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Fabrication and activity evaluation of electrode catalysts with intermetallic compound nanoclusters uniformly supported on organic molecular substrates

Research Project

Project/Area Number 21K18939
Research Category

Grant-in-Aid for Challenging Research (Exploratory)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 32:Physical chemistry, functional solid state chemistry, and related fields
Research InstitutionKeio University

Principal Investigator

Nakajima Atsushi  慶應義塾大学, 理工学部(矢上), 教授 (30217715)

Project Period (FY) 2021-07-09 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥6,370,000 (Direct Cost: ¥4,900,000、Indirect Cost: ¥1,470,000)
Fiscal Year 2022: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2021: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Keywordsナノクラスター電極触媒 / 金属間化合物 / 有機分子基板 / 担体表面 / ナノクラスター / 電極触媒 / 構造活性相関
Outline of Research at the Start

既報の溶液還元法や原子共蒸着法での触媒作成の不均一性を解決するため、高出力インパルスマグネトロンスパッタリングによる高強度ナノクラスター生成法を用いて、金属間化合物の合金ナノクラスターを対象に、構成原子数と組成を精密に分離して担体表面上に担持して触媒を創成する方法を構築する。担体表面に予め有機分子蒸着を施し、分子間相互作用の局所性によって触媒の表面拡散の抑制と適切な有機分子の選択による電極触媒の活性化を実現する。この電極触媒を用いて、二酸化炭素還元反応などにおける電極触媒の活性を、X線光電子分光法による構造と電子物性と併せて評価し、ナノクラスター触媒の活性と構造、電子物性の相関を解明する。

Outline of Final Research Achievements

Nanoclusters of palladium, platinum, platinum/terbium alloys were synthesized in a gas phase. After selecting the number of atoms and composition with a mass spectrometer, the nanocluster ions were deposited on a substrate pre-decorated by organic molecules. The electronic states were evaluated by x-ray photoelectron spectroscopy and by oxygen gas exposures. By changing the type of organic molecule to electron-donor or electron-acceptor, the charge states of the substrate were designed, resulting in that the reactivity of the nanoclusters against oxygen gas could be controlled by the supporting substrate. The result indicates the importance of the substrate effect; the catalytic activity of the deposited nanoclusters can be controlled by the organic molecule modification. This experimental approach opens up a new molecular science of nanocluster-supported catalysts, in which the number of constituent metal atoms and composition are precisely controlled on an organic substrate.

Academic Significance and Societal Importance of the Research Achievements

表面に予め有機分子蒸着を施すことで担体表面上での均一性を向上させ、分子間相互作用によって触媒の表面拡散の抑制と適切な有機分子による電荷制御で、元素の複合化による合金化と併せて、ナノクラスター触媒の活性化を実現した。この研究は表面担持された合金ナノクラスターに対して基板の担持効果の位置づけを解明し、パラジムや白金、および、その合金ナノクラスターの触媒作用機構を分子論に基づいて理解することに基礎を与えるものである。この成果によって、表面担持ナノクラスターの触媒活性を制御する方策の1つが得られたもので、パラジウムや白金などの希少元素に対して、少ない原子数のナノクラスター触媒が活用される道を拓いた。

Report

(3 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • Research Products

    (22 results)

All 2023 2022 2021 Other

All Journal Article (6 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 6 results,  Open Access: 1 results) Presentation (15 results) (of which Int'l Joint Research: 4 results,  Invited: 3 results) Remarks (1 results)

  • [Journal Article] Two-Photon Photoemission Spectroscopy and Microscopy for Electronic and Plasmonic Characterizations of Molecularly Designed Organic Surfaces2023

    • Author(s)
      Shibuta Masahiro、Nakajima Atsushi
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 14 Issue: 13 Pages: 3285-3295

    • DOI

      10.1021/acs.jpclett.3c00043

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Molecularly Designed Cluster?Surface Interaction for Halogen-like and Alkali-like Metal-Encapsulating Silicon Cage Superatoms on n- and p-Type Organic Substrates2022

    • Author(s)
      Kamoshida Toshiaki、Shibuta Masahiro、Ohta Tsutomu、Eguchi Toyoaki、Nakajima Atsushi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 26 Pages: 10889-10899

    • DOI

      10.1021/acs.jpcc.2c02196

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Spectroscopic imaging of photoexcited states at a polycrystalline copper metal surface via two-photon photoelectron emission microscopy2022

    • Author(s)
      Shibuta Masahiro、Nakajima Atsushi
    • Journal Title

      Chemical Physics Letters

      Volume: 804 Pages: 139909-139909

    • DOI

      10.1016/j.cplett.2022.139909

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Superatom Generation and Deposition of Alkali-like Ta@Si<sub>16</sub> and Halogen-like Al<sub>13</sub> via Atomic Aggregation2022

