Mechanochemically assisted hydrothermal synthesis of Sn-substituted MFI-type silicates

Sci Technol Adv Mater. 2018 Aug 6;19(1):545-553. doi: 10.1080/14686996.2018.1497404. eCollection 2018.

Abstract

Substitution of Al atoms in a zeolite framework by catalytic metal atoms has attracted considerable attention because the catalytic behavior can be tuned by the substituted atoms. In the present study, Sn-substituted MFI-type silicates were synthesized using a hydrothermal reaction of an amorphous Si-O-Sn precursor prepared by mechanochemical grinding of SiO2 and Sn(OH)4. The mechanochemical treatment was found to be a key technique for obtaining the amorphous Si-O-Sn precursor, where tetrahedral Sn4+ species were incorporated into the amorphous matrix. The Sn content in the framework of the MFI-type silicates was successfully controlled by the initial HCl/Si molar ratio of the hydrothermal procedures. Optical reflectance measurements revealed that the Sn4+ ions were dispersedly incorporated into the silicate framework while preserving the initial tetrahedrally coordinated species. Infrared results imply that the resulting Sn-substituted MFI-type silicate has Brønsted acid character. Precise control of the Brønsted and Lewis acid properties by Sn doping is a promising approach to the development of novel types of zeolite-based catalytic materials.

Keywords: 10 Engineering and Structural materials; 102 Porous / Nanoporous / Nanostructured materials; 301 Chemical syntheses / processing; MFI; Mechanochemical; hydrothermal; silicate; zeolite.

Grants and funding

This work was supported by the Japan Society for the Promotion of Science [15H04181]; JST-CREST.