Rapid direct synthesis of nano-H-ZSM-5 from leached illite via solid-like-state conversion-based crystallization

摘要

The direct synthesis of H-ZSM-5 catalysts from natural aluminosilicate clays is important for the conversion of raw clay resources to high-value-added products. Herein, the solid-like-state conversion was used to directly prepare nano-H-ZSM-5 with uniform morphology and particle size (similar to 300 nm) from leached illite (ISR) as both Si and Al source. Crystallization kinetics indicated that the reactivity of ISR is similar to that of commercially fabricated products and ISR could be rapidly (within 5 h) converted into nano-H-ZSM-5, the crystallinity, morphology, and crystal size of which were strongly affected by the amount of tetrapropylammonium hydroxide (TPAOH). Additionally, the residual Al of ISR uniformly intruded the H-ZSM-5 framework to provide active sites for the methanol-to-aromatics reaction. The catalytic performance stability and BTX selectivity of nano-H-ZSM-5 for this reaction surpassed those of a commercial ZSM-5 catalyst because of the synergistic effect among the specific surface area and volume of micropores, uniform morphology and particle size, and homogeneously distributed acidic sites. This rapid, efficient, and cleaner synthesis reported herein was shown to have no necessity of ion exchange with ammonium salts, to be H-form of ZSM-5 as well as improve the productivity of HZSM-5 catalysts. And consequently, it is expected to reduce the cost of synthesis and provide an opportunity for the comprehensive development and utilization of illite clay resources.