A Facile and Green Synthesis Strategy for Full-Crystalline Shaped Mordenite Zeolite with Excellent Catalytic Performance and Mechanical Strength

Zeolites are indispensable catalysts in industrial processes, yet the incorporation of inert binders during shaping often leads to active site dilution and pore blockage, compromising catalytic efficiency. Herein, we develop a green, efficient, and robust strategy for fabricating full-crystalline shaped zeolites by converting binders into zeolite frameworks via steam-assisted crystallization. This template-free approach reduced the environmental negative impact while enabling the direct formation of binder-free zeolite bodies. The resulting catalysts exhibit high crystallinity, enhanced mass transport, and considerable mechanical strength (129.4 ± 28.3 N/cm), together delivering superior catalytic performance (1003.3 g·kgcat⁻¹·h⁻¹) in dimethyl ether (DME) carbonylation compared with conventional shaped zeolite (632.5 g·kgcat⁻¹·h⁻¹) and the parent powders (839.8 g·kgcat⁻¹·h⁻¹). Comprehensive characterization by Ar physisorption, SEM, NH₃-TPD, IR, and DME adsorption confirms that increased acidity and improved pore connectivity account for the performance enhancement, while intergrown zeolite domains strengthen particle cohesion and mechanical integrity. Furthermore, the steam-assisted method demonstrates broad applicability across a wide range of sol-gel formula. Time-resolved crystallization investigation demonstrates that the full crystallization can be achieved within a short duration (12 h). Overall, this work establishes an eco-friendly and efficient route for synthesizing engineering-grade, full-crystalline shaped MOR zeolite, providing practical guidance for next-generation industrial catalysts.