MOR nanosheets with tunable c-axis thickness and their catalytic performance in DME carbonylation

Abstract

Controlling the anisotropic growth of crystals to achieve desired morphology is a challenge in zeolite crystallization, which often requires the use of bulky organic surfactants or additional crystal growth modifiers. Here, MOR crystals with tunable c-axis thickness (12-MR channel direction) were readily synthesized with commercial tetraethylammonium hydroxide (TEAOH) as an organic-structure directing agent (OSDA). It is revealed that the relative growth rates of different crystal faces of MOR zeolite can be tuned by the crystallization temperature and TEAOH amount in the developed gel system. Higher temperature and lower TEAOH concentration can effectively retard the growth of MOR crystals along the c-axis, yielding MOR nanosheets with short c-axis thickness (ca. 40 nm). Investigation on the crystallization process demonstrates that the crystal growth follows a particle attachment mechanism. Theoretical calculation was further employed to elucidate the c-axis thickness variation of MOR zeolite under different conditions. A kilogram-scale synthesis of MOR nanosheets has been realized with a 10 L autoclave, achieving high solid yield of 92 %. The MOR nanosheets, offering short 12-MR diffusion path, exhibit substantially enhanced catalytic activity and stability in the dimethyl ether (DME) carbonylation to methyl acetate reaction.