NDLI: Methanol-to-olefins process over zeolite catalysts with DDR topology: effect of composition and structural defects on catalytic performance

Content Provider	Royal Society of Chemistry (RSC)
Author	Yarulina, Irina Ruiz-Martinez, Javier Gascon, Jorge Goetze, Joris Kapteijn, Freek Gücüyener, Canan Weckhuysen, Bert M. Thiel, Leonard van Dikhtiarenko, Alla
Copyright Year	2016
Abstract	A systematic study of the effect of physicochemical properties affecting catalyst deactivation, overall olefin selectivity and ethylene/propylene ratio during the methanol-to-olefins (MTO) reaction is presented for two zeolites with the DDR topology, namely Sigma-1 and ZSM-58. Both catalysts show high selectivity towards light olefins and completely suppress the formation of hydrocarbons bigger than C4, with selectivity to ethane not exceeding 1% and some traces of propane. By applying seeded growth approach, a series of Sigma-1 zeolites with tunable crystal size and acidity was synthesized. For this series the highest methanol throughput at 450 °C before deactivation was found for crystals 0.5 μm in size with an acidity corresponding to 0.5 Al atoms per zeolite cage, and a selectivity to ethylene and propylene reaching 90%. Comparison between ZSM-58 and Sigma-1 catalysts with similar morphologies and acidity under the same reaction conditions revealed a three times higher throughput of methanol in case of ZSM-58. The analysis of functional surface groups, assessed through FT-IR, revealed the presence of silanol defects in Sigma-1 responsible for faster catalyst deactivation. These silanol defects can be selectively removed (confirmed by FT-IR) from the zeolite framework by applying a mild treatment in presence of NaOH/CTAB, leading to an improved catalyst lifetime. Co-feeding experiments with short olefins and water show low reactivity of primary MTO products, which only react at the surface of the catalyst particles. These results demonstrate that migration of the reaction zone in case of DDR catalysts hardly affects catalyst stability, product composition and nature of deactivating species. The nature of these species depends mostly on reaction temperature: at low temperatures deactivation occurs mainly due to the formation of inert adamantane species, while at high temperatures poly-condensed aromatic hydrocarbons play the major role in deactivation.
Starting Page	2663
Ending Page	2678
Page Count	16
File Format	HTM / HTML PDF
ISSN	20444753
Volume Number	6
Issue Number	8
Journal	Catalysis Science & Technology
DOI	10.1039/c5cy02140e
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Subscribed
Subject Keyword	Silanol Propene Alkene Adamantane Ethylene Sigma Micrometre Topology Zeolite Fourier-transform infrared spectroscopy Propane Methanol
Content Type	Text
Resource Type	Article
Subject	Catalysis

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