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Spectroscopic study on dynamical structures of electrode/electrolyte interfaces using surface-enhanced electronic and vibrational Raman scattering

Research Project

Project/Area Number 21H01882
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionNagoya Institute of Technology

Principal Investigator

Ikeda Katsuyoshi  名古屋工業大学, 工学(系)研究科(研究院), 教授 (50321899)

Co-Investigator(Kenkyū-buntansha) 本林 健太  名古屋工業大学, 工学(系)研究科(研究院), 准教授 (60609600)
浦長瀬 正幸  名古屋工業大学, 工学(系)研究科(研究院), 研究員 (00512766)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,550,000 (Direct Cost: ¥13,500,000、Indirect Cost: ¥4,050,000)
Fiscal Year 2023: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2022: ¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2021: ¥8,320,000 (Direct Cost: ¥6,400,000、Indirect Cost: ¥1,920,000)
Keywordsテラヘルツ振動 / イオン液体 / 水素結合 / 界面計測 / その場観察 / 動的構造 / テラヘルツ / 電気二重層 / 電気化学反応 / 界面分光 / 電気化学界面
Outline of Research at the Start

電極/電解質の接する電気化学界面に形成される電気2重層は、電池等においてエネルギー変換の行われる「反応場」である。電気2重層の微視的構造は、界面電子移動に大きな影響を与えるが、イオン間あるいは電極表面との物理化学的相互作用により、その動的挙動は複雑である。本研究では、「電極側の界面電子情報」、「電解質側の界面化学種情報」、「帯電粒子間の相互作用を伴う二重層の動的構造」を全て同時にin-situ測定することで、界面の構造とダイナミクスを明らかにする。特に、イオン間の相互作用や電極との相互作用に伴う短距離秩序形成が電極反応に与える影響を調べ、次世代電池開発に資する界面現象の知見蓄積を目指す。

Outline of Final Research Achievements

In this project, surface enhanced electronic and vibrational Raman scattering (SERS) spectroscopy has been applied to study structures and dynamics of ionic liquids and aqueous electrolyte solutions on a metal electrode surface. For vibrational SERS, the detectable frequency range was extended into the terahertz region so that anion-cation interactions and hydrogen bond vibrations were measured. We successfully observed adsorption and desorption of anions, creation and breaking of anion-cation pairs, and hydrogen bond breaking under potential application in the vibrational spectra. We were also able to measure the changes of surface charge induced by interfacial structure changes in the electronic spectra. These results clearly shows that simultaneous observation of vibrational and electronic information at electrochemical interfaces is quite useful to understand electrochemical processes at the molecular level.

Academic Significance and Societal Importance of the Research Achievements

電極/電解質界面は、電気エネルギーと化学エネルギーの変換において電子を授受する場である。したがって、印加電位に対して電極近傍の電解質イオンや溶媒分子の挙動を分子レベルで理解することは、エネルギー変換デバイスを設計する上で不可欠である。溶媒としての水は水素結合による特異な性質を示す。また、次世代電解液として期待されるイオン液体は、中性溶媒分子を含まないため、界面近傍のイオン分布(界面構造)やそのダイナミクスが従来とは大きく異なると考えられている。本研究の成果は、水系電解液とイオン液体電解液のそれぞれが界面近傍で示す挙動を理解する上で、極めて有効な分光手法を提示するものである。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (49 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (1 results) Journal Article (11 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 11 results,  Open Access: 4 results) Presentation (36 results) (of which Int'l Joint Research: 5 results,  Invited: 3 results) Book (1 results)

  • [Int'l Joint Research] Key Lab of Materials Physics/Institute of Solid State Physics(中国)

    • Related Report
      2023 Annual Research Report
  • [Journal Article] Revisit of the plasmon-mediated chemical transformation of<i>para</i>-aminothiophenol2023

    • Author(s)
      Kondo Toshiki、Inagaki Motoharu、Tanaka Shohei、Tsukiji Shinya、Motobayashi Kenta、Ikeda Katsuyoshi
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 25 Issue: 20 Pages: 14618-14626

    • DOI

      10.1039/d3cp00924f

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Probing collective terahertz vibrations of a hydrogen-bonded water network at buried electrochemical interfaces2023

