Abstract
Manipulating the geometries and electronic structures of oxygen vacancies (Ovs) in oxides to increase their catalytic activity has been a critical focus of research, but the processes remain challenging, particularly because of the significant interference caused by ubiquitous water vapour. In this work, we employ a nanocrystal-to-crystal transformation methodology to integrate a single atom of bismuth (Bi) into MnO(2), resulting in the formation of Bi-Ov-Mn entities. This single site reduces the formation energy of ˙OOOH species, facilitating the formation of reactive oxygen species (ROS), particularly ˙OH, due to the nonuniform electron distribution in the presence of both ozone and water. Therefore, this unique asymmetric defective linkage provides excellent water vapour resistance (1.8 vol%), which significantly improves its performance in the removal of volatile organic compounds. In this study, a pioneering paradigm utilizing asymmetric active sites is introduced, which expands the potential of catalytic ozonation for VOC abatement.