Fluorine and nitrogen dual-doped carbon material as metal-free peroxymonosulfate activator for efficient tetracycline degradation: Radical-free mechanism

Persulfate-based advanced oxidation technology holds great potential for antibiotic treatment. However, its low activity, metal ion leaching, and poor stability mainly limit the practical application. Fluorine-nitrogen heteroatomic dual-doping carbon material (F,N-CM) was successfully prepared using ZIF-8 metal-organic frameworks as a precursor. F,N-CM exhibited high peroxymonosulfate (PMS) activation capability for tetracycline (TC) degradation. The incorporation of F and N dopants in F,N-CM created abundant defects and active sites, facilitating the activation of PMS. Notably, the presence of fluorine atomic lone electron pairs significantly enhanced electron transfer from PMS to TC. The high degradation performance of the F,N-CM/PMS system was primarily attributed to radical-free pathways involving singlet oxygen and electron transfer. Furthermore, F,N-CM demonstrated good stability for PMS activation and could be regenerated through simple calcination. This research provides a novel strategy for developing metal-free carbon materials with dual-doped heteroatoms as effective catalyst for PMS activation and degradation of refractory organic pollutants.