Methanol-to-hydrocarbons conversion over MoO sub(3)/H-ZSM-5 catalysts prepared via lower temperature calcination: a route to tailor the distribution and evolution of promoter Mo species, and their corresponding catalytic properties
A series of MoO sub(3)/H-ZSM-5 (Si/Al = 25) catalysts were prepared via calcination at a lower-than-usual temperature (400 degree C) and subsequently evaluated in the methanol-to-hydrocarbon reaction at that same temperature. The catalytic properties of those catalysts were compared with the sample...
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Veröffentlicht in: | Chemical science (Cambridge) 2015-08, Vol.6 (9), p.5152-5163 |
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Sprache: | eng |
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Zusammenfassung: | A series of MoO sub(3)/H-ZSM-5 (Si/Al = 25) catalysts were prepared via calcination at a lower-than-usual temperature (400 degree C) and subsequently evaluated in the methanol-to-hydrocarbon reaction at that same temperature. The catalytic properties of those catalysts were compared with the sample prepared at the more conventional, higher temperature of 500 degree C. For the lower temperature preparations, molybdenum oxide was preferentially dispersed over the zeolite external surface, while only the higher loading level of MoO sub(3) (7.5 wt% or higher) led to observable inner migration of the Mo species into the zeolite channels, with concomitant partial loss of the zeolite Broensted acidity. On the MoO sub(3) modified samples, the early-period gas yield, especially for valuable propylene and C sub(4) products, was noticeably accelerated, and is gradually converted into an enhanced liquid aromatic formation. The 7.5 wt% MoO sub(3)/H-ZSM-5 sample prepared at 400 degree C thereby achieved a balance between the zeolite surface dispersion of Mo species, their inner channel migration and the corresponding effect on the intrinsic Broensted acidity of the acidic zeolite. That loading level also possessed the highest product selectivity (after 5 h reaction) to benzene, toluene and xylenes, as well as higher early-time valuable gas product yields in time-on-stream experiments. However, MoO sub(3) loading levels of 7.5 wt% and above also resulted in earlier catalyst deactivation by enhanced coke accumulation at, or near, the zeolite channel openings. Our research illustrates that the careful adoption of moderate/lower temperature dispersion processes for zeolite catalyst modification gives considerable potential for tailoring and optimizing the system's catalytic performance. |
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ISSN: | 2041-6520 2041-6539 |
DOI: | 10.1039/c5sc01825k |