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Tuning electrochemical reactions via reaction field design

Research Project

Project/Area Number 22K14542
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionOsaka University

Principal Investigator

Katayama Yu  大阪大学, 産業科学研究所, 准教授 (70819284)

Project Period (FY) 2022-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2023: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2022: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Keywordsナノ反応場 / 電極触媒 / オペランド分光 / 水素結合ネットワーク / ルイス酸性 / オペランド分光法 / エネルギー変換反応 / 物質変換反応 / 電気化学 / 界面化学
Outline of Research at the Start

層状酸化物の層間に触媒活性サイトを導入し、層間を反応の舞台(=ナノ反応場)に見立てる。これにより、「触媒反応が実際に進行する」活性サイトとその周囲の環境の精密設計を目指す。具体的には、金属錯体を活性サイトと捉え、その (1)配位状態、(2)距離を配位子設計により最適化する。さらに、反応場が狭小であることを用いて、(3)溶媒である水分子の相互作用を制御する。さらに、オペランド分光法を用いることでナノ反応場で進行する反応のメカニズムを解明し、触媒材料設計にフィードバックする。これらにより、反応素過程の選択的制御を実現し、真に目的反応に最適化された革新的触媒を創成する。

Outline of Final Research Achievements

We have succeeded in synthesizing electrocatalysts in which catalytically active sites consisting of metal complexes are introduced between the layers of layered manganese oxides, and the layers are regarded as a reaction field (= nano reaction field). Specifically, in addition to using a single metal complex as the active site, we have succeeded in synthesizing electrocatalysts in which multiple metal complexes exist in a coexistent state. Furthermore, the interlayer environment during various electrochemical reactions was successfully observed using operando spectroscopy. These results led us to propose (1) a concerted reaction mechanism between adjacent active sites specific to nano-reaction fields and (2) the modulation effect of solvent on the hydrogen bonding network, as factors controlling the activity of electrocatalytic reactions in nano-reaction fields.

Academic Significance and Societal Importance of the Research Achievements

本研究で設計に成功したナノ反応場は、電気化学反応に必要な要素(触媒、溶媒、第三体分子)が収容され、目的とする反応基質のみがアクセス可能な電気化学反応場である。ナノ反応場の設計が深化すれば、電気エネルギーによる物質変換(Power-to-X)を担う電気化学反応の理想形である「普遍的な原料から、所望の生成物のみを、必要最小限のエネルギーで得ること」の実現に一歩近づく。

Report

(3 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Research-status Report
  • Research Products

    (26 results)

All 2024 2023 2022 Other

All Int'l Joint Research (4 results) Journal Article (8 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 8 results,  Open Access: 5 results) Presentation (13 results) (of which Int'l Joint Research: 7 results,  Invited: 7 results) Remarks (1 results)

  • [Int'l Joint Research] インペリアルカレッジロンドン(英国)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] マサチューセッツ工科大学(米国)

    • Related Report
      2023 Annual Research Report
  • [Int'l Joint Research] Massachusetts Institute of Technology(米国)

    • Related Report
      2022 Research-status Report
  • [Int'l Joint Research] Imperial College London(英国)

    • Related Report
      2022 Research-status Report
  • [Journal Article] Role of Electrolyte pH on Water Oxidation for Iridium Oxides2024

    • Author(s)
      Liang Caiwu、Katayama Yu、Tao Yemin、Morinaga Asuka、Moss Benjamin、Celorrio Ver?nica、Ryan Mary、Stephens Ifan E. L.、Durrant James R.、Rao Reshma R.
    • Journal Title

      Journal of the American Chemical Society

      Volume: 146 Issue: 13 Pages: 8928-8938

    • DOI

      10.1021/jacs.3c12011

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] <i>Operando</i> Spectroscopy-Inspired Design of Electrochemical Interface2023

    • Author(s)
      KATAYAMA Yu
    • Journal Title

      Electrochemistry

      Volume: 91 Issue: 10 Pages: 101004-101004

    • DOI

      10.5796/electrochemistry.23-00059

    • ISSN
      1344-3542, 2186-2451
    • Year and Date
      2023-10-05
    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Water Increases the Faradaic Selectivity of Li-Mediated Nitrogen Reduction2023

    • Author(s)
      Spry Matthew、Westhead Olivia、Tort Romain、Moss Benjamin、Katayama Yu、Titirici Maria-Magdalena、Stephens Ifan E. L.、Bagger Alexander
    • Journal Title

      ACS Energy Letters

      Volume: 8 Issue: 2 Pages: 1230-1235

    • DOI

      10.1021/acsenergylett.2c02792

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Searching for the Rules of Electrochemical Nitrogen Fixation2023

    • Author(s)
      Tort Romain、Bagger Alexander、Westhead Olivia、Kondo Yasuyuki、Khobnya Artem、Winiwarter Anna、Davies Bethan J. V.、Walsh Aron、Katayama Yu、Yamada Yuki、Ryan Mary P.、Titirici Maria-Magdalena、Stephens Ifan E. L.
    • Journal Title

      ACS Catalysis

      Volume: 13 Issue: 22 Pages: 14513-14522

    • DOI

      10.1021/acscatal.3c03951

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electrospun CuO?Fe<sub>3</sub>O<sub>4</sub> Tube Catalyst for the Decomposition of Organic Matter via an Accelerated Heterogeneous Fenton-like Process2023

