Cobalt single atoms anchored in crystalline carbon nitride for efficient peroxymonosulfate activation to combat...

Antibiotic resistance poses considerable risks worldwide due to its threats to human health and ecosystem stability. Notably, aquatic ecosystems are recognized as reservoirs of antibiotic resistance contaminants. Therefore, developing effective strategies to mitigate antibiotic resistance in aquatic environments is urgently required. Herein, a cobalt single-atom-crystalline carbon nitride (Co-CCN) catalyst was fabricated and employed to activate peroxymonosulfate (PMS) for antibiotic-resistant bacteria (ARB) inactivation and antibiotic-resistance genes (ARGs) elimination. Notably, the Co-CCN/PMS system attained approximately 6-7-log inactivation of diverse ARB within 20 min, and ARB membrane disruption was further verified based on cellular morphology imaging and protein leakage measurements. Additionally, the removal efficiency of tetA exceeded a 4-log reduction within 120 min. Electron paramagnetic resonance (EPR) and quenching tests confirmed that the Co-CCN/PMS system generated •OH, SO₄•^-, •O₂ ^-, and ¹O₂ for highly efficient ARB inactivation and ARG removal. Besides, the Co-CCN/PMS system also demonstrated exceptional environmental robustness and high efficiency for treating real water. Density functional theory (DFT) calculations indicated that single Co atoms adsorb oxygen atoms from PMS via electrostatic interactions, accompanied by electron transfer from Co-CCN to activate PMS. Our findings provide atomic-level insights into PMS activation for mitigating antibiotic resistance in aquatic settings.