Xu Le, Ma Tianqiong, Shen Yihan, Wang Yong, Han Lu, Chaikittisilp Watcharop, Yokoi Toshiyuki, Sun Junliang, Wakihara Toru, Okubo Tatsuya
Department of Chemical System Engineering, The University of Tokyo, Tokyo, 113-8656, Japan.
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
Angew Chem Int Ed Engl. 2020 Nov 2;59(45):19934-19939. doi: 10.1002/anie.202009336. Epub 2020 Aug 31.
Unit-cell-thin zeolitic nanosheets have emerged as fascinating materials for catalysis and separation. The controllability of nanosheet stacking is extremely challenging in the chemistry of two-dimensional zeolitic materials. To date, the organization of zeolitic nanosheets in hydrothermal synthesis has been limited by the lack of tunable control over the guest-host interactions between organic structure-directing agents (OSDAs) and zeolitic nanosheets. A direct synthetic methodology is reported that enables systematic manipulation of the aluminosilicate MWW-type nanosheet stacking. Variable control of guest-host interactions is rationally achieved by synergistically altering the charge density of OSDAs and synthetic silica-to-alumina composition. These finely controlled interactions allow successful preparation of a series of three-dimensional (3D) zeolites, with MWW-layer stacking in wide ranges from variably disorder to fully ordered, leading to tunable catalytic activity in the cracking reaction. These results highlight unprecedented opportunities to modulate zeolitic nanosheets arrangement in 3D zeolites whose structure can be tailored for catalysis and separation.
