: ¥3,400,000)
Fiscal Year 2004: ¥500,000 (Direct Cost: ¥500,000)
Fiscal Year 2003: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 2002: ¥1,900,000 (Direct Cost: ¥1,900,000)
Keywords超臨界二酸化炭素 / 白金 / 銅 / 高圧電気化学 / 電流効率 / 修飾電極 / 電界還元 / 白金修飾銅 / 二酸化炭素還元 / 高圧電源 / 超臨界流体 / 銅電極
Research Abstract

超臨界二酸化炭素、あるいは高圧二酸化酸素雰囲気下での電極反応に用いるために、酸性溶液中での置換メッキ法を利用した新規白金修飾銅電極を作製した。この手法は、銅電極の形状および、結晶性を問わず、浸漬時間と錯体の濃度によって、白金の量を容易に制御可能であった。また、金、銀、電極上に作製した自己組織化単分子膜に塩化白金酸イオンを静電的に結合させた後、電気化学的に還元、更に、有機膜であるチオールの膜を還元脱離法によるて脱離して作製した、白金/金電極も作製した。
電極の作成法としては、比較的濃度の低い1mM塩化白金酸溶液を用いて浸漬時間を変化させることで修飾する白金の量を変化させて、白金を薄く修飾することができた。実験条件を検討した結果、白金修飾銅電極の作製には低濃度の塩化白金酸を使用するほうが望ましいことがわかった。
酸素の還元において白金修飾銅電極は、白金の修飾時間が短時間(10sec,30sec)である場合、銅と似た挙動を示した。酸素の還元電位は、Cu電極上での酸素還元の場合に比べて100mVほどネガティブシフトし、水素発生はわずかながらポジティブシフトした。
また白金の修飾時間が長時間(5min,10min)の場合、酸素還元において白金とほぼ同じ電位で酸素の還元が生じ、銅と同様に水素発生が確認された。すなをち、銅と白金の両方の特徴が見られた。二酸化炭素の還元においてギ酸生成の電流効率は白金修飾銅電極(10sec:37.0%,30sec:25.8%,300sec:30.3%)は銅電極の場合(6.9%)よりも高くなった。一方、メタンの生成の電流効率は、白金を短時間(10sec)で修飾したもの(17.6%)において、銅電極の場合(118%)よりも高い値が得られた。つまり二酸化炭素の還元においては比較的少量の白金を修飾した白金修飾銅電極が高い触媒効果を示すと考えられる。

Report

(3 results)
  • 2004 Annual Research Report
  • 2003 Annual Research Report
  • 2002 Annual Research Report
  • Research Products

    (14 results)

All 2005 2004 Other

All Journal Article (4 results) Publications (10 results)

  • [Journal Article] Notable deuterium effect on the electron transfer rate of myoglobin2005

    • Author(s)
      Y.Mie
    • Journal Title

      Chem.Commun (In press)

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Superoxide Dismutase (SOD) Modified Electrodes2004

    • Author(s)
      K.Nishiyama
    • Journal Title

      Journal of The Surface Science Society of Japan 25

      Pages: 285-289

    • NAID

      10012929664

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Functional Evaluation of Heme Vinyl Groups in Myoglobin with Symmetric Protoheme Isomers2004

    • Author(s)
      Y.Mie
    • Journal Title

      Biochemistry 43

      Pages: 13149-13155

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Preparation and Characterization of Metal Monolayer Using Complexation of Cationic Self-assembled Monolayer with Metal Anion2004

    • Author(s)
      H.Hanazono
    • Journal Title

      Joint International Joint Meeting, Meeting of the Electrochemical Society, Fall Meeting of the Electrochemical Society of Japan

    • Related Report
      2004 Annual Research Report
  • [Publications] S.Yoshimoto: "Formation of Well-Defined p-tert-Butylcalix[4]arenedithiolate Monolayer on a Au(100)-(1x1) Surface Studies by In Situ Scanning Tunneling Microscopy"Langumuir. 19・(20). 8130 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] T.Yamada: "Detection of C-Si Covalent Bond in CH3 Adsorbate Formed by Chemical Reaction of CH3MgBr and H : Si(111)"J.Am.Chem.Soc.. 125・(26). 8039 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] I.Taniguchi: "Surface functions of 2-mercapropyridine, 2-mercaptopyrazine and 2-mercaptoquinoxaline modified Au(111) electrodes for rapid electron transfer of cytochrome c"Electrochemistry Communications. 5・(10). 857 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Nishiyama: "Photochemical and photo-triggered reduction of NADP+ by reconstituted myoglobin and cytochrome c and its application to photobioreacter"Proceedings of International Tenth Beijing Conference and Exhibition on Instrumental Analysis F.Electroanalytical Chemistry. F115 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 西山勝彦: "表面化学"スーパオキサイドディスムターゼ(SOD)修飾電極(In press). (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] Katushiko Nishiyama, Atsuhi Kubo, Akihiko Ueda, Isao Taniguchi: "Surface pKa of Amine-Terminated Self-assmebled Monolayers Evaluated by Direct Observation of Counter Anion by FT-Surface Enhanced Raman Spectroscopy"Chemistry Letters. 17. 80-81 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Atsushi Kubo, Katsuhiko Nishiyama, Isao Taniguchi: "Evaluation of pKa for Amine-Terminated Self-assmebled Monolayers by FT-Surface Enhanced Raman Spectroscopy"Asian Conference on Electrochemistry 2002 and The 5^<th> Korea-Japan Joint Seminar on Electrochemistry. 326-327 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Taro Yamada, Nao Takano, Tomoyuki Inoue, Tetsuya Osaka, Katsuhiko Nishiyama, Hiroshi Harada, Yosuke Tanaka, Isao Taniguchi: "Organic Ultra Thin Films Covalently Bonded n Si(111) Prepared by Grignard Reaction"Asian Conference on Electrochemistry 2002 and The 5^<th> Korea-Japan Joint Seminar on Electrochemistry. 360-361 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Katsuhiko Nishiyama, Yasuhiro Mie, Chiho Yamada, Midori Kishita, Hideyuki Nagai, Isao Taniguchi: "Photoinduced Enzyme Reaction of Reconstituted Myoglobin"、14^<th> International Conference on Photochemical Conversion and Storage of Solar Energy"14^<th> International Conference on Photochemical Conversion and Storage of Solar Energy. W3-P-5 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Taro Yamada, Nao Takano, Tomoyuki Inoue, Tetsuya Osaka, Hiroshi Harada, Katsuhiko Nishiyama, Isao Taniguchi: "C-Si Single Covalent Bonds Fixing CH_3 Groups Prepared by Chemical Reaction of CH_3MgBr and H : Si(111)"Surface Science. (In press.).

    • Related Report
      2002 Annual Research Report

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Published: 2002-04-01   Modified: 2016-04-21  

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