Reaction Mechanisms of H-2 Reduction and N2O Decomposition on Fe/ZSM-5 Zeolite: A Density Functional Theoretical Study
文献类型：期刊论文
| 作者 | Yang, Gang1,2; Zhou, Lijun2; Liu, Xianchun1; Han, Xiuwen1; Bao, Xinhe1 |
| 刊名 | journal of physical chemistry c
 |
| 出版日期 | 2009-10-22 |
| 卷号 | 113期号:42页码:18184-18190 |
| 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. |
| 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 |
| 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 |
| 收录类别 | SCI |
| 语种 | 英语 |
| WOS记录号 | WOS:000270671100030 |
| 公开日期 | 2015-11-17 |
| 源URL | [http://159.226.238.44/handle/321008/141263]  |
| 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.NE Forestry Univ, Minist Educ, Key Lab Forest Plant Ecol, Harbin 150040, Peoples R China |
| 推荐引用方式 GB/T 7714 | 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. |
| APA | Yang, Gang,Zhou, Lijun,Liu, Xianchun,Han, Xiuwen,&Bao, Xinhe.(2009).Reaction Mechanisms of H-2 Reduction and N2O Decomposition on Fe/ZSM-5 Zeolite: A Density Functional Theoretical Study.journal of physical chemistry c,113(42),18184-18190. |
| MLA | Yang, Gang,et al."Reaction Mechanisms of H-2 Reduction and N2O Decomposition on Fe/ZSM-5 Zeolite: A Density Functional Theoretical Study".journal of physical chemistry c 113.42(2009):18184-18190. |
入库方式： OAI收割
来源：大连化学物理研究所
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