    • Author(s)
      Isogai Taichi、Uranagase Masayuki、Motobayashi Kenta、Ogata Shuji、Ikeda Katsuyoshi
    • Journal Title

      Chemical Science

      Volume: 14 Issue: 24 Pages: 6531-6537

    • DOI

      10.1039/d3sc01734f

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Origin of Temperature-Dependent Overpotential of Co Electrodeposition in an Ionic Liquid2023

    • Author(s)
      Motobayashi Kenta、Nakagawa Hayato、Shibamura Yuhei、Ikeda Katsuyoshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 128 Issue: 2 Pages: 819-826

    • DOI

      10.1021/acs.jpcc.3c07750

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Surface mass analysis of heterogeneous reactions using low-frequency surface-enhanced Raman scattering2023

    • Author(s)
      Ikeda Katsuyoshi
    • Journal Title

      Current Opinion in Electrochemistry

      Volume: 41 Pages: 101355-101355

    • DOI

      10.1016/j.coelec.2023.101355

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] In-situ Surface-Enhanced Raman Spectroscopy Reveals a Mars?van Krevelen-Type Gas Sensing Mechanism in Au@SnO<sub>2</sub> Nanoparticle-Based Chemiresistors2023

    • Author(s)
      Bao Haoming、Motobayashi Kenta、Zhang Hongwen、Cai Weiping、Ikeda Katsuyoshi
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 14 Issue: 17 Pages: 4113-4118

    • DOI

      10.1021/acs.jpclett.3c00562

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] In Situ Spectroscopic Characterization of an Intermediate of CO<sub>2</sub> Electroreduction on a Au Electrode in Room-Temperature Ionic Liquids2022

    • Author(s)
      Motobayashi Kenta、Maeno Yoshiki、Ikeda Katsuyoshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 29 Pages: 11981-11986

    • DOI

      10.1021/acs.jpcc.2c03012

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Engineered Au@CuO Nanoparticles for Wide-Range Quantitation of Sulfur Ions by Surface-Enhanced Raman Spectroscopy2022

    • Author(s)
      Bao Haoming、Motobayashi Kenta、Ikeda Katsuyoshi
    • Journal Title

      Analytical Chemistry

      Volume: 94 Issue: 49 Pages: 17169-17176

    • DOI

      10.1021/acs.analchem.2c03631

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] In situ mass analysis of surface reactions using surface-enhanced Raman spectroscopy covering a wide range of frequencies2022

    • Author(s)
      Toshiki Kondo, Motoharu Inagaki, Kenta Motobayashi, Katsuyoshi Ikeda
    • Journal Title

      Catalysis Science & Technology

      Volume: 12 Issue: 8 Pages: 2670-2676

    • DOI

      10.1039/d2cy00229a

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Surface-enhanced electronic Raman scattering at various metal surfaces2022

    • Author(s)
      Ryuto Kamimura, Toshiki Kondo, Kenta Motobayashi, Katsuyoshi Ikeda
    • Journal Title

      Physica Status Solidi B: Basic Solid State Physics

      Volume: - Issue: 9

    • DOI

      10.1002/pssb.202100589

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] A single spectroscopic probe for in-situ analysis of electronic and vibrational information at both sides of electrode/electrolyte interfaces using surface-enhanced Raman scattering2021

    • Author(s)
      Taichi Isogai, Kenta Motobayashi, Katsuyoshi Ikeda
    • Journal Title

      The Journal of Chemical Physics

      Volume: 155 Issue: 20 Pages: 204702-204702

    • DOI

      10.1063/5.0067355

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Competing characters of Li+‐Glyme complex in a solvate ionic liquid: High stability in the bulk and rapid desolvation on an electrode surface2021

    • Author(s)
      Motobayashi Kenta、Matsumoto Kosuke、Tsuzuki Seiji、Ikeda Katsuyoshi
    • Journal Title

      Electrochemical Science Advances

      Volume: Early View Issue: 6

    • DOI

      10.1002/elsa.202100150

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] 表面増強電子-振動ラマン散乱によるAu電極/イオン液体界面の両相における電気化学応答の同時観察2024

    • Author(s)
      上野領、本林健太、池田勝佳
    • Organizer
      電気化学会第91回大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Electrochemical Hydrogen Evolution using Proton Transport through Two Dimensional Monolayers2024

