Nitrogen/Sulfur Co-Doped Biochar for Peroxymonosulfate Activation in Paracetamol Degradation: Mechanism Insight and Toxicity Evaluation

Advanced oxidation processes based on either peroxydisulfate (PDS) or peroxymonosulfate (PMS), collectively termed persulfate-based advanced oxidation processes (PS-AOPs), show potential in wastewater treatment applications. In this work, the nitrogen (N) and sulfur (S) co-doped biochar (NSBC) was prepared via a one-step pyrolysis of coffee grounds at 400 to 800 °C as a PMS activator for degrading paracetamol (PCT). The non-metallic NSBC demonstrated exceptional catalytic activity in activating PMS. In the NSBC-800/PMS system, 100% of PCT was completely degraded within 20 min, with a high reaction rate constant (k_obs) of 0.2412 min⁻¹. The system’s versatility was highlighted by its degradation potential across a wide pH range (3–11) and in the presence of various background ions and humic acids. The results of various experiments and characterization techniques showed that the system relied on an NSBC-800-mediated electron transfer as the main mechanism for PCT degradation. Additionally, there was a minor involvement of ¹O₂ in a non-radical degradation pathway. The graphitic N and thiophene-S (C-S-C) moieties introduced by N/S co-doping, as well as the carbonyl (C=O) groups of the biochar, were considered active sites promoting ¹O₂ generation. The total organic carbon (TOC) removal rate reached 37% in 120 min, while the assessment of the toxicity of the degradation products also affirmed the system’s environmental safety. This research provides a novel method for preparing environmentally friendly and cost-effective carbon-based catalysts for environmental remediation.