Ethane aromatization and evolution of carbon deposits over nanosized and microsized Zn/ZSM-5 catalysts

Abstract

Rapid deactivation by coke deposition is the main obstacle of ethane aromatization over Zn/ZSM-5. In this work, using the prepared nanosized Zn/HZSM-5, an almost threefold product yield and significantly improved stability were achieved in comparison with those of the microsized catalyst. XRD and XPS analyses indicated that a higher percentage of reactive [ZnOZn]²⁺ species was maintained during ethane aromatization over nano-Zn/HZSM-5 than micro-Zn/HZSM-5. In addition, the evolution of carbon deposits over nanosized and microsized Zn/ZSM-5 was investigated during prolonged ethane aromatization reaction using Raman spectroscopy and thermogravimetry measurements. Compared to the microsized catalyst, the nanosized zeolite facilitated the faster escape of light aromatics and the precursors of carbon deposits from the zeolite pores, thus suppressing the accumulation of coke deposits and improving the catalyst stability. Based on the nanosized Zn/HZSM-5, a protocol of isothermal reaction followed by regeneration was developed by periodically removing carbonaceous deposits, and an ∼25–35% product yield was achieved after 10 reaction–regeneration cycles.