Study of Methane Dehydroaromatization on Impregnated Mo/ZSM-5 Catalysts and Characterization of Nanostructured Molybdenum Phases and Carbonaceous Deposits Научная публикация
Журнал |
Industrial and Engineering Chemistry Research
ISSN: 0888-5885 , E-ISSN: 1520-5045 |
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Вых. Данные | Год: 2007, Том: 46, Номер: 12, Страницы: 4063-4074 Страниц : 12 DOI: 10.1021/ie0609564 | ||||
Ключевые слова | Catalysts; Molybdenum; Nanostructured materials; X ray diffraction analysis | ||||
Авторы |
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Организации |
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Информация о финансировании (1)
1 | Netherlands Organisation for Scientific Research | 047.15.012 |
Реферат:
Methane dehydroaromatization was studied over a series of impregnated Mo/ZSM-5 catalysts with different molybdenum contents and Si/Al atomic ratios in the parent H-ZSM-5 zeolites. The maximum catalytic activity (∼14% CH4 conversion) and benzene formation selectivity (∼70%) were observed for the samples with 2%−5% molybdenum. The activity and selectivity are improved when the Si/Al ratio is decreased from 45 to 17. After pretreatment in argon and reaction at 720 °C, the catalysts have been characterized by textural methods, X-ray diffractometry (XRD), differential thermal analysis (DTA), high-resolution transmission electron microscopy (HRTEM), and energy-dispersive X-ray spectroscopy (EDX). As determined by HRTEM, after the pretreatment, the MoOx phase is highly dispersed on the external surface of the zeolite. During the reaction, molybdenum carbide nanoparticles 2−15 nm in size are formed on the external surface, and the molybdenum-containing clusters are deposited in the zeolite channels. The carbonaceous deposits (CDs) are formed as graphite layers on the surface of Mo2C nanoparticles that were >2 nm in size, and as friable layers with a disordered structure on the external surface of the zeolite. According to EDX, XRD, and DTA studies, the content of the CD and the extent of their condensation (the C/H ratio) increase with the time-on-stream. For all the studied molybdenum contents (1%−10%) and time-on-stream values (0.5−6 h), the CDs formed on the catalysts with Si/Al = 17 are characterized by one maximum of the exothermic burn-out effect in DTA, whereas on the catalysts with Si/Al = 30 and 45, they are characterized by two such maxima. A correlation between the catalyst activity, the selectivity versus nanostructure, and the location of the molybdenum phases and CDs is discussed.
Библиографическая ссылка:
Matus E.V.
, Ismagilov I.Z.
, Sukhova O.B.
, Zaikovskii V.I.
, Tsikoza L.T.
, Ismagilov Z.R.
, Moulijn J.A.
Study of Methane Dehydroaromatization on Impregnated Mo/ZSM-5 Catalysts and Characterization of Nanostructured Molybdenum Phases and Carbonaceous Deposits
Industrial and Engineering Chemistry Research. 2007. V.46. N12. P.4063-4074. DOI: 10.1021/ie0609564 WOS Scopus РИНЦ CAPlusCA OpenAlex
Study of Methane Dehydroaromatization on Impregnated Mo/ZSM-5 Catalysts and Characterization of Nanostructured Molybdenum Phases and Carbonaceous Deposits
Industrial and Engineering Chemistry Research. 2007. V.46. N12. P.4063-4074. DOI: 10.1021/ie0609564 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Опубликована online: | 12 июн. 2006 г. |
Поступила в редакцию: | 22 июл. 2006 г. |
Принята к публикации: | 20 окт. 2006 г. |
Опубликована в печати: | 1 июн. 2007 г. |
Идентификаторы БД:
Web of science: | WOS:000246803800022 |
Scopus: | 2-s2.0-34250828435 |
РИНЦ: | 13550746 |
Chemical Abstracts: | 2006:1269252 |
Chemical Abstracts (print): | 146:464837 |
OpenAlex: | W2088247876 |