Atomically Precise Control of Silver Species Encaged in Zeolite Catalysts with Minimal Loading for Maximal Performance

Atom-efficient metal catalysts with structural precision in the zeolite matrix are of great significance for maximizing the resource efficiency, but it remains challenging. In this study, atomically precise silver catalysts consisting of single atoms and subnanometric trimers were successfully encaged into the Y zeolite. Furthermore, we discriminate through experiments and DFT calculations the interplay among the electronic structure, coordination environment, and catalytic reactivity of silver atoms and trimers in silane oxidation. Interestingly, the single-atom catalyst with a minimal loading of 0.02 wt % reached the highest TOF of 16 043 h –1 at room temperature among the silver-based catalysts in the literature, but the silver trimer exhibited extremely poor capacities. This striking difference is attributed to the local chemistry and specific location within zeolites; the interactions between single atoms and adsorbed reactants can significantly cleave Si–H bonds. This work makes a critical comparison among zeolite-confined single atoms and minuscule clusters and provides a promising approach for the scale-up of atomically precise catalysts.