Nashrieh Shimi va Mohandesi Shimi Iran

Nashrieh Shimi va Mohandesi Shimi Iran

Influence of Various Types of Zeolitic Supports on Catalytic Properties and Performance of Cr-Based Nanocatalysts Used in C2H6/CO2 Oxidative Dehydrogenation Process

Document Type : Research Article

Authors
Farhad Rahmani 1
Mohammad Haghighi 2
1 Chemical Engineering Faculty, Sahand University of Technology, P.O. Box 51335-1996, Tabriz, I.R. IRAN
2 Chemical Engineering Faculty, Sahand University of Technology, P.O. Box 51335-1996 , Tabriz, I.R. IRAN
Abstract
In this study, the applicability of zeolitic supports and effect of zeolitic supports on catalytic properties and performance of Cr-based nanocatalysts used in oxidative dehydrogenation of ethane with CO2 were investigated. In this regard, a series of chromium oxide-based catalysts containing 3.4 wt.% of Cr were prepared by incipient wetness impregnation of clinoptilolite, SAPO-34 and HZSM-5 chosen among the natural zeolites, zeo-type materials and synthetic zeolites, respectively. To this aim, clinoptilolite was purchased and SAPO-34 and HZSM-5 were successfully synthesized via the hydrothermal method as evidenced by XRD, FESEM, BET and EDX techniques. The formation of fewer agglomerations and better dispersion of surface nanoparticles over cubic-like particles of ZSM-5 compared to other zeolitic supports were
confirmed by FESEM images. The TPD-NH3 results revealed that more desirable acidic properties were obtained by employing clinoptilolite compared to other zeolitic supports, resulting in high stability. Based on the EDX results, a higher dispersion of chromium species could be achieved using synthetic supports especially HZSM-5 due to their much higher specific surface area. This reflects in the higher content of redox Cr species stabilized in comparison with SAPO-34 and clinoptilolite, which alongside homogenous and fine surface nanoparticles and fewer agglomerations account for the superior catalytic performance of Cr/ZSM-5. Based on the characterization results, the low surface area of clinoptilolite and low dispersion of Cr species in Cr/Clinoptilolite and surface coverage and micropore blockage in Cr/SAPO-34 are mainly responsible for low ethylene yield of this catalyst compared with implementing ZSM-5 support. It was found that Cr/ZSM5 effectively dehydrogenated ethane to ethylene in the presence of CO2 at 700 °C, giving 45.4% ethylene yield. Coke deposition as a result of the presence of strong acid sites is mainly responsible for decreasing trend observed for catalytic performance with increasing reaction time.
Keywords
Zeolitic suppored nanocatalyst
Oxidative dehydrogenation
Ethane
ethylene
Carbon dioxide

Subjects

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