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Creation of Ni(0) with superparamagnetic nature and Ni(I) species and their characterization

Research Project

Project/Area Number 16H04118
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic chemistry
Research InstitutionOkayama University

Principal Investigator

Kuroda Yasushige  岡山大学, 自然科学研究科, 特任教授 (40116455)

Co-Investigator(Kenkyū-buntansha) 大久保 貴広  岡山大学, 自然科学研究科, 准教授 (30385554)
砂月 幸成  岡山大学, 自然生命科学研究支援センター, 助教 (80362987)
Project Period (FY) 2016-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥17,940,000 (Direct Cost: ¥13,800,000、Indirect Cost: ¥4,140,000)
Fiscal Year 2018: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2017: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2016: ¥15,210,000 (Direct Cost: ¥11,700,000、Indirect Cost: ¥3,510,000)
Keywordsゼオライト / ゼオライトを利用した新奇電子状態創出 / 超常磁性ニッケル種 / ニッケルクラスター / ニッケル超酸化物形成 / 室温でのCO酸化反応 / 亜鉛イオン-オキシル種 / 室温でのメタン活性化 / ゼオライト細孔 / 一価ニッケルイオン / X線微細構造解析 / 振動電子遷移 / 亜鉛-オキシル種 / 一価カドミウム二量体 / コバルト酸素活性種 / 新奇電子状態創出 / CO分子の活性化 / 磁気特性 / 新物質創出場 / ニッケル微粒子 / 超常磁性 / ゼオライト空間 / 一価ニッケルイオン創出 / 電子スピン共鳴法 / 紫外可視吸収分光法 / 赤外線吸収分光法 / イオン交換遷移金属イオン / 小分子の活性化 / 微粒子創出法
Outline of Final Research Achievements

We have succeeded in creating sub-nano sized stable Ni-cluster by utilizing zeolite as a nano-reaction pot and found its prominent superparamagenetic property, and also preparing a novel monovalent nickel ion which accelerates the CO-oxidation reaction even at 300 K. In addition, a monovalent zinc ion, as well as an atomic zinc species, were prepared in zeolite which activate dioxygen at 300 K, resulting in the formation of zinc-oxyl species via zinc ozonide. It has been clarified that thus formed zinc oxyl species activates methane to form methanol at 300 K. On the basis of these data, it has become apparent that the zeolite-lattice as a specific reaction field confers unprecedented electronic states onto the exchanged ions. As a future perspective, it is expected that these fascinating results will give new guidlines for developing efficient materials which exhibit helpful functionalities in both academic and applied fields.

Academic Significance and Societal Importance of the Research Achievements

我々はゼオライトを特異反応場創製のためのリアクションポットとして利用することによって,今までにない,金属イオンの新奇な(表面新物質としての)特性を創出できることを提案している.本研究により,電荷をもたないサブナノサイズのニッケルクラスター,一価ニッケル種や原子状亜鉛種,一価亜鉛種などがゼオライト中で安定に存在できるという驚くべき発見となった.これらの成果により,分布幅の狭い状態でニッケルクラスターや一価ニッケル種および原子状亜鉛種,一価亜鉛種などの磁気特性や触媒能を利用した系への展開が期待される.以上のように,本研究は画期的な内容であり,学術的にも応用化学の面でも意義深い研究である.

Report

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

    (15 results)

All 2019 2018 2017 2016

All Journal Article (7 results) (of which Peer Reviewed: 7 results,  Open Access: 1 results,  Acknowledgement Compliant: 1 results) Presentation (8 results) (of which Invited: 1 results)

  • [Journal Article] Room-Temperature Activation of the C-H bond in Methane over Terminal ZnII-Oxyl Species in an MFI Zeolite: A Combined Spectroscopic and Computational Study of the Reactive Frontier Molecular Orbitals and Their Origins (selected as supplementary cover art)2019

    • Author(s)
      A. Oda, T. Ohkubo, T. Yumura, H. Kobayashi, and Y.Kuroda
    • Journal Title

      Inorg. Chem.

      Volume: 58 Pages: 327-338

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Room Temperature O Transfer from NO to CO Mediated by Nearest Cd(I) Ions in MFI Zeolite Cavity (selected as Front inside cover)2019

    • Author(s)
      A. Oda, T. Ohkubo, and Y. Kuroda
    • Journal Title

      Dalton Trans.

