Effect of Cage Size on the Selective Conversion of Methanol to Light Olefins

Abstract

Zeolites that contain eight-membered ring pores but different cavity geometries (LEV, CHA, and AFX structure types) are synthesized at similar Si/Al ratios and crystal sizes. These materials are tested as catalysts for the selective conversion of methanol to light olefins. At 400 °C, atmospheric pressure, and 100% conversion of methanol, the ethylene selectivity decreases as the cage size increases. Variations in the Si/Al ratio of the LEV and CHA show that the maximum selectivity occurs at Si/Al = 15–18. Because lower Si/Al ratios tend to produce faster deactivation rates and poorer selectivities, reactivity comparisons between frameworks are performed with solids having a ratio Si/Al = 15–18. With LEV and AFX, the data are the first from materials with this high Si/Al. At similar Si/Al and primary crystallite size, the propylene selectivity for the material with the CHA structure exceeds those from either the LEV or AFX structure. The AFX material gives the shortest reaction lifetime, but has the lowest amount of carbonaceous residue after reaction. Thus, there appears to be an intermediate cage size for maximizing the production of light olefins and propylene selectivities equivalent to or exceeding ethylene selectivities.