Two-dimensional (2-D) exfoliated nanomaterials have attracted tremendous attentions because of the unique surface structures and increased reactive sites for various applications. Herein, a one-step pyrolysis method was used to fabricate ultrathin C₃N₄ photocatalysts, which had significant advantages over conventional post-exfoliation strategies with labor-intensive and time-consuming procedures. We found that oxygen doping by atmospheric air could effectively break the interlayer and intralayer interactions in polymeric C₃N₄, forming 2-D ultrathin nanocatalysts with high activity for persulfate activation. The integration of photocatalysis and persulfate oxidation resulted in 21- and 15-fold enhancement in the degradation of Bisphenol A pollutants compared to the individual reactions. The significant contributions of atmospheric oxygen doping to the charge separation and surface reactions were fundamentally investigated. This work not only provides a facile strategy to exfoliate polymeric semiconductor into ultrathin nanostructures, but also reveals valuable insight into the exploration of high-performance catalysts for the synergistic removal of environmental contaminants.

二维（2-D）剥落的纳米材料由于其独特的表面结构和增加的用于各种应用的反应位而备受关注。本文中，采用一步热解法制备超薄的C ₃ N ₄光催化剂，与传统的剥离后策略相比，该方法具有劳动强度大，耗时长的优点。我们发现大气中的氧掺杂可以有效地破坏聚合物C ₃ N _4中的层间和层内相互作用，形成了对过硫酸盐活化具有高活性的二维超薄纳米催化剂。与单独的反应相比，光催化和过硫酸盐氧化的整合导致双​​酚A污染物降解的增加21倍和15倍。从根本上研究了大气氧掺杂对电荷分离和表面反应的重大贡献。这项工作不仅提供了一种将聚合物半导体剥离为超薄纳米结构的简便策略，而且还揭示了对探索用于协同去除环境污染物的高性能催化剂的宝贵见解。