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题名: Reaction Mechanisms of H-2 Reduction and N2O Decomposition on Fe/ZSM-5 Zeolite: A Density Functional Theoretical Study
作者: Yang, Gang1, 2;  Zhou, Lijun2;  Liu, Xianchun1;  Han, Xiuwen1;  Bao, Xinhe1
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2009-10-22
DOI: 10.1021/jp906426j
卷: 113, 期:42, 页:18184-18190
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Science & Technology - Other Topics ;  Materials Science
英文摘要: The Fe/ZSM-5 catalysts are usually prepared with H-2 pretreatment. In this work, the reaction mechanisms of H-2 reduction and N2O decomposition on Fe/ZSM-5 zeolite were studied with B3LYP density functional calculations, Before reduction, the vertical H-2 adsorption mode oil the high-spin Fe(III)/ZSM-5 zeolite must transform into the parallel mode, which is almost barrierless. Both high- and low-spin Fe(III)/ZSM-5 zeolites play an important role during the H-2 reduction processes; in addition, Fe(III)/ZSM-5 zeolite is readily reduced by H-2 pretreatment at moderate temperatures, because the ZPE-corrected energy barriers of the high- and low-spin states equal 46.22 and 18.61 kJ mol(-1), respectively. Albeit with large H-2 adsorption energies, Fe(III)/ZSM-5 zeolite may not be Suitable for H-2 Storage due to the difficulty of releasing the H-2 molecules. On the H-2-reduced Fe(II)/ZSM-5 zeolite, the energy barrier of N2O decomposition was calculated at 117.77 kJ mol(-1), which is less than those of the high- and low-spin Fe(III)/ZSM-5 zeolites. In Fe(III)/ZSM-5 zeolite, the high-spin state predominates the N2O decomposition process due to the higher structural stabilities, where the ZPE-corrected energy barrier is equal to 148.14 kJ mol(-1) and in good agreement with the previous data. Accordingly, the N2O decomposition reactions are facilitated by H-2 pretreatment. In addition, the "alpha-oxygen" species produced by N2O decomposition over the reduced Fe(II)/ZSM-5 zeolite should be responsible for the reaction activities of the monoiron species.
关键词[WOS]: NITROUS-OXIDE DECOMPOSITION ;  DIRECT BENZENE HYDROXYLATION ;  BRIDGED IRON SITES ;  MOLECULAR-HYDROGEN ;  COMPREHENSIVE DFT ;  ZSM-5 ZEOLITE ;  ACTIVE-SITES ;  FE-ZEOLITES ;  FE-ZSM-5 ;  ADSORPTION
语种: 英语
WOS记录号: WOS:000270671100030
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141263
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.NE Forestry Univ, Minist Educ, Key Lab Forest Plant Ecol, Harbin 150040, Peoples R China

Recommended Citation:
Yang, Gang,Zhou, Lijun,Liu, Xianchun,et al. Reaction Mechanisms of H-2 Reduction and N2O Decomposition on Fe/ZSM-5 Zeolite: A Density Functional Theoretical Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2009,113(42):18184-18190.
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