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题名: The promotional effect of NO on N2O decomposition over the bi-nuclear Fe sites in Fe/ZSM-5
作者: Xia, Haian1;  Sun, Keqiang1;  Liu, Zhimin1;  Feng, Zhaochi1;  Ying, Pinliang1;  Li, Can1
关键词: Fe/ZSM-5 ;  N2O decomposition ;  Bi-nuclear ;  Transient response ;  Raman
刊名: JOURNAL OF CATALYSIS
发表日期: 2010-03-22
DOI: 10.1016/j.jcat.2009.12.014
卷: 270, 期:1, 页:103-109
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Engineering, Chemical
研究领域[WOS]: Chemistry ;  Engineering
英文摘要: Combining transient response method, steady-state kinetics, in situ IR, and in situ Raman spectroscopic techniques, the effect of NO on N2O decomposition over Fe/ZSM-5 catalyst was investigated in detail, which reveals that the active sites are bi-nuclear Fe sites. The presence of NO increases the desorption rate of O-2 and lowers the apparent activation energy of N2O decomposition. Trace amount of water vapor can lead to the deactivation of the Fe/ZSM-5 catalyst due to the oxidation of the active Fe2+ sites during N2O decomposition. On the other hand, NO treatment causes the regeneration of the inactive Fe sites by releasing O-2 at relatively low temperature. For the first time, it was found that a Raman band at 743 cm(-1), assigned to the bi-nuclear Fe sites, changes accordingly with the deactivation and regeneration of the Fe/ZSM-5 catalyst. The in situ IR spectroscopic study reveals that NO treatment of the deactivated catalyst can remove the hydroxyl groups bound to the inactive Fe3+ species. These results demonstrate that H2O and NO play important roles in the structural transformation between the hydroxylated bi-nuclear Fe3+ sites and the dehydroxylated bi-nuclear Fe2+ sites in Fe/ZSM-5. Our conclusion is that the positive effect of NO on N2O decomposition is due to the dehydroxylation of the hydroxylated bi-nuclear Fe sites facilitated by NO, as well as the enhancement of the O-2 desorption rate regulated by NO. (C) 2009 Elsevier Inc. All rights reserved.
关键词[WOS]: NITROUS-OXIDE DECOMPOSITION ;  HIGH-TEMPERATURE TREATMENT ;  CHEMICAL-VAPOR-DEPOSITION ;  SELECTIVE CATALYTIC-REDUCTION ;  RESONANCE RAMAN-SPECTROSCOPY ;  OVER-EXCHANGED FE/ZSM5 ;  IRON-CONTAINING ZSM-5 ;  NITRIC-OXIDE ;  MFI ZEOLITES ;  PHYSICOCHEMICAL CHARACTERIZATION
语种: 英语
WOS记录号: WOS:000275966100014
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141736
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Xia, Haian,Sun, Keqiang,Liu, Zhimin,et al. The promotional effect of NO on N2O decomposition over the bi-nuclear Fe sites in Fe/ZSM-5[J]. JOURNAL OF CATALYSIS,2010,270(1):103-109.
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