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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
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 Matus Ekaterina V. 1 , Ismagilov Ilyas Z. 1 , Sukhova Olga B. 1 , Zaikovskii Vladimir I. 1 , Tsikoza Lidiya T. 1 , Ismagilov Zinfer R. 1 , Moulijn Jacob A. 2
Организации
1 Boreskov Institute of Catalysis SB RAS, pr. Akademika LaVrentieVa, 5, Novosibirsk, 630090, Russia
2 Delft University of Technology, Delft, The Netherlands

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
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
Цитирование в БД:
БД Цитирований
Web of science 99
Scopus 107
РИНЦ 106
OpenAlex 108
Альметрики: