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アルカン選択的活性化のための触媒反応場設計

Research Project

Project/Area Number 13126210
Research Category

Grant-in-Aid for Scientific Research on Priority Areas

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

Principal Investigator

服部 忠  名古屋大学, 大学院・工学研究科, 教授 (50023172)

Co-Investigator(Kenkyū-buntansha) 吉田 寿雄  名古屋大学, 難処理人工物研究センター, 助教授 (80273267)
薩摩 篤  名古屋大学, 大学院・工学研究科, 助教授 (00215758)
鬼頭 繁治  愛知工業大学, 教授 (20023343)
Project Period (FY) 2001 – 2004
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥20,600,000 (Direct Cost: ¥20,600,000)
Fiscal Year 2003: ¥4,800,000 (Direct Cost: ¥4,800,000)
Fiscal Year 2002: ¥7,700,000 (Direct Cost: ¥7,700,000)
Fiscal Year 2001: ¥8,100,000 (Direct Cost: ¥8,100,000)
Keywords触媒反応工学 / アルカン / 触媒 / 選択還元 / 選択酸化 / 反応雰囲気 / 光触媒 / ニューラルネットワーク / in-situ IR / in-situ UV-Vis
Research Abstract

触媒の活性制御因子はしばしば反応雰囲気に著しく依存するため、触媒システムの最適化には触媒反応場と触媒作用との因果関係の解明が重要な課題となる。本年度は以下に示す成果を得た。担持Ag触媒上でのNO選択還元反応において、反応場へ添加した水素がAg種を還元・凝集させ、高活性種であるAg^<δ+>クラスターを形成する現象が見いだされた。ゼオライトを用いて、担体効果を検討したところ、MFI, BEAでは水素添加によりNO還元活性が飛躍的に向上するが、MORやYでは水素の効果は大きくなかった。Ag-MFI,-MORの反応ガス処理後のUV-Visスペクトルを比較したところ、H_2共存下で250,285nmにAg^<δ+>クラスターに帰属される新たな吸収が観察された。一方MORでは高濃度の水素を共存させることによって初めてAgnd+clusterの吸収が観察された。Ag^<δ+>クラスター形成と水素による促進効果に相関性が見られ、水素により還元凝集したAg^<δ+>クラスターの形成によりNO選択還元反応の活性が向上すること見いだされた。Agnd+clusterの形成が可逆的であり、ゼオライト酸強度、すなわちゼオライトのアニオンとしての強度に依存することから、Ag^+イオンとAg^<δ+>クラスターは一種の平衡状態で触媒上に存在すると理解された。さらにこの知見をアルミナ担持Ag触媒に拡張するため、各種添加物で修飾したアルミナを担体としたAg触媒を用いて担体効果を検討した。MgおよびZnでのアルミナの修飾によって、NO転化率の向上が見られた。表面積に大差はなく、活性向上は表面積以外の因子による。酸量の多い担体ほどNO転化率が高いことから、Ag-ゼオライトの場合と同様に、担体の酸量が活性に依存していることが示唆された。

Report

(3 results)
  • 2003 Annual Research Report
  • 2002 Annual Research Report
  • 2001 Annual Research Report
  • Research Products

    (20 results)

All Other

All Publications (20 results)

