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Insight into the Electrochemical Oxidation Mechanism of Carbon Materials by Deuterium-Labeled Temperature-Programmed Desorption

Research Project

Project/Area Number 20H02833
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 36020:Energy-related chemistry
Research InstitutionGunma University

Principal Investigator

Ishii Takafumi  群馬大学, 大学院理工学府, 助教 (50750155)

Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥16,770,000 (Direct Cost: ¥12,900,000、Indirect Cost: ¥3,870,000)
Fiscal Year 2022: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2021: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2020: ¥14,170,000 (Direct Cost: ¥10,900,000、Indirect Cost: ¥3,270,000)
Keywords炭素材料 / 電気化学的酸化 / 表面分析 / 燃料電池 / キャパシタ / エネルギー貯蔵材料 / PEFC / 活性炭 / カーボンブラック / 電気化学 / エネルギー貯蔵
Outline of Research at the Start

電気化学的酸化による炭素電極の劣化が問題視されている.これを解決するためには,炭素材料の酸化機構を知ることが必要不可欠であるが,その理解は未だに不十分である.炭素の酸化反応は,複雑な化学構造をもつ炭素エッジ面の化学反応であり,その反応機構を明らかにするためには,炭素エッジ面の化学構造を精密に分析する必要がある.申請者は,これまで重水素標識昇温脱離(TPD)分析によって,炭素エッジ面の化学構造を精密に分析できることを見出している.本研究では,この炭素エッジ面精密分析手法を用いて,水系電解液中での電気化学的酸化による炭素エッジ面の化学構造変化を追跡し,炭素材料の電気化学的酸化機構を解明する.

Outline of Final Research Achievements

In this study, the electrochemical oxidation behavior of carbon materials was investigated by D-TPD analysis. It was found that phenolic hydroxyl groups (Ph2), ethers, and carbonyls were preferentially formed on the carbon surface by electrochemical oxidation. It is generally believed that electrochemical oxidation proceeds from the edge sites. However, in the results of this study, carbon samples with fewer edge sites showed higher reactivity to electrochemical oxidation. We attempted to understand this electrochemical oxidation behavior by proposing two hypotheses. Future investigation of the validity of these hypotheses will lead to a better understanding of the electrochemical oxidation mechanism.

Academic Significance and Societal Importance of the Research Achievements

炭素材料は電極材としてキャパシタ,燃料電池など多くの電気化学用途で利用されている.炭素材料は酸化反応に弱いという欠点があり,電気化学的酸化による炭素電極の劣化が問題視されている.本研究成果は,炭素エッジ面精密分析手法を用いて,水系電解液中での電気化学的酸化による炭素エッジ面の化学構造変化を追跡し,炭素材料の電気化学的酸化メカニズムを解明へ向けた知見を示すものである.この成果により,炭素材料の耐久性向上へ向けた材料設計指針を与えると期待される.

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • Research Products

    (16 results)

All 2023 2022 2021 2020

All Journal Article (10 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 8 results) Presentation (6 results) (of which Invited: 2 results)

  • [Journal Article] Chemical modification of carbon edge sites using trimethylaluminum to enhance the oxidation resistance of carbon materials2023

    • Author(s)
      Yano Aika、Ishii Takafumi
    • Journal Title

      Carbon

      Volume: 207 Pages: 231-239

    • DOI

      10.1016/j.carbon.2023.02.059

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] What can we learn by analyzing the edge sites of carbon materials?2022

    • Author(s)
      Kyotani Takashi、Ozaki Jun-ichi、Ishii Takafumi
    • Journal Title

      Carbon Reports

      Volume: 1 Issue: 4 Pages: 188-205

    • DOI

      10.7209/carbon.010406

    • ISSN
      2436-5831
    • Year and Date
      2022-12-01
    • Related Report
      2022 Annual Research Report
  • [Journal Article] Estimation of the spatial distribution of carbon edge sites in a carbon structure using H2 desorption kinetics in temperature programmed desorption2022

    • Author(s)
      Ishii Takafumi、Ozaki Jun-ichi
    • Journal Title

      Carbon

      Volume: 196 Pages: 1054-1062

    • DOI

      10.1016/j.carbon.2022.06.006

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Modulation of the electronic state of carbon thin films by inorganic substrates2022

    • Author(s)
      Ishii Takafumi、Okuhara Daichi、Kobayashi Rieko、Ozaki Jun-ichi
    • Journal Title

