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题名: Highly efficient catalytic conversion of chloromethane to light olefins over HSAPO-34 as studied by catalytic testing and in situ FTIR
作者: Wei, YX;  Zhang, DZ;  Liu, ZM;  Su, BL
关键词: SAPO-34 ;  chloromethane conversion ;  FTIR ;  catalytic testing ;  light alkenes ;  HCl ;  reaction mechanism
刊名: JOURNAL OF CATALYSIS
发表日期: 2006-02-15
DOI: 10.1016/j.jcat.2005.11.021
卷: 238, 期:1, 页:46-57
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Engineering, Chemical
研究领域[WOS]: Chemistry ;  Engineering
英文摘要: The catalytic conversion of chloromethane over HSAPO-34 was followed by in situ Fourier transform infrared (FTIR) spectroscopy and catalytic testing. Our detailed IR investigation allowed the identification of the active sites and the adsorbed species. HSAPO-34 has high activity and selectivity for the production of light olefins. The FTIR results demonstrated that the conversion starts at 350 degrees C with the formation of alkoxy groups as intermediate products. On adsorption and conversion of chloromethane, three distinct shifts of -OH bands associated with the Si(OH)Al acidic sites were observed, attributed to the interaction between Si(OH)AI with CH3Cl, HCl and C=C groups. In the 350-500 degrees C temperature range, chloromethane is converted to ethylene, propylene, and butylenes with 70-80% selectivity. Increasing reaction temperature increases conversion and enhances the yield of lighter olefins. The detailed FTIR study of chloromethane conversion at 450 degrees C at different system chloromethane loadings reveals that increasing system CH3Cl loading increased the conversion rate. This is attributed to the participation of gas-phase chloromethane molecules with adsorbed species enhancing the reaction rate, while at lower chloromethane loadings, the reactions may just occur between the adsorbed species. The IR studies also reveal the reversible breaking of Al-O-P bonds on adsorption of HCl, a main product of the reaction, to generate large amounts of P-OH groups. The Al-O-P bonding was restored after removal of HCl by evacuation at 150 degrees C. These IR observations combined with the catalytic test results allow us to propose a realistic reaction mechanism. (c) 2005 Elsevier Inc. All rights reserved.
关键词[WOS]: HIGHER HYDROCARBONS ;  ZEOLITE CATALYSTS ;  SAPO-34 CATALYST ;  METHYL-CHLORIDE ;  BASIC ZEOLITES ;  ACID CATALYST ;  METHANOL ;  ADSORPTION ;  TEMPLATE ;  CAVITIES
语种: 英语
WOS记录号: WOS:000235372900007
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/140282
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, Nat Gas Utilizat & Appl Catalysis Lab, Dalian 116023, Peoples R China
2.Fac Univ Notre Dame Paix, Lab CMI, B-5000 Namur, Belgium

Recommended Citation:
Wei, YX,Zhang, DZ,Liu, ZM,et al. Highly efficient catalytic conversion of chloromethane to light olefins over HSAPO-34 as studied by catalytic testing and in situ FTIR[J]. JOURNAL OF CATALYSIS,2006,238(1):46-57.
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