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• W2024447259 abstract "The direct conversion of methane to aromatics such as benzene and naphthalene has been studied on a series of Mo-supported catalysts using HZSM-5, FSM-16, mordenite, USY, SiO2, and Al2O3as the supporting materials. Among all the supports used, the HZSM-5-supported Mo catalysts exhibit the highest yield of aromatic products, achieving over 70% total selectivity of the hydrocarbons on a carbon basis at 5–12% methane conversion at 973 K and 1 atm. By contrast, less than 20% of the converted methane is transformed to hydrocarbon products on the other Mo-supported catalysts, which are drastically deactivated, owing to serious coke formation. The XANES/EXAFS and TG/DTA/mass studies reveal that the zeolite-supported Mo oxide is endothermally converted with methane around 955 K to molybdenum carbide (Mo2C) cluster (Mo-C, C.N.=1,R=2.09 Å; Mo-Mo, C.N.=2.3–3.5;R=2.98 Å), which initiates the methane aromatization yielding benzene and naphthalene at 873–1023 K. Although both Mo2C and HZSM-5 support alone have a very low activity for the reaction, physically mixed hybrid catalysts consisting of 3 wt% Mo/SiO2+HZSM-5 and Mo2C+HZSM-5 exhibited a remarkable promotion to enhance the yields of benzene and naphthalene over 100–300 times more than either component alone. On the other hand, it was demonstrated by the IR measurement in pyridine adsorption that the Mo/HZSM-5 catalysts having the optimum SiO2/Al2O3ratios, around 40, show maximum Brönsted acidity among the catalysts with SiO2/Al2O3ratios of 20–1900. There is a close correlation between the activity of benzene formation in methane aromatization and the Brönsted acidity of Mo/HZSM-5, but not Lewis aciditiy. It was found that maximum benzene formation was obtained on the Moz/HZSM-5 having SiO2/Al2O3ratios of 20–49, but substantially poor activities on those with SiO2/Al2O3ratios smaller and higher than 40. The results suggest that methane is dissociated on the molybdenum carbide cluster supported on HZSM-5 having optimum Brönsted acidity to form CHx(x>1) and C2-species as the primary intermediates which are oligomerized subsequently to aromatics such as benzene and naphthalene at the interface of Mo2C and HZSM-5 zeolite having the optimum Brönsted acidity. The bifunctional catalysis of Mo/HZSM for methane conversion towards aromatics is discussed by analogy with the promotion mechanism on the Pt/Al2O3catalyst for the dehydro-aromatization of alkanes." @default.
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• W2024447259 date "1999-01-01" @default.
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• W2024447259 title "Bifunctional Catalysis of Mo/HZSM-5 in the Dehydroaromatization of Methane to Benzene and Naphthalene XAFS/TG/DTA/MASS/FTIR Characterization and Supporting Effects" @default.
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• W2024447259 doi "https://doi.org/10.1006/jcat.1998.2310" @default.
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