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Improvement of catalyst for selective reduction of NO by controlling reaction atmospheres

Research Project

Project/Area Number 14350425
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionNagoya University

Principal Investigator

SATSUMA Atsushi  Nagoya University, Graduate School of Engineering, Professor, 工学研究科, 教授 (00215758)

Co-Investigator(Kenkyū-buntansha) YOSHIDA Hisao  Nagoya University, Eco Topia Science Institute, Associate Professor, エコトピア科学研究機構, 助教授 (80273267)
SHIMIZU Ken-ichi  Nagoya University, Graduate School of Engineering, Research Associate, 工学研究科, 助手 (60324000)
服部 忠  名古屋大学, 工学研究科, 教授 (50023172)
Project Period (FY) 2002 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥14,200,000 (Direct Cost: ¥14,200,000)
Fiscal Year 2004: ¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 2003: ¥5,000,000 (Direct Cost: ¥5,000,000)
Fiscal Year 2002: ¥7,000,000 (Direct Cost: ¥7,000,000)
KeywordsNOx / Selective Reduction / Catalyst / Reaction atmospheres / Reaction mechanism / in-situ spectroscopy / Dynamics of active species / Diesel engine
Research Abstract

The addition of hydrogen in the reaction atmosphere is effective in promoting the activity of Ag/alumina and Ag-zeolites on the selective reduction of NO by hydrocarbons (HC-SCR) at low temperatures. The increment of NO conversion over Ag-MFI corresponds to the periodic addition of hydrogen into C_3H_8-SCR conditions. The UV-Vis spectra of Ag-MFI have revealed that the addition of hydrogen results in the formation of Ag_n^<□+> clusters due to partial reduction and agglomeration of Ag species The coincidence of the formation of the Ag_n^<□+> clusters and the increment of NO conversion suggests that Ag_n^<□+> clusters are the highly active species for HC-SCR. From analysis by H_2-TPR, UV-Vis, and EXAFS, the structure of Ag_n^<□+> clusters on Ag-MFI is identified as being Ag_4^<2+> on average. The formation of Ag clusters was strongly affected by the type of zeolites : The major Ag species are Ag^+ ions for MOR, Ag_n^<□+> clusters for MFI and BEA, and relatively large metallic Ag_m particles for Y. The sequence of Ag agglomeration (MOR<MFI<BEA<Y) is in accordance with the strength of the acid sites of zeolites. It can be expected that the interaction between the positive charge of Ag_n^<□+> clusters and acid sites, i.e., the ion-exchange site of zeolites, stabilizes Ag_n^<□+> clusters. The type of Ag species under HC-SCR conditions depends on the concentration of gas-phase oxidants (NO,O_2) and reductants (H_2,HC), and also on the number and strength of the zeolite acid sites.

Report

(4 results)
  • 2004 Annual Research Report   Final Research Report Summary
  • 2003 Annual Research Report
  • 2002 Annual Research Report
  • Research Products

    (20 results)

All 2004 Other

All Journal Article (7 results) Publications (13 results)

  • [Journal Article] Ag Cluster as Active Species for SCR of NO by propane in the Presence of Hydrogen over Ag-MFI2004

    • Author(s)
      J.Shibata, Y.Takada, A.Shichi, S.Satokawa, A.Satsuma, T.Hattori
    • Journal Title

      Journal of Catalysis 222

      Pages: 368-376

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Drastic Enhancement of SCR of NO over Ir Catalyst through Formation of Metallic Iridium on Na-zeolite2004

    • Author(s)
      J.Shibata, H.Yoshida, A.Satsuma, T.Hattori
    • Journal Title

      Chemistry Letters 33

      Pages: 800-801

    • NAID

      10013284289

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Adsorption-controlled Diffusion in Catalytic Reduction of NO with Hydrocarbons over Zeolite Catalysts2004

    • Author(s)
      A.Shichi, A.Satsuma, T.Hattori
    • Journal Title

      Catalysis Today 93-95

      Pages: 777-781

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Structure of active Ag clusters in Ag-zeolites for SCR of NO by propane in the presence of hydrogen2004

    • Author(s)
      J.Shibata, K.Shimizu, Y.Takada, A.Shichi, S.Satokawa, A.Satsuma, T.Hattori
    • Journal Title

      Journal of Catalysis 227

      Pages: 367-374

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Influence of zeolite support on activity enhancement by addition of hydrogen for SCR of NO by propane over Ag-zeolites2004

    • Author(s)
      J.Shibata, Y.Takada, A.Shichi, S.Satokawa, A.Satsuma, T.Hattori
    • Journal Title

      Applied Catalysis B : Environmental 54

      Pages: 137-144

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Factors controlling activity and selectivity for SCR of NO by hydrogen over supported Pt catalysts2004

    • Author(s)
      J.Shibata, M.Hashimoto, K.Shimizu, H.Yoshida, T.Hattori, A.Satsuma
    • Journal Title

      Journal of Physical Chemistry, B 108

      Pages: 18327-18335

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Annual Research Report 2004 Final Research Report Summary
  • [Journal Article] Factors controlling activity and selectivity for SCR of NO by hydrogen over supported Pt catalysts2004

    • Author(s)
      J.Shibata, M.Hashimoto, K.Shimizu, H.Yoshida, T.Hattori, A.Satsuma
    • Journal Title

      Journal of Physical Chemistry B 108

      Pages: 18327-18335

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [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, M.Hashimoto, J.Shibata, H.Yoshida, T.Hattori: "Nitrous oxide free pathway for selective reduction of NO by hydrogen over supported Pt catalysts"Chem.Commun.. 2003. 1698-1699 (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. 42-51 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.Satsuma, K.Shimizu: "In-situ FT/IR Study of Selective Catalytic Reduction of NO over Alumina-based Catalysts"Progress in Energy and Combustion Science. 29. 71-84 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 薩摩 篤, 柴田順二, 服部 忠: "UV-visibleスペクトルによる固体触媒表面のin-situ観察"Jasco Report. 45. 5-9 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] T.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] A.Satsuma他4名: "Influence of Hydrocarbon Structure on Selective Catalytic Reduction of NO over Cu-Al_2O_3"Appl. Catal. B. 37. 197-204 (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(6). 35-37 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] 志知明, 薩摩篤, 服部忠: "ゼオライト触媒上での炭化水素脱硝における細孔内拡散の影響"化学工業, 53(9), 696-699(2002). 53(9). 696-699 (2002)

    • Related Report
      2002 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. 42-51 (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Satsuma他4名: "In-situ UV-visible Spectroscopic Study for Dynamic Analysis of Silver Catalyst"Abst. 4^<th> Tokyo Conf. Adv. Catal. Sci. Tech.. 4. 20 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Satsuma他4名: "In-situ FT/IR Study of Selective Catalytic Reduction of NO over Alumina-based Catalysts"Progress in Energy and Combustion Science. (印刷中).

    • Related Report
      2002 Annual Research Report
  • [Publications] 薩摩篤, 柴田順二, 服部忠: "UV-visibleスペクトルによる固体触媒表面のin-situ観察"Jasco Report. (印刷中).

    • Related Report
      2002 Annual Research Report

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Published: 2002-04-01   Modified: 2016-04-21  

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