The importance of Fe loading on the N2O reduction with NH3 over Fe-MFI:: Effect of acid site formation on Fe species

被引：37

作者：

Sugawara, Kou

Nobukawa, Takeshi

Yoshida, Masanori

Sato, Yoshihiro

Okumura, Kazu

Tomishige, Keiichi

Kunimori, Kimio

机构：

[1] Univ Tsukuba, Inst Mat Sci, Tsukuba, Ibaraki 305573, Japan

[2] Tottori Univ, Fac Engn, Dept Mat Sci, Tottori 6808552, Japan

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2007年 / 69卷 / 3-4期

基金：

日本学术振兴会;

关键词：

N2O reduction; ammonia; methane; Fe-MFI; acid sites;

D O I：

10.1016/j.apcatb.2006.06.027

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Effect of the loading amount of Fe over ion-exchanged Fe-MFI catalysts on the catalytic performance of N2O reduction with NH3 was investigated, and the results indicated that the turnover frequency (TOF) was almost constant in the Fe/Al range between 0.05 and 0.40. The activity of N2O + NH3 reaction was much lower than that of N2O + CH4 reaction over Fe-MFI (Fe/Al = 0.40), and the preadsorption of NH3 decreased drastically the activity of N2O + CH4 reaction. The temperature-programmed desorption (TPD) of NH3 showed the formation of stronger acid sites on Fe-MFI (Fe/Al = 0.24 and 0.40), and the amount of the acid sites agrees well with the desorption amount O-2 in O-2-TPD in the low temperature range. The acid sites gave a 3610 cm(-1) peak (Bronsted acid) in FTIR observation. These results suggest that the acid sites were formed on the bridge oxide ions in binuclear Fe species. Adsorbed NH3 on the strong acid sites inhibited N2O dissociation, which can be related to the low activity of N2O + NH3 reaction over Fe-MFI with high Fe loading. (c) 2006 Elsevier B.V. All rights reserved.

引用

页码：154 / 163

页数：10

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