Methane dehydroaromatization–A study on hydrogen use for catalyst reduction, role of molybdenum, the nature of catalyst support and significance of Bronsted acid sites

论文摘要

Methane dehydroaromatization was studied over Mo/SiO2 and Mo/HZSM-5 with different Mo loadings（2, 5, 10 wt%） at 973 K and 1023 K in a recirculating batch reactor. H2 pretreatment at 1023 K prior to methane activation has significantly improved the catalyst activity with increase in Mo loading and reduced the induction time on benzene formation in both Mo/SiO2 and Mo/HZSM-5. 10 wt% Mo/HZSM-5 gave a maximum methane conversion of 19% and ～67% benzene selectivity at 1023 K. The XRD analysis of used catalysts revealed that the Mo O3 species were converted to β-Mo2C phase. Studies on Mo/SiO2 catalysts showed that benzene was formed even in the absence of acidic zeolite sites. Reactions of ethylene in the presence of pure silica, HZSM-5 and in a blank reactor revealed that conversion of ethylene to aromatics was similar in case of the blank reactor and silica. Thus, it is believed that molybdenum carbide sites act as active sites only for C–H bond activation of methane and ethylene formation. Even though, ethylene can undergo subsequent oligomerization without any catalytic aid to form benzene at973 K and above addition of acidic zeolites improved the selectivity of benzene.

论文目录

• 1. Introduction
• 2. Experimental
•   2.1. Catalyst preparation
•     2.1.1. Incipient wetness impregnation （IWI） method
•     2.1.2. Sol–gel synthesis
•   2.2. Catalytic reaction system
•   2.3. Catalyst characterization
•     2.3.1. Brunauer–Emmett–Teller （BET） surface area
•     2.3.2. Scanning Electron Microscopy （SEM）
•     2.3.3. X-ray diffraction （XRD）
•     2.3.4. n-Propylamine–temperature-programmed desorption （NPA-TPD）
•     2.3.5. Temperature-programmed reduction （TPR）
• 3. Results and discussion
•   3.1. Catalyst characterization
•     3.1.1. Surface area
•     3.1.2. X-ray diffraction （XRD） analysis
•     3.1.3. Scanning electron microscope （SEM） analysis
•     3.1.4. n-Propylamine–temperature-programmed desorption （NPA-TPD）
•     3.1.5. Temperature-programmed reduction （TPR）
•   3.2. Conversion of CH4on Mo/Si O2 （IWI） , Mo/SiO2 （SG） and Mo/HZSM-5 （IWI）
•   3.3. Selectivity of C6H6, C2 and carbon on Mo/SiO2 （IWI） , Mo/SiO2 （SG） and Mo/HZSM-5 （IWI）
•   3.4. Methane activation over 10 wt%Mo/HZSM-5 （IWI） catalyst
•   3.5. Role of molybdenum in methane activation
•   3.6. Methane dimerization and aromatization
• 4. Conclusions
• Declarations of interest

文章来源

类型: 期刊论文

作者: Vaidheeshwar Ramasubramanian,Hema Ramsurn,Geoffrey L.Price

来源: Journal of Energy Chemistry 2019年07期

年度: 2019

分类: 工程科技Ⅰ辑

专业: 化学

单位: Russell School of Chemical Engineering, The University of Tulsa

基金: financial support from the University of Tulsa (Faculty Development Summer Fellowship),ACS-PRF (PRF# 56052-DNI9) are gratefully acknowledged

分类号: O643.36;O621.251

页码: 20-32

总页数: 13

文件大小: 1631K

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