      Volume: 48 Issue: 7 Pages: 2308-2317

    • DOI

      10.1039/c8dt04425b

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Idenitification of a stable ZnII-Oxyl species produced in an MFI zeolite and its reversible reactivity with O2 at room temperature2017

    • Author(s)
      A. Oda, T. Ohkubo, T. Yumura, H. Kobayashi, Y. Kuroda
    • Journal Title

      Angew. Chem. Int. Ed.

      Volume: 56 Issue: 33 Pages: 9715-9718

    • DOI

      10.1002/anie.201702570

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Surplus adsorption of bromide ion into pi-conjugated carbon nanospaces assisted by proton coadsorption2017

    • Author(s)
      T. Ohkubo, M. Nishi, M. Yamasaki, H. Takagi, and Y. Kuroda
    • Journal Title

      J. Colloid Interface Sci.

      Volume: 508 Pages: 415-418

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Why do zeolites induce unprecedented electronic state on exchanged metal ions?2017

    • Author(s)
      A. Oda, T. Ohkubo, T. Yumura, H. Kobayashi, and Y. Kuroda
    • Journal Title

      Phys. Chem. Chem. Phys.

      Volume: 19 Issue: 36 Pages: 25105-25114

    • DOI

      10.1039/c7cp02669b

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Utilizing Super-atom Orbital Ideas to Understand Properties of Silver Clusters inside ZSM-5 Zeolite2017

    • Author(s)
      Yumura, T.; Kumondai, M.; Wakasugi, T.; Kuroda, Y.; Kobayashi, H.
    • Journal Title

      RSC Advances

      Volume: 7 Issue: 9 Pages: 4950-4959

    • DOI

      10.1039/c6ra26492a

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Tubular nitrogen-doped TiO2 samples with efficient photocatalytic properties based on long-lived charge separation under visible-light irradiation: synthesis, characterization and reactivity2017

    • Author(s)
      Y. Hirose, A. Itadani, T. Ohkubo, H. Hashimoto, J. Takada, S. Kittaka, and Y. Kuroda
    • Journal Title

      Dalton Trans.

      Volume: 46 Issue: 13 Pages: 4435-4451

    • DOI

      10.1039/c6dt04914a

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Presentation] 新奇な吸着・活性化場および物質創出場としてのゼオライト2018

    • Author(s)
      黒田 泰重
    • Organizer
      第28回吸着シンポジウム(吸着夏の学校)
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] M FI型ゼオライト特有のサイト上で創出されたCoの新奇な酸素活性化能:[Co(III)O2]+形成サイトの局所構造解析2018

    • Author(s)
      豆成優樹,織田晃,大久保貴広,黒田泰重
    • Organizer
      第32回日本吸着学会研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] MFI型ゼオライトを反応場としたNi+種の創製とその酸化・還元特性2017

    • Author(s)
      南條翼・織田晃・砂月幸成・大久保貴広・黒田泰重
    • Organizer
      日本化学会第97春季年会
    • Place of Presentation
      慶應義塾大学 日吉キャンパス
    • Year and Date
      2017-03-16
    • Related Report
      2016 Annual Research Report
  • [Presentation] MFI 型ゼオライトを反応場としたNi+種の創製とその酸化・ 還元特性2017

    • Author(s)
      南條翼・織田晃・大久保貴広・黒田泰重
    • Organizer
      日本化学会 第97春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] ゼオライト場を利用したNiⅡ超酸化物種の創製とCOの常温酸化2017

    • Author(s)
      南條翼・織田晃・大久保貴広・黒田泰重
    • Organizer
      第25回 ゼオライト夏の学校
    • Related Report
      2017 Annual Research Report
  • [Presentation] Co(I)イオン交換ゼオライト上で起る室温における酸素の二電子還元:Co(III)-peroxoの形の形成機構,電子構造,案ラビに反応性の形成機構,電子構造,ならびに反応性2017

    • Author(s)
      豆成優樹,織田晃,大久保貴広,黒田 泰重
    • Organizer
      日本化学会 第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] RT hydroxylation of methane over Zu(II)-Oxyl created in MFI zeolite2017

    • Author(s)
      Oda Akira, Ohkubo Takahiro, Kuroda Yasushige
    • Organizer
      日本化学会 第98春季年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] ゼオライト場を利用したニッケルの新奇電子状態創出とその特性2016

    • Author(s)
      南條翼・織田晃・砂月幸成・大久保貴広・黒田泰重
    • Organizer
      コロイドおよび界面化学討論会
    • Place of Presentation
      北海道教育大学 旭川校
    • Year and Date
      2016-09-22
    • Related Report
      2016 Annual Research Report

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Published: 2016-04-21   Modified: 2020-03-30  

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