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题名: Density functional theory study on structure of molybdenum carbide loaded on MCM-22 zeolite and mechanism for methane activation
作者: Zhu Hongyuan;  Zhang Yuan;  Zhou Danhong;  Guan Jing;  Bao Xinhe
关键词: MCM-22 zeolite ;  molybdenum carbide ;  density functional theory ;  methane ;  activation energy
刊名: CHINESE JOURNAL OF CATALYSIS
发表日期: 2007-02-01
卷: 28, 期:2, 页:180-186
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Applied ;  Chemistry, Physical ;  Engineering, Chemical
研究领域[WOS]: Chemistry ;  Engineering
英文摘要: Density functional theory was employed to study the geometric and electronic structure of molybdenum carbide loaded on MCM-22 zeolite and predict the mechanism for CH4 activation. Two models of active center, Mo(CH2)(2) (Model A) and Mo(CH)CH2 (Model B), were designed; they were located on the T4 site of the supercage in MCM-22 zeolite. The geometry optimization and electronic structure analysis of the models were performed based on 3T cluster model. The optimized geometry showed that the Mo connected with CH2 terminal group by double bond (bond length 0.18-0.19 nm) and with CH terminal group by triple bond (bond length 0.17 nm). The natural bond orbital calculation revealed that the Mo was bonded to framework oxygen through a bond. In terms of the composition and the energy of the frontier orbitals, it was suggested that the CH4 activation on Mo carbide active center would happen between the HOMO of CH4 molecule and the LUMO of Mo carbide. Namely, electrons preferred to transfer from the sigma-orbital of C-H bond to the pi * -orbital of Mo-C bond. After heterogenous splitting of C-H bond, the H3C- group was bonded to Mo and the H+ was bonded to C in Mo carbide species. The calculated activation energy on Model A was 119.97 kJ/mol. On Model B, there were two possible pathways, in which the hydrogen in CH4 could attach to CH2 and CH terminal groups. The corresponding activation energy was 91.37 and 79.07 kJ/mol, respectively.
关键词[WOS]: DEHYDRO-AROMATIZATION ;  ACID SITES ;  MO/MCM-22 CATALYSTS ;  MO/HZSM-5 CATALYSTS ;  MO ;  DEHYDROAROMATIZATION ;  CONVERSION ;  BENZENE ;  DEHYDROGENATION ;  OXYGEN
语种: 英语
WOS记录号: WOS:000244994000018
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/140459
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.Liaoning Normal Univ, Coll Chem & Chem Engn, Inst Chem Functionalized Mat, Dalian 116029, Liaoning, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China

Recommended Citation:
Zhu Hongyuan,Zhang Yuan,Zhou Danhong,et al. Density functional theory study on structure of molybdenum carbide loaded on MCM-22 zeolite and mechanism for methane activation[J]. CHINESE JOURNAL OF CATALYSIS,2007,28(2):180-186.
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