Catalytic ozonation of VOC over high-entropy MnCePrZrY oxide: unveiling the role of high-entropy configuration in ozone activation

High-entropy oxides (HEOs) have emerged as promising catalytic materials owing to their unique multi-metal synergy and tunable defect structures. However, their application in the catalytic ozonation of gaseous volatile organic compounds (VOCs) remains largely unexplored. Herein, a novel fluorite-type HEO, (MnCePrZrY)O 2 , was synthesized via a self-propagating combustion method and employed for the low-temperature catalytic ozonation of acetone. The HEO achieved complete catalytic ozonation of acetone at 90 °C while maintaining stable activity over an 18 h test. Comparative experiments using O 2 and O 3 as oxidants revealed that the promotional effect of the high-entropy structure was substantially more pronounced in catalytic ozonation than in conventional catalytic oxidation, highlighting the critical role of the HEO in amplifying the promoting effect of O 3 . Mechanistic investigations demonstrated that the local lattice distortion induced by the high-entropy configuration lowered the oxygen-vacancy formation energy, thereby promoting the generation of oxygen-deficient structures and enhancing ozone adsorption. Meanwhile, multimetallic coupling induced pronounced electronic redistribution and reduced the charge-transfer resistance, facilitating the activation of adsorbed ozone and its conversion into ROS, particularly highly oxidative hydroxyl radicals, which accelerated the oxidation of acetone-derived intermediates. This work elucidates how high-entropy configurations enhance ozone activation and promote the low-temperature deep oxidation of VOCs, providing new insights into the rational design of efficient catalysts for catalytic ozonation.