In this study, Se@NC-x decorated with Se was successfully prepared via two-step calcination with zeolitic imidazole framework (ZIF) as a precursor. Mechanistic studies show that PMS would be adsorbed onto the surface of Se@NC-900 to form an active complex (Se@NC-900/PMS*), and the active Se@NC-900/PMS* could oxidize phenol by the rapid decomposition of PMS. Specifically, electrons are extracted by Se@NC-900/PMS* and then transferred to the surface of Se@NC-900, which can trigger the degradation of phenol. Notably, it is found that the local charge redistribution caused by the doping of Se can activate the catalytic potential of the intrinsically inert carbon skeleton through density flooding theory (DFT) calculations. The XLogP, ΔE, VIP, and E_{LUMO (Se@NC/PMS)-HOMO (pollutants)} and degradation rate constants of different micropollutants were correlated well linearly. This indicates that the Se@NC-900/PMS system has a great selectivity for the degradation of pollutants. Overall, these findings not only illustrate the role of Se in tuning the electronic structure of Se@NC-x to enhance the activation of PMS, but also bridge the gap in our knowledge about the physicochemical properties and degradation performance of Se@NC catalysts.

在这项研究中，以沸石咪唑骨架 (ZIF) 为前体，通过两步煅烧成功制备了 Se 修饰的 Se@NC-x。机理研究表明，PMS 会吸附到 Se@NC-900 表面形成活性复合物（Se@NC-900/PMS*），活性 Se@NC-900/PMS* 可以快速氧化苯酚PMS的分解。具体来说，电子被 Se@NC-900/PMS* 提取，然后转移到 Se@NC-900 的表面，从而引发苯酚的降解。值得注意的是，通过密度驱替理论 (DFT) 计算发现，由 Se 掺杂引起的局部电荷重新分布可以激活本征惰性碳骨架的催化潜力。XLogP、ΔE、VIP 和 E _{LUMO (Se@NC/PMS)-HOMO（污染物）}和不同微污染物的降解速率常数呈线性相关。这表明 Se@NC-900/PMS 系统对污染物的降解具有很好的选择性。总的来说，这些发现不仅说明了 Se 在调整 Se@NC-x 的电子结构以增强 PMS 活化方面的作用，而且弥合了我们对 Se@NC 催化剂的物理化学性质和降解性能的了解。