2007 Fiscal Year Final Research Report Summary
Ag Cluster Catalyst-Research of Reaction Mechanism and Development of Diesel deNOx Catalyst
| Project/Area Number |
17360386
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Catalyst/Resource chemical process
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| Research Institution | Nagoya University |
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Principal Investigator |
SATSUMA Atsushi Nagoya University, Graduate School ofEngineering, Professor (00215758)
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| Co-Investigator(Kenkyū-buntansha) |
SHIMIZU Kenichi Nagoya University, Graduate Sehml ofEngineering, Assistant Professor (60324000)
SAWABE Kyoichi Nagoya University, Graduate School of Engineering, Lecturer (80235473)
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| Project Period (FY) |
2005 – 2007
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| Keywords | Silver / Cluster / Selective Reduction of NOx / Diesel engines / in-situ Spectroscopy / DFT calculation / Active oxygen / Reaction mechanism |
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| Research Abstract |
Reduction of NOx from diesel engine cars is serious problem from environmental points of view. We have found that Ag duster having the Size of nano to sub-nano scale is very effective for the selective reduction of NOx by unburned hydrocarbons RIC-SCR) in the excess of oxygen. The aim of this project is to reveal the dynamics and the reaction mechanism of HC-SCR over Ag duster by using in-situ spectroscopy and DET calculations in order to guide the design of practical catalysts. The following results have been obtained in the term of the project.
1.Reactivity and reaction mechanism of Ag duster : It was hind by ESR spectrometer that the contact of gaseous oxygen and Ag duster formed by a slight reduction of Ag-alumina by hydrogen results in the formation of super-oxide species. The important role of Ag duster on the activation of oxygen was clarified. Furthermore, the role of hydrogen on the activation of oxygen and the formation of Ag cluster was suggested.
2. Evaluation of reaction mechanism by DFP calculation: Formation of Ag duster by hydrogen and activation of oxygen on its surface was evaluated by DFP calculation. Ag 4-membered cluster (Ag_4^<2+>) is the most stable in zeolite cage, which is in harmony with the experimental results by EKAFS. The contact of hydrogenated Ag duster (H-H-Ag_4^<2+>) with oxygen results in the formation of hydrogen peroxide. The experimental results can be rationalized by this model, because the hydrogen peroxide is active for both oxidation of hydrocarbons ns to oxygenated species and NO to NO2
3. SOx tolerance of Ag duster in the presence of hydrogen: High SOx tolerance of Ag duster was achieved through optimization of the kind of reductants, temperature, and co-feeding of hydrogen. The high SIX tolerance is caused by migration of SOx from Ag surface to gas phase or alumina support.
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[Journal Article] Atsushi Satsuma, Reactive Activation of 02 with HZ-Reduced Silver Clusters a Key Step in the H2-Promoted Selective Catalytic Reduction of NO with C3Hg over Ag/AI2032007
Author(s)
Ken-ichi, Shimizu, Masao, Tsuzuki, Kazuo, Kato, Shigeru, Yokota, Kazu, Okumura
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Journal Title
J. Phys. Chem. C 111
Pages: 950-959
Description
「研究成果報告書概要(欧文)」より
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[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
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Journal Title
J. Phys. Chem. C 111(4)
Pages: 1683-1688
Description
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[Journal Article] Atsushi Satsuma, Reaction Mechanism of H2-Promoted Selective Catalytic Reduction of NO with C3H8 over Ag-MFI Zeolites2007
Author(s)
Ken-ichi, Shimizu, Kenji, Sugino, Kazuo, Kato, Shigeru, Yokota, Kant, Okumura
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Journal Title
J. Phys. Chem. C 111
Pages: 6481-6487
Description
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[Journal Article] Stability of Pd(II) ion in side pocket of mordenite under hydrothermal conditions2005
Author(s)
Atsushi, Satsuma, Yasuhiro, Sahashi, Junji, Shibata, Koji, Nishi, Shigeo, Satokawa, Keiji, Itabashi, Shin-ichi, Komai, Hisao, Yoshida, Tadashi, Hattori
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Journal Title
Micro. Meso. Mater 81
Pages: 135-138
Description
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[Presentation] ,Effect of Supports on Formation and Reduction Rate of Stored Nitrates on NSR Catalysts as Investigated by in-situ FUR2007
Author(s)
Ken-ichi, Shimizu, Yoshinori, Saito, Takeshi, Nobukawa, Naoto, Miyoshi, Atsushi, Satsuma
Organizer
3rd China-Japan Workshop on Environmental Catalysis and Eco-Materials, Tsinghua University
Place of Presentation
Beijing, China
Year and Date
20071010-12
Description
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[Presentation] Oxidation State of Supported-Metal (Ag, Pt, Ir) Species as an Important Factor for the Selective Catalytic Reduction of NO in Hydrogen Containing Atmosphere2005
Author(s)
Atsushi, Satsuma, Junji, Shibata, Ken-ichi, Shimizu, Hisao, Yoshida, Tadashi, Hattori
Organizer
5th Japan-Korea Symposium on Catalysts
Place of Presentation
Matsue, Japan
Year and Date
20050511-13
Description
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