Multi-heteroatom-doping promotes molecular oxygen activation on polymeric carbon nitride for simultaneous generation of H2O2 and degradation of oxcarbazepine

Abstract

Simultaneously realizing the efficient generation of H₂O₂ and degradation of pollutants is of great significance for environmental remediation. However, most polymeric semiconductors only show moderate performance in molecular oxygen (O₂) activation due to the sluggish electron–hole pair dissociation and charge transfer dynamics. Herein, we develop a simple thermal shrinkage strategy to construct multi-heteroatom-doped polymeric carbon nitride (K, P, O-CN_x). The resultant K, P, O-CN_x not only improves the separation efficiency of charge carriers, but also improves the adsorption/activation capacity of O₂. K, P, O-CN_x significantly increases the production of H₂O₂ and the degradation activity of oxcarbazepine (OXC) under visible light. K, P, O-CN₅ shows a high H₂O₂ production rate (1858 μM h⁻¹ g⁻¹) in water under visible light, far surpassing that of pure PCN. The apparent rate constant for OXC degradation by K, P, O-CN₅ increases to 0.0491 min⁻¹, which is 8.47 times that of PCN. Density functional theory (DFT) calculations show that the adsorption energy of O₂ near phosphorus atoms in K, P, O-CN_x is the highest. This work provides a new idea for the efficient degradation of pollutants and generation of H₂O₂ at the same time.