Material-enhanced heterogonous peroxymonosulfate (PMS) activation on emerging organic pollutant degradation has attracted intensive attention, and a challenge is the electron transfer efficiency from material to PMS for radical production. Herein, an interface architecture of Co­(OH)2 nanosheets growing on the KNbO3 perovskite [Co­(OH)2/KNbO3] was developed, which showed high catalytic activity in PMS activation. A high reaction rate constant (k 1) of 0.631 min–1 and complete removal of pazufloxacin within 5 min were achieved. X-ray photoelectron spectroscopy, X-ray absorption near edge structure spectra, and density functional theory (DFT) calculations revealed the successful construction of the material interface and modulated electronic structure for Co­(OH)2/KNbO3, resulting in the hole accumulation on Co­(OH)2 and electron accumulation on KNbO3. Bader topological analysis on charge density distribution further indicates that the occupations of Co-3d and O-2p orbitals in Co­(OH)2/KNbO3 are pushed above the Fermi level to form antibonding states (σ*), leading to high chemisorption affinity to PMS. In addition, more reactive Co­(II) with the closer d-band center to the Fermi level results in higher electron transfer efficiency and lower decomposition energy of PMS to SO4 •–. Moreover, the reactive sites of pazufloxacin for SO4 •– attack were precisely identified based on DFT calculation on the Fukui index. The pazufloxacin pathways proceeded as decarboxylation, nitroheterocyclic ring opening reaction, defluorination, and hydroxylation. This work can provide a potential route in developing advanced catalysts based on manipulation of the interface and electronic structure for enhanced Fenton-like reaction such as PMS activation.

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