Organic Structure-Directing Agent-Free Synthesis of Mordenite-Type Zeolites Driven by Al-Rich Amorphous Aluminosilicates

Mordenite (MOR)-type zeolites with a Si/AI molar ratio of up to 13 with crystallite sizes of ca. 60 nm were successfully synthesized from Al-rich aluminosilicates with a Si/Al ratio of 2 and additional SiO2 under seed-assisted hydrothermal conditions for 6 h or longer without any organic structure-directing agents (OSDAs). In stark contrast, under the same hydrothermal conditions for 6 h, control experiments using starting reagent(s), such as Al-poor aluminosilicate, pure SiO2, tetraethyl orthosilicate, and Al(NO3)(3), all of which are typically employed for zeolite synthesis, failed to yield MOR-type zeolites. The pentacoordinated Al species, which are present in Al-rich aluminosilicates and are more reactive than the tetra- and hexa-coordinated Al species typically found in alumina and Al-poor aluminosilicates, played a decisive role in the OSDA-free synthesis of MOR-type zeolites.

Automated summary

MOR-type zeolites with a Si/Al ratio of up to 13 and crystallite sizes of around 60 nm were successfully synthesized from Al-rich aluminosilicates with additional SiO2 under seed-assisted hydrothermal conditions. The presence of pentacoordinated Al species in the Al-rich aluminosilicates played a decisive role in the OSDA-free synthesis of MOR-type zeolites, while control experiments using other starting reagents failed to yield the desired product.