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题名: Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5
作者: Sun, KQ;  Xia, H;  Hensen, E;  van Santen, R;  Li, C
通讯作者: 李灿
关键词: N2O decomposition ;  mechanism ;  Fe/ZSM-5 ;  transient-response ;  iron species ;  active site ;  Fe-O-Al species
刊名: JOURNAL OF CATALYSIS
发表日期: 2006-02-15
DOI: 10.1016/j.jcat.2005.12.013
卷: 238, 期:1, 页:186-195
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: Nitrous oxide decomposition on Fe/ZSM-5 catalysts, prepared by solid-state ion exchange followed by calcination in O-2 at 823 K or high-temperature treatment in He at 1173 K, was studied by steady-state reaction and transient-response techniques. High-temperature treatment induces profound changes in the distribution of iron species, most notably a substantial fraction of oligonuclear and cationic Fe species are converted to Fe species stabilized by extra-framework Al (Fe-O-Al species) in zeolite micropores. Nitrous oxide decomposition is much slower over calcined Fe/ZSM-5 than over its high-temperature-treated counterpart. Only over the latter catalysts is inhibition of N2O conversion by molecular oxygen observed. Transient response experiments show that molecular oxygen and nitrogen evolve simultaneously for calcined Fe/ZSM-5. It is proposed that the reaction proceeds over isolated Fe3+ sites in cationic species or oligonuclear Fe oxide species via a scavenging mechanism in which adsorbed oxygen species react with gaseous nitrous oxide to give molecular nitrogen and oxygen. In contrast, transient-response experiments for the high-temperature-treated catalyst show slow oxygen desorption compared with nitrogen formation, pointing to recombinative oxygen desorption being rate-limiting. This agrees with the finding that the rate is inhibited by molecular oxygen. It is proposed that ferrous ions in the high-temperature-treated catalyst show a much higher reactivity in nitrous oxide decomposition than Fe3+ sites. The Fe2+ species are most likely associated with the mixed iron and aluminium species formed upon high-temperature treatment. (c) 2005 Elsevier Inc. All rights reserved.
关键词[WOS]: NITROUS-OXIDE DECOMPOSITION ;  EX-FRAMEWORK FEZSM-5 ;  SURFACE-CHEMISTRY ;  FE/MFI CATALYSTS ;  OXYGEN FORMATION ;  NOX REDUCTION ;  FE-SILICALITE ;  MAS NMR ;  ZEOLITES ;  IRON
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000235372900020
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/98237
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
2.Eindhoven Univ Technol, Schuit Inst Catalysis, NL-5600 MB Eindhoven, Netherlands

Recommended Citation:
Sun, KQ,Xia, H,Hensen, E,et al. Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5[J]. JOURNAL OF CATALYSIS,2006,238(1):186-195.
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