High‐Entropy Oxides Stabilized Single‐Atom Pt Triggers Mechanism Transition for Efficient Catalytic Oxidation

ABSTRACT The diesel oxidation catalysts (DOC) have been challenged by the high cost of noble metal and limited reactivity at low temperature. Herein, we report PtSmMnCoNb high‐entropy oxide nanoparticles supported single‐atom Pt catalyst, which achieves 90% conversion for CO at 100°C, for C 3 H 6 at 208°C, and 50% conversion for NO x at 203°C. This catalyst also achieves a thermodynamically stabilized configuration, which exhibits a long‐term durability benefited from high‐entropy effects. A combined experimental and theoretical analysis reveals the electron‐rich character of Pt δ+ sites derived by the strong interaction involved in abundant Pt‐O‐Metal interfaces, which accounts for the effective activation for reactants, leading to a transition in the reaction mechanism from Mars‐van Krevelen to Eley‐Rideal. This work provides a design paradigm of advanced catalysts for the integrated removal of multi‐pollutants.