    • Author(s)
      セカル バラニタラヌ,保田諭,本林健太, 池田勝佳
    • Organizer
      電気化学会第91回大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 表面増強電子-振動ラマン散乱によるイオン液体/Au 電極界面の観察2023

    • Author(s)
      上野領、本林健太、池田勝佳
    • Organizer
      第23回日本表面真空学会中部支部学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] イオン液体のカチオン種に依存した Zn 電析過電圧:表面増強赤外分光による検討2023

    • Author(s)
      武内幹生、池田勝佳、本林健太
    • Organizer
      第23回日本表面真空学会中部支部学術講演会
    • Related Report
      2023 Annual Research Report
  • [Presentation] In-Situ Vibrational Spectroscopic Analysis of Solid Layer Formation at a Superconcentrated Electrolyte/Electrode Interface2023

    • Author(s)
      Kenta Motobayashi, Masanori Nagasaka, Katsuyoshi Ikeda
    • Organizer
      2023 Materials Research Society Fall Meeting & Exhibit
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Sn 電析進行下におけるイオン液体/電極界面の in-situ 構造観測2023

    • Author(s)
      間瀬智也, 池田勝佳, 本林健太
    • Organizer
      第13回イオン液体討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] イオン液体中の金属電析における過電圧の起源: 界面構造のin situ 観測に基づく考察2023

    • Author(s)
      本林健太, 中川隼人, 武内幹生, 芝村悠平, 池田勝佳
    • Organizer
      第13回イオン液体討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Overpotential of Co Electrodeposition in an Ionic Liquid Originated from Interfacial Restructuring2023

    • Author(s)
      Kenta Motobayashi, Hyato Nakagawa, Yuhei Shibamura, Katsuyoshi Ikeda
    • Organizer
      2023 Joint Symposium on Molten Salts
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Sn電析進行下におけるイオン液体/電極界面構造のその場振動分光観測2023

    • Author(s)
      間瀬 智大, 池田 勝佳, 本林 健太
    • Organizer
      第54回中部化学関係学協会支部連合秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] コバルト錯体修飾電極における水素発生反応の評価2023

    • Author(s)
      池俣 篤希, 本林 健太, 池田 勝佳
    • Organizer
      第54回中部化学関係学協会支部連合秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Overpotential of Co electrodeposition in an ionic liquid: mechanistic study using surface enhanced infrared absorption spectroscopy2023

    • Author(s)
      Kenta Motobayashi, Hyato Nakagawa, Yuhei Shibamura, Katsuyoshi Ikeda
    • Organizer
      Annual Meeting of the Japan Society of Vacuum and Surface Science 2023
    • Related Report
      2023 Annual Research Report
  • [Presentation] Probing Dielectric Relaxation of Water at Electrochemical Interfaces with Low-Frequency SERS Spectroscopy2023

    • Author(s)
      Katsuyoshi Ikeda
    • Organizer
      244th ECS Meeting
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 電極界面における水の誘電緩和応答のTHz-SERS測定2023

    • Author(s)
      池田勝佳
    • Organizer
      第17回分子科学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 水電解中のカソード表面における水素結合状態変化のラマン観察2023

    • Author(s)
      上村龍豊,本林健太,池田勝佳
    • Organizer
      2023電気化学会秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] アミノベンゼンチオールのプラズモン誘起アゾ化反応の再検討2023

    • Author(s)
      池田勝佳
    • Organizer
      2023年光化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] In-Situ Low-Frequency SERS Observation at Various Electrochemical Interfaces2023

    • Author(s)
      Katsuyoshi Ikeda
    • Organizer
      243rd ECS Meeting
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] テラヘルツ領域の SERS測定による各種電解液中での電極界面のその場観察2023

    • Author(s)
      上村龍豊, 上野領, 本林健太, 池田勝佳
    • Organizer
      電気化学会第90回大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] イオン液体/金電極界面における CO2電解還元反応の表面増強赤外分光観測2023

    • Author(s)
      本林健太, 前野義貴, 池田勝佳
    • Organizer
      電気化学会第90回大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Origin of Temperature-Dependent Onset Potentials of Co Electrodeposition in an Ionic Liquid Proved by Interfacial Vibrational Spectroscopy2022

