Impregnating Subnanometer Metallic Nanocatalysts into Self-Pillared Zeolite Nanosheets

Impregnation is the most commonly used approach to prepare supported metal catalysts in industry. However, this method suffers from formation of large particles with uneven dispersion, poor thermal stability, and thus unsatisfied catalytic performance. Here, we demonstrate that self-pillared MFI zeolite (silicalite-1 ZSM-5) nanosheets larger surface area abundant Si-OH groups are ideal supports immobilize ultrasmall monometallic (e.g., Rh Ru) various bimetallic clusters via simple incipient wetness impregnation method. The loaded subnanometric uniformly dispersed within sinusoidal five-membered rings remain stable at high temperatures. Rh/SP-S-1 highly efficient ammonia borane (AB) hydrolysis, showing a TOF value 430 molH2 molRh-1 min-1 298 K, which more than 6-fold improvement over nanosized zeolite-supported catalyst even comparable single-atom catalyst. Because synergistic effect between Rh-Ru acidity, H2 generation rate AB hydrolysis Rh0.8Ru0.2/SP-ZSM-5-100 reaches up 1006 molmetal-1 also shows record activities cascade hydrogenation nitroarenes by coupling AB. This work demonstrates excellent anchor diverse metallic species method, obtained nanocatalysts can be applied industrially important reactions.