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DXAFS法によるゼオライトでの金属ナノクラスターの動的構造変化観察

Research Project

Project/Area Number 17034044
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionTottori University

Principal Investigator

奥村 和  鳥取大学, 工学部, 助手 (30294341)

Co-Investigator(Kenkyū-buntansha) 加藤 和男  高輝度光科学研究センター, 利用研究促進部門, 研究員
Project Period (FY) 2005 – 2006
Project Status Completed (Fiscal Year 2006)
Budget Amount *help
¥4,900,000 (Direct Cost: ¥4,900,000)
Fiscal Year 2006: ¥2,600,000 (Direct Cost: ¥2,600,000)
Fiscal Year 2005: ¥2,300,000 (Direct Cost: ¥2,300,000)
Keywordsゼオライト / クラスター / 時間分解EXAFS / パラジウム / 触媒 / EXAFS / ヘテロポリ酸 / フリーデル-クラフツ反応 / PROX反応 / モルデナイト / 白金
Research Abstract

ゼオライト細孔内に内包された金属クラスターは有用な触媒として機能するが、形成されるクラスターの構造は担体であるゼオライトの構造や酸性質の影響を強く受ける。本研究ではDXAFSやQXAFSといった手法によって水素雰囲気下でクラスターが形成される過程、または酸素によって再分散する過程を追跡し、触媒の活性点の形成に及ぼす担体の酸点の影響を調べることを目指した。酸型のモルデナイトやZSM-5にPdを担持し、水素雰囲気下でのクラスターの形成過程をDXAFSによって追跡した。その結果、一旦安定な6核クラスターを形成し、その後外表面上で凝集することがわかった。さらに500℃で酸素を導入すると、単分子状の酸化物として酸点上に再分散する様子が観察された。このような金属クラスターの形成・再分散は可逆的に見られた。H-Y型ゼオライトを担体とした場合には13核程度のクラスターが形成していた。このクラスター上ではHeck反応が溶媒に溶出せずに効率的に進行し、再利用も可能であることがわかった。H-Y型ゼオライトにAuを担持させたところ、0℃においてCO-O_2反応に高活性を示した。Na-Y型ゼオライトでは著しくAuが凝集していたのに対し、H-Yを使うとAuの凝集が抑制されていた。前処理時に酸点および気相にH_2が存在することにより高分散なAuクラスターが形成され、高活性を示したものと考えられる。

Report

(2 results)
  • 2006 Annual Research Report
  • 2005 Annual Research Report
  • Research Products

    (24 results)

All 2007 2006 2005

All Journal Article (23 results) Book (1 results)

  • [Journal Article] Formation and Redispersion of Silver Clusters in Ag-MFI Zeolite as Investigated by Time-Resolved QXAFS and UV-Vis2007

    • Author(s)
      Ken-ichi Shimizu, Kenji Sugino, Kazuo Kato, Shigeru Yokota, Kazu Okumura, Atsushi Satsuma
    • Journal Title

      J. Phys. Chem. C 111

      Pages: 1683-1688

    • Related Report
      2006 Annual Research Report
  • [Journal Article] The importance of Fe loading on the N_2O reduction with NH_3 over Fe-MFI : Effect of acid site formation on Fe species2007

    • Author(s)
      Kou Sugawara, Takeshi Nobukawa, Masanori Yoshida, Yoshihiro Sato, Kazu Okumura, Keiichi Tomishige, Kimio Kunimori
    • Journal Title

      Appl. Catal. B 69

      Pages: 154-163

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Surface modification of Ni catalysts with trace Pd and Rh for oxidative steam reforming of methane2007

    • Author(s)
      Yuya Mukainakano, Baitao Li, Shigeru Kado, Tomohisa Miyazawa, Kazu Okumura, Toshihiro Miyao, Shuichi Naito, Kimio Kunimori, Keiichi Tomishige
    • Journal Title

      Appl. Catal. A 318

      Pages: 252-252

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Reductive Activation of O_2 with H_2 Reduced Silver Clusters as a Key Step in the H_2-Promoted Selective Catalytic Reduction of NO with C_3H_8 over Ag/Al_2O_32007

    • Author(s)
      Ken-ichi Shimizu, Masao Tsuzuki, Kazuo Kato, Shigeru Yokota, Kazu Okumura, Atsushi Satsuma
    • Journal Title

      J. Phys. Chem. C 111

      Pages: 950-959

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Role of active oxygen transients in selective catalytic reduction of N_2O with CH_4 over Fe-zeolite catalysts2007

    • Author(s)
      Takeshi Nobukawa, Kou Sugawara, Kazu Okumura, Keiichi Tomishige, Kimio Kunimori
    • Journal Title

      Appl. Catal. B : Environmental 70

      Pages: 342-352

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Neutron diffraction an X-ray absorption study of Ag5Pb2O62007

    • Author(s)
      K.Yoshii, M.Mizumaki, K.Kato, T.Uruga, H.Abe, A.Nakamura, Y.Shimojo, Y.Ishii, Y.Morii
    • Journal Title

      J. Solid State Chem. 3180

      Pages: 377-381

    • Related Report
      2006 Annual Research Report
  • [Journal Article] ime-Resolved Energy-Dispersive XAFS Station for Wide-Energy Range at SPring-82007

    • Author(s)
      Kazuo Kato., Tomoya Uruga, Hajime Tanida, Shigeru Yokota, Kazu Okumura, Yasuhiko Imai
    • Journal Title

      AIP Conference Proceeding i87

      Pages: 1214-1217

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Development of Ni catalysts for tar removal by steamgasification of biomass2006