    • Author(s)
      Inoue Tomoya、Ichikawa Takumi、Matsunaga Kimika、Birumachi Ryuki、Nakamura Kanata、Nakajima Atsushi
    • Journal Title

      Journal of The Electrochemical Society

      Volume: 169 Issue: 10 Pages: 102511-102511

    • DOI

      10.1149/1945-7111/ac9a0a

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Size-Dependent Oxidative Stability of Silicon Nanoclusters Mixed with a Tantalum Atom2022

    • Author(s)
      Shibuta Masahiro、Huber Maximilian、Kamoshida Toshiaki、Terasaka Kazuya、Hatanaka Miho、Niedner-Schatteburg Gereon、Nakajima Atsushi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 126 Issue: 9 Pages: 4423-4432

    • DOI

      10.1021/acs.jpcc.1c10895

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Al13- and B@Al12- superatoms on a molecularly decorated substrate2022

    • Author(s)
      Shibuta Masahiro、Inoue Tomoya、Kamoshida Toshiaki、Eguchi Toyoaki、Nakajima Atsushi
    • Journal Title

      Nature Communications

      Volume: 13 Issue: 1 Pages: 1336-1336

    • DOI

      10.1038/s41467-022-29034-9

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] Plasmonic Silver Nanoclusters for Sensitizing Surface Plasmon Polaritons Propagating at Buried Organic/Metal Interfaces2022

    • Author(s)
      Atsushi Nakajima
    • Organizer
      Symposium on Cluster Surface Interaction (CSI2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Nucleation and Growth of Small Atomic Aggregates into Superatom Nanoclusters2022

    • Author(s)
      Atsushi Nakajima
    • Organizer
      The 241st Spring Electrochemical Society Meeting
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Oxidation Reactivities of Two Ta@Si16 and B@Al12 Superatoms on an Organic Substrate2022

    • Author(s)
      Atsushi Nakajima
    • Organizer
      Symposium on Size Selected Clusters (S3C)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Study on the chemical reactivity of boron-doped aluminum nanoclusters supported on organic surfaces2022

    • Author(s)
      INOUE, Tomoya; NAKAJIMA, Atsushi
    • Organizer
      第37回化学反応討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Electronic states and reactivities of palladium nanoclusters on organic substrates2022

    • Author(s)
      SHINOMIYA, Koh; INOUE, Tomoya; NAKAJIMA, Atsushi
    • Organizer
      第37回化学反応討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 8,9族原子内包シリコンケージナノクラスターの有機表面上における化学的特性2022

    • Author(s)
      市川 琢己,寺坂 一也,中嶋 敦
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 有機基板上にソフトランディングさせた単一サイズ銀ナノクラスターの局在表面プラズモン共鳴2022

    • Author(s)
      溝口 凱斗,井上 朋也,渋田 昌弘,中嶋 敦
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 燃料電池正極の酸素還元反応におけるPt-Tb合金ナノクラスター触媒の活性評価2022

    • Author(s)
      松永 季実果,中嶋 敦
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 単一組成の白金パラジウム合金ナノクラスターを電極触媒とする酸素還元反応における活性評価2022

    • Author(s)
      美留町 竜輝,松永 季実果,中嶋 敦
    • Organizer
      第16回分子科学討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 二光子光電子顕微分光による電子励起状態の局所観測2022

    • Author(s)
      渋田昌弘, 中嶋敦
    • Organizer
      第16回 表面・界面スペクトロスコピー 2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] 気相ナノクラスターを用いた機能表面科学の開拓2022

    • Author(s)
      中嶋敦, 渋田昌弘, 井上朋也
    • Organizer
      第16回 表面・界面スペクトロスコピー 2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] 有機表面上に担持された13族超原子の化学的反応性2022

    • Author(s)
      井上朋也、中嶋 敦
    • Organizer
      日本化学会 第102 春季年会(2022)
    • Related Report
      2021 Research-status Report
  • [Presentation] 有機基板とサイズによる表面担持されたアルミニウムナノクラスターの反応性制御2021

    • Author(s)
      井上 朋也,渋田 昌弘,中嶋 敦
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 有機分子基板上に担持したパラジウムナノクラスターの電荷状態と反応性2021

    • Author(s)
      四ノ宮 康,井上 朋也,中嶋 敦
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] Superatom Chemistry of Metal-Encapsulating Silicon Cage Nanoclusters2021

    • Author(s)
      Atsushi Nakajima
    • Organizer
      The International Chemical Congress of Pacific Basin Societies 2021
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Remarks] 研究室ホームページ

    • URL

      http://chem.keio.ac.jp/nakajima-lab/index.html

    • Related Report
      2021 Research-status Report

URL: 

Published: 2021-07-13   Modified: 2024-01-30  

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