Dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion

This work reports for the first time a dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion observed during an induction period. The OXZEO (oxide-zeolite) bifunctional catalyst concept has enabled selective syngas conversion to a series of value-added chemicals and fuels such as light olefins, aromatics and gasoline. Herein we report for the first time a dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion observed during an induction period. Structured illumination microscopy, intelligent gravimetric analysis, UV-Raman, X-ray diffraction, thermogravimetry and gas chromatography-mass spectrometer analysis indicate that this is attributed to the evolution of carbonaceous species as the reaction proceeds, which gradually reduces the effective space inside the cage. Consequently, the diffusion of molecules is hindered and the hindering is much more prominent for larger molecules such as C4+. As a result, the selectivity of ethylene is enhanced whereas that of C4+ is suppressed. Beyond the induction period, the product selectivity levels off. For instance, ethylene selectivity levels off at 44% and propylene selectivity at 31%, as well as CO conversion at 27%. The findings here bring a new fundamental understanding that will guide further development of selective catalysts for olefin synthesis based on the OXZEO concept.

Automated summary

This study reports the dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion during an induction period. The evolution of carbonaceous species reduces the effective space inside the cages, hindering the diffusion of molecules, especially larger ones. As a result, the selectivity of ethylene is enhanced while the selectivity of C4+ is suppressed.