Project/Area Number |
14350425
|
Research Category |
Grant-in-Aid for Scientific Research (B)
|
Allocation Type | Single-year Grants |
Section | 一般 |
Research Field |
触媒・化学プロセス
|
Research Institution | Nagoya 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)
|
Keywords | NOx / 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.
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