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Lattice defects (nano-twin) and origin of activity for bulk metallic catalysts

Research Project

Project/Area Number 15H02299
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Research Field Structural/Functional materials
Research InstitutionTohoku University

Principal Investigator

Tsai Anpang  東北大学, 多元物質科学研究所, 教授 (90225681)

Co-Investigator(Kenkyū-buntansha) 寺内 正己  東北大学, 多元物質科学研究所, 教授 (30192652)
亀岡 聡  東北大学, 多元物質科学研究所, 准教授 (60312823)
高倉 洋礼  北海道大学, 工学研究院, 准教授 (30284483)
野澤 和生  鹿児島大学, 理工学域理学系, 准教授 (00448763)
西本 一恵  東北大学, 多元物質科学研究所, 助教 (10586168)
青野 祐美  防衛大学校(総合教育学群、人文社会科学群、応用科学群、電気情報学群及びシステム工学群), 電気情報学群, 准教授 (80531988)
Project Period (FY) 2015-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥40,170,000 (Direct Cost: ¥30,900,000、Indirect Cost: ¥9,270,000)
Fiscal Year 2018: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Fiscal Year 2017: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Fiscal Year 2016: ¥8,580,000 (Direct Cost: ¥6,600,000、Indirect Cost: ¥1,980,000)
Fiscal Year 2015: ¥17,030,000 (Direct Cost: ¥13,100,000、Indirect Cost: ¥3,930,000)
Keywords格子欠陥 / ナノ双晶 / 配位数 / CO酸化 / 触媒活性 / リーチング / 双晶
Outline of Final Research Achievements

We have proposed a new mechanism for creation of catalytically active sites in porous Au. The existence of low-coordinated atomic sites on the surface is essential for understanding the catalytic activity of nanostructured Au. Samples of porous Au prepared by leaching Al2Au exhibit high catalytic activity towards CO oxidation. The presence of quite common nano-twins in the fcc lattice of porous Au significantly correlates with the catalytic activity. On the {211} surfaces of porous Au the twin boundaries can form chains of atoms with coordination number CN=6, which is denoted as W-chains. In contrast to the usually considered isolated low-coordinated active sites in Au as the corners of nanoparticles or the kinks on stepped of surfaces the W-chains form long rows of active Au sites. DFT calculations show that on the W-chains O2 chemisorbs and activated.

Academic Significance and Societal Importance of the Research Achievements

双晶は金属材料中では敬遠される格子欠陥であるが、触媒作用において活性点を作り出すサイトになる。双晶は金属ではよく知られているが、触媒化学分野では全く知られない。しかし、この双晶が触媒に多く活性サイトを形成することは、触媒活性の起源に新しい概念を与えている。金属と触媒の両分野において新しい境界分野を形成することで大いに学術的意義が存在する。また、表面積の小さなバルク金属であっても、大量の双晶を導入することで高い触媒活性を達成するという、高活性のバルク金属触媒の開発に新しい指針を与えており、現実の有害ガス除去の触媒開発に拍車がかかることで社会的深い意義をもっている。

Report

(5 results)
  • 2018 Annual Research Report   Final Research Report ( PDF )
  • 2017 Annual Research Report
  • 2016 Annual Research Report
  • 2015 Annual Research Report
  • Research Products

    (17 results)

All 2019 2018 2017 2016 2015

All Journal Article (8 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 8 results,  Acknowledgement Compliant: 1 results,  Open Access: 1 results) Presentation (9 results) (of which Int'l Joint Research: 1 results,  Invited: 5 results)

  • [Journal Article] Highly Selective Semi-hydrogenation of Acetylene over Porous Au with Twin Boundary Defects2019

    • Author(s)
      S. Kameoka, M. Krajci, A.P. Tsai,
    • Journal Title

      Appl. Catal

      Volume: A569 Pages: 101-109

    • DOI

      10.1016/j.apcata.2018.10.027

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effects of Cu oxidation states on the catalysis of NO +CO and N2O+CO reactions2019

    • Author(s)
      H. Iwamoto, S. Kameoka, Y. Xu, C. Nishimura, A.P. Tsai
    • Journal Title

      J. Phys, Chem. Solids,

      Volume: 125 Pages: 64-73

    • DOI

      10.1016/j.jpcs.2018.10.013

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Fast Oxidation of Porous Cu Induced by Nano-Twinning2018

    • Author(s)
      Kazue Nishimoto, Marian Krajci, Takayuki Sakurai, Hirone Iwamoto, Mitsuko Onoda, Chikashi Nishimura, Jeng-Ting Tsai, Sea-Fue Wang, Satoshi Kameoka, and An-Pang Tsai
    • Journal Title

