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题名: Enhanced activation and decomposition of CH4 by the addition of C2H4 or C2H2 for hydrogen and carbon nanotube production
作者: Qian, Weizhong1;  Tian, Tao1;  Guo, Chenyi1;  Wen, Qian1;  Li, Kuangjie2;  Zhang, Hongbo3;  Shi, Haibo1;  Wang, Dezheng1;  Liu, Yi1;  Zhang, Qiang1;  Zhang, Yongxiong2;  Wei, Fei1;  Wang, Zhanwen1;  Li, Xiaodong2;  Li, Yongdan4
刊名: JOURNAL OF PHYSICAL CHEMISTRY C
发表日期: 2008-05-22
DOI: 10.1021/jp800016m
卷: 112, 期:20, 页:7588-7593
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 decomposition of CH4 in the presence of C2H4 or C2H2 using a nanosized iron or nickel based catalyst with volume ratios of C2H4 or C2H2 to CH4 of 1.75:1 to 0.55:1 was investigated. The presence of C2H4 or C2H2 increased the conversion of CH4 to 3 to 5 times that with no C2H4 or C2H2; that is, it significantly increased the production rate of carbon from 20-30 to 45-75 g/gcat/h at 723-873 K. The online detection of the time dependent composition of the product gas and experiments in which the feeding sequence of CH4 and C2H4/C2H2 was changed allowed us to propose a mechanism for the enhanced decomposition as follows. First, the facile exothermic adsorption and decomposition of C2H4 or C2H2 provides the driving force for the in situ endothermic decomposition of CH4. Subsequently, the thermodynamically favored intermediate products of aromatics or poly aromatics are formed by the insertion of CH4 into adsorbed C2H4 or C2H2 fragments. Finally, the intermediate products are rapidly dehydrogenated on the high activity catalyst to form carbon nanotubes (CNTs). The enhancement effect is dependent on the ratio of C2H4 to CH4 but independent of the ratio of C2H2 to CH4, which was explained as being due to the different exothermicities of the C2H4 and C2H2 reactions. This finding provides a new stimulus for methane activation at low temperature to produce hydrogen and CNTs with high efficiency.
关键词[WOS]: CATALYTIC DECOMPOSITION ;  METHANE DECOMPOSITION ;  GAS ;  ADSORPTION ;  ACETYLENE ;  ETHYLENE
语种: 英语
WOS记录号: WOS:000255905400015
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/141004
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.Tsinghua Univ, Dept Chem Engn, Beijing Key Lab Green Chem React Engn & Technol, Beijing 100084, Peoples R China
2.Beijing Inst Technol, Sch Mat Sci & Engn, Beijing 100081, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
4.Tianjin Univ, Sch Chem Engn, Tianjin Key Lab Appl Catalysis Sci & Technol, Tianjin 300072, Peoples R China

Recommended Citation:
Qian, Weizhong,Tian, Tao,Guo, Chenyi,et al. Enhanced activation and decomposition of CH4 by the addition of C2H4 or C2H2 for hydrogen and carbon nanotube production[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2008,112(20):7588-7593.
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