Two-dimensional carbon materials with various N atom proportions (2D-CNMs) are constructed to clarify the optimal catalyst for carbamazepine (CBZ) oxidation and the inner mechanism for persulfate-based advanced oxidation processes (P-AOPs). Results show that peroxydisulfate (PDS) can be activated by all 2D-CNMs with the order of C₃N > C₇₁N > graphene > C₂N > CN, while C₃N is the only catalyst for peroxymonosulfate (PMS) activation. The C₃N with the maximum graphitic N can activate PDS and PMS in a wide temperature range at any pH, and demonstrates the optimal CBZ oxidation performance. Notably, the graphitic N atoms promote P-AOPs from five aspects: (i) electron structure, (ii) electrical conductivity, (iii) electron transfer from persulfate to catalysts, (iv) electron jump of co-system before and after activation, (v) interaction between catalyst and persulfate. The most vigorous activity of C₃N is attributed to the greatest number of graphitic N. This work clarifies the essential role of graphitic N atoms with implications for the catalyst design, and facilitates the environmental applications of P-AOPs for micropollutant abatement.

构建具有不同N原子比例的二维碳材料（2D-CNMs），以阐明卡马西平（CBZ）氧化的最佳催化剂和过硫酸盐基高级氧化过程（P-AOPs）的内在机理。结果表明，所有 2D-CNMs 均能以 C ₃ N > C ₇₁ N > 石墨烯 > C ₂ N > CN 的顺序活化过二硫酸盐 (PDS)，而 C ₃ N 是过一硫酸盐 (PMS) 活化的唯一催化剂。C ₃具有最大石墨N的N可以在任何pH下在很宽的温度范围内激活PDS和PMS，并表现出最佳的CBZ氧化性能。值得注意的是，石墨N原子从五个方面促进P-AOPs：（i）电子结构，（ii）导电性，（iii）从过硫酸盐到催化剂的电子转移，（iv）活化前后共系统的电子跃迁， (v) 催化剂和过硫酸盐之间的相互作用。_{C 3} N最活跃的活性归因于最多数量的石墨 N。这项工作阐明了石墨 N 原子对催化剂设计的重要作用，并促进了 P-AOP 在微污染物减排中的环境应用。