      Inorg. Chem

      Volume: 57(5) Issue: 5 Pages: 2908-2916

    • DOI

      10.1021/acs.inorgchem.7b03225

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Probing Single Pt Atoms in Complex Intermetallic Al13Fe42018

    • Author(s)
      Yamada Tsunetomo、Kojima Takayuki、Abe Eiji、Kameoka Satoshi、Murakami Yumi、Gille Peter、Tsai An Pang
    • Journal Title

      Journal of the American Chemical Society

      Volume: 140 Issue: 11 Pages: 3838-3841

    • DOI

      10.1021/jacs.7b13658

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Understanding the Catalytic Activity of Nanoporous Gold: Role of Twinning in FCC Lattice2017

    • Author(s)
      M. Krajci, S. Kameoka, A.P. Tsai,
    • Journal Title

      J. Chem. Phys.

      Volume: 147 Issue: 4 Pages: 044713-044713

    • DOI

      10.1063/1.4994701

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Intermetallic: A Pseudoelement for Catalysis2017

    • Author(s)
      Tsai A. P.、Kameoka S.、Nozawa K.、Shimoda M.、Ishii Y.
    • Journal Title

      Accounts of Chemical Research

      Volume: 50 Issue: 12 Pages: 2879-2885

    • DOI

      10.1021/acs.accounts.7b00476

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Twinning in fcc lattice crates low-coordinated catalytically active sites in porous gold2016

    • Author(s)
      marian Krajci, Satoshi Kameoka, Anpang Tsai
    • Journal Title

      J. Chem. Phys.

      Volume: 145 Pages: 1-6

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
  • [Journal Article] Insights into the dominant factors of porous gold for CO oxidation2016

    • Author(s)
      Satoshi Kameoka, Toyokazu Tanabe, Kanji Miyamoto, and An Pang Tsai
    • Journal Title

      The Journal of Chemical Physics

      Volume: 144 Issue: 3 Pages: 034703-34703

    • DOI

      10.1063/1.4940307

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] The role of twinning   defects on catalysis in Au and Cu2018

    • Author(s)
      An-Pang Tsai, Satoshi Kameoka, Marian Marian Krajci
    • Organizer
      Pre-conference of TOCAT8 and the 5th  International Symposium of Institute for Catalysis
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Roles of defects and electronic structure in catalysis ;Twinning and concept of pseudoelement-2018

    • Author(s)
      蔡 安邦
    • Organizer
      Johnson Matthey Academic Conference 2018
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 金属学に基づく触媒作用の理解および触媒設計2018

    • Author(s)
      蔡 安邦
    • Organizer
      触媒学会つくば地区講演会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Al基金属間化合物のリーチング処理によるナノ・バルクハイブリット触媒材料の創製2018

    • Author(s)
      亀岡聡, 蔡安邦
    • Organizer
      日本金属学会2018年春期講演大会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 金の触媒作用における新しいメカニズムの提案 ― ナノ双晶の役割 ―2017

    • Author(s)
      蔡 安邦
    • Organizer
      第119回触媒討論会
    • Place of Presentation
      首都大学(東京都八王子市)
    • Year and Date
      2017-03-21
    • Related Report
      2016 Annual Research Report
  • [Presentation] ナノポーラスCuとAl2Cuのリーチング界面のTEM観察2017

    • Author(s)
      西本一恵
    • Organizer
      日本金属学会2017年春期講演大会
    • Place of Presentation
      首都大学(東京都八王子市)
    • Year and Date
      2017-03-15
    • Related Report
      2016 Annual Research Report
  • [Presentation] Twinning and Catalytic Activity of Carbon Monoxide Conversion in Nanoporous Silver Catalysts2017

    • Author(s)
      劉 珉宏
    • Organizer
      日本金属学会2017年春期講演大会
    • Place of Presentation
      首都大学(東京都八王子市)
    • Year and Date
      2017-03-15
    • Related Report
      2016 Annual Research Report
  • [Presentation] ポーラス金におけるナノ双晶による高い触媒活性の発現機構2017

    • Author(s)
      蔡安邦, 亀岡聡, M. Krajci
    • Organizer
      日本金属学会2017年秋期講演大会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] ラネー型触媒の微細組織とCO酸化特性2015

    • Author(s)
      櫻井孝之,西本一恵,大橋諭,亀岡聡,蔡安邦
    • Organizer
      日本金属学会2015年秋期講演大会
    • Place of Presentation
      九州大学
    • Year and Date
      2015-09-16
    • Related Report
      2015 Annual Research Report

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Published: 2015-04-16   Modified: 2020-03-30  

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