The effect of Br− and F− on the synthesis of ZSM-11 zeolites with tetrabutylammonium salts and the catalytic performance of methanol to olefins
摘要
ZSM-11 zeolites were systematically synthesized by a simple two-stage crystallization method with TBABr and TBAF template respectively. The physical and chemical properties of the obtained samples were characterized by using XRD, FTIR, SEM, N2 physical adsorption & desorption and NH3-TPD. The effects of Br− and F− on the morphologies, structure, acidities as well as the catalytic performance of methanol to olefins (MTO) process were elaborately investigated. The findings suggested that the F− anion facilitated the aggregation of nanocrystalline grains and a more refined MEL structure, thereby resulting in a larger BET surface, abundant mesopores and moderate acidity, which effectively improved diffusion ability and suppressed coke deposition. In contrast, the Br− contributed to the morphology of rod-like crystals aggregation and the co-crystalline ZSM-11/5 zeolites. As a result, the ZSM-11 zeolite prepared with TBAF template exhibited significantly superior catalytic performance in MTO process with a longer lifetime and higher selectivity to propylene and butene, compared to the ZSM-11 synthesized using TBABr template.