    • Author(s)
      中川 隼人,池田 勝佳,本林 健太
    • Organizer
      第12回イオン液体討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] In-situ Evaluation of Mechanical Properties of a Solid Layer Formed at Superconcentrated Electrolyte/Electrode Interface2022

    • Author(s)
      小林 明斗,湊 丈俊,池田 勝佳,本林 健太
    • Organizer
      第12回イオン液体討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] イオン液体中におけるCO2 電解還元反応の表面増強赤外観測2022

    • Author(s)
      本林健太, 前野義貴, 池田勝佳
    • Organizer
      2022年電気化学会 東北支部・東海支部合同シンポジウム
    • Related Report
      2022 Annual Research Report
  • [Presentation] 表面増強ラマン散乱による水/白金系電極界面の水素結合ネットワークの観察2022

    • Author(s)
      上村龍豊, 本林健太, 池田勝佳
    • Organizer
      2022年電気化学会 東北支部・東海支部合同シンポジウム
    • Related Report
      2022 Annual Research Report
  • [Presentation] 溶媒和イオン液体/電極界面で起こる脱溶媒和現象のその場観測2022

    • Author(s)
      松本 晃輔,池田 勝佳,本林 健太
    • Organizer
      第 54 回溶融塩化学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 表面選択的な振動分光法による電極界面の水素結合ネットワークの直接観察2022

    • Author(s)
      上村 龍豊,磯貝 太一,本林 健太, 池田 勝佳
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 電極表面のアミノベンゼンチオールはSERS測定中にプラズモン誘起反応を起こすか?2022

    • Author(s)
      池田勝佳
    • Organizer
      2022年電気化学秋季大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 電位により誘起されるイオン液体/電極二重層界面の構造変化:温度による影響2022

    • Author(s)
      中川隼人, 池田勝佳, 本林健太
    • Organizer
      2022年電気化学秋季大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 表面増強分光で探る帯電界面の構造とダイナミクス2022

    • Author(s)
      池田勝佳
    • Organizer
      第9回森野ディスカッション
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Surface-enhanced Raman spectroscopy at electrified interfaces: electronic SERS and low-frequency vibrational SERS2022

    • Author(s)
      Katsuyoshi Ikeda
    • Organizer
      SPIE Optics + Photonics meeting
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 各種金属電極表面における表面増強電子ラマン散乱測定2022

    • Author(s)
      上村龍豊, 本林健太, 池田勝佳
    • Organizer
      電気化学会第89回大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] In-situ Vibrational Observation of a Superconcentrated Electrolyte/Electrode Interface2021

    • Author(s)
      Masanori Nagasaka, Katsuyoshi Ikeda, Kenta Motobayashi
    • Organizer
      The 9th International Symposium on Surface Science
    • Related Report
      2021 Annual Research Report
  • [Presentation] In-situ Observation of the Potential-dependent Structure of a Superconcentrated Electrolyte/Electrode Interface2021

    • Author(s)
      長坂昌憲, 池田勝佳, 本林健太
    • Organizer
      第11回イオン液体討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Temperature dependence of potential-induced restructuring of an ionic liquid/Au electrode interface2021

    • Author(s)
      中川隼人, 池田勝佳, 本林健太
    • Organizer
      第11回イオン液体討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 表面増強ラマン散乱による電極界面のテラヘルツ振動構造の観察2021

    • Author(s)
      池田勝佳
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] ニトロベンゼンチオールの光及び電気化学反応過程の低振動表面増強ラマン観察2021

    • Author(s)
      近藤利樹, 本林健太, 池田勝佳
    • Organizer
      2021年電気化学秋季大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] リチウム塩濃厚電解液中における電極界面構造の直接観測2021

    • Author(s)
      長坂昌憲, 池田勝佳, 本林健太
    • Organizer
      2021年電気化学秋季大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 表面増強赤外吸収法(SEIRAS)と表面増強ラマン散乱法(SERS)による電極/電解液界面のin-situ計測2021

    • Author(s)
      池田勝佳
    • Organizer
      素材プロセシング第69委員会第2分科会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Book] ラマン分光スペクトルデータ解析事例集2022

    • Author(s)
      池田勝佳
    • Total Pages
      405
    • Publisher
      (株)技術情報協会
    • ISBN
      9784861048722
    • Related Report
      2021 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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