Janus Electronic State of Supported Metal Oxide Catalysts Governs Removal of Multiple Pollutants

ABSTRACT Orchestrating adsorption and activation of multiple pollutants at specific sites in environmental catalysis remains challenging. Here, we report a Janus electronic state in the catalysts by dispersing nanosized MnO 2 on hydroxylated TiO 2 , comprising interface‐proximal electron‐enriched Mn 3+ sites and interface‐distal electron‐deficient Mn 4+ sites, arising from spatially asymmetric charge distribution induced by strong oxide‐support interaction. This structure was elucidated through atomic‐resolution scanning transmission electron microscopy, electron energy loss spectroscopy, X‐ray absorption spectroscopy probing the interface between nanosized MnO 2 and hydroxylated TiO 2 , complemented by density functional theory calculations. Taking the synergistic catalytic conversion of nitrogen oxide and volatile organic compounds as a model reaction for environmental catalysis, this Janus electronic state catalyst exhibits remarkable molecule‐site specificity, channelling nitrogen oxide reduction to electron‐enriched Mn 3+ sites and volatile organic compound oxidation to electron‐deficient Mn 4+ sites. This work highlights the potential of the Janus electronic state for precise catalysis in removal of multiple pollutants.