    • Author(s)
      Takeo Kimura, Tomohisa Miyazawa, Jin Nishikawa, Shigeru Kado, Kazu Okumura, Toshihiro Miyao, Shuichi Naito, Kimio Kunimori, Keiichi Tomishige
    • Journal Title

      Applied Catalysis B : Environmental 68

      Pages: 160-170

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Oxidative steam reforming of methane under atmospheric and pressurized conditions over Pd/NiO-MgO2006

    • Author(s)
      Mohammad Nurunnabi, Yuya Mukainakano, Shigeru Kado, Tomohisa Miyazawa, Kazu Okumura, Toshihiro Miyao, Shuichi Naito, Kimihito Suzuki
    • Journal Title

      Appl. Catal. A 308

      Pages: 1-1

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Pd loaded on high silica support active for the total oxidation of diluted methane in the presence of water vapor2006

    • Author(s)
      Kazu Okumura, Eishi Shinohara, Miki Niwa
    • Journal Title

      Catal. Today 117

      Pages: 577-583

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Strong Inhibition Effect of Sulfur Impurities in Alumina Suports on the Catalytic Activity of Rh in the CH_4-CO_2 Reforming Reaction2006

    • Author(s)
      Shigeru Yokota, Kazu Okumura, Miki Niwa
    • Journal Title

      Appl. Catal. A 310

      Pages: 122-126

    • Related Report
      2006 Annual Research Report
  • [Journal Article] Speciation of iodine in solid environmentaI samples by iodine K-edge XANES : application to soils and ferromanganese oxides2006

    • Author(s)
      Sayuri Kodama, Yoshio Takahashi, Kazu Okumura, Tomoya Uruga
    • Journal Title

      Science of the Total Environment 363

      Pages: 275-284

    • Related Report
      2006 Annual Research Report
  • [Journal Article] The Active and Reusable Catalyst in the Friedel-Crafts Alkylation Derived from a Heteropoly Acid2005

    • Author(s)
      K.Okumura, K.Yamashita, M.Hirano, M.Niwa
    • Journal Title

      Journal of Catalysis 234(2)

      Pages: 300-300

    • NAID

      10015544076

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Quick XAFS Studies on the Y-Type Zeolite Supported Au Catalysts for CO-O_2 Reaction2005

    • Author(s)
      K.Okumura, K.Yoshino, K.Kato, M.Niwa
    • Journal Title

      Journal of Physical Chemistry B 109(25)

      Pages: 12380-12380

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Active and Reusable Catalyst in the Friedel-Crafts Alkylation Derived from a Heteropoly Acid2005

    • Author(s)
      K.Okumura, K.Yamashita, M.Hirano, M.Niwa
    • Journal Title

      Chemistry Letters 34

      Pages: 716-716

    • NAID

      10015544076

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Catalytic Performance and Elution of Pd in the Heck Reaction over Zeolite Supported Pd Cluster Catalyst2005

    • Author(s)
      K.Okumura, K.Nota, K.Yoshida, M.Niwa
    • Journal Title

      Journal of Catalysis 231

      Pages: 245-245

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Fe-MFI触媒上のN_2O還元反応における還元剤の種類による影響と活性点の構造解析2005

    • Author(s)
      菅原康, 信川健, 野口義雄, 奥村和, 他
    • Journal Title

      表面科学 26

      Pages: 385-385

    • NAID

      10016588026

    • Related Report
      2005 Annual Research Report
  • [Journal Article] X線吸収微細構造法によるゼオライト細孔内における金属クラスターの形成過程観察2005

    • Author(s)
      奥村 和, 加藤和男
    • Journal Title

      表面 42

      Pages: 233-233

    • NAID

      40006646310

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Speciation of osmium in an iron meteorite and a platinum ore specimen based on X-ray absorption fine-structure spectroscopy2005

    • Author(s)
      N.Sakakibara, Y.Takahashi, K.Okumura, et al.
    • Journal Title

      Geochemical Journal 39

      Pages: 383-383

    • NAID

      40006831412

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Selective Catalytic Reduction of NO by Methane over Pd Loaded on heteropolyacids/SiO_2 at Low Temperature2005

    • Author(s)
      K.Okumura, R.Yoshimoto, K.Suzuki, M.Niwa
    • Journal Title

      Bulletin of Chemical Society of Japan 78

      Pages: 361-361

    • NAID

      10014367069

    • Related Report
      2005 Annual Research Report
  • [Journal Article] 環境触媒としてのパラジウム触媒におけるゼオライトの担体効果2005

    • Author(s)
      奥村和, 丹羽幹
    • Journal Title

      触媒 47

      Pages: 21-21

    • NAID

      10014095002

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Effect of reductants in N_2O reduction over Fe-MFI catalysts2005

    • Author(s)
      T.Nobukawa, M.Yoshida, K.Okumura, et al.
    • Journal Title

      Journal of Catalysis 229

      Pages: 374-374

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Spontaneous Dispersion of PdO and Generation of Metal Pd cluster in Zeolites Studied by Means of in situ DXAFS2005

    • Author(s)
      K.Okumura, R Yoshimoto, S Yokota, Kazuo Kato, et al.
    • Journal Title

      Physica Scripta T115

      Pages: 816-816

    • Related Report
      2005 Annual Research Report
  • [Book] SPring-8の高輝度放射光を利用した先端触媒開発2006

    • Author(s)
      奥村和・丹羽幹
    • Total Pages
      477
    • Publisher
      エヌ・ティー・エス
    • Related Report
      2006 Annual Research Report

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Published: 2005-04-01   Modified: 2018-03-28  

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