Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5
文献类型：期刊论文
| 作者 | Sun, KQ; Xia, H; Hensen, E; van Santen, R; Li, C |
| 刊名 | journal of catalysis
 |
| 出版日期 | 2006-02-15 |
| 卷号 | 238期号:1页码:186-195 |
| 关键词 | N2O decomposition mechanism Fe/ZSM-5 transient-response iron species active site Fe-O-Al species |
| 产权排序 | 1;1 |
| 通讯作者 | 李灿 |
| 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. |
| WOS标题词 | science & technology ; physical sciences ; technology |
| 类目[WOS] | chemistry, physical ; engineering, chemical |
| 研究领域[WOS] | chemistry ; engineering |
| 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 |
| 收录类别 | SCI |
| 原文出处 | true |
| 语种 | 英语 |
| WOS记录号 | WOS:000235372900020 |
| 公开日期 | 2010-11-30 |
| 源URL | [http://159.226.238.44/handle/321008/98237]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 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 |
| 推荐引用方式 GB/T 7714 | 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. |
| APA | Sun, KQ,Xia, H,Hensen, E,van Santen, R,&Li, C.(2006).Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5.journal of catalysis,238(1),186-195. |
| MLA | Sun, KQ,et al."Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5".journal of catalysis 238.1(2006):186-195. |
入库方式： OAI收割
来源：大连化学物理研究所
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