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Characterization of atomic structure of single Pt atoms on N-doped graphene

Research Project

Project/Area Number 19K15439
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 29020:Thin film/surface and interfacial physical properties-related
Research InstitutionHokkaido University

Principal Investigator

Yamazaki Kenji  北海道大学, 工学研究院, 助教 (10732985)

Project Period (FY) 2019-04-01 – 2021-03-31
Project Status Completed (Fiscal Year 2020)
Budget Amount *help
¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2020: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2019: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Keywords金属単原子 / 単原子触媒 / TEM / グラフェン / 単原子スパッタリング / TEM、STEM / 電子顕微鏡
Outline of Research at the Start

本研究課題では単原子触媒材料として期待されるPt単原子分散体の原子分解能、3次元でのイメージングを行う。申請者独自のPt単原子分散手法を用いたサンプルに対して収差補正透過型電子顕微鏡による原子分解能イメージング、原子分解能EELS解析を行い窒素ドープグラフェンにアンカーされたPt単原子の3次元原子配置を示すことによって、Pt単原子の安定化に対する窒素の作用を明らかにする。

Outline of Final Research Achievements

Single-atom catalysts are attracting attention due to their superior catalytic activity and cost. Nitrogen (N) enhances the stability of single platinum (Pt) atoms on graphene because Pt atoms dispersed by plasma sputtering in an N2 atmosphere are less likely to aggregate. However, the atomic structure of Pt and N on graphene has not been clarified. Here, we experimentally revealed the atomic arrangement of Pt, N, and carbon (C) by scanning transmission electron microscopy and electron energy loss spectroscopy. Pt and N atoms were adsorbed near the step edge of nanographene stacked on single-layer pristine graphene, rather than on the terrace. DFT calculation using the experimental structure confirmed that the single Pt atom has high stability because N strengthens the bond between Pt and C at the step edge. In addition to a large decrease in the population of Pt 5dxy-orbital, an increase in the population of 5dyz-orbital was observed.

Academic Significance and Societal Importance of the Research Achievements

単原子触媒の化学反応活性の高さは吸着構造に大きく影響する。これまでにグラフェン上のPt単原子の多くがグラフェンのステップエッジに多く吸着し、ステップエッジでの原子配置を明らかにしたが、より単原子が安定に存在する窒素ドープグラフェンの原子配置を明らかにした例はこれまでなかった。本研究では収差補正走査透過型顕微鏡(STEM)を用いた電子エネルギー損失分光(EELS)マッピングによって窒素ドープグラフェン上のPt単原子の原子配置を始めて明らかにし、理論計算によって吸着構造の電子状態を明らかにした。

Report

(3 results)
  • 2020 Annual Research Report   Final Research Report ( PDF )
  • 2019 Research-status Report
  • Research Products

    (7 results)

All 2021 2020 2019

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

  • [Journal Article] Single Pt Atoms on N-Doped Graphene: Atomic Structure and Local Electronic States2021

    • Author(s)
      Sugimoto Ryo、Segawa Yuhiro、Suzuta Akio、Kunisada Yuji、Uchida Tsutomu、Yamazaki Kenji、Gohara Kazutoshi
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 125 Issue: 5 Pages: 2900-2906

    • DOI

      10.1021/acs.jpcc.0c08811

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Quasi-static 3D structure of graphene ripple measured using aberration-corrected TEM2021

    • Author(s)
      Segawa Yuhiro、Yamazaki Kenji、Yamasaki Jun、Gohara Kazutoshi
    • Journal Title

      Nanoscale

      Volume: 13 Issue: 11 Pages: 5847-5856

    • DOI

      10.1039/d1nr00237f

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electron Microscopic Observation of an Icosahedral Au13 Core in Au25(SePh)18 and Reversible Isomerization between Icosahedral and Face-Centered Cubic Cores in Au144(SC2H4Ph)602020

    • Author(s)
      Takahata Ryo、Yamazoe Seiji、Maehara Yosuke、Yamazaki Kenji、Takano Shinjiro、Kurashige Wataru、Negishi Yuichi、Gohara Kazutoshi、Tsukuda Tatsuya
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 124 Issue: 12 Pages: 6907-6912

    • DOI

      10.1021/acs.jpcc.9b11412

    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Presentation] Atomic structure of Single Pt atoms anchored on nanographene2019

    • Author(s)
      K. Yamazaki, Y. Maehara, and K. Gohara
    • Organizer
      2019MRSFallMeeting
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Single-atom dispersion of platinum on graphene using plasma sputtering2019

    • Author(s)
      K. Gohara, K. Yamazaki
    • Organizer
      MRM2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Spatiotemporal pattern of graphene ripple structure measured using aberration corrected TEM2019

    • Author(s)
      Y. Segawa, K. Yamazaki, K. Gohara
    • Organizer
      MRM2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] In-situ observation of the motion of single metal atoms on graphene using aberration corrected electron microscopy2019

    • Author(s)
      A. Suzuta, T. Uchida, K. Yamazaki, R.Sugimoto, K. Gohara
    • Organizer
      MRM2019
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research

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Published: 2019-04-18   Modified: 2022-01-27  

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