Peroxydisulfate activation by sulfur-doped ordered mesoporous carbon: Insight into the intrinsic relationship between defects and 1O2 generation

Abstract

The carbon-catalyzed persulfate-based advanced oxidation process (PS-AOP) has recently received much focus owing to the green, economical, and sustainable nature of carbon catalysts. In this study, sulfur-doped ordered mesoporous carbons (S-OMCs) were utilized to activate peroxydisulfate (PDS) for ciprofloxacin (CIP) removal. A synthesis temperature gradient was set to regulate the defect level of S-OMCs, since the thermal decomposition of oxygen- and sulfur-containing groups at different temperatures could release S and O and then create defects. In all S-OMCs/PDS systems, ¹O₂ dominated CIP degradation. Interestingly, a high linear correlation (R² = 0.9091) between defect level and ¹O₂ yield was found, confirming the structure-activity relationship between defects and ¹O₂ generation. Moreover, the impacts of several important reaction conditions and water matrix on S-OMC-1000/PDS activation system were surveyed. In the S-OMC-1000/PDS activation system, CIP removal could attain 85.84% under the condition of unadjusted pH (pH = 5.3) and small amount of S-OMC-1000 (50 mg/L). The S-OMC-1000/PDS activation system also exhibited relatively stable or even better performance in the presence of common inorganic anions and natural organic matter (NOM), manifesting its good potential for practical applications. In addition, the reusability of S-OMC-1000 was investigated. This study provides a practical and high-efficiency way for decontaminating antibiotic-polluted water, and gives an alternative approach for identifying the active site of catalysts.

Keywords: (1)O(2); Ciprofloxacin; Defects; Peroxydisulfate activation; S-doped ordered mesoporous carbon; Structure-activity relationship.