Insights into persulfate activation by dicyandiamide-derived carbon for 2,4-dichlorophenol degradation: Roles of nitrogen doping and defective carbon atoms

Abstract

In this study, a dicyandiamide residue-derived carbon material (DWC-800) was fabricated through a two-step process involving ball-milling nitrogen (N) doping and high-temperature annealing, and then utilized for peroxodisulfate (PDS) activation in the removal of 2,4-dichlorophenol (2,4-DCP). The obtained DWC-800, with very low N content (0.52 at.%), exhibited highly efficient PDS activation, resulting in complete removal of 2,4-DCP in 60 min. This performance was superior to that of the material with high N content (15.4 at.%), which was prepared using only one-step ball-milling N doping. The N-doped process increased the defective degree of carbocatalyst, and these reactive carbon defects rather than N species greatly improved the adsorption and catalytic activity. The results of quenching experiments and electron paramagnetic resonance demonstrated that PDS activation by DWC-800 for 2,4-DCP degradation followed a nonradical pathway, leading to the production of both singlet oxygen (1O2) and carbon-PDS* complex. Notably, electron transfer mediated by the carbon-PDS* complex played a significant role in the degradation of 2,4-DCP. Overall, this study gets new insights into the role of N doping in mediating the structural properties of the carbocatalyst and its catalytic performance, and provides a theoretical basis for the utilization of dicyandiamide waste residue for wastewater remediation.