Role of active oxygen transients in selective catalytic reduction of N2O with CH4 over Fe-zeolite catalysts

Takeshi Nobukawa; Kou Sugawara; Kazu Okumura; Keiichi Tomishige; Kimio Kunimori

doi:10.1016/j.apcatb.2005.11.032

Role of active oxygen transients in selective catalytic reduction of N₂O with CH₄ over Fe-zeolite catalysts

Takeshi Nobukawa, Kou Sugawara, Kazu Okumura, Keiichi Tomishige, Kimio Kunimori

ENG - Applied Chemistry

Research output: Contribution to journal › Article › peer-review

35 Citations (Scopus)

Abstract

Sharp NO and O₂ desorption peaks, which were caused by the decomposition of nitro and nitrate species over Fe species, were observed in the range of 520-673 K in temperature-programmed desorption (TPD) from Fe-MFI after H₂ treatment at 773 K or high-temperature (HT) treatment at 1073 K followed by N₂O treatment. The amounts of O₂ and NO desorption were dependent on the pretreatment pressure of N₂O in the H₂ and N₂O treatment. The adsorbed species could be regenerated by the H₂ and N₂O treatment after TPD, and might be considered to be active oxygen species in selective catalytic reduction (SCR) of N₂O with CH₄. However, the reaction rate of CH₄ activation by the adsorbed species formed after the H₂ and N₂O or the HT and N₂O treatment was not so high as that of the CH₄ + N₂O reaction over the catalyst after O₂ treatment. The simultaneous presence of CH₄ and N₂O is essential for the high activity of the reaction, which suggests that nascent oxygen species formed by N₂O dissociation can activate CH₄ in the SCR of N₂O with CH₄.

Original language	English
Pages (from-to)	342-352
Number of pages	11
Journal	Applied Catalysis B: Environmental
Volume	70
Issue number	1-4
DOIs	https://doi.org/10.1016/j.apcatb.2005.11.032
Publication status	Published - 2007 Jan 31

Keywords

EXAFS
Fe-MFI
FTIR
Methane activation
Nascent oxygen
Nitrous oxide
TPD

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10.1016/j.apcatb.2005.11.032

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title = "Role of active oxygen transients in selective catalytic reduction of N2O with CH4 over Fe-zeolite catalysts",

abstract = "Sharp NO and O2 desorption peaks, which were caused by the decomposition of nitro and nitrate species over Fe species, were observed in the range of 520-673 K in temperature-programmed desorption (TPD) from Fe-MFI after H2 treatment at 773 K or high-temperature (HT) treatment at 1073 K followed by N2O treatment. The amounts of O2 and NO desorption were dependent on the pretreatment pressure of N2O in the H2 and N2O treatment. The adsorbed species could be regenerated by the H2 and N2O treatment after TPD, and might be considered to be active oxygen species in selective catalytic reduction (SCR) of N2O with CH4. However, the reaction rate of CH4 activation by the adsorbed species formed after the H2 and N2O or the HT and N2O treatment was not so high as that of the CH4 + N2O reaction over the catalyst after O2 treatment. The simultaneous presence of CH4 and N2O is essential for the high activity of the reaction, which suggests that nascent oxygen species formed by N2O dissociation can activate CH4 in the SCR of N2O with CH4.",

keywords = "EXAFS, Fe-MFI, FTIR, Methane activation, Nascent oxygen, Nitrous oxide, TPD",

author = "Takeshi Nobukawa and Kou Sugawara and Kazu Okumura and Keiichi Tomishige and Kimio Kunimori",

note = "Funding Information: This research has been supported by the approval of the Photon Factory Advisory Committee (Proposal No. 2003G255). The authors are grateful to the Chemical Analysis Center, University of Tsukuba, for ICP analysis. T. Nobukawa is grateful for his Research Fellowship from the Japan Society for Promotion of Science (JSPS) for Young Scientists. ",

year = "2007",

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doi = "10.1016/j.apcatb.2005.11.032",

language = "English",

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T1 - Role of active oxygen transients in selective catalytic reduction of N2O with CH4 over Fe-zeolite catalysts

AU - Nobukawa, Takeshi

AU - Sugawara, Kou

AU - Okumura, Kazu

AU - Tomishige, Keiichi

AU - Kunimori, Kimio

N1 - Funding Information: This research has been supported by the approval of the Photon Factory Advisory Committee (Proposal No. 2003G255). The authors are grateful to the Chemical Analysis Center, University of Tsukuba, for ICP analysis. T. Nobukawa is grateful for his Research Fellowship from the Japan Society for Promotion of Science (JSPS) for Young Scientists.

PY - 2007/1/31

Y1 - 2007/1/31

N2 - Sharp NO and O2 desorption peaks, which were caused by the decomposition of nitro and nitrate species over Fe species, were observed in the range of 520-673 K in temperature-programmed desorption (TPD) from Fe-MFI after H2 treatment at 773 K or high-temperature (HT) treatment at 1073 K followed by N2O treatment. The amounts of O2 and NO desorption were dependent on the pretreatment pressure of N2O in the H2 and N2O treatment. The adsorbed species could be regenerated by the H2 and N2O treatment after TPD, and might be considered to be active oxygen species in selective catalytic reduction (SCR) of N2O with CH4. However, the reaction rate of CH4 activation by the adsorbed species formed after the H2 and N2O or the HT and N2O treatment was not so high as that of the CH4 + N2O reaction over the catalyst after O2 treatment. The simultaneous presence of CH4 and N2O is essential for the high activity of the reaction, which suggests that nascent oxygen species formed by N2O dissociation can activate CH4 in the SCR of N2O with CH4.

AB - Sharp NO and O2 desorption peaks, which were caused by the decomposition of nitro and nitrate species over Fe species, were observed in the range of 520-673 K in temperature-programmed desorption (TPD) from Fe-MFI after H2 treatment at 773 K or high-temperature (HT) treatment at 1073 K followed by N2O treatment. The amounts of O2 and NO desorption were dependent on the pretreatment pressure of N2O in the H2 and N2O treatment. The adsorbed species could be regenerated by the H2 and N2O treatment after TPD, and might be considered to be active oxygen species in selective catalytic reduction (SCR) of N2O with CH4. However, the reaction rate of CH4 activation by the adsorbed species formed after the H2 and N2O or the HT and N2O treatment was not so high as that of the CH4 + N2O reaction over the catalyst after O2 treatment. The simultaneous presence of CH4 and N2O is essential for the high activity of the reaction, which suggests that nascent oxygen species formed by N2O dissociation can activate CH4 in the SCR of N2O with CH4.

KW - EXAFS

KW - Fe-MFI

KW - FTIR

KW - Methane activation

KW - Nascent oxygen

KW - Nitrous oxide

KW - TPD

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JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

IS - 1-4

ER -

Role of active oxygen transients in selective catalytic reduction of N₂O with CH₄ over Fe-zeolite catalysts

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Keywords

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