Iron-based catalysts are widely used in peroxysulfate-based AOPs but suffering from low catalytic performance at neutral pH conditions, which limits the application in groundwater remediation. Herein, this study investigated the efficacy, mechanism and long-term durability of Fe-doped nitrogen carbon (Fe@NC) armor catalysts toward peroxysulfate activation for the degradation of anthropogenic phenolics (APs) in groundwater matrices. The results showed that nonradical activation of Oxone (i.e., HSO₅^–) was obtained over the as-prepared Fe-3 % @NC-700 catalyst, high-valent Fe species (Fe(IV)O) and ¹O₂ were identified as the dominant reactive species for the efficient degradation of APs by experiments and density functional theory (DFT) calculations. Notably, the DFT results indicated that HSO₅^– was favorably adsorbed on the Fe atoms owing to the electrostatic interaction, which transformed exothermically into SO₄^2– and ¹O₂ over Fe₃C, accompanied by the generation of Fe(IV)O. Additionally, the Fe-3 % @NC-700 catalyst displayed long-term activity for in situ activation of Oxone in groundwater matrices without pH adjustment, resulting in ΔAPs: ΔOxone stoichiometry efficiencies at 4.2–5.0 % . Wheat seeds germination tests revealed that the biotoxicity of the treated water was reduced notably by the present catalytic system, which holds large potential application in treatment of APs-contaminated groundwater.

铁基催化剂广泛用于过硫酸盐基AOP，但在中性pH条件下催化性能较低，限制了其在地下水修复中的应用。在此，本研究研究了铁掺杂氮碳（Fe@NC）铠装催化剂对过氧硫酸盐活化降解地下水基质中人为酚类（AP）的功效、机制和长期耐久性。结果表明，在所制备的 Fe-3 % @NC-700 催化剂上实现了Oxone（即 HSO ₅ ^– ）的非自由基活化，鉴定出高价 Fe 物种（ Fe(IV) O）和¹ O ₂通过实验和密度泛函理论（DFT）计算，将其作为有效降解AP的主要反应物种。值得注意的是，DFT结果表明，由于静电相互作用， HSO ₅ ^–有利地吸附在Fe原子上，在Fe _{3 C上放热转化为SO 4} ^2–和¹ O ₂，​​同时生成Fe(IV) O此外，Fe-3% @NC-700 催化剂在无需调节 pH 的情况下，在地下水基质中显示出对 Oxone 进行原位活化的长期活性，导致 ΔAPs：ΔOxone 化学计量效率为 4.2–5.0%。小麦种子发芽试验表明，本催化系统显着降低了处理水的生物毒性，在处理APs污染的地下水方面具有巨大的应用潜力。