Zeolite Y-Encapsulated Pd Single Atoms and Clusters: Unlocking Stepwise Synergy for Low-Temperature Propane Oxidation

We report the rational design and precise construction of Y zeolite-encapsulated Pd catalysts featuring coexisting single atoms and clusters (Pd 1+ n @Y) that enable the efficient and low-temperature total oxidation of propane. Fine tuning of Pd loading and synthesis conditions in a PVP-assisted one-pot hydrothermal approach affords controllable confinement of dual active sites (isolated Pd single atoms and clusters). Catalytic evaluations reveal that Pd 1+ n @Y exhibits a T 90 of only 265 °C, significantly outperforming the single-site counterparts (Pd 1 @Y and Pd n @Y). Combining density functional theory (DFT) calculations with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies elucidates a stepwise synergistic mechanism wherein Pd single atoms preferentially activate the C–H bond in propane to form alkyl intermediates, while Pd clusters facilitate O 2 activation and C–C bond cleavage to complete oxidation. This work establishes a robust “single atom–cluster” synergistic paradigm for designing advanced catalysts for the abatement of light alkanes.