  • [Publications] J.Shibata, K.Shimizu, S.Satokawa, A.Satsuma, T.Hattori: "Promotion effect of hydrogen on surface steps in SCR of NO by propane over alumina-based silver catalyst as examined by transient FT-IR"Phys.Chem.Chem.Phys.. 5. 2154-2160 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.Satsuma, A.Shichi, T.Hattori: "Zeolite Micropore as Unique Reaction Field for the Selective Catalytic Reduction of NO by Hydrocarbons"CATTECH. 7. 6-14 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] J.Shibata, Y.Takada, A.Shichi, S.Satokawa, A.Satsuma, T.Hattori: "Ag Cluster as Active Species for SCR of NO by propane in the Presence of Hydrogen over Ag-MFI"J.Catal.. (印刷中). (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yoshida, M.G.Chaskar, Y.Kato, T.Hattori: "Active sites on silica-supported zirconium oxide for photoinduced direct methane conversion and photoluminescence"J.Photochem.Photobio.A. 160. 47-53 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yoshida, N.Matsushita, Y.Kato, T.Hattori: "Synergistic active sites on SiO_2-Al_2-TiO_2photocatalysts for direct methane coupling"J.Phys.Chem.B. 107. 8355-8362 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Yoshida, 他5名: "Active Ag species in MFI Zeolite for Direct Methane Conversion in the light and dark"Res.Chem.Intermed.. 29. 897-910 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] Y.Kato, H.Yoshida, T.Hattori: "Photo-induced non-oxidative coupling of methane over H-zeolite around room temperature"Micropor.Mesopor.Mater.. 51. 223-231 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Kato, N.Matsushita, H.Yoshida, T.Hattori: "Highly active silica-alumina-titania catalyst for photoinduced non-oxidative methane coupling"Catal.Commun.. 3. 99-103 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] H.Yoshida, N.Matsushita, Y.Kato, T.Hattori: "Active sites in sol-gel prepared silica-alumina for photoinduced non-oxidative methane coupling"Phys.Chem.Chem.Phys.. 4. 2459-2465 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] H.Yoshida, M.G.Chaskar, Y.Kato, T.Hattori: "Fine structural photoluminescence spectra of silica-supported zirconium oxide and its photoactivity in direct methane conversion"Chem.Commun.. 2002. 2014-2015 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Nishi, S.Komai, K.Inagaki, A.Satsuma, T.Hattori: "Structure and Catalytic Properties of Ga-MFI in Propane Aromatization"Appl.Catal.A : General. 223. 187-193 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] 薩摩 篤, 柴田順二, 里川重夫: "反応場による触媒の高機能化-Ag触媒上でのNO選択還元を例として-"化学工学. 66. 35-37 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] J.Shibata, K.Shimizu, A.Satsuma, T.Hattori: "Influence of Hydrocarbon Structure on Selective Catalytic Reduction of NO over Cu-Al_2O_3"Appl.Catal.B : Environmental. 37. 197-204 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Shichi, A.Satsuma, T.Hattori: "Influence of hydrocarbon molecular size on the selective catalytic reduction of NO by hydrocarbons over Cu-MFI zeolite"Appl.Catal.A. 207. 315-321 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Shimizu, J.Shibata, H.Yoshida, A.Satsuma, T.Hattori: "Silver-alumina catalysts for selective reduction of NO by higher hydrocarbons : structure of active sites and reaction mechanism"Appl.Catal.B. 30. 151-162 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] J.Shibata, K.Shimizu, A.Satsuma, T.Hattori: "Influence of hydrocarbon structure on selective catalytic reduction of NO by hydrocarbons over Cu-Al2O3"Appl.Catal.B. (印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.Shichi, Y.Kawamura, A.Satsuma, T.Hattori: "Effect of carbon number in hydrocarbon reductant on the selective catalytic reduction of NO over cation-exchanged MFI zeolites"Stud.Surf.Sci.Catal.. 135. 30-O-03 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Shimizu, J.Shibata, A.Satsuma, T.Hattori: "Mechanistic causes of hydrocarbon effect on the activity of Ag-Al2O3 catalyst for selective reduction NO"Phys.Chem.Chem.Phys.. 3. 880-884 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.Satsuma, 他5名: "Insertion of iron-complex to lamellar vanadyl benzylphosphate for preparation of well-defined catalyst"Catal.Today. 71. 161-167 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Shimizu, A.Satsuma, T.Hattori: "Metal oxide catalysts for selective reduction of NOx by hydrocarbons : toward molecular basis for catalyst design"Catalysis Survey from Japan. 4. 115-123 (2001)

    • Related Report
      2001 Annual Research Report

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Published: 2001-04-01   Modified: 2018-03-28  

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