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Highly efficient catalytic conversion of chloromethane to light olefins over HSAPO-34 as studied by catalytic testing and in situ FTIR
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
2006-02-15
DOI10.1016/j.jcat.2005.11.021
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
关键词[WOS]HIGHER HYDROCARBONS ; ZEOLITE CATALYSTS ; SAPO-34 CATALYST ; METHYL-CHLORIDE ; BASIC ZEOLITES ; ACID CATALYST ; METHANOL ; ADSORPTION ; TEMPLATE ; CAVITIES
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.
语种英语
WOS记录号WOS:000235372900007
引用统计
被引频次:73[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/140282
专题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, Nat Gas Utilizat & Appl Catalysis Lab, Dalian 116023, Peoples R China
2.Fac Univ Notre Dame Paix, Lab CMI, B-5000 Namur, Belgium
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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.
APA Wei, YX,Zhang, DZ,Liu, ZM,&Su, BL.(2006).Highly efficient catalytic conversion of chloromethane to light olefins over HSAPO-34 as studied by catalytic testing and in situ FTIR.JOURNAL OF CATALYSIS,238(1),46-57.
MLA Wei, YX,et al."Highly efficient catalytic conversion of chloromethane to light olefins over HSAPO-34 as studied by catalytic testing and in situ FTIR".JOURNAL OF CATALYSIS 238.1(2006):46-57.
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