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题名: Active sites in Fe/ZSM-5 for nitrous oxide decomposition and benzene hydroxylation with nitrous oxide
作者: Sun, Keqiang2;  Xia, Haian2;  Feng, Zhaochi2;  van Santen, Rutger1;  Hensen, Emiel1;  Li, Can2
通讯作者: Emiel Hensen ;  李灿
关键词: zeolite ;  ZSM-5 ;  iron ;  Raman and infrared spectroscopy ;  nitrous oxide decomposition ;  benzene hydroxylation
刊名: JOURNAL OF CATALYSIS
发表日期: 2008-03-10
DOI: 10.1016/j.jcat.2008.01.017
卷: 254, 期:2, 页:383-396
收录类别: SCI
文章类型: Article
部门归属: 5
项目归属: 503
产权排名: 1;1
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: The effect of the iron content and the pretreatment conditions of Fe/ZSM-5 catalysts on the Fe speciation and the catalytic activities in nitrous oxide decomposition and benzene hydroxylation with nitrous oxide has been investigated. Iron-containing ZSM-5 zeolites with varying iron content (Fe/Al = 0.1-1.0) were prepared by solid-state ion exchange of HZSM-5 zeolite with FeCl3 followed by hydrolysis and finally calcination at 823 K. In a second step, the catalysts were treated at 1] 73 K in He flow. The catalysts were characterized by FT-infrared, UV-vis and Raman spectroscopy. The number of Fe2+ centers was determined by low-temperature nitrous oxide decomposition and the subsequent methane titration. The highest activity for catalytic nitrous oxide decomposition was achieved for catalysts with intermediate iron loading (Fe/Al = 0.66). The activity after high-temperature treatment was about three times higher than after calcination. Whereas the calcined catalysts showed negligible activity in benzene hydroxylation, high-temperature treatment resulted in dramatic improvements in activity and selectivity. The selectivity to phenol decreased strongly with increasing Fe content. The profound changes in catalytic reactivity are related to the changes in iron speciation upon high-temperature treatment. Besides considerable extraction of Al from framework positions, resonance Raman spectroscopy points to changes in the structure of the iron oxide species of low nuclearity. A useful model is the reconstruction of charge-compensating cationic iron species to iron species stabilized by extraframework Al species located in the zeolite micropores. Further analysis of spectroscopic data suggests that oligonuclear, perhaps binuclear, iron sites appear most favorable for nitrous oxide decomposition, whereas the mononuclear iron sites are active for benzene hydroxylation to phenol. (C) 2008 Elsevier Inc. All rights reserved.
关键词[WOS]: HIGH-TEMPERATURE TREATMENT ;  CHEMICAL-VAPOR-DEPOSITION ;  DIRECT N2O DECOMPOSITION ;  ONE-STEP OXIDATION ;  SELECTIVE OXIDATION ;  FE/MFI CATALYSTS ;  SURFACE OXYGEN ;  NOX REDUCTION ;  PHYSICOCHEMICAL CHARACTERIZATION ;  FE-SILICALITE
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000255533700025
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/101299
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.Eindhoven Univ Technol, Schuit Inst Catalysis, NL-5600 MB Eindhoven, Netherlands
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Sun, Keqiang,Xia, Haian,Feng, Zhaochi,et al. Active sites in Fe/ZSM-5 for nitrous oxide decomposition and benzene hydroxylation with nitrous oxide[J]. JOURNAL OF CATALYSIS,2008,254(2):383-396.
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