Nanocarbon materials are emerging as alternative activators of peroxymonosulfate (PMS) for organics decomposition. However, the relatively low activity and complex syntheses hindered their practical application and innovation with respect to rational design of carbocatalysts is highly desired. Herein, an in situ replication and transformation strategy was employed to facilely convert porous Fe₃O₄ microspheres into novel Fe/N codoped large-pore mesoporous carbon spheres (M‑Fe/NC) as Fenton-like catalysts for PMS activation. Benefiting from the abundance of active sites induced by dual heteroatom doping, the enhanced active site exposure due to the unique mesoporous structure, and the high stability of carbon component, the derived M‑Fe/NC was superior to the pristine Fe₃O₄ for PMS activation to degrade various organics and was efficient over a wide pH range (2–9). Compared with the proposed mechanisms of previous reports, both radical (surface-bound SO₄⁻ and OH) and nonradical (¹O₂ and direct oxidation) pathways are involved in the M‑Fe/NC/PMS system. Furthermore, experimental observations in combination with DFT calculations reveal that graphitic N and FeN₄ sites serve as dual reaction centers in the catalysis. This research opened an avenue for development of novel multi-doped carbocatalysts used to activate PMS for sustainable remediation.

纳米碳材料正在作为有机过氧化物分解的过氧单硫酸盐（PMS）的替代活化剂而出现。然而，相对低的活性和复杂的合成阻碍了它们的实际应用，并且高度期望关于碳催化剂的合理设计的创新。本文中，采用原位复制和转化策略轻松地转化多孔Fe ₃ O ₄的微球转变成新型的Fe / N共掺杂的大孔介孔碳球（M‑Fe / NC），作为PMS活化的类Fenton催化剂。得益于双重杂原子掺杂诱导的大量活性位点，由于独特的介孔结构而增加的活性位点暴露，以及碳组分的高稳定性，所得到的M‑Fe / NC优于原始的Fe ₃ O ₄。 PMS活化可降解各种有机物，并且在很宽的pH范围内（2–9）有效。与以前的报告中所提出的机制相比，两个自由基（表面结合的SO ₄ ^-和OH）和非自由基（¹ Ò ₂M‑Fe / NC / PMS系统中包含了直接和直接氧化途径）。此外，结合DFT计算的实验观察表明，石墨N和Fe N ₄位点在催化中充当双重反应中心。这项研究为开发新型多掺杂碳催化剂以激活PMS进行可持续修复开辟了道路。