Synergistic oxytetracycline adsorption and peroxydisulfate-driven oxidation on nitrogen and sulfur co-doped porous carbon spheres

Abstract

Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment. Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs₉₀₀-OH) were synthesized using glucose and L-cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs₉₀₀-10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min⁻¹ (k_0–15 min). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs₉₀₀-10%-OH ensured the efficient oxidation of OTC. N,S-CSs₉₀₀-10%-OH reduced the activation energy of the OTC degradation reaction (Ea=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O₂^•−, ¹O₂, SO₄^•− and •OH, of which O₂^•− was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.