Amino-assisted MOF-derived hierarchical Pt@CeO2 microspheres with highly dispersed Pt for efficient toluene oxidation

Amino-ligand-assisted MOF derivation forms hierarchical Pt@CeO 2 microspheres. • -NH 2 groups anchor Pt species, preventing aggregation and maintaining pores. • The catalyst shows exceptional toluene oxidation, achieving a low T 90 of 177 °C. • In situ DRIFTS elucidates a sequential Mars-van Krevelen oxidation pathway. A novel amino-ligand-assisted MOF-derivation strategy was developed to fabricate hierarchically structured Pt@CeO 2 microspheres with highly dispersed Pt species (0.34 wt. %). The -NH 2 functional groups effectively anchored Pt precursors, preventing aggregation and preserving hierarchical porosity during calcination. The resulting catalyst exhibited exceptional toluene oxidation performance, achieving T 50 and T 90 values of 155 and 177 °C, respectively, significantly outperforming conventional impregnation-derived counterparts. Characterization revealed abundant surface oxygen vacancies, enhanced Ce 3+ concentration, and superior low-temperature reducibility due to strong metal-support interaction. In situ DRIFTS analysis confirmed a Mars-van Krevelen mechanism with sequential degradation pathway: toluene → benzyl alcohol → benzaldehyde → benzoate → anhydride → CO 2 and H 2 O. The superior catalytic performance arises from the synergistic effects of the hierarchically oriented mesoporous structure, inherently enlarged specific surface area, and the highly dispersed active Pt species confined within the CeO 2 matrix. This work establishes a versatile platform for designing high-performance catalysts with controlled metal dispersion and hierarchical porosity for VOC abatement and oxidation reactions. Download: Download high-res image (202KB) Download: Download full-size image