      Carbon

      Volume: 196 Pages: 313-319

    • DOI

      10.1016/j.carbon.2022.04.079

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Preparation of Chemically Structure-Controlled BN-Doped Carbons for the Molecular Understanding of Their Surface Active Sites for Oxygen Reduction Reaction2022

    • Author(s)
      Ishii Takafumi、Philavanh Malisa、Negishi Junpei、Inukai Eiji、Ozaki Jun-ichi
    • Journal Title

      ACS Catalysis

      Volume: 12 Issue: 2 Pages: 1288-1297

    • DOI

      10.1021/acscatal.1c04806

    • Related Report
      2021 Annual Research Report
  • [Journal Article] Direct conversion of lignin to high-quality graphene-based materials <i>via</i> catalytic carbonization2021

    • Author(s)
      Ishii Takafumi、Mori Mikaru、Hisayasu Shiguma、Tamura Ryusuke、Ikuta Yuki、Fujishiro Fumito、Ozaki Jun-ichi、Itabashi Hideyuki、Mori Masanobu
    • Journal Title

      RSC Advances

      Volume: 11 Issue: 31 Pages: 18702-18707

    • DOI

      10.1039/d1ra02491d

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Benzene hydrogenation activities of Ni catalyst supported on N- and B-doped carbons2021

    • Author(s)
      Ishii Takafumi、Kitamura Yuki、Hasegawa Seiya、Sasaki Chiaki、Ozaki Jun-ichi
    • Journal Title

      Diamond and Related Materials

      Volume: 119 Pages: 108550-108550

    • DOI

      10.1016/j.diamond.2021.108550

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Sulfur-Doped Carbons from Durian Peels, Their Surface Characteristics, and Electrochemical Behaviors2021

    • Author(s)
      Desa Susilo Sudarman、Ishii Takafumi、Nueangnoraj Khanin
    • Journal Title

      ACS Omega

      Volume: 6 Issue: 38 Pages: 24902-24909

    • DOI

      10.1021/acsomega.1c03760

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct evidence for highly developed graphene in PAN-based carbon fibers2021

    • Author(s)
      Ono Kiminori、Tomai Takaaki、Ishii Takafumi、Kurushima Kosuke、Inamoto Shin、Rutz Benjamin H.、Tanaka Fumihiko
    • Journal Title

      Carbon Trends

      Volume: 5 Pages: 100136-100136

    • DOI

      10.1016/j.cartre.2021.100136

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] In-Depth Analysis of Key Factors Affecting the Catalysis of Oxidized Carbon Blacks for Cellulose Hydrolysis2021

    • Author(s)
      Gabe Atsushi、Takatsuki Akira、Hiratani Masahiko、Kaneeda Masato、Kurihara Yoshiaki、Aoki Takayuki、Mashima Hiroki、Ishii Takafumi、Ozaki Jun-ichi、Nishihara Hirotomo、Kyotani Takashi
    • Journal Title

      ACS Catalysis

      Volume: 12 Issue: 2 Pages: 892-905

    • DOI

      10.1021/acscatal.1c04054

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] 昇温脱離法による炭素表面官能基の分析2022

    • Author(s)
      石井孝文
    • Organizer
      2022年度第2回CPC研究会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] H2脱離反応速度解析によるエッジサイト空間分布の評価2022

    • Author(s)
      石井孝文,尾崎純一
    • Organizer
      第49回炭素材料学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] H2脱離反応速度解析の重水素標識昇温脱離分析への適用2022

    • Author(s)
      石井孝文,尾崎純一
    • Organizer
      第49回炭素材料学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 金属酸化物コアシェルカーボンの物性と触媒担体効果2022

    • Author(s)
      石井孝文,宮下峻,長島日向子,関川あかね,奥原 大地,小林 里江子,尾崎 純一
    • Organizer
      第49回炭素材料学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 昇温脱離法による炭素材料表面の精密分析と炭素構造解析2021

    • Author(s)
      石井孝文
    • Organizer
      第48回炭素材料学会年会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] カーボンブラックの水系電解液中における電気化学的酸化挙動の追跡2020

    • Author(s)
      髙木大地,石井孝文,尾崎純一
    • Organizer
      第47回炭素材料学会年会
    • Related Report
      2020 Annual Research Report

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Published: 2020-04-28   Modified: 2024-01-30  

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