    • Author(s)
      Morinaga Asuka、Kijima Michika、Katayama Yu、Tsutsumi Hiromori
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 44 Pages: 21552-21560

    • DOI

      10.1021/acs.jpcc.3c05481

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] The role of ion solvation in lithium mediated nitrogen reduction2023

    • Author(s)
      Westhead O.、Spry M.、Bagger A.、Shen Z.、Yadegari H.、Favero S.、Tort R.、Titirici M.、Ryan M. P.、Jervis R.、Katayama Y.、Aguadero A.、Regoutz A.、Grimaud A.、Stephens I. E. L.
    • Journal Title

      Journal of Materials Chemistry A

      Volume: - Issue: 24 Pages: 12746-12758

    • DOI

      10.1039/d2ta07686a

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Layered Manganese Dioxide Thin Films Intercalated with Ag<sup>+</sup> Ions Reduceable In Situ for Oxygen Reduction Reaction2022

    • Author(s)
      Marukawa Ryuichi、Kiso Takayuki、Shimizu Tomohito、Katayama Yu、Nakayama Masaharu
    • Journal Title

      ACS Omega

      Volume: 7 Issue: 18 Pages: 15854-15861

    • DOI

      10.1021/acsomega.2c00967

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Carboxamide-Directed Stereospecific Couplings of Chiral Tertiary Alkyl Halides with Terminal Alkynes2022

    • Author(s)
      Akagawa Hiroki、Tsuchiya Naoki、Morinaga Asuka、Katayama Yu、Sumimoto Michinori、Nishikata Takashi
    • Journal Title

      ACS Catalysis

      Volume: 12 Issue: 16 Pages: 9831-9838

    • DOI

      10.1021/acscatal.2c02433

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Presentation] Operando Spectroscopy to Probe Electrolyte-Electrode Interface: Implication in Energy Storage and Electrolysis Applications2024

    • Author(s)
      Yu Katayama
    • Organizer
      MATSUS Spring 2024
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 積層2Dナノ層間内の水分子ネットワーク構造制御による酸素発生反応活性の向上2024

    • Author(s)
      宇都宮友彦,Qing Su,森永明日香,近藤靖幸,片山祐,山田裕貴
    • Organizer
      電気化学会第91回大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Operando Spectroscopy to Probe Electrolyte-Electrode Interface: Role of Electrolyte-Adsorbate Interaction2023

    • Author(s)
      Yu Katayama
    • Organizer
      ISE2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Probing Electrochemical Interfaces by Operando Spectroscopic Techniques2023

    • Author(s)
      Yu Katayama
    • Organizer
      2023 CSC Canadian Chemistry Conference and Exhibition
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] オペランド反応機構解析に立脚した水電解用触媒ー電解液界面の統合設計2023

    • Author(s)
      片山 祐
    • Organizer
      2023年度 第2回関西電気化学研究会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Activate N2-selective Pathways for Electrochemical Ammonia Oxidation: Dual Active Site Tandem Catalysis in 2D Layered Nanospace2022

    • Author(s)
      Asuka Morinaga, Keisuke Shirai, Hiromori Tsutsumi, Masaharu Nakayama, Yu Katayama
    • Organizer
      MRS Fall Meeting 2022
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] Operando Analysis of the Electrochemical Process in Confined Space2022

    • Author(s)
      Yu Katayama
    • Organizer
      Imperial College London, Electrochemistry Network Seminar
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Atomic Scale Understanding of the Electrochemical Interfaces:Operando Surface-Enhanced Infrared Absorption Spectroscopy (SEIRAS)2022

    • Author(s)
      Yu Katayama
    • Organizer
      nanoGe Fall Meeting 2022
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Revealing the Electrochemical Process in Confined Space by Operando Spectroscopy2022

    • Author(s)
      Yu Katayama
    • Organizer
      MIT Special Seminar
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 表面増強赤外分光法による Ni(II)-Cu(II)共存ナノ空間でのアンモニア酸化反応のオペランド観測2022

    • Author(s)
      森永明日香、白井敬介、小野隆太郎、村上愛、堤宏守、藤井健太、中山雅晴、片山祐
    • Organizer
      第82回分析化学討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] 層状ナノ空間でのサブナノ Pd粒子の電気化学的合成2022

    • Author(s)
      安藤 岬、小野 隆太郎、森永 明日香、近藤 靖幸、山田 裕貴、片山 祐、堤 宏守
    • Organizer
      2022年電気化学秋季大会
    • Related Report
      2022 Research-status Report
  • [Presentation] 二次元層状空間をメタル化反応場とした微細 Pd 粒子の合成とその電気化学特性2022

    • Author(s)
      安藤 岬、小野 隆太郎、森永 明日香、近藤 靖幸、山田 裕貴、片山 祐、堤 宏守
    • Organizer
      2022年日本化学会中国四国支部大会
    • Related Report
      2022 Research-status Report
  • [Presentation] 層状 MnO2内における Pt 単原子の合成およびその電気化学特性2022

    • Author(s)
      小野隆太郎、堤宏守、片山祐
    • Organizer
      2022年日本化学会中国四国支部大会
    • Related Report
      2022 Research-status Report
  • [Remarks] 研究者個人HP

    • URL

      https://sites.google.com/view/electrocatalysislab/home?authuser=1

    • Related Report
      2022 Research-status Report

URL: 

Published: 2022-04-19   Modified: 